---
_id: '13989'
abstract:
- lang: eng
text: Characterizing and controlling entanglement in quantum materials is crucial
for the development of next-generation quantum technologies. However, defining
a quantifiable figure of merit for entanglement in macroscopic solids is theoretically
and experimentally challenging. At equilibrium the presence of entanglement can
be diagnosed by extracting entanglement witnesses from spectroscopic observables
and a nonequilibrium extension of this method could lead to the discovery of novel
dynamical phenomena. Here, we propose a systematic approach to quantify the time-dependent
quantum Fisher information and entanglement depth of transient states of quantum
materials with time-resolved resonant inelastic x-ray scattering. Using a quarter-filled
extended Hubbard model as an example, we benchmark the efficiency of this approach
and predict a light-enhanced many-body entanglement due to the proximity to a
phase boundary. Our work sets the stage for experimentally witnessing and controlling
entanglement in light-driven quantum materials via ultrafast spectroscopic measurements.
article_number: '3512'
article_processing_charge: No
article_type: original
arxiv: 1
author:
- first_name: Jordyn
full_name: Hales, Jordyn
last_name: Hales
- first_name: Utkarsh
full_name: Bajpai, Utkarsh
last_name: Bajpai
- first_name: Tongtong
full_name: Liu, Tongtong
last_name: Liu
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Mingda
full_name: Li, Mingda
last_name: Li
- first_name: Matteo
full_name: Mitrano, Matteo
last_name: Mitrano
- first_name: Yao
full_name: Wang, Yao
last_name: Wang
citation:
ama: Hales J, Bajpai U, Liu T, et al. Witnessing light-driven entanglement using
time-resolved resonant inelastic X-ray scattering. Nature Communications.
2023;14. doi:10.1038/s41467-023-38540-3
apa: Hales, J., Bajpai, U., Liu, T., Baykusheva, D. R., Li, M., Mitrano, M., &
Wang, Y. (2023). Witnessing light-driven entanglement using time-resolved resonant
inelastic X-ray scattering. Nature Communications. Springer Nature. https://doi.org/10.1038/s41467-023-38540-3
chicago: Hales, Jordyn, Utkarsh Bajpai, Tongtong Liu, Denitsa Rangelova Baykusheva,
Mingda Li, Matteo Mitrano, and Yao Wang. “Witnessing Light-Driven Entanglement
Using Time-Resolved Resonant Inelastic X-Ray Scattering.” Nature Communications.
Springer Nature, 2023. https://doi.org/10.1038/s41467-023-38540-3.
ieee: J. Hales et al., “Witnessing light-driven entanglement using time-resolved
resonant inelastic X-ray scattering,” Nature Communications, vol. 14. Springer
Nature, 2023.
ista: Hales J, Bajpai U, Liu T, Baykusheva DR, Li M, Mitrano M, Wang Y. 2023. Witnessing
light-driven entanglement using time-resolved resonant inelastic X-ray scattering.
Nature Communications. 14, 3512.
mla: Hales, Jordyn, et al. “Witnessing Light-Driven Entanglement Using Time-Resolved
Resonant Inelastic X-Ray Scattering.” Nature Communications, vol. 14, 3512,
Springer Nature, 2023, doi:10.1038/s41467-023-38540-3.
short: J. Hales, U. Bajpai, T. Liu, D.R. Baykusheva, M. Li, M. Mitrano, Y. Wang,
Nature Communications 14 (2023).
date_created: 2023-08-09T13:06:59Z
date_published: 2023-06-14T00:00:00Z
date_updated: 2023-08-22T06:50:04Z
day: '14'
doi: 10.1038/s41467-023-38540-3
extern: '1'
external_id:
arxiv:
- '2209.02283'
pmid:
- '37316515'
intvolume: ' 14'
keyword:
- General Physics and Astronomy
- General Biochemistry
- Genetics and Molecular Biology
- General Chemistry
- Multidisciplinary
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.1038/s41467-023-38540-3
month: '06'
oa: 1
oa_version: Published Version
pmid: 1
publication: Nature Communications
publication_identifier:
eissn:
- 2041-1723
publication_status: published
publisher: Springer Nature
quality_controlled: '1'
scopus_import: '1'
status: public
title: Witnessing light-driven entanglement using time-resolved resonant inelastic
X-ray scattering
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 14
year: '2023'
...
---
_id: '13990'
abstract:
- lang: eng
text: Many-body entanglement in condensed matter systems can be diagnosed from equilibrium
response functions through the use of entanglement witnesses and operator-specific
quantum bounds. Here, we investigate the applicability of this approach for detecting
entangled states in quantum systems driven out of equilibrium. We use a multipartite
entanglement witness, the quantum Fisher information, to study the dynamics of
a paradigmatic fermion chain undergoing a time-dependent change of the Coulomb
interaction. Our results show that the quantum Fisher information is able to witness
distinct signatures of multipartite entanglement both near and far from equilibrium
that are robust against decoherence. We discuss implications of these findings
for probing entanglement in light-driven quantum materials with time-resolved
optical and x-ray scattering methods.
article_number: '106902'
article_processing_charge: No
article_type: original
arxiv: 1
author:
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Mona H.
full_name: Kalthoff, Mona H.
last_name: Kalthoff
- first_name: Damian
full_name: Hofmann, Damian
last_name: Hofmann
- first_name: Martin
full_name: Claassen, Martin
last_name: Claassen
- first_name: Dante M.
full_name: Kennes, Dante M.
last_name: Kennes
- first_name: Michael A.
full_name: Sentef, Michael A.
last_name: Sentef
- first_name: Matteo
full_name: Mitrano, Matteo
last_name: Mitrano
citation:
ama: Baykusheva DR, Kalthoff MH, Hofmann D, et al. Witnessing nonequilibrium entanglement
dynamics in a strongly correlated fermionic chain. Physical Review Letters.
2023;130(10). doi:10.1103/physrevlett.130.106902
apa: Baykusheva, D. R., Kalthoff, M. H., Hofmann, D., Claassen, M., Kennes, D. M.,
Sentef, M. A., & Mitrano, M. (2023). Witnessing nonequilibrium entanglement
dynamics in a strongly correlated fermionic chain. Physical Review Letters.
American Physical Society. https://doi.org/10.1103/physrevlett.130.106902
chicago: Baykusheva, Denitsa Rangelova, Mona H. Kalthoff, Damian Hofmann, Martin
Claassen, Dante M. Kennes, Michael A. Sentef, and Matteo Mitrano. “Witnessing
Nonequilibrium Entanglement Dynamics in a Strongly Correlated Fermionic Chain.”
Physical Review Letters. American Physical Society, 2023. https://doi.org/10.1103/physrevlett.130.106902.
ieee: D. R. Baykusheva et al., “Witnessing nonequilibrium entanglement dynamics
in a strongly correlated fermionic chain,” Physical Review Letters, vol.
130, no. 10. American Physical Society, 2023.
ista: Baykusheva DR, Kalthoff MH, Hofmann D, Claassen M, Kennes DM, Sentef MA, Mitrano
M. 2023. Witnessing nonequilibrium entanglement dynamics in a strongly correlated
fermionic chain. Physical Review Letters. 130(10), 106902.
mla: Baykusheva, Denitsa Rangelova, et al. “Witnessing Nonequilibrium Entanglement
Dynamics in a Strongly Correlated Fermionic Chain.” Physical Review Letters,
vol. 130, no. 10, 106902, American Physical Society, 2023, doi:10.1103/physrevlett.130.106902.
short: D.R. Baykusheva, M.H. Kalthoff, D. Hofmann, M. Claassen, D.M. Kennes, M.A.
Sentef, M. Mitrano, Physical Review Letters 130 (2023).
date_created: 2023-08-09T13:07:24Z
date_published: 2023-03-10T00:00:00Z
date_updated: 2023-08-22T07:18:01Z
day: '10'
doi: 10.1103/physrevlett.130.106902
extern: '1'
external_id:
arxiv:
- '2209.02081'
pmid:
- '36962013'
intvolume: ' 130'
issue: '10'
keyword:
- General Physics and Astronomy
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://arxiv.org/abs/2209.02081
month: '03'
oa: 1
oa_version: Preprint
pmid: 1
publication: Physical Review Letters
publication_identifier:
eissn:
- 1079-7114
issn:
- 0031-9007
publication_status: published
publisher: American Physical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Witnessing nonequilibrium entanglement dynamics in a strongly correlated fermionic
chain
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 130
year: '2023'
...
---
_id: '13991'
abstract:
- lang: eng
text: The prediction and realization of topological insulators have sparked great
interest in experimental approaches to the classification of materials1,2,3. The
phase transition between non-trivial and trivial topological states is important,
not only for basic materials science but also for next-generation technology,
such as dissipation-free electronics4. It is therefore crucial to develop advanced
probes that are suitable for a wide range of samples and environments. Here we
demonstrate that circularly polarized laser-field-driven high-harmonic generation
is distinctly sensitive to the non-trivial and trivial topological phases in the
prototypical three-dimensional topological insulator bismuth selenide5. The phase
transition is chemically initiated by reducing the spin–orbit interaction strength
through the substitution of bismuth with indium atoms6,7. We find strikingly different
high-harmonic responses of trivial and non-trivial topological surface states
that manifest themselves as a conversion efficiency and elliptical dichroism that
depend both on the driving laser ellipticity and the crystal orientation. The
origins of the anomalous high-harmonic response are corroborated by calculations
using the semiconductor optical Bloch equations with pairs of surface and bulk
bands. As a purely optical approach, this method offers sensitivity to the electronic
structure of the material, including its nonlinear response, and is compatible
with a wide range of samples and sample environments.
article_processing_charge: No
article_type: original
author:
- first_name: Christian
full_name: Heide, Christian
last_name: Heide
- first_name: Yuki
full_name: Kobayashi, Yuki
last_name: Kobayashi
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Deepti
full_name: Jain, Deepti
last_name: Jain
- first_name: Jonathan A.
full_name: Sobota, Jonathan A.
last_name: Sobota
- first_name: Makoto
full_name: Hashimoto, Makoto
last_name: Hashimoto
- first_name: Patrick S.
full_name: Kirchmann, Patrick S.
last_name: Kirchmann
- first_name: Seongshik
full_name: Oh, Seongshik
last_name: Oh
- first_name: Tony F.
full_name: Heinz, Tony F.
last_name: Heinz
- first_name: David A.
full_name: Reis, David A.
last_name: Reis
- first_name: Shambhu
full_name: Ghimire, Shambhu
last_name: Ghimire
citation:
ama: Heide C, Kobayashi Y, Baykusheva DR, et al. Probing topological phase transitions
using high-harmonic generation. Nature Photonics. 2022;16(9):620-624. doi:10.1038/s41566-022-01050-7
apa: Heide, C., Kobayashi, Y., Baykusheva, D. R., Jain, D., Sobota, J. A., Hashimoto,
M., … Ghimire, S. (2022). Probing topological phase transitions using high-harmonic
generation. Nature Photonics. Springer Nature. https://doi.org/10.1038/s41566-022-01050-7
chicago: Heide, Christian, Yuki Kobayashi, Denitsa Rangelova Baykusheva, Deepti
Jain, Jonathan A. Sobota, Makoto Hashimoto, Patrick S. Kirchmann, et al. “Probing
Topological Phase Transitions Using High-Harmonic Generation.” Nature Photonics.
Springer Nature, 2022. https://doi.org/10.1038/s41566-022-01050-7.
ieee: C. Heide et al., “Probing topological phase transitions using high-harmonic
generation,” Nature Photonics, vol. 16, no. 9. Springer Nature, pp. 620–624,
2022.
ista: Heide C, Kobayashi Y, Baykusheva DR, Jain D, Sobota JA, Hashimoto M, Kirchmann
PS, Oh S, Heinz TF, Reis DA, Ghimire S. 2022. Probing topological phase transitions
using high-harmonic generation. Nature Photonics. 16(9), 620–624.
mla: Heide, Christian, et al. “Probing Topological Phase Transitions Using High-Harmonic
Generation.” Nature Photonics, vol. 16, no. 9, Springer Nature, 2022, pp.
620–24, doi:10.1038/s41566-022-01050-7.
short: C. Heide, Y. Kobayashi, D.R. Baykusheva, D. Jain, J.A. Sobota, M. Hashimoto,
P.S. Kirchmann, S. Oh, T.F. Heinz, D.A. Reis, S. Ghimire, Nature Photonics 16
(2022) 620–624.
date_created: 2023-08-09T13:07:51Z
date_published: 2022-09-01T00:00:00Z
date_updated: 2023-08-22T07:20:09Z
day: '01'
doi: 10.1038/s41566-022-01050-7
extern: '1'
intvolume: ' 16'
issue: '9'
keyword:
- Atomic and Molecular Physics
- and Optics
- Electronic
- Optical and Magnetic Materials
language:
- iso: eng
month: '09'
oa_version: None
page: 620-624
publication: Nature Photonics
publication_identifier:
eissn:
- 1749-4893
issn:
- 1749-4885
publication_status: published
publisher: Springer Nature
quality_controlled: '1'
scopus_import: '1'
status: public
title: Probing topological phase transitions using high-harmonic generation
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 16
year: '2022'
...
---
_id: '13992'
abstract:
- lang: eng
text: Understanding the chirality of molecular reaction pathways is essential for
a broad range of fundamental and applied sciences. However, the current ability
to probe chirality on the time scale of primary processes underlying chemical
reactions remains very limited. Here, we demonstrate time-resolved photoelectron
circular dichroism (TRPECD) with ultrashort circularly polarized vacuum-ultraviolet
(VUV) pulses from a tabletop source. We demonstrate the capabilities of VUV-TRPECD
by resolving the chirality changes in time during the photodissociation of atomic
iodine from two chiral molecules. We identify several general key features of
TRPECD, which include the ability to probe dynamical chirality along the complete
photochemical reaction path, the sensitivity to the local chirality of the evolving
scattering potential, and the influence of electron scattering off dissociating
photofragments. Our results are interpreted by comparison with high-level ab-initio
calculations of transient PECDs from molecular photoionization calculations. Our
experimental and theoretical techniques define a general approach to femtochirality.
article_number: abq2811
article_processing_charge: No
article_type: original
arxiv: 1
author:
- first_name: Vít
full_name: Svoboda, Vít
last_name: Svoboda
- first_name: Niraghatam Bhargava
full_name: Ram, Niraghatam Bhargava
last_name: Ram
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Daniel
full_name: Zindel, Daniel
last_name: Zindel
- first_name: Max D. J.
full_name: Waters, Max D. J.
last_name: Waters
- first_name: Benjamin
full_name: Spenger, Benjamin
last_name: Spenger
- first_name: Manuel
full_name: Ochsner, Manuel
last_name: Ochsner
- first_name: Holger
full_name: Herburger, Holger
last_name: Herburger
- first_name: Jürgen
full_name: Stohner, Jürgen
last_name: Stohner
- first_name: Hans Jakob
full_name: Wörner, Hans Jakob
last_name: Wörner
citation:
ama: Svoboda V, Ram NB, Baykusheva DR, et al. Femtosecond photoelectron circular
dichroism of chemical reactions. Science Advances. 2022;8(28). doi:10.1126/sciadv.abq2811
apa: Svoboda, V., Ram, N. B., Baykusheva, D. R., Zindel, D., Waters, M. D. J., Spenger,
B., … Wörner, H. J. (2022). Femtosecond photoelectron circular dichroism of chemical
reactions. Science Advances. American Association for the Advancement of
Science. https://doi.org/10.1126/sciadv.abq2811
chicago: Svoboda, Vít, Niraghatam Bhargava Ram, Denitsa Rangelova Baykusheva, Daniel
Zindel, Max D. J. Waters, Benjamin Spenger, Manuel Ochsner, Holger Herburger,
Jürgen Stohner, and Hans Jakob Wörner. “Femtosecond Photoelectron Circular Dichroism
of Chemical Reactions.” Science Advances. American Association for the
Advancement of Science, 2022. https://doi.org/10.1126/sciadv.abq2811.
ieee: V. Svoboda et al., “Femtosecond photoelectron circular dichroism of
chemical reactions,” Science Advances, vol. 8, no. 28. American Association
for the Advancement of Science, 2022.
ista: Svoboda V, Ram NB, Baykusheva DR, Zindel D, Waters MDJ, Spenger B, Ochsner
M, Herburger H, Stohner J, Wörner HJ. 2022. Femtosecond photoelectron circular
dichroism of chemical reactions. Science Advances. 8(28), abq2811.
mla: Svoboda, Vít, et al. “Femtosecond Photoelectron Circular Dichroism of Chemical
Reactions.” Science Advances, vol. 8, no. 28, abq2811, American Association
for the Advancement of Science, 2022, doi:10.1126/sciadv.abq2811.
short: V. Svoboda, N.B. Ram, D.R. Baykusheva, D. Zindel, M.D.J. Waters, B. Spenger,
M. Ochsner, H. Herburger, J. Stohner, H.J. Wörner, Science Advances 8 (2022).
date_created: 2023-08-09T13:08:04Z
date_published: 2022-07-15T00:00:00Z
date_updated: 2023-08-22T07:24:01Z
day: '15'
doi: 10.1126/sciadv.abq2811
extern: '1'
external_id:
arxiv:
- '2206.04099'
pmid:
- '35857523'
intvolume: ' 8'
issue: '28'
keyword:
- Multidisciplinary
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.1126/sciadv.abq2811
month: '07'
oa: 1
oa_version: Published Version
pmid: 1
publication: Science Advances
publication_identifier:
eissn:
- 2375-2548
publication_status: published
publisher: American Association for the Advancement of Science
quality_controlled: '1'
scopus_import: '1'
status: public
title: Femtosecond photoelectron circular dichroism of chemical reactions
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 8
year: '2022'
...
---
_id: '13993'
abstract:
- lang: eng
text: Photoionization is a process taking place on attosecond time scales. How its
properties evolve from isolated particles to the condensed phase is an open question
of both fundamental and practical relevance. Here, we review recent work that
has advanced the study of photoionization dynamics from atoms to molecules, clusters
and the liquid phase. The first measurements of molecular photoionization delays
have revealed the attosecond dynamics of electron emission from a molecular shape
resonance and their sensitivity to the molecular potential. Using electron-ion
coincidence spectroscopy these measurements have been extended from isolated molecules
to clusters. A continuous increase of the delays with the water-cluster size has
been observed up to a size of 4-5 molecules, followed by a saturation towards
larger clusters. Comparison with calculations has revealed a correlation of the
time delay with the spatial extension of the created electron hole. Using cylindrical
liquid-microjet techniques, these measurements have also been extended to liquid
water, revealing a delay relative to isolated water molecules that was very similar
to the largest water clusters studied. Detailed modeling based on Monte-Carlo
simulations confirmed that these delays are dominated by the contributions of
the first two solvation shells, which agrees with the results of the cluster measurements.
These combined results open the perspective of experimentally characterizing the
delocalization of electronic wave functions in complex systems and studying their
evolution on attosecond time scales.
article_processing_charge: No
article_type: original
author:
- first_name: Xiaochun
full_name: Gong, Xiaochun
last_name: Gong
- first_name: Inga
full_name: Jordan, Inga
last_name: Jordan
- first_name: Martin
full_name: Huppert, Martin
last_name: Huppert
- first_name: Saijoscha
full_name: Heck, Saijoscha
last_name: Heck
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Denis
full_name: Jelovina, Denis
last_name: Jelovina
- first_name: Axel
full_name: Schild, Axel
last_name: Schild
- first_name: Hans Jakob
full_name: Wörner, Hans Jakob
last_name: Wörner
citation:
ama: 'Gong X, Jordan I, Huppert M, et al. Attosecond photoionization dynamics: from
molecules over clusters to the liquid phase. Chimia. 2022;76(6):520-528.
doi:10.2533/chimia.2022.520'
apa: 'Gong, X., Jordan, I., Huppert, M., Heck, S., Baykusheva, D. R., Jelovina,
D., … Wörner, H. J. (2022). Attosecond photoionization dynamics: from molecules
over clusters to the liquid phase. Chimia. Swiss Chemical Society. https://doi.org/10.2533/chimia.2022.520'
chicago: 'Gong, Xiaochun, Inga Jordan, Martin Huppert, Saijoscha Heck, Denitsa Rangelova
Baykusheva, Denis Jelovina, Axel Schild, and Hans Jakob Wörner. “Attosecond Photoionization
Dynamics: From Molecules over Clusters to the Liquid Phase.” Chimia. Swiss
Chemical Society, 2022. https://doi.org/10.2533/chimia.2022.520.'
ieee: 'X. Gong et al., “Attosecond photoionization dynamics: from molecules
over clusters to the liquid phase,” Chimia, vol. 76, no. 6. Swiss Chemical
Society, pp. 520–528, 2022.'
ista: 'Gong X, Jordan I, Huppert M, Heck S, Baykusheva DR, Jelovina D, Schild A,
Wörner HJ. 2022. Attosecond photoionization dynamics: from molecules over clusters
to the liquid phase. Chimia. 76(6), 520–528.'
mla: 'Gong, Xiaochun, et al. “Attosecond Photoionization Dynamics: From Molecules
over Clusters to the Liquid Phase.” Chimia, vol. 76, no. 6, Swiss Chemical
Society, 2022, pp. 520–28, doi:10.2533/chimia.2022.520.'
short: X. Gong, I. Jordan, M. Huppert, S. Heck, D.R. Baykusheva, D. Jelovina, A.
Schild, H.J. Wörner, Chimia 76 (2022) 520–528.
date_created: 2023-08-09T13:08:15Z
date_published: 2022-06-29T00:00:00Z
date_updated: 2023-08-22T07:26:39Z
day: '29'
doi: 10.2533/chimia.2022.520
extern: '1'
intvolume: ' 76'
issue: '6'
keyword:
- General Medicine
- General Chemistry
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.2533/chimia.2022.520
month: '06'
oa: 1
oa_version: Published Version
page: 520-528
publication: Chimia
publication_identifier:
eissn:
- 2673-2424
issn:
- 0009-4293
publication_status: published
publisher: Swiss Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: 'Attosecond photoionization dynamics: from molecules over clusters to the liquid
phase'
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 76
year: '2022'
...
---
_id: '13994'
abstract:
- lang: eng
text: "Ultrafast lasers are an increasingly important tool to control and stabilize
emergent phases in quantum materials. Among a variety of possible excitation protocols,
a particularly intriguing route is the direct light engineering of microscopic
electronic parameters, such as the electron hopping and the local Coulomb repulsion
(Hubbard \r\nU). In this work, we use time-resolved x-ray absorption spectroscopy
to demonstrate the light-induced renormalization of the Hubbard U in a cuprate
superconductor, La1.905Ba0.095CuO4. We show that intense femtosecond laser pulses
induce a substantial redshift of the upper Hubbard band while leaving the Zhang-Rice
singlet energy unaffected. By comparing the experimental data to time-dependent
spectra of single- and three-band Hubbard models, we assign this effect to an
approximately 140-meV reduction of the on-site Coulomb repulsion on the copper
sites. Our demonstration of a dynamical Hubbard U renormalization in a copper
oxide paves the way to a novel strategy for the manipulation of superconductivity
and magnetism as well as to the realization of other long-range-ordered phases
in light-driven quantum materials."
article_number: '011013'
article_processing_charge: No
article_type: original
arxiv: 1
author:
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Hoyoung
full_name: Jang, Hoyoung
last_name: Jang
- first_name: Ali A.
full_name: Husain, Ali A.
last_name: Husain
- first_name: Sangjun
full_name: Lee, Sangjun
last_name: Lee
- first_name: Sophia F. R.
full_name: TenHuisen, Sophia F. R.
last_name: TenHuisen
- first_name: Preston
full_name: Zhou, Preston
last_name: Zhou
- first_name: Sunwook
full_name: Park, Sunwook
last_name: Park
- first_name: Hoon
full_name: Kim, Hoon
last_name: Kim
- first_name: Jin-Kwang
full_name: Kim, Jin-Kwang
last_name: Kim
- first_name: Hyeong-Do
full_name: Kim, Hyeong-Do
last_name: Kim
- first_name: Minseok
full_name: Kim, Minseok
last_name: Kim
- first_name: Sang-Youn
full_name: Park, Sang-Youn
last_name: Park
- first_name: Peter
full_name: Abbamonte, Peter
last_name: Abbamonte
- first_name: B. J.
full_name: Kim, B. J.
last_name: Kim
- first_name: G. D.
full_name: Gu, G. D.
last_name: Gu
- first_name: Yao
full_name: Wang, Yao
last_name: Wang
- first_name: Matteo
full_name: Mitrano, Matteo
last_name: Mitrano
citation:
ama: Baykusheva DR, Jang H, Husain AA, et al. Ultrafast renormalization of the on-site
Coulomb repulsion in a cuprate superconductor. Physical Review X. 2022;12(1).
doi:10.1103/physrevx.12.011013
apa: Baykusheva, D. R., Jang, H., Husain, A. A., Lee, S., TenHuisen, S. F. R., Zhou,
P., … Mitrano, M. (2022). Ultrafast renormalization of the on-site Coulomb repulsion
in a cuprate superconductor. Physical Review X. American Physical Society.
https://doi.org/10.1103/physrevx.12.011013
chicago: Baykusheva, Denitsa Rangelova, Hoyoung Jang, Ali A. Husain, Sangjun Lee,
Sophia F. R. TenHuisen, Preston Zhou, Sunwook Park, et al. “Ultrafast Renormalization
of the On-Site Coulomb Repulsion in a Cuprate Superconductor.” Physical Review
X. American Physical Society, 2022. https://doi.org/10.1103/physrevx.12.011013.
ieee: D. R. Baykusheva et al., “Ultrafast renormalization of the on-site
Coulomb repulsion in a cuprate superconductor,” Physical Review X, vol.
12, no. 1. American Physical Society, 2022.
ista: Baykusheva DR, Jang H, Husain AA, Lee S, TenHuisen SFR, Zhou P, Park S, Kim
H, Kim J-K, Kim H-D, Kim M, Park S-Y, Abbamonte P, Kim BJ, Gu GD, Wang Y, Mitrano
M. 2022. Ultrafast renormalization of the on-site Coulomb repulsion in a cuprate
superconductor. Physical Review X. 12(1), 011013.
mla: Baykusheva, Denitsa Rangelova, et al. “Ultrafast Renormalization of the On-Site
Coulomb Repulsion in a Cuprate Superconductor.” Physical Review X, vol.
12, no. 1, 011013, American Physical Society, 2022, doi:10.1103/physrevx.12.011013.
short: D.R. Baykusheva, H. Jang, A.A. Husain, S. Lee, S.F.R. TenHuisen, P. Zhou,
S. Park, H. Kim, J.-K. Kim, H.-D. Kim, M. Kim, S.-Y. Park, P. Abbamonte, B.J.
Kim, G.D. Gu, Y. Wang, M. Mitrano, Physical Review X 12 (2022).
date_created: 2023-08-09T13:08:26Z
date_published: 2022-01-20T00:00:00Z
date_updated: 2023-08-22T07:28:38Z
day: '20'
doi: 10.1103/physrevx.12.011013
extern: '1'
external_id:
arxiv:
- '2109.13229'
intvolume: ' 12'
issue: '1'
keyword:
- General Physics and Astronomy
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.1103/PhysRevX.12.011013
month: '01'
oa: 1
oa_version: Published Version
publication: Physical Review X
publication_identifier:
eissn:
- 2160-3308
publication_status: published
publisher: American Physical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Ultrafast renormalization of the on-site Coulomb repulsion in a cuprate superconductor
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 12
year: '2022'
...
---
_id: '13995'
abstract:
- lang: eng
text: Shape resonances play a central role in many areas of science, but the real-time
measurement of the associated many-body dynamics remains challenging. Here, we
present measurements of recoil frame angle-resolved photoionization delays in
the vicinity of shape resonances of CF4. This technique provides insights into
the spatiotemporal photoionization dynamics of molecular shape resonances. We
find delays of up to ∼600 as in the ionization out of the highest occupied molecular
orbital (HOMO) with a strong dependence on the emission direction and a pronounced
asymmetry along the dissociation axis. Comparison with quantum-scattering calculations
traces the asymmetries to the interference of a small subset of partial waves
at low kinetic energies and, additionally, to the interference of two overlapping
shape resonances in the HOMO-1 channel. Our experimental and theoretical results
establish a broadly applicable approach to space- and time-resolved photoionization
dynamics in the molecular frame.
article_number: abj8121
article_processing_charge: No
article_type: original
author:
- first_name: Saijoscha
full_name: Heck, Saijoscha
last_name: Heck
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Meng
full_name: Han, Meng
last_name: Han
- first_name: Jia-Bao
full_name: Ji, Jia-Bao
last_name: Ji
- first_name: Conaill
full_name: Perry, Conaill
last_name: Perry
- first_name: Xiaochun
full_name: Gong, Xiaochun
last_name: Gong
- first_name: Hans Jakob
full_name: Wörner, Hans Jakob
last_name: Wörner
citation:
ama: Heck S, Baykusheva DR, Han M, et al. Attosecond interferometry of shape resonances
in the recoil frame of CF4. Science Advances. 2021;7(49). doi:10.1126/sciadv.abj8121
apa: Heck, S., Baykusheva, D. R., Han, M., Ji, J.-B., Perry, C., Gong, X., &
Wörner, H. J. (2021). Attosecond interferometry of shape resonances in the recoil
frame of CF4. Science Advances. American Association for the Advancement
of Science. https://doi.org/10.1126/sciadv.abj8121
chicago: Heck, Saijoscha, Denitsa Rangelova Baykusheva, Meng Han, Jia-Bao Ji, Conaill
Perry, Xiaochun Gong, and Hans Jakob Wörner. “Attosecond Interferometry of Shape
Resonances in the Recoil Frame of CF4.” Science Advances. American Association
for the Advancement of Science, 2021. https://doi.org/10.1126/sciadv.abj8121.
ieee: S. Heck et al., “Attosecond interferometry of shape resonances in the
recoil frame of CF4,” Science Advances, vol. 7, no. 49. American Association
for the Advancement of Science, 2021.
ista: Heck S, Baykusheva DR, Han M, Ji J-B, Perry C, Gong X, Wörner HJ. 2021. Attosecond
interferometry of shape resonances in the recoil frame of CF4. Science Advances.
7(49), abj8121.
mla: Heck, Saijoscha, et al. “Attosecond Interferometry of Shape Resonances in the
Recoil Frame of CF4.” Science Advances, vol. 7, no. 49, abj8121, American
Association for the Advancement of Science, 2021, doi:10.1126/sciadv.abj8121.
short: S. Heck, D.R. Baykusheva, M. Han, J.-B. Ji, C. Perry, X. Gong, H.J. Wörner,
Science Advances 7 (2021).
date_created: 2023-08-09T13:09:02Z
date_published: 2021-12-03T00:00:00Z
date_updated: 2023-08-22T07:30:25Z
day: '03'
doi: 10.1126/sciadv.abj8121
extern: '1'
external_id:
pmid:
- '34860540'
intvolume: ' 7'
issue: '49'
keyword:
- Multidisciplinary
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.1126/sciadv.abj8121
month: '12'
oa: 1
oa_version: Published Version
pmid: 1
publication: Science Advances
publication_identifier:
eissn:
- 2375-2548
publication_status: published
publisher: American Association for the Advancement of Science
quality_controlled: '1'
scopus_import: '1'
status: public
title: Attosecond interferometry of shape resonances in the recoil frame of CF4
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 7
year: '2021'
...
---
_id: '13996'
abstract:
- lang: eng
text: We report the observation of an anomalous nonlinear optical response of the
prototypical three-dimensional topological insulator bismuth selenide through
the process of high-order harmonic generation. We find that the generation efficiency
increases as the laser polarization is changed from linear to elliptical, and
it becomes maximum for circular polarization. With the aid of a microscopic theory
and a detailed analysis of the measured spectra, we reveal that such anomalous
enhancement encodes the characteristic topology of the band structure that originates
from the interplay of strong spin–orbit coupling and time-reversal symmetry protection.
The implications are in ultrafast probing of topological phase transitions, light-field
driven dissipationless electronics, and quantum computation.
article_processing_charge: No
article_type: original
arxiv: 1
author:
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Alexis
full_name: Chacón, Alexis
last_name: Chacón
- first_name: Jian
full_name: Lu, Jian
last_name: Lu
- first_name: Trevor P.
full_name: Bailey, Trevor P.
last_name: Bailey
- first_name: Jonathan A.
full_name: Sobota, Jonathan A.
last_name: Sobota
- first_name: Hadas
full_name: Soifer, Hadas
last_name: Soifer
- first_name: Patrick S.
full_name: Kirchmann, Patrick S.
last_name: Kirchmann
- first_name: Costel
full_name: Rotundu, Costel
last_name: Rotundu
- first_name: Ctirad
full_name: Uher, Ctirad
last_name: Uher
- first_name: Tony F.
full_name: Heinz, Tony F.
last_name: Heinz
- first_name: David A.
full_name: Reis, David A.
last_name: Reis
- first_name: Shambhu
full_name: Ghimire, Shambhu
last_name: Ghimire
citation:
ama: Baykusheva DR, Chacón A, Lu J, et al. All-optical probe of three-dimensional
topological insulators based on high-harmonic generation by circularly polarized
laser fields. Nano Letters. 2021;21(21):8970-8978. doi:10.1021/acs.nanolett.1c02145
apa: Baykusheva, D. R., Chacón, A., Lu, J., Bailey, T. P., Sobota, J. A., Soifer,
H., … Ghimire, S. (2021). All-optical probe of three-dimensional topological insulators
based on high-harmonic generation by circularly polarized laser fields. Nano
Letters. American Chemical Society. https://doi.org/10.1021/acs.nanolett.1c02145
chicago: Baykusheva, Denitsa Rangelova, Alexis Chacón, Jian Lu, Trevor P. Bailey,
Jonathan A. Sobota, Hadas Soifer, Patrick S. Kirchmann, et al. “All-Optical Probe
of Three-Dimensional Topological Insulators Based on High-Harmonic Generation
by Circularly Polarized Laser Fields.” Nano Letters. American Chemical
Society, 2021. https://doi.org/10.1021/acs.nanolett.1c02145.
ieee: D. R. Baykusheva et al., “All-optical probe of three-dimensional topological
insulators based on high-harmonic generation by circularly polarized laser fields,”
Nano Letters, vol. 21, no. 21. American Chemical Society, pp. 8970–8978,
2021.
ista: Baykusheva DR, Chacón A, Lu J, Bailey TP, Sobota JA, Soifer H, Kirchmann PS,
Rotundu C, Uher C, Heinz TF, Reis DA, Ghimire S. 2021. All-optical probe of three-dimensional
topological insulators based on high-harmonic generation by circularly polarized
laser fields. Nano Letters. 21(21), 8970–8978.
mla: Baykusheva, Denitsa Rangelova, et al. “All-Optical Probe of Three-Dimensional
Topological Insulators Based on High-Harmonic Generation by Circularly Polarized
Laser Fields.” Nano Letters, vol. 21, no. 21, American Chemical Society,
2021, pp. 8970–78, doi:10.1021/acs.nanolett.1c02145.
short: D.R. Baykusheva, A. Chacón, J. Lu, T.P. Bailey, J.A. Sobota, H. Soifer, P.S.
Kirchmann, C. Rotundu, C. Uher, T.F. Heinz, D.A. Reis, S. Ghimire, Nano Letters
21 (2021) 8970–8978.
date_created: 2023-08-09T13:09:15Z
date_published: 2021-10-22T00:00:00Z
date_updated: 2023-08-22T07:32:00Z
day: '22'
doi: 10.1021/acs.nanolett.1c02145
extern: '1'
external_id:
arxiv:
- '2109.15291'
pmid:
- '34676752'
intvolume: ' 21'
issue: '21'
keyword:
- Mechanical Engineering
- Condensed Matter Physics
- General Materials Science
- General Chemistry
- Bioengineering
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.1021/acs.nanolett.1c02145
month: '10'
oa: 1
oa_version: Published Version
page: 8970-8978
pmid: 1
publication: Nano Letters
publication_identifier:
eissn:
- 1530-6992
issn:
- 1530-6984
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: All-optical probe of three-dimensional topological insulators based on high-harmonic
generation by circularly polarized laser fields
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 21
year: '2021'
...
---
_id: '13997'
abstract:
- lang: eng
text: We investigate theoretically the strong-field regime of light-matter interactions
in the topological-insulator class of quantum materials. In particular, we focus
on the process of nonperturbative high-order harmonic generation from the paradigmatic
three-dimensional topological insulator bismuth selenide (Bi2Se3) subjected to
intense midinfrared laser fields. We analyze the contributions from the spin-orbit-coupled
bulk states and the topological surface bands separately and reveal a major difference
in how their harmonic yields depend on the ellipticity of the laser field. Bulk
harmonics show a monotonic decrease in their yield as the ellipticity increases,
in a manner reminiscent of high harmonic generation in gaseous media. However,
the surface contribution exhibits a highly nontrivial dependence, culminating
with a maximum for circularly polarized fields. We attribute the observed anomalous
behavior to (i) the enhanced amplitude and the circular pattern of the interband
dipole and the Berry connections in the vicinity of the Dirac point and (ii) the
influence of the higher-order, hexagonal warping terms in the Hamiltonian, which
are responsible for the hexagonal deformation of the energy surface at higher
momenta. The latter are associated directly with spin-orbit-coupling parameters.
Our results thus establish the sensitivity of strong-field-driven high harmonic
emission to the topology of the band structure as well as to the manifestations
of spin-orbit interaction.
article_number: '023101'
article_processing_charge: No
article_type: original
arxiv: 1
author:
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Alexis
full_name: Chacón, Alexis
last_name: Chacón
- first_name: Dasol
full_name: Kim, Dasol
last_name: Kim
- first_name: Dong Eon
full_name: Kim, Dong Eon
last_name: Kim
- first_name: David A.
full_name: Reis, David A.
last_name: Reis
- first_name: Shambhu
full_name: Ghimire, Shambhu
last_name: Ghimire
citation:
ama: Baykusheva DR, Chacón A, Kim D, Kim DE, Reis DA, Ghimire S. Strong-field physics
in three-dimensional topological insulators. Physical Review A. 2021;103(2).
doi:10.1103/physreva.103.023101
apa: Baykusheva, D. R., Chacón, A., Kim, D., Kim, D. E., Reis, D. A., & Ghimire,
S. (2021). Strong-field physics in three-dimensional topological insulators. Physical
Review A. American Physical Society. https://doi.org/10.1103/physreva.103.023101
chicago: Baykusheva, Denitsa Rangelova, Alexis Chacón, Dasol Kim, Dong Eon Kim,
David A. Reis, and Shambhu Ghimire. “Strong-Field Physics in Three-Dimensional
Topological Insulators.” Physical Review A. American Physical Society,
2021. https://doi.org/10.1103/physreva.103.023101.
ieee: D. R. Baykusheva, A. Chacón, D. Kim, D. E. Kim, D. A. Reis, and S. Ghimire,
“Strong-field physics in three-dimensional topological insulators,” Physical
Review A, vol. 103, no. 2. American Physical Society, 2021.
ista: Baykusheva DR, Chacón A, Kim D, Kim DE, Reis DA, Ghimire S. 2021. Strong-field
physics in three-dimensional topological insulators. Physical Review A. 103(2),
023101.
mla: Baykusheva, Denitsa Rangelova, et al. “Strong-Field Physics in Three-Dimensional
Topological Insulators.” Physical Review A, vol. 103, no. 2, 023101, American
Physical Society, 2021, doi:10.1103/physreva.103.023101.
short: D.R. Baykusheva, A. Chacón, D. Kim, D.E. Kim, D.A. Reis, S. Ghimire, Physical
Review A 103 (2021).
date_created: 2023-08-09T13:09:26Z
date_published: 2021-02-01T00:00:00Z
date_updated: 2023-08-22T07:33:43Z
day: '01'
doi: 10.1103/physreva.103.023101
extern: '1'
external_id:
arxiv:
- '2008.01265'
intvolume: ' 103'
issue: '2'
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://arxiv.org/abs/2008.01265
month: '02'
oa: 1
oa_version: Preprint
publication: Physical Review A
publication_identifier:
eissn:
- 2469-9934
issn:
- 2469-9926
publication_status: published
publisher: American Physical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Strong-field physics in three-dimensional topological insulators
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 103
year: '2021'
...
---
_id: '13998'
abstract:
- lang: eng
text: The interaction of strong near-infrared (NIR) laser pulses with wide-bandgap
dielectrics produces high harmonics in the extreme ultraviolet (XUV) wavelength
range. These observations have opened up the possibility of attosecond metrology
in solids, which would benefit from a precise measurement of the emission times
of individual harmonics with respect to the NIR laser field. Here we show that,
when high-harmonics are detected from the input surface of a magnesium oxide crystal,
a bichromatic probing of the XUV emission shows a clear synchronization largely
consistent with a semiclassical model of electron–hole recollisions in bulk solids.
On the other hand, the bichromatic spectrogram of harmonics originating from the
exit surface of the 200 μm-thick crystal is strongly modified, indicating the
influence of laser field distortions during propagation. Our tracking of sub-cycle
electron and hole re-collisions at XUV energies is relevant to the development
of solid-state sources of attosecond pulses.
article_number: '144003'
article_processing_charge: No
article_type: original
arxiv: 1
author:
- first_name: Giulio
full_name: Vampa, Giulio
last_name: Vampa
- first_name: Jian
full_name: Lu, Jian
last_name: Lu
- first_name: Yong Sing
full_name: You, Yong Sing
last_name: You
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Mengxi
full_name: Wu, Mengxi
last_name: Wu
- first_name: Hanzhe
full_name: Liu, Hanzhe
last_name: Liu
- first_name: Kenneth J
full_name: Schafer, Kenneth J
last_name: Schafer
- first_name: Mette B
full_name: Gaarde, Mette B
last_name: Gaarde
- first_name: David A
full_name: Reis, David A
last_name: Reis
- first_name: Shambhu
full_name: Ghimire, Shambhu
last_name: Ghimire
citation:
ama: 'Vampa G, Lu J, You YS, et al. Attosecond synchronization of extreme ultraviolet
high harmonics from crystals. Journal of Physics B: Atomic, Molecular and Optical
Physics. 2020;53(14). doi:10.1088/1361-6455/ab8e56'
apa: 'Vampa, G., Lu, J., You, Y. S., Baykusheva, D. R., Wu, M., Liu, H., … Ghimire,
S. (2020). Attosecond synchronization of extreme ultraviolet high harmonics from
crystals. Journal of Physics B: Atomic, Molecular and Optical Physics.
IOP Publishing. https://doi.org/10.1088/1361-6455/ab8e56'
chicago: 'Vampa, Giulio, Jian Lu, Yong Sing You, Denitsa Rangelova Baykusheva, Mengxi
Wu, Hanzhe Liu, Kenneth J Schafer, Mette B Gaarde, David A Reis, and Shambhu Ghimire.
“Attosecond Synchronization of Extreme Ultraviolet High Harmonics from Crystals.”
Journal of Physics B: Atomic, Molecular and Optical Physics. IOP Publishing,
2020. https://doi.org/10.1088/1361-6455/ab8e56.'
ieee: 'G. Vampa et al., “Attosecond synchronization of extreme ultraviolet
high harmonics from crystals,” Journal of Physics B: Atomic, Molecular and
Optical Physics, vol. 53, no. 14. IOP Publishing, 2020.'
ista: 'Vampa G, Lu J, You YS, Baykusheva DR, Wu M, Liu H, Schafer KJ, Gaarde MB,
Reis DA, Ghimire S. 2020. Attosecond synchronization of extreme ultraviolet high
harmonics from crystals. Journal of Physics B: Atomic, Molecular and Optical Physics.
53(14), 144003.'
mla: 'Vampa, Giulio, et al. “Attosecond Synchronization of Extreme Ultraviolet High
Harmonics from Crystals.” Journal of Physics B: Atomic, Molecular and Optical
Physics, vol. 53, no. 14, 144003, IOP Publishing, 2020, doi:10.1088/1361-6455/ab8e56.'
short: 'G. Vampa, J. Lu, Y.S. You, D.R. Baykusheva, M. Wu, H. Liu, K.J. Schafer,
M.B. Gaarde, D.A. Reis, S. Ghimire, Journal of Physics B: Atomic, Molecular and
Optical Physics 53 (2020).'
date_created: 2023-08-09T13:09:51Z
date_published: 2020-06-17T00:00:00Z
date_updated: 2023-08-22T07:36:36Z
day: '17'
doi: 10.1088/1361-6455/ab8e56
extern: '1'
external_id:
arxiv:
- '2001.09951'
intvolume: ' 53'
issue: '14'
keyword:
- Condensed Matter Physics
- Atomic and Molecular Physics
- and Optics
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://arxiv.org/abs/2001.09951
month: '06'
oa: 1
oa_version: Preprint
publication: 'Journal of Physics B: Atomic, Molecular and Optical Physics'
publication_identifier:
eissn:
- 1361-6455
issn:
- 0953-4075
publication_status: published
publisher: IOP Publishing
quality_controlled: '1'
scopus_import: '1'
status: public
title: Attosecond synchronization of extreme ultraviolet high harmonics from crystals
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 53
year: '2020'
...
---
_id: '13999'
abstract:
- lang: eng
text: Attosecond chronoscopy has revealed small but measurable delays in photoionization,
characterized by the ejection of an electron on absorption of a single photon.
Ionization-delay measurements in atomic targets provide a wealth of information
about the timing of the photoelectric effect, resonances, electron correlations
and transport. However, extending this approach to molecules presents challenges,
such as identifying the correct ionization channels and the effect of the anisotropic
molecular landscape on the measured delays. Here, we measure ionization delays
from ethyl iodide around a giant dipole resonance. By using the theoretical value
for the iodine atom as a reference, we disentangle the contribution from the functional
ethyl group, which is responsible for the characteristic chemical reactivity of
a molecule. We find a substantial additional delay caused by the presence of a
functional group, which encodes the effect of the molecular potential on the departing
electron. Such information is inaccessible to the conventional approach of measuring
photoionization cross-sections. The results establish ionization-delay measurements
as a valuable tool in investigating the electronic properties of molecules.
article_processing_charge: No
article_type: original
author:
- first_name: Shubhadeep
full_name: Biswas, Shubhadeep
last_name: Biswas
- first_name: Benjamin
full_name: Förg, Benjamin
last_name: Förg
- first_name: Lisa
full_name: Ortmann, Lisa
last_name: Ortmann
- first_name: Johannes
full_name: Schötz, Johannes
last_name: Schötz
- first_name: Wolfgang
full_name: Schweinberger, Wolfgang
last_name: Schweinberger
- first_name: Tomáš
full_name: Zimmermann, Tomáš
last_name: Zimmermann
- first_name: Liangwen
full_name: Pi, Liangwen
last_name: Pi
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Hafiz A.
full_name: Masood, Hafiz A.
last_name: Masood
- first_name: Ioannis
full_name: Liontos, Ioannis
last_name: Liontos
- first_name: Amgad M.
full_name: Kamal, Amgad M.
last_name: Kamal
- first_name: Nora G.
full_name: Kling, Nora G.
last_name: Kling
- first_name: Abdullah F.
full_name: Alharbi, Abdullah F.
last_name: Alharbi
- first_name: Meshaal
full_name: Alharbi, Meshaal
last_name: Alharbi
- first_name: Abdallah M.
full_name: Azzeer, Abdallah M.
last_name: Azzeer
- first_name: Gregor
full_name: Hartmann, Gregor
last_name: Hartmann
- first_name: Hans J.
full_name: Wörner, Hans J.
last_name: Wörner
- first_name: Alexandra S.
full_name: Landsman, Alexandra S.
last_name: Landsman
- first_name: Matthias F.
full_name: Kling, Matthias F.
last_name: Kling
citation:
ama: Biswas S, Förg B, Ortmann L, et al. Probing molecular environment through photoemission
delays. Nature Physics. 2020;16(7):778-783. doi:10.1038/s41567-020-0887-8
apa: Biswas, S., Förg, B., Ortmann, L., Schötz, J., Schweinberger, W., Zimmermann,
T., … Kling, M. F. (2020). Probing molecular environment through photoemission
delays. Nature Physics. Springer Nature. https://doi.org/10.1038/s41567-020-0887-8
chicago: Biswas, Shubhadeep, Benjamin Förg, Lisa Ortmann, Johannes Schötz, Wolfgang
Schweinberger, Tomáš Zimmermann, Liangwen Pi, et al. “Probing Molecular Environment
through Photoemission Delays.” Nature Physics. Springer Nature, 2020. https://doi.org/10.1038/s41567-020-0887-8.
ieee: S. Biswas et al., “Probing molecular environment through photoemission
delays,” Nature Physics, vol. 16, no. 7. Springer Nature, pp. 778–783,
2020.
ista: Biswas S, Förg B, Ortmann L, Schötz J, Schweinberger W, Zimmermann T, Pi L,
Baykusheva DR, Masood HA, Liontos I, Kamal AM, Kling NG, Alharbi AF, Alharbi M,
Azzeer AM, Hartmann G, Wörner HJ, Landsman AS, Kling MF. 2020. Probing molecular
environment through photoemission delays. Nature Physics. 16(7), 778–783.
mla: Biswas, Shubhadeep, et al. “Probing Molecular Environment through Photoemission
Delays.” Nature Physics, vol. 16, no. 7, Springer Nature, 2020, pp. 778–83,
doi:10.1038/s41567-020-0887-8.
short: S. Biswas, B. Förg, L. Ortmann, J. Schötz, W. Schweinberger, T. Zimmermann,
L. Pi, D.R. Baykusheva, H.A. Masood, I. Liontos, A.M. Kamal, N.G. Kling, A.F.
Alharbi, M. Alharbi, A.M. Azzeer, G. Hartmann, H.J. Wörner, A.S. Landsman, M.F.
Kling, Nature Physics 16 (2020) 778–783.
date_created: 2023-08-09T13:10:07Z
date_published: 2020-07-01T00:00:00Z
date_updated: 2023-08-22T07:38:04Z
day: '01'
doi: 10.1038/s41567-020-0887-8
extern: '1'
intvolume: ' 16'
issue: '7'
keyword:
- General Physics and Astronomy
language:
- iso: eng
month: '07'
oa_version: None
page: 778-783
publication: Nature Physics
publication_identifier:
eissn:
- 1745-2481
issn:
- 1745-2473
publication_status: published
publisher: Springer Nature
quality_controlled: '1'
scopus_import: '1'
status: public
title: Probing molecular environment through photoemission delays
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 16
year: '2020'
...
---
_id: '14000'
abstract:
- lang: eng
text: This chapter presents an overview of the state of the art in attosecond time-resolved
spectroscopy. The theoretical foundations of strong-field light–matter interaction
and attosecond pulse generation are described. The enabling laser technologies
are reviewed from chirped-pulse amplification and carrier-envelope-phase stabilization
to the generation and characterization of attosecond pulses. The applications
of attosecond pulses and pulse trains in electron- or ion-imaging experiments
are presented, followed by attosecond electron spectroscopy in larger molecules.
After this, high-harmonic spectroscopy and its applications to probing charge
migration on attosecond time scales is reviewed. The rapidly evolving field of
molecular photoionization delays is discussed. Finally, the applications of attosecond
transient absorption to probing molecular dynamics are presented.
article_processing_charge: No
author:
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Hans Jakob
full_name: Wörner, Hans Jakob
last_name: Wörner
citation:
ama: 'Baykusheva DR, Wörner HJ. Attosecond Molecular Dynamics and Spectroscopy.
In: Marquardt R, Quack M, eds. Molecular Spectroscopy and Quantum Dynamics.
1st ed. Elsevier; 2020:113-161. doi:10.1016/b978-0-12-817234-6.00009-x'
apa: Baykusheva, D. R., & Wörner, H. J. (2020). Attosecond Molecular Dynamics
and Spectroscopy. In R. Marquardt & M. Quack (Eds.), Molecular Spectroscopy
and Quantum Dynamics (1st ed., pp. 113–161). Elsevier. https://doi.org/10.1016/b978-0-12-817234-6.00009-x
chicago: Baykusheva, Denitsa Rangelova, and Hans Jakob Wörner. “Attosecond Molecular
Dynamics and Spectroscopy.” In Molecular Spectroscopy and Quantum Dynamics,
edited by Roberto Marquardt and Martin Quack, 1st ed., 113–61. Elsevier, 2020.
https://doi.org/10.1016/b978-0-12-817234-6.00009-x.
ieee: D. R. Baykusheva and H. J. Wörner, “Attosecond Molecular Dynamics and Spectroscopy,”
in Molecular Spectroscopy and Quantum Dynamics, 1st ed., R. Marquardt and
M. Quack, Eds. Elsevier, 2020, pp. 113–161.
ista: 'Baykusheva DR, Wörner HJ. 2020.Attosecond Molecular Dynamics and Spectroscopy.
In: Molecular Spectroscopy and Quantum Dynamics. , 113–161.'
mla: Baykusheva, Denitsa Rangelova, and Hans Jakob Wörner. “Attosecond Molecular
Dynamics and Spectroscopy.” Molecular Spectroscopy and Quantum Dynamics,
edited by Roberto Marquardt and Martin Quack, 1st ed., Elsevier, 2020, pp. 113–61,
doi:10.1016/b978-0-12-817234-6.00009-x.
short: D.R. Baykusheva, H.J. Wörner, in:, R. Marquardt, M. Quack (Eds.), Molecular
Spectroscopy and Quantum Dynamics, 1st ed., Elsevier, 2020, pp. 113–161.
date_created: 2023-08-09T13:10:23Z
date_published: 2020-09-25T00:00:00Z
date_updated: 2023-08-22T09:25:07Z
day: '25'
doi: 10.1016/b978-0-12-817234-6.00009-x
edition: '1'
editor:
- first_name: Roberto
full_name: Marquardt, Roberto
last_name: Marquardt
- first_name: Martin
full_name: Quack, Martin
last_name: Quack
extern: '1'
language:
- iso: eng
month: '09'
oa_version: None
page: 113-161
publication: Molecular Spectroscopy and Quantum Dynamics
publication_identifier:
eisbn:
- '0128172355'
isbn:
- '9780128172353'
publication_status: published
publisher: Elsevier
quality_controlled: '1'
scopus_import: '1'
status: public
title: Attosecond Molecular Dynamics and Spectroscopy
type: book_chapter
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
year: '2020'
...
---
_id: '14028'
abstract:
- lang: eng
text: 'The present review addresses the technical advances and the theoretical developments
to realize and rationalize attosecond-science experiments that reveal a new dynamical
time scale (10−15-10−18 s), with a particular emphasis on molecular systems and
the implications of attosecond processes for chemical dynamics. After a brief
outline of the theoretical framework for treating non-perturbative phenomena in
Section 2, we introduce the physical mechanisms underlying high-harmonic generation
and attosecond technology. The relevant technological developments and experimental
schemes are covered in Section 3. Throughout the remainder of the chapter, we
report on selected applications in molecular attosecond physics, thereby addressing
specific phenomena mediated by purely electronic dynamics: charge localization
in molecular hydrogen, charge migration in biorelevant molecules, high-harmonic
spectroscopy, and delays in molecular photoionization.'
article_processing_charge: No
arxiv: 1
author:
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Hans Jakob
full_name: Wörner, Hans Jakob
last_name: Wörner
citation:
ama: Baykusheva DR, Wörner HJ. Attosecond molecular spectroscopy and dynamics. doi:10.48550/arXiv.2002.02111
apa: Baykusheva, D. R., & Wörner, H. J. (n.d.). Attosecond molecular spectroscopy
and dynamics. https://doi.org/10.48550/arXiv.2002.02111
chicago: Baykusheva, Denitsa Rangelova, and Hans Jakob Wörner. “Attosecond Molecular
Spectroscopy and Dynamics,” n.d. https://doi.org/10.48550/arXiv.2002.02111.
ieee: D. R. Baykusheva and H. J. Wörner, “Attosecond molecular spectroscopy and
dynamics.” .
ista: Baykusheva DR, Wörner HJ. Attosecond molecular spectroscopy and dynamics.
10.48550/arXiv.2002.02111.
mla: Baykusheva, Denitsa Rangelova, and Hans Jakob Wörner. Attosecond Molecular
Spectroscopy and Dynamics. doi:10.48550/arXiv.2002.02111.
short: D.R. Baykusheva, H.J. Wörner, (n.d.).
date_created: 2023-08-10T06:47:45Z
date_published: 2020-02-01T00:00:00Z
date_updated: 2023-08-22T09:17:34Z
day: '01'
doi: 10.48550/arXiv.2002.02111
extern: '1'
external_id:
arxiv:
- '2002.02111'
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.48550/arXiv.2002.02111
month: '02'
oa: 1
oa_version: Preprint
page: '2002.02111'
publication_status: submitted
status: public
title: Attosecond molecular spectroscopy and dynamics
type: preprint
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
year: '2020'
...
---
_id: '14001'
abstract:
- lang: eng
text: Chiral molecules interact and react differently with other chiral objects,
depending on their handedness. Therefore, it is essential to understand and ultimately
control the evolution of molecular chirality during chemical reactions. Although
highly sophisticated techniques for the controlled synthesis of chiral molecules
have been developed, the observation of chirality on the natural femtosecond time
scale of a chemical reaction has so far remained out of reach in the gas phase.
Here, we demonstrate a general experimental technique, based on high-harmonic
generation in tailored laser fields, and apply it to probe the time evolution
of molecular chirality during the photodissociation of 2-iodobutane. These measurements
show a change in sign and a pronounced increase in the magnitude of the chiral
response over the first 100 fs, followed by its decay within less than 500 fs,
revealing the photodissociation to achiral products. The observed time evolution
is explained in terms of the variation of the electric and magnetic transition-dipole
moments between the lowest electronic states of the cation as a function of the
reaction coordinate. These results open the path to investigations of the chirality
of molecular-reaction pathways, light-induced chirality in chemical processes,
and the control of molecular chirality through tailored laser pulses.
article_processing_charge: No
article_type: original
arxiv: 1
author:
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Daniel
full_name: Zindel, Daniel
last_name: Zindel
- first_name: Vít
full_name: Svoboda, Vít
last_name: Svoboda
- first_name: Elias
full_name: Bommeli, Elias
last_name: Bommeli
- first_name: Manuel
full_name: Ochsner, Manuel
last_name: Ochsner
- first_name: Andres
full_name: Tehlar, Andres
last_name: Tehlar
- first_name: Hans Jakob
full_name: Wörner, Hans Jakob
last_name: Wörner
citation:
ama: Baykusheva DR, Zindel D, Svoboda V, et al. Real-time probing of chirality during
a chemical reaction. Proceedings of the National Academy of Sciences. 2019;116(48):23923-23929.
doi:10.1073/pnas.1907189116
apa: Baykusheva, D. R., Zindel, D., Svoboda, V., Bommeli, E., Ochsner, M., Tehlar,
A., & Wörner, H. J. (2019). Real-time probing of chirality during a chemical
reaction. Proceedings of the National Academy of Sciences. Proceedings
of the National Academy of Sciences. https://doi.org/10.1073/pnas.1907189116
chicago: Baykusheva, Denitsa Rangelova, Daniel Zindel, Vít Svoboda, Elias Bommeli,
Manuel Ochsner, Andres Tehlar, and Hans Jakob Wörner. “Real-Time Probing of Chirality
during a Chemical Reaction.” Proceedings of the National Academy of Sciences.
Proceedings of the National Academy of Sciences, 2019. https://doi.org/10.1073/pnas.1907189116.
ieee: D. R. Baykusheva et al., “Real-time probing of chirality during a chemical
reaction,” Proceedings of the National Academy of Sciences, vol. 116, no.
48. Proceedings of the National Academy of Sciences, pp. 23923–23929, 2019.
ista: Baykusheva DR, Zindel D, Svoboda V, Bommeli E, Ochsner M, Tehlar A, Wörner
HJ. 2019. Real-time probing of chirality during a chemical reaction. Proceedings
of the National Academy of Sciences. 116(48), 23923–23929.
mla: Baykusheva, Denitsa Rangelova, et al. “Real-Time Probing of Chirality during
a Chemical Reaction.” Proceedings of the National Academy of Sciences,
vol. 116, no. 48, Proceedings of the National Academy of Sciences, 2019, pp. 23923–29,
doi:10.1073/pnas.1907189116.
short: D.R. Baykusheva, D. Zindel, V. Svoboda, E. Bommeli, M. Ochsner, A. Tehlar,
H.J. Wörner, Proceedings of the National Academy of Sciences 116 (2019) 23923–23929.
date_created: 2023-08-09T13:10:36Z
date_published: 2019-11-13T00:00:00Z
date_updated: 2023-08-22T07:40:05Z
day: '13'
doi: 10.1073/pnas.1907189116
extern: '1'
external_id:
arxiv:
- '1906.10818'
pmid:
- '31723044'
intvolume: ' 116'
issue: '48'
keyword:
- Multidisciplinary
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.1073/pnas.1907189116
month: '11'
oa: 1
oa_version: Published Version
page: 23923-23929
pmid: 1
publication: Proceedings of the National Academy of Sciences
publication_identifier:
eissn:
- 1091-6490
issn:
- 0027-8424
publication_status: published
publisher: Proceedings of the National Academy of Sciences
quality_controlled: '1'
scopus_import: '1'
status: public
title: Real-time probing of chirality during a chemical reaction
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 116
year: '2019'
...
---
_id: '14002'
abstract:
- lang: eng
text: The advancement of attosecond chronoscopy has made it possible to reveal ultrashort
time dynamics of photoionization [1]. Ionization delay measurements in atomic
targets provide a wealth of information about the timing of the photoelectric
effect [2], resonances, electron correlations and transport. The extension of
this approach to molecules, however, presents great challenges. In addition to
the difficulty of identifying correct ionization channels, it is hard to disentangle
the role of the anisotropic molecular landscape from the delays inherent to the
excitation process itself. Here, we present the measurements of ionization delays
from ethyl iodide around the 4d giant dipole resonance of iodine. We employ attosecond
streaking spectroscopy, which enables to disentangle the contribution to the delay
from the functional ethyl group, being responsible for the characteristic chemical
reactivity of the molecule. An attosecond extreme ultraviolet (XUV) pulse ionizes
the molecule around the energy of the giant resonance and the released electron
is exposed to the ponderomotive force of a synchronized near-infrared (NIR) field,
which yields a streaking spectrogram (see figure). Comparative phase analysis
of the spectrograms corresponding to iodine 4d and neon 2p emission permits extracting
overall photoemission delays for ethyl iodide. The data is recorded for multiple
photon energies around the iodine 4d resonance and compared to classical Wigner
propagation [3] and quantum scattering [4] calculations. Here the outgoing electron,
produced via inner shell ionization of the iodine atom in ethyl iodide, and thereby
hardly influenced by the molecular potential during the birth process, acquires
the necessary information about the influence of the functional ethyl group during
its propagation. We find significant delay contributions that can distinguish
between different functional groups, providing a sensitive probe of the local
molecular environment [5]. This would stimulate to perform further angle resolved
measurements in molecules to probe the potential landscape in three dimension.
article_number: '8871819'
article_processing_charge: No
author:
- first_name: Shubhadeep
full_name: Biswas, Shubhadeep
last_name: Biswas
- first_name: I.
full_name: Liontos, I.
last_name: Liontos
- first_name: A. M.
full_name: Kamal, A. M.
last_name: Kamal
- first_name: N. G.
full_name: Kling, N. G.
last_name: Kling
- first_name: A. F.
full_name: Alharbi, A. F.
last_name: Alharbi
- first_name: M.
full_name: Alharbi, M.
last_name: Alharbi
- first_name: A. M.
full_name: Azzeer, A. M.
last_name: Azzeer
- first_name: H. J.
full_name: Worner, H. J.
last_name: Worner
- first_name: A. S.
full_name: Landsman, A. S.
last_name: Landsman
- first_name: M. F.
full_name: Kling, M. F.
last_name: Kling
- first_name: B.
full_name: Forg, B.
last_name: Forg
- first_name: J.
full_name: Schotz, J.
last_name: Schotz
- first_name: W.
full_name: Schweinberger, W.
last_name: Schweinberger
- first_name: L.
full_name: Ortmann, L.
last_name: Ortmann
- first_name: T.
full_name: Zimmermann, T.
last_name: Zimmermann
- first_name: L.-W.
full_name: Pi, L.-W.
last_name: Pi
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: H. A.
full_name: Masood, H. A.
last_name: Masood
citation:
ama: 'Biswas S, Liontos I, Kamal AM, et al. Probing molecular influence on photoemission
delays. In: 2019 Conference on Lasers and Electro-Optics Europe & European
Quantum Electronics Conference. Institute of Electrical and Electronics Engineers;
2019. doi:10.1109/cleoe-eqec.2019.8871819'
apa: 'Biswas, S., Liontos, I., Kamal, A. M., Kling, N. G., Alharbi, A. F., Alharbi,
M., … Masood, H. A. (2019). Probing molecular influence on photoemission delays.
In 2019 Conference on Lasers and Electro-Optics Europe & European Quantum
Electronics Conference. Munich, Germany: Institute of Electrical and Electronics
Engineers. https://doi.org/10.1109/cleoe-eqec.2019.8871819'
chicago: Biswas, Shubhadeep, I. Liontos, A. M. Kamal, N. G. Kling, A. F. Alharbi,
M. Alharbi, A. M. Azzeer, et al. “Probing Molecular Influence on Photoemission
Delays.” In 2019 Conference on Lasers and Electro-Optics Europe & European
Quantum Electronics Conference. Institute of Electrical and Electronics Engineers,
2019. https://doi.org/10.1109/cleoe-eqec.2019.8871819.
ieee: S. Biswas et al., “Probing molecular influence on photoemission delays,”
in 2019 Conference on Lasers and Electro-Optics Europe & European Quantum
Electronics Conference, Munich, Germany, 2019.
ista: 'Biswas S, Liontos I, Kamal AM, Kling NG, Alharbi AF, Alharbi M, Azzeer AM,
Worner HJ, Landsman AS, Kling MF, Forg B, Schotz J, Schweinberger W, Ortmann L,
Zimmermann T, Pi L-W, Baykusheva DR, Masood HA. 2019. Probing molecular influence
on photoemission delays. 2019 Conference on Lasers and Electro-Optics Europe &
European Quantum Electronics Conference. CLEO: European Conference on Lasers and
Electro-Optics, 8871819.'
mla: Biswas, Shubhadeep, et al. “Probing Molecular Influence on Photoemission Delays.”
2019 Conference on Lasers and Electro-Optics Europe & European Quantum
Electronics Conference, 8871819, Institute of Electrical and Electronics Engineers,
2019, doi:10.1109/cleoe-eqec.2019.8871819.
short: S. Biswas, I. Liontos, A.M. Kamal, N.G. Kling, A.F. Alharbi, M. Alharbi,
A.M. Azzeer, H.J. Worner, A.S. Landsman, M.F. Kling, B. Forg, J. Schotz, W. Schweinberger,
L. Ortmann, T. Zimmermann, L.-W. Pi, D.R. Baykusheva, H.A. Masood, in:, 2019 Conference
on Lasers and Electro-Optics Europe & European Quantum Electronics Conference,
Institute of Electrical and Electronics Engineers, 2019.
conference:
end_date: 2019-06-27
location: Munich, Germany
name: 'CLEO: European Conference on Lasers and Electro-Optics'
start_date: 2019-06-23
date_created: 2023-08-09T13:10:49Z
date_published: 2019-10-17T00:00:00Z
date_updated: 2023-08-22T09:32:56Z
day: '17'
doi: 10.1109/cleoe-eqec.2019.8871819
extern: '1'
language:
- iso: eng
month: '10'
oa_version: None
publication: 2019 Conference on Lasers and Electro-Optics Europe & European Quantum
Electronics Conference
publication_identifier:
eisbn:
- '9781728104690'
isbn:
- '9781728104706'
publication_status: published
publisher: Institute of Electrical and Electronics Engineers
quality_controlled: '1'
scopus_import: '1'
status: public
title: Probing molecular influence on photoemission delays
type: conference
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
year: '2019'
...
---
_id: '14003'
abstract:
- lang: eng
text: "Molecular chirality plays an essential role in most biochemical processes.
The observation and quantification of chirality-sensitive signals, however, remains
extremely challenging, especially on ultrafast timescales and in dilute media.
Here, we describe the experimental realization of an all-optical and ultrafast
scheme for detecting chiral dynamics in molecules. This technique is based on
high-harmonic generation by a combination of two-color counterrotating femtosecond
laser pulses with polarization states tunable from linear to circular. We demonstrate
two different implementations of chiral-sensitive high-harmonic spectroscopy on
an ensemble of randomly oriented methyloxirane molecules in the gas phase. Using
two elliptically polarized fields, we observe that the ellipticities maximizing
the harmonic signal reach up to \r\n4.4\r\n±\r\n0.2\r\n%\r\n (at 17.6 eV). Using
two circularly polarized fields, we observe circular dichroisms ranging up to
\r\n13\r\n±\r\n6\r\n%\r\n (28.3–33.1 eV). Our theoretical analysis confirms that
the observed chiral response originates from subfemtosecond electron dynamics
driven by the magnetic component of the driving laser field. This assignment is
supported by the experimental observation of a strong intensity dependence of
the chiral effects and its agreement with theory. We moreover report and explain
a pronounced variation of the signal strength and dichroism with the driving-field
ellipticities and harmonic orders. Finally, we demonstrate the sensitivity of
the experimental observables to the shape of the electron hole. This technique
for chiral discrimination will yield femtosecond temporal resolution when integrated
in a pump-probe scheme and subfemtosecond resolution on chiral charge migration
in a self-probing scheme."
article_number: '031060'
article_processing_charge: No
article_type: original
author:
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Hans Jakob
full_name: Wörner, Hans Jakob
last_name: Wörner
citation:
ama: Baykusheva DR, Wörner HJ. Chiral discrimination through bielliptical high-harmonic
spectroscopy. Physical Review X. 2018;8(3). doi:10.1103/physrevx.8.031060
apa: Baykusheva, D. R., & Wörner, H. J. (2018). Chiral discrimination through
bielliptical high-harmonic spectroscopy. Physical Review X. American Physical
Society. https://doi.org/10.1103/physrevx.8.031060
chicago: Baykusheva, Denitsa Rangelova, and Hans Jakob Wörner. “Chiral Discrimination
through Bielliptical High-Harmonic Spectroscopy.” Physical Review X. American
Physical Society, 2018. https://doi.org/10.1103/physrevx.8.031060.
ieee: D. R. Baykusheva and H. J. Wörner, “Chiral discrimination through bielliptical
high-harmonic spectroscopy,” Physical Review X, vol. 8, no. 3. American
Physical Society, 2018.
ista: Baykusheva DR, Wörner HJ. 2018. Chiral discrimination through bielliptical
high-harmonic spectroscopy. Physical Review X. 8(3), 031060.
mla: Baykusheva, Denitsa Rangelova, and Hans Jakob Wörner. “Chiral Discrimination
through Bielliptical High-Harmonic Spectroscopy.” Physical Review X, vol.
8, no. 3, 031060, American Physical Society, 2018, doi:10.1103/physrevx.8.031060.
short: D.R. Baykusheva, H.J. Wörner, Physical Review X 8 (2018).
date_created: 2023-08-10T06:34:48Z
date_published: 2018-07-01T00:00:00Z
date_updated: 2023-08-22T07:42:07Z
day: '01'
doi: 10.1103/physrevx.8.031060
extern: '1'
intvolume: ' 8'
issue: '3'
keyword:
- General Physics and Astronomy
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.1103/PhysRevX.8.031060
month: '07'
oa: 1
oa_version: Published Version
publication: Physical Review X
publication_identifier:
eissn:
- 2160-3308
publication_status: published
publisher: American Physical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Chiral discrimination through bielliptical high-harmonic spectroscopy
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 8
year: '2018'
...
---
_id: '14004'
abstract:
- lang: eng
text: High-harmonic spectroscopy driven by circularly polarized laser pulses and
their counterrotating second harmonic is a new branch of attosecond science which
currently lacks quantitative interpretations. We extend this technique to the
midinfrared regime and record detailed high-harmonic spectra of several rare-gas
atoms. These results are compared with the solution of the Schrödinger equation
in three dimensions and calculations based on the strong-field approximation that
incorporate accurate scattering-wave recombination matrix elements. A quantum-orbit
analysis of these results provides a transparent interpretation of the measured
intensity ratios of symmetry-allowed neighboring harmonics in terms of (i) a set
of propensity rules related to the angular momentum of the atomic orbitals, (ii)
atom-specific matrix elements related to their electronic structure, and (iii)
the interference of the emissions associated with electrons in orbitals corotating
or counterrotating with the laser fields. These results provide the foundation
for a quantitative understanding of bicircular high-harmonic spectroscopy.
article_number: '203201'
article_processing_charge: No
article_type: original
arxiv: 1
author:
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Simon
full_name: Brennecke, Simon
last_name: Brennecke
- first_name: Manfred
full_name: Lein, Manfred
last_name: Lein
- first_name: Hans Jakob
full_name: Wörner, Hans Jakob
last_name: Wörner
citation:
ama: Baykusheva DR, Brennecke S, Lein M, Wörner HJ. Signatures of electronic structure
in bicircular high-harmonic spectroscopy. Physical Review Letters. 2017;119(20).
doi:10.1103/physrevlett.119.203201
apa: Baykusheva, D. R., Brennecke, S., Lein, M., & Wörner, H. J. (2017). Signatures
of electronic structure in bicircular high-harmonic spectroscopy. Physical
Review Letters. American Physical Society. https://doi.org/10.1103/physrevlett.119.203201
chicago: Baykusheva, Denitsa Rangelova, Simon Brennecke, Manfred Lein, and Hans
Jakob Wörner. “Signatures of Electronic Structure in Bicircular High-Harmonic
Spectroscopy.” Physical Review Letters. American Physical Society, 2017.
https://doi.org/10.1103/physrevlett.119.203201.
ieee: D. R. Baykusheva, S. Brennecke, M. Lein, and H. J. Wörner, “Signatures of
electronic structure in bicircular high-harmonic spectroscopy,” Physical Review
Letters, vol. 119, no. 20. American Physical Society, 2017.
ista: Baykusheva DR, Brennecke S, Lein M, Wörner HJ. 2017. Signatures of electronic
structure in bicircular high-harmonic spectroscopy. Physical Review Letters. 119(20),
203201.
mla: Baykusheva, Denitsa Rangelova, et al. “Signatures of Electronic Structure in
Bicircular High-Harmonic Spectroscopy.” Physical Review Letters, vol. 119,
no. 20, 203201, American Physical Society, 2017, doi:10.1103/physrevlett.119.203201.
short: D.R. Baykusheva, S. Brennecke, M. Lein, H.J. Wörner, Physical Review Letters
119 (2017).
date_created: 2023-08-10T06:35:51Z
date_published: 2017-11-17T00:00:00Z
date_updated: 2023-08-22T08:21:10Z
day: '17'
doi: 10.1103/physrevlett.119.203201
extern: '1'
external_id:
arxiv:
- '1710.04474'
intvolume: ' 119'
issue: '20'
keyword:
- General Physics and Astronomy
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://arxiv.org/abs/1710.04474
month: '11'
oa: 1
oa_version: Preprint
publication: Physical Review Letters
publication_identifier:
eissn:
- 1079-7114
issn:
- 0031-9007
publication_status: published
publisher: American Physical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Signatures of electronic structure in bicircular high-harmonic spectroscopy
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 119
year: '2017'
...
---
_id: '14005'
abstract:
- lang: eng
text: Strong-field photoelectron holography and laser-induced electron diffraction
(LIED) are two powerful emerging methods for probing the ultrafast dynamics of
molecules. However, both of them have remained restricted to static systems and
to nuclear dynamics induced by strong-field ionization. Here we extend these promising
methods to image purely electronic valence-shell dynamics in molecules using photoelectron
holography. In the same experiment, we use LIED and photoelectron holography simultaneously,
to observe coupled electronic-rotational dynamics taking place on similar timescales.
These results offer perspectives for imaging ultrafast dynamics of molecules on
femtosecond to attosecond timescales.
article_number: '15651'
article_processing_charge: No
article_type: original
author:
- first_name: Samuel G.
full_name: Walt, Samuel G.
last_name: Walt
- first_name: Niraghatam
full_name: Bhargava Ram, Niraghatam
last_name: Bhargava Ram
- first_name: Marcos
full_name: Atala, Marcos
last_name: Atala
- first_name: Nikolay I
full_name: Shvetsov-Shilovski, Nikolay I
last_name: Shvetsov-Shilovski
- first_name: Aaron
full_name: von Conta, Aaron
last_name: von Conta
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Manfred
full_name: Lein, Manfred
last_name: Lein
- first_name: Hans Jakob
full_name: Wörner, Hans Jakob
last_name: Wörner
citation:
ama: Walt SG, Bhargava Ram N, Atala M, et al. Dynamics of valence-shell electrons
and nuclei probed by strong-field holography and rescattering. Nature Communications.
2017;8. doi:10.1038/ncomms15651
apa: Walt, S. G., Bhargava Ram, N., Atala, M., Shvetsov-Shilovski, N. I., von Conta,
A., Baykusheva, D. R., … Wörner, H. J. (2017). Dynamics of valence-shell electrons
and nuclei probed by strong-field holography and rescattering. Nature Communications.
Springer Nature. https://doi.org/10.1038/ncomms15651
chicago: Walt, Samuel G., Niraghatam Bhargava Ram, Marcos Atala, Nikolay I Shvetsov-Shilovski,
Aaron von Conta, Denitsa Rangelova Baykusheva, Manfred Lein, and Hans Jakob Wörner.
“Dynamics of Valence-Shell Electrons and Nuclei Probed by Strong-Field Holography
and Rescattering.” Nature Communications. Springer Nature, 2017. https://doi.org/10.1038/ncomms15651.
ieee: S. G. Walt et al., “Dynamics of valence-shell electrons and nuclei
probed by strong-field holography and rescattering,” Nature Communications,
vol. 8. Springer Nature, 2017.
ista: Walt SG, Bhargava Ram N, Atala M, Shvetsov-Shilovski NI, von Conta A, Baykusheva
DR, Lein M, Wörner HJ. 2017. Dynamics of valence-shell electrons and nuclei probed
by strong-field holography and rescattering. Nature Communications. 8, 15651.
mla: Walt, Samuel G., et al. “Dynamics of Valence-Shell Electrons and Nuclei Probed
by Strong-Field Holography and Rescattering.” Nature Communications, vol.
8, 15651, Springer Nature, 2017, doi:10.1038/ncomms15651.
short: S.G. Walt, N. Bhargava Ram, M. Atala, N.I. Shvetsov-Shilovski, A. von Conta,
D.R. Baykusheva, M. Lein, H.J. Wörner, Nature Communications 8 (2017).
date_created: 2023-08-10T06:36:09Z
date_published: 2017-06-15T00:00:00Z
date_updated: 2023-08-22T08:26:06Z
day: '15'
doi: 10.1038/ncomms15651
extern: '1'
external_id:
pmid:
- '28643771'
intvolume: ' 8'
keyword:
- General Physics and Astronomy
- General Biochemistry
- Genetics and Molecular Biology
- General Chemistry
- Multidisciplinary
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.1038/ncomms15651
month: '06'
oa: 1
oa_version: Published Version
pmid: 1
publication: Nature Communications
publication_identifier:
eissn:
- 2041-1723
publication_status: published
publisher: Springer Nature
quality_controlled: '1'
scopus_import: '1'
status: public
title: Dynamics of valence-shell electrons and nuclei probed by strong-field holography
and rescattering
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 8
year: '2017'
...
---
_id: '14006'
abstract:
- lang: eng
text: We present a theoretical formalism for the calculation of attosecond delays
in molecular photoionization. It is shown how delays relevant to one-photon-ionization,
also known as Eisenbud-Wigner-Smith delays, can be obtained from the complex dipole
matrix elements provided by molecular quantum scattering theory. These results
are used to derive formulae for the delays measured by two-photon attosecond interferometry
based on an attosecond pulse train and a dressing femtosecond infrared pulse.
These effective delays are first expressed in the molecular frame where maximal
information about the molecular photoionization dynamics is available. The effects
of averaging over the emission direction of the electron and the molecular orientation
are introduced analytically. We illustrate this general formalism for the case
of two polyatomic molecules. N2O serves as an example of a polar linear molecule
characterized by complex photoionization dynamics resulting from the presence
of molecular shape resonances. H2O illustrates the case of a non-linear molecule
with comparably simple photoionization dynamics resulting from a flat continuum.
Our theory establishes the foundation for interpreting measurements of the photoionization
dynamics of all molecules by attosecond metrology.
article_number: '124306'
article_processing_charge: No
article_type: original
author:
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Hans Jakob
full_name: Wörner, Hans Jakob
last_name: Wörner
citation:
ama: Baykusheva DR, Wörner HJ. Theory of attosecond delays in molecular photoionization.
The Journal of Chemical Physics. 2017;146(12). doi:10.1063/1.4977933
apa: Baykusheva, D. R., & Wörner, H. J. (2017). Theory of attosecond delays
in molecular photoionization. The Journal of Chemical Physics. AIP Publishing.
https://doi.org/10.1063/1.4977933
chicago: Baykusheva, Denitsa Rangelova, and Hans Jakob Wörner. “Theory of Attosecond
Delays in Molecular Photoionization.” The Journal of Chemical Physics.
AIP Publishing, 2017. https://doi.org/10.1063/1.4977933.
ieee: D. R. Baykusheva and H. J. Wörner, “Theory of attosecond delays in molecular
photoionization,” The Journal of Chemical Physics, vol. 146, no. 12. AIP
Publishing, 2017.
ista: Baykusheva DR, Wörner HJ. 2017. Theory of attosecond delays in molecular photoionization.
The Journal of Chemical Physics. 146(12), 124306.
mla: Baykusheva, Denitsa Rangelova, and Hans Jakob Wörner. “Theory of Attosecond
Delays in Molecular Photoionization.” The Journal of Chemical Physics,
vol. 146, no. 12, 124306, AIP Publishing, 2017, doi:10.1063/1.4977933.
short: D.R. Baykusheva, H.J. Wörner, The Journal of Chemical Physics 146 (2017).
date_created: 2023-08-10T06:36:19Z
date_published: 2017-03-28T00:00:00Z
date_updated: 2023-08-22T08:30:59Z
day: '28'
doi: 10.1063/1.4977933
extern: '1'
external_id:
pmid:
- '28388142'
intvolume: ' 146'
issue: '12'
keyword:
- Physical and Theoretical Chemistry
- General Physics and Astronomy
language:
- iso: eng
month: '03'
oa_version: None
pmid: 1
publication: The Journal of Chemical Physics
publication_identifier:
eissn:
- 1089-7690
issn:
- 0021-9606
publication_status: published
publisher: AIP Publishing
quality_controlled: '1'
scopus_import: '1'
status: public
title: Theory of attosecond delays in molecular photoionization
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 146
year: '2017'
...
---
_id: '14007'
abstract:
- lang: eng
text: 'In a recent article by Hockett et al (2016 J. Phys. B: At. Mol. Opt. Phys.
49 095602), time delays arising in the context of molecular single-photon ionization
are investigated from a theoretical point of view. We argue that one of the central
equations given in this article is incorrect and present a reformulation that
is consistent with the established treatment of angle-dependent scattering delays
(Eisenbud 1948 PhD Thesis Princeton University; Wigner 1955 Phys. Rev. 98 145–7;
Smith 1960 Phys. Rev. 118 349–6; Nussenzveig 1972 Phys. Rev. D 6 1534–42).'
article_number: '078002'
article_processing_charge: No
article_type: letter_note
arxiv: 1
author:
- first_name: Denitsa Rangelova
full_name: Baykusheva, Denitsa Rangelova
id: 71b4d059-2a03-11ee-914d-dfa3beed6530
last_name: Baykusheva
- first_name: Hans Jakob
full_name: Wörner, Hans Jakob
last_name: Wörner
citation:
ama: 'Baykusheva DR, Wörner HJ. Comment on ‘Time delays in molecular photoionization.’
Journal of Physics B: Atomic, Molecular and Optical Physics. 2017;50(7).
doi:10.1088/1361-6455/aa62b5'
apa: 'Baykusheva, D. R., & Wörner, H. J. (2017). Comment on ‘Time delays in
molecular photoionization.’ Journal of Physics B: Atomic, Molecular and Optical
Physics. IOP Publishing. https://doi.org/10.1088/1361-6455/aa62b5'
chicago: 'Baykusheva, Denitsa Rangelova, and Hans Jakob Wörner. “Comment on ‘Time
Delays in Molecular Photoionization.’” Journal of Physics B: Atomic, Molecular
and Optical Physics. IOP Publishing, 2017. https://doi.org/10.1088/1361-6455/aa62b5.'
ieee: 'D. R. Baykusheva and H. J. Wörner, “Comment on ‘Time delays in molecular
photoionization,’” Journal of Physics B: Atomic, Molecular and Optical Physics,
vol. 50, no. 7. IOP Publishing, 2017.'
ista: 'Baykusheva DR, Wörner HJ. 2017. Comment on ‘Time delays in molecular photoionization’.
Journal of Physics B: Atomic, Molecular and Optical Physics. 50(7), 078002.'
mla: 'Baykusheva, Denitsa Rangelova, and Hans Jakob Wörner. “Comment on ‘Time Delays
in Molecular Photoionization.’” Journal of Physics B: Atomic, Molecular and
Optical Physics, vol. 50, no. 7, 078002, IOP Publishing, 2017, doi:10.1088/1361-6455/aa62b5.'
short: 'D.R. Baykusheva, H.J. Wörner, Journal of Physics B: Atomic, Molecular and
Optical Physics 50 (2017).'
date_created: 2023-08-10T06:36:29Z
date_published: 2017-03-15T00:00:00Z
date_updated: 2023-08-22T08:32:43Z
day: '15'
doi: 10.1088/1361-6455/aa62b5
extern: '1'
external_id:
arxiv:
- '1611.09352'
intvolume: ' 50'
issue: '7'
keyword:
- Condensed Matter Physics
- Atomic and Molecular Physics
- and Optics
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://arxiv.org/abs/1611.09352
month: '03'
oa: 1
oa_version: Preprint
publication: 'Journal of Physics B: Atomic, Molecular and Optical Physics'
publication_identifier:
eissn:
- 1361-6455
issn:
- 0953-4075
publication_status: published
publisher: IOP Publishing
quality_controlled: '1'
scopus_import: '1'
status: public
title: Comment on ‘Time delays in molecular photoionization’
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 50
year: '2017'
...