---
_id: '13251'
abstract:
- lang: eng
text: A rotating organic cation and a dynamically disordered soft inorganic cage
are the hallmark features of organic-inorganic lead-halide perovskites. Understanding
the interplay between these two subsystems is a challenging problem, but it is
this coupling that is widely conjectured to be responsible for the unique behavior
of photocarriers in these materials. In this work, we use the fact that the polarizability
of the organic cation strongly depends on the ambient electrostatic environment
to put the molecule forward as a sensitive probe of the local crystal fields inside
the lattice cell. We measure the average polarizability of the C/N–H bond stretching
mode by means of infrared spectroscopy, which allows us to deduce the character
of the motion of the cation molecule, find the magnitude of the local crystal
field, and place an estimate on the strength of the hydrogen bond between the
hydrogen and halide atoms. Our results pave the way for understanding electric
fields in lead-halide perovskites using infrared bond spectroscopy.
acknowledgement: "We thank Bingqing Cheng and Hong-Zhou Ye for valuable discussions;
Y.W.’s work at IST Austria was supported through ISTernship summer internship program
funded by OeADGmbH; D.L. and Z.A. acknowledge support by IST Austria (ISTA); M.L.
acknowledges support by the European Research Council (ERC) Starting Grant No. 801770
(ANGULON).\r\nA.A.Z. and O.M.B. acknowledge support by KAUST."
article_processing_charge: Yes (via OA deal)
article_type: original
arxiv: 1
author:
- first_name: Yujing
full_name: Wei, Yujing
id: 0c5ff007-2600-11ee-b896-98bd8d663294
last_name: Wei
orcid: 0000-0001-8913-9719
- first_name: Artem
full_name: Volosniev, Artem
id: 37D278BC-F248-11E8-B48F-1D18A9856A87
last_name: Volosniev
orcid: 0000-0003-0393-5525
- first_name: Dusan
full_name: Lorenc, Dusan
id: 40D8A3E6-F248-11E8-B48F-1D18A9856A87
last_name: Lorenc
- first_name: Ayan A.
full_name: Zhumekenov, Ayan A.
last_name: Zhumekenov
- first_name: Osman M.
full_name: Bakr, Osman M.
last_name: Bakr
- first_name: Mikhail
full_name: Lemeshko, Mikhail
id: 37CB05FA-F248-11E8-B48F-1D18A9856A87
last_name: Lemeshko
orcid: 0000-0002-6990-7802
- first_name: Zhanybek
full_name: Alpichshev, Zhanybek
id: 45E67A2A-F248-11E8-B48F-1D18A9856A87
last_name: Alpichshev
orcid: 0000-0002-7183-5203
citation:
ama: Wei Y, Volosniev A, Lorenc D, et al. Bond polarizability as a probe of local
crystal fields in hybrid lead-halide perovskites. The Journal of Physical Chemistry
Letters. 2023;14(27):6309-6314. doi:10.1021/acs.jpclett.3c01158
apa: Wei, Y., Volosniev, A., Lorenc, D., Zhumekenov, A. A., Bakr, O. M., Lemeshko,
M., & Alpichshev, Z. (2023). Bond polarizability as a probe of local crystal
fields in hybrid lead-halide perovskites. The Journal of Physical Chemistry
Letters. American Chemical Society. https://doi.org/10.1021/acs.jpclett.3c01158
chicago: Wei, Yujing, Artem Volosniev, Dusan Lorenc, Ayan A. Zhumekenov, Osman M.
Bakr, Mikhail Lemeshko, and Zhanybek Alpichshev. “Bond Polarizability as a Probe
of Local Crystal Fields in Hybrid Lead-Halide Perovskites.” The Journal of
Physical Chemistry Letters. American Chemical Society, 2023. https://doi.org/10.1021/acs.jpclett.3c01158.
ieee: Y. Wei et al., “Bond polarizability as a probe of local crystal fields
in hybrid lead-halide perovskites,” The Journal of Physical Chemistry Letters,
vol. 14, no. 27. American Chemical Society, pp. 6309–6314, 2023.
ista: Wei Y, Volosniev A, Lorenc D, Zhumekenov AA, Bakr OM, Lemeshko M, Alpichshev
Z. 2023. Bond polarizability as a probe of local crystal fields in hybrid lead-halide
perovskites. The Journal of Physical Chemistry Letters. 14(27), 6309–6314.
mla: Wei, Yujing, et al. “Bond Polarizability as a Probe of Local Crystal Fields
in Hybrid Lead-Halide Perovskites.” The Journal of Physical Chemistry Letters,
vol. 14, no. 27, American Chemical Society, 2023, pp. 6309–14, doi:10.1021/acs.jpclett.3c01158.
short: Y. Wei, A. Volosniev, D. Lorenc, A.A. Zhumekenov, O.M. Bakr, M. Lemeshko,
Z. Alpichshev, The Journal of Physical Chemistry Letters 14 (2023) 6309–6314.
date_created: 2023-07-18T11:13:17Z
date_published: 2023-07-05T00:00:00Z
date_updated: 2023-07-19T06:59:19Z
day: '05'
ddc:
- '530'
department:
- _id: MiLe
- _id: ZhAl
doi: 10.1021/acs.jpclett.3c01158
ec_funded: 1
external_id:
arxiv:
- '2304.14198'
isi:
- '001022811500001'
file:
- access_level: open_access
checksum: c0c040063f06a51b9c463adc504f1a23
content_type: application/pdf
creator: dernst
date_created: 2023-07-19T06:55:39Z
date_updated: 2023-07-19T06:55:39Z
file_id: '13253'
file_name: 2023_JourPhysChemistry_Wei.pdf
file_size: 2121252
relation: main_file
success: 1
file_date_updated: 2023-07-19T06:55:39Z
has_accepted_license: '1'
intvolume: ' 14'
isi: 1
issue: '27'
keyword:
- General Materials Science
- Physical and Theoretical Chemistry
language:
- iso: eng
month: '07'
oa: 1
oa_version: Published Version
page: 6309-6314
project:
- _id: 2688CF98-B435-11E9-9278-68D0E5697425
call_identifier: H2020
grant_number: '801770'
name: 'Angulon: physics and applications of a new quasiparticle'
publication: The Journal of Physical Chemistry Letters
publication_identifier:
eissn:
- 1948-7185
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
status: public
title: Bond polarizability as a probe of local crystal fields in hybrid lead-halide
perovskites
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 14
year: '2023'
...
---
_id: '14261'
abstract:
- lang: eng
text: In this work, a generalized, adapted Numerov implementation capable of determining
band structures of periodic quantum systems is outlined. Based on the input potential,
the presented approach numerically solves the Schrödinger equation in position
space at each momentum space point. Thus, in addition to the band structure, the
method inherently provides information about the state functions and probability
densities in position space at each momentum space point considered. The generalized,
adapted Numerov framework provided reliable estimates for a variety of increasingly
complex test suites in one, two, and three dimensions. The accuracy of the proposed
methodology was benchmarked against results obtained for the analytically solvable
Kronig-Penney model. Furthermore, the presented numerical solver was applied to
a model potential representing a 2D optical lattice being a challenging application
relevant, for example, in the field of quantum computing.
acknowledgement: Financial supports for this work via a PhD scholarship for J. Gamper
issued by the Leopold-Franzens-University of Innsbruck (Vicerector Prof. Dr Ulrike
Tanzer) are gratefully acknowledged. The computational results presented have been
achieved (in part) using the HPC infrastructure of the University of Innsbruck.
article_processing_charge: Yes (in subscription journal)
article_type: original
author:
- first_name: Jakob
full_name: Gamper, Jakob
last_name: Gamper
- first_name: Florian
full_name: Kluibenschedl, Florian
id: 7499e70e-eb2c-11ec-b98b-f925648bc9d9
last_name: Kluibenschedl
- first_name: Alexander K.H.
full_name: Weiss, Alexander K.H.
last_name: Weiss
- first_name: Thomas S.
full_name: Hofer, Thomas S.
last_name: Hofer
citation:
ama: Gamper J, Kluibenschedl F, Weiss AKH, Hofer TS. Accessing position space wave
functions in band structure calculations of periodic systems - a generalized,
adapted numerov implementation for one-, two-, and three-dimensional quantum problems.
Journal of Physical Chemistry Letters. 2023;14(33):7395-7403. doi:10.1021/acs.jpclett.3c01707
apa: Gamper, J., Kluibenschedl, F., Weiss, A. K. H., & Hofer, T. S. (2023).
Accessing position space wave functions in band structure calculations of periodic
systems - a generalized, adapted numerov implementation for one-, two-, and three-dimensional
quantum problems. Journal of Physical Chemistry Letters. American Chemical
Society. https://doi.org/10.1021/acs.jpclett.3c01707
chicago: Gamper, Jakob, Florian Kluibenschedl, Alexander K.H. Weiss, and Thomas
S. Hofer. “Accessing Position Space Wave Functions in Band Structure Calculations
of Periodic Systems - a Generalized, Adapted Numerov Implementation for One-,
Two-, and Three-Dimensional Quantum Problems.” Journal of Physical Chemistry
Letters. American Chemical Society, 2023. https://doi.org/10.1021/acs.jpclett.3c01707.
ieee: J. Gamper, F. Kluibenschedl, A. K. H. Weiss, and T. S. Hofer, “Accessing position
space wave functions in band structure calculations of periodic systems - a generalized,
adapted numerov implementation for one-, two-, and three-dimensional quantum problems,”
Journal of Physical Chemistry Letters, vol. 14, no. 33. American Chemical
Society, pp. 7395–7403, 2023.
ista: Gamper J, Kluibenschedl F, Weiss AKH, Hofer TS. 2023. Accessing position space
wave functions in band structure calculations of periodic systems - a generalized,
adapted numerov implementation for one-, two-, and three-dimensional quantum problems.
Journal of Physical Chemistry Letters. 14(33), 7395–7403.
mla: Gamper, Jakob, et al. “Accessing Position Space Wave Functions in Band Structure
Calculations of Periodic Systems - a Generalized, Adapted Numerov Implementation
for One-, Two-, and Three-Dimensional Quantum Problems.” Journal of Physical
Chemistry Letters, vol. 14, no. 33, American Chemical Society, 2023, pp. 7395–403,
doi:10.1021/acs.jpclett.3c01707.
short: J. Gamper, F. Kluibenschedl, A.K.H. Weiss, T.S. Hofer, Journal of Physical
Chemistry Letters 14 (2023) 7395–7403.
date_created: 2023-09-03T22:01:16Z
date_published: 2023-08-11T00:00:00Z
date_updated: 2023-09-06T11:04:31Z
day: '11'
ddc:
- '530'
- '540'
department:
- _id: GradSch
doi: 10.1021/acs.jpclett.3c01707
external_id:
isi:
- '001048165800001'
pmid:
- '37566743'
file:
- access_level: open_access
checksum: 637454e2b3a357498d8d622d241c4bf6
content_type: application/pdf
creator: dernst
date_created: 2023-09-06T07:32:39Z
date_updated: 2023-09-06T07:32:39Z
file_id: '14272'
file_name: 2023_JourPhysChemistry_Gamper.pdf
file_size: 4986859
relation: main_file
success: 1
file_date_updated: 2023-09-06T07:32:39Z
has_accepted_license: '1'
intvolume: ' 14'
isi: 1
issue: '33'
language:
- iso: eng
month: '08'
oa: 1
oa_version: Published Version
page: 7395-7403
pmid: 1
publication: Journal of Physical Chemistry Letters
publication_identifier:
eissn:
- 1948-7185
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Accessing position space wave functions in band structure calculations of periodic
systems - a generalized, adapted numerov implementation for one-, two-, and three-dimensional
quantum problems
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: c635000d-4b10-11ee-a964-aac5a93f6ac1
volume: 14
year: '2023'
...
---
_id: '9681'
abstract:
- lang: eng
text: One of the most prominent consequences of the quantum nature of light atomic
nuclei is that their kinetic energy does not follow a Maxwell–Boltzmann distribution.
Deep inelastic neutron scattering (DINS) experiments can measure this effect.
Thus, the nuclear quantum kinetic energy can be probed directly in both ordered
and disordered samples. However, the relation between the quantum kinetic energy
and the atomic environment is a very indirect one, and cross-validation with theoretical
modeling is therefore urgently needed. Here, we use state of the art path integral
molecular dynamics techniques to compute the kinetic energy of hydrogen and oxygen
nuclei in liquid, solid, and gas-phase water close to the triple point, comparing
three different interatomic potentials and validating our results against equilibrium
isotope fractionation measurements. We will then show how accurate simulations
can draw a link between extremely precise fractionation experiments and DINS,
therefore establishing a reliable benchmark for future measurements and providing
key insights to increase further the accuracy of interatomic potentials for water.
article_processing_charge: No
article_type: letter_note
author:
- first_name: Bingqing
full_name: Cheng, Bingqing
id: cbe3cda4-d82c-11eb-8dc7-8ff94289fcc9
last_name: Cheng
orcid: 0000-0002-3584-9632
- first_name: Jörg
full_name: Behler, Jörg
last_name: Behler
- first_name: Michele
full_name: Ceriotti, Michele
last_name: Ceriotti
citation:
ama: 'Cheng B, Behler J, Ceriotti M. Nuclear quantum effects in water at the triple
point: Using theory as a link between experiments. The Journal of Physical
Chemistry Letters. 2016;7(12):2210-2215. doi:10.1021/acs.jpclett.6b00729'
apa: 'Cheng, B., Behler, J., & Ceriotti, M. (2016). Nuclear quantum effects
in water at the triple point: Using theory as a link between experiments. The
Journal of Physical Chemistry Letters. American Chemical Society. https://doi.org/10.1021/acs.jpclett.6b00729'
chicago: 'Cheng, Bingqing, Jörg Behler, and Michele Ceriotti. “Nuclear Quantum Effects
in Water at the Triple Point: Using Theory as a Link between Experiments.” The
Journal of Physical Chemistry Letters. American Chemical Society, 2016. https://doi.org/10.1021/acs.jpclett.6b00729.'
ieee: 'B. Cheng, J. Behler, and M. Ceriotti, “Nuclear quantum effects in water at
the triple point: Using theory as a link between experiments,” The Journal
of Physical Chemistry Letters, vol. 7, no. 12. American Chemical Society,
pp. 2210–2215, 2016.'
ista: 'Cheng B, Behler J, Ceriotti M. 2016. Nuclear quantum effects in water at
the triple point: Using theory as a link between experiments. The Journal of Physical
Chemistry Letters. 7(12), 2210–2215.'
mla: 'Cheng, Bingqing, et al. “Nuclear Quantum Effects in Water at the Triple Point:
Using Theory as a Link between Experiments.” The Journal of Physical Chemistry
Letters, vol. 7, no. 12, American Chemical Society, 2016, pp. 2210–15, doi:10.1021/acs.jpclett.6b00729.'
short: B. Cheng, J. Behler, M. Ceriotti, The Journal of Physical Chemistry Letters
7 (2016) 2210–2215.
date_created: 2021-07-19T08:57:32Z
date_published: 2016-06-16T00:00:00Z
date_updated: 2023-02-23T14:04:49Z
day: '16'
doi: 10.1021/acs.jpclett.6b00729
extern: '1'
external_id:
pmid:
- '27203358'
intvolume: ' 7'
issue: '12'
language:
- iso: eng
month: '06'
oa_version: None
page: 2210-2215
pmid: 1
publication: The Journal of Physical Chemistry Letters
publication_identifier:
eissn:
- 1948-7185
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: 'Nuclear quantum effects in water at the triple point: Using theory as a link
between experiments'
type: journal_article
user_id: 6785fbc1-c503-11eb-8a32-93094b40e1cf
volume: 7
year: '2016'
...