---
_id: '7968'
abstract:
- lang: eng
text: Organic materials are known to feature long spin-diffusion times, originating
in a generally small spin–orbit coupling observed in these systems. From that
perspective, chiral molecules acting as efficient spin selectors pose a puzzle
that attracted a lot of attention in recent years. Here, we revisit the physical
origins of chiral-induced spin selectivity (CISS) and propose a simple analytic
minimal model to describe it. The model treats a chiral molecule as an anisotropic
wire with molecular dipole moments aligned arbitrarily with respect to the wire’s
axes and is therefore quite general. Importantly, it shows that the helical structure
of the molecule is not necessary to observe CISS and other chiral nonhelical molecules
can also be considered as potential candidates for the CISS effect. We also show
that the suggested simple model captures the main characteristics of CISS observed
in the experiment, without the need for additional constraints employed in the
previous studies. The results pave the way for understanding other related physical
phenomena where the CISS effect plays an essential role.
article_processing_charge: Yes (via OA deal)
article_type: original
author:
- first_name: Areg
full_name: Ghazaryan, Areg
id: 4AF46FD6-F248-11E8-B48F-1D18A9856A87
last_name: Ghazaryan
orcid: 0000-0001-9666-3543
- first_name: Yossi
full_name: Paltiel, Yossi
last_name: Paltiel
- first_name: Mikhail
full_name: Lemeshko, Mikhail
id: 37CB05FA-F248-11E8-B48F-1D18A9856A87
last_name: Lemeshko
orcid: 0000-0002-6990-7802
citation:
ama: Ghazaryan A, Paltiel Y, Lemeshko M. Analytic model of chiral-induced spin selectivity.
The Journal of Physical Chemistry C. 2020;124(21):11716-11721. doi:10.1021/acs.jpcc.0c02584
apa: Ghazaryan, A., Paltiel, Y., & Lemeshko, M. (2020). Analytic model of chiral-induced
spin selectivity. The Journal of Physical Chemistry C. American Chemical
Society. https://doi.org/10.1021/acs.jpcc.0c02584
chicago: Ghazaryan, Areg, Yossi Paltiel, and Mikhail Lemeshko. “Analytic Model of
Chiral-Induced Spin Selectivity.” The Journal of Physical Chemistry C.
American Chemical Society, 2020. https://doi.org/10.1021/acs.jpcc.0c02584.
ieee: A. Ghazaryan, Y. Paltiel, and M. Lemeshko, “Analytic model of chiral-induced
spin selectivity,” The Journal of Physical Chemistry C, vol. 124, no. 21.
American Chemical Society, pp. 11716–11721, 2020.
ista: Ghazaryan A, Paltiel Y, Lemeshko M. 2020. Analytic model of chiral-induced
spin selectivity. The Journal of Physical Chemistry C. 124(21), 11716–11721.
mla: Ghazaryan, Areg, et al. “Analytic Model of Chiral-Induced Spin Selectivity.”
The Journal of Physical Chemistry C, vol. 124, no. 21, American Chemical
Society, 2020, pp. 11716–21, doi:10.1021/acs.jpcc.0c02584.
short: A. Ghazaryan, Y. Paltiel, M. Lemeshko, The Journal of Physical Chemistry
C 124 (2020) 11716–11721.
date_created: 2020-06-16T14:29:59Z
date_published: 2020-05-04T00:00:00Z
date_updated: 2023-09-05T12:07:15Z
day: '04'
ddc:
- '530'
department:
- _id: MiLe
doi: 10.1021/acs.jpcc.0c02584
ec_funded: 1
external_id:
isi:
- '000614616200006'
file:
- access_level: open_access
checksum: 25932bb1d0b0a955be0bea4d17facd49
content_type: application/pdf
creator: kschuh
date_created: 2020-10-20T14:39:47Z
date_updated: 2020-10-20T14:39:47Z
file_id: '8683'
file_name: 2020_PhysChemC_Ghazaryan.pdf
file_size: 1543429
relation: main_file
success: 1
file_date_updated: 2020-10-20T14:39:47Z
has_accepted_license: '1'
intvolume: ' 124'
isi: 1
issue: '21'
language:
- iso: eng
month: '05'
oa: 1
oa_version: Published Version
page: 11716-11721
project:
- _id: 260C2330-B435-11E9-9278-68D0E5697425
call_identifier: H2020
grant_number: '754411'
name: ISTplus - Postdoctoral Fellowships
- _id: 26031614-B435-11E9-9278-68D0E5697425
call_identifier: FWF
grant_number: P29902
name: Quantum rotations in the presence of a many-body environment
- _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 C
publication_identifier:
eissn:
- 1932-7455
issn:
- 1932-7447
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Analytic model of chiral-induced spin selectivity
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: 124
year: '2020'
...
---
_id: '7301'
abstract:
- lang: eng
text: Several problems arise at the O2 (positive) electrode in the Li-air battery,
including solvent/electrode decomposition and electrode passivation by insulating
Li2O2. Progress partially depends on exploring the basic electrochemistry of O2
reduction. Here we describe the effect of complexing-cations on the electrochemical
reduction of O2 in DMSO in the presence and absence of a Li salt. The solubility
of alkaline peroxides in DMSO is enhanced by the complexing-cations, consistent
with their strong interaction with reduced O2. The complexing-cations also increase
the rate of the 1-electron O2 reduction to O2•– by up to six-fold (k° = 2.4 ×10–3
to 1.5 × 10–2 cm s–1) whether or not Li+ ions are present. In the absence of Li+,
the complexing-cations also promote the reduction of O2•– to O22–. In the presence
of Li+ and complexing-cations, and despite the interaction of the reduced O2 with
the latter, SERS confirms that the product is still Li2O2.
article_processing_charge: No
article_type: original
author:
- first_name: Chunmei
full_name: Li, Chunmei
last_name: Li
- first_name: Olivier
full_name: Fontaine, Olivier
last_name: Fontaine
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
- first_name: Lee
full_name: Johnson, Lee
last_name: Johnson
- first_name: Sylvie
full_name: Grugeon, Sylvie
last_name: Grugeon
- first_name: Stéphane
full_name: Laruelle, Stéphane
last_name: Laruelle
- first_name: Peter G.
full_name: Bruce, Peter G.
last_name: Bruce
- first_name: Michel
full_name: Armand, Michel
last_name: Armand
citation:
ama: 'Li C, Fontaine O, Freunberger SA, et al. Aprotic Li–O2 battery: Influence
of complexing agents on oxygen reduction in an aprotic solvent. The Journal
of Physical Chemistry C. 2014;118(7):3393-3401. doi:10.1021/jp4093805'
apa: 'Li, C., Fontaine, O., Freunberger, S. A., Johnson, L., Grugeon, S., Laruelle,
S., … Armand, M. (2014). Aprotic Li–O2 battery: Influence of complexing agents
on oxygen reduction in an aprotic solvent. The Journal of Physical Chemistry
C. ACS. https://doi.org/10.1021/jp4093805'
chicago: 'Li, Chunmei, Olivier Fontaine, Stefan Alexander Freunberger, Lee Johnson,
Sylvie Grugeon, Stéphane Laruelle, Peter G. Bruce, and Michel Armand. “Aprotic
Li–O2 Battery: Influence of Complexing Agents on Oxygen Reduction in an Aprotic
Solvent.” The Journal of Physical Chemistry C. ACS, 2014. https://doi.org/10.1021/jp4093805.'
ieee: 'C. Li et al., “Aprotic Li–O2 battery: Influence of complexing agents
on oxygen reduction in an aprotic solvent,” The Journal of Physical Chemistry
C, vol. 118, no. 7. ACS, pp. 3393–3401, 2014.'
ista: 'Li C, Fontaine O, Freunberger SA, Johnson L, Grugeon S, Laruelle S, Bruce
PG, Armand M. 2014. Aprotic Li–O2 battery: Influence of complexing agents on oxygen
reduction in an aprotic solvent. The Journal of Physical Chemistry C. 118(7),
3393–3401.'
mla: 'Li, Chunmei, et al. “Aprotic Li–O2 Battery: Influence of Complexing Agents
on Oxygen Reduction in an Aprotic Solvent.” The Journal of Physical Chemistry
C, vol. 118, no. 7, ACS, 2014, pp. 3393–401, doi:10.1021/jp4093805.'
short: C. Li, O. Fontaine, S.A. Freunberger, L. Johnson, S. Grugeon, S. Laruelle,
P.G. Bruce, M. Armand, The Journal of Physical Chemistry C 118 (2014) 3393–3401.
date_created: 2020-01-15T12:17:28Z
date_published: 2014-01-29T00:00:00Z
date_updated: 2021-01-12T08:12:53Z
day: '29'
doi: 10.1021/jp4093805
extern: '1'
intvolume: ' 118'
issue: '7'
language:
- iso: eng
month: '01'
oa_version: None
page: 3393-3401
publication: The Journal of Physical Chemistry C
publication_identifier:
issn:
- 1932-7447
- 1932-7455
publication_status: published
publisher: ACS
quality_controlled: '1'
status: public
title: 'Aprotic Li–O2 battery: Influence of complexing agents on oxygen reduction
in an aprotic solvent'
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 118
year: '2014'
...
---
_id: '6370'
abstract:
- lang: eng
text: 'The molecular and supramolecular origins of the superior nonlinear optical
(NLO) properties observed in the organic phenolic triene material, OH1 (2-(3-(4-hydroxystyryl)-5,5-dimethylcyclohex-2-enylidene)malononitrile),
are presented. The molecular charge-transfer distribution is topographically mapped,
demonstrating that a uniformly delocalized passive electronic medium facilitates
the charge-transfer between the phenolic electron donor and the cyano electron
acceptors which lie at opposite ends of the molecule. Its ability to act as a
“push–pull” π-conjugated molecule is quantified, relative to similar materials,
by supporting empirical calculations; these include bond-length alternation and
harmonic-oscillator stabilization energy (HOSE) tests. Such tests, together with
frontier molecular orbital considerations, reveal that OH1 can exist readily in
its aromatic (neutral) or quinoidal (charge-separated) state, thereby overcoming
the “nonlinearity-thermal stability trade-off”. The HOSE calculation also reveals
a correlation between the quinoidal resonance contribution to the overall structure
of OH1 and the UV–vis absorption peak wavelength in the wider family of configurationally
locked polyene framework materials. Solid-state tensorial coefficients of the
molecular dipole, polarizability, and the first hyperpolarizability for OH1 are
derived from the first-, second-, and third-order electronic moments of the experimental
charge-density distribution. The overall solid-state molecular dipole moment is
compared with those from gas-phase calculations, revealing that crystal field
effects are very significant in OH1. The solid-state hyperpolarizability derived
from this charge-density study affords good agreement with gas-phase calculations
as well as optical measurements based on hyper-Rayleigh scattering (HRS) and electric-field-induced
second harmonic (EFISH) generation. This lends support to the further use of charge-density
studies to calculate solid-state hyperpolarizability coefficients in other organic
NLO materials. Finally, this charge-density study is also employed to provide
an advanced classification of hydrogen bonds in OH1, which requires more stringent
criteria than those from conventional structure analysis. As a result, only the
strongest OH···NC interaction is so classified as a true hydrogen bond. Indeed,
it is this electrostatic interaction that influences the molecular charge transfer:
the other four, weaker, nonbonded contacts nonetheless affect the crystal packing.
Overall, the establishment of these structure–property relationships lays a blueprint
for designing further, more NLO efficient, materials in this industrially leading
organic family of compounds.'
author:
- first_name: Tze-Chia
full_name: Lin, Tze-Chia
last_name: Lin
- first_name: Jacqueline M.
full_name: Cole, Jacqueline M.
last_name: Cole
- first_name: Andrew P
full_name: Higginbotham, Andrew P
id: 4AD6785A-F248-11E8-B48F-1D18A9856A87
last_name: Higginbotham
orcid: 0000-0003-2607-2363
- first_name: Alison J.
full_name: Edwards, Alison J.
last_name: Edwards
- first_name: Ross O.
full_name: Piltz, Ross O.
last_name: Piltz
- first_name: Javier
full_name: Pérez-Moreno, Javier
last_name: Pérez-Moreno
- first_name: Ji-Youn
full_name: Seo, Ji-Youn
last_name: Seo
- first_name: Seung-Chul
full_name: Lee, Seung-Chul
last_name: Lee
- first_name: Koen
full_name: Clays, Koen
last_name: Clays
- first_name: O-Pil
full_name: Kwon, O-Pil
last_name: Kwon
citation:
ama: 'Lin T-C, Cole JM, Higginbotham AP, et al. Molecular origins of the high-performance
nonlinear optical susceptibility in a phenolic polyene chromophore: Electron density
distributions, hydrogen bonding, and ab initio calculations. The Journal of
Physical Chemistry C. 2013;117(18):9416-9430. doi:10.1021/jp400648q'
apa: 'Lin, T.-C., Cole, J. M., Higginbotham, A. P., Edwards, A. J., Piltz, R. O.,
Pérez-Moreno, J., … Kwon, O.-P. (2013). Molecular origins of the high-performance
nonlinear optical susceptibility in a phenolic polyene chromophore: Electron density
distributions, hydrogen bonding, and ab initio calculations. The Journal of
Physical Chemistry C. American Chemical Society (ACS). https://doi.org/10.1021/jp400648q'
chicago: 'Lin, Tze-Chia, Jacqueline M. Cole, Andrew P Higginbotham, Alison J. Edwards,
Ross O. Piltz, Javier Pérez-Moreno, Ji-Youn Seo, Seung-Chul Lee, Koen Clays, and
O-Pil Kwon. “Molecular Origins of the High-Performance Nonlinear Optical Susceptibility
in a Phenolic Polyene Chromophore: Electron Density Distributions, Hydrogen Bonding,
and Ab Initio Calculations.” The Journal of Physical Chemistry C. American
Chemical Society (ACS), 2013. https://doi.org/10.1021/jp400648q.'
ieee: 'T.-C. Lin et al., “Molecular origins of the high-performance nonlinear
optical susceptibility in a phenolic polyene chromophore: Electron density distributions,
hydrogen bonding, and ab initio calculations,” The Journal of Physical Chemistry
C, vol. 117, no. 18. American Chemical Society (ACS), pp. 9416–9430, 2013.'
ista: 'Lin T-C, Cole JM, Higginbotham AP, Edwards AJ, Piltz RO, Pérez-Moreno J,
Seo J-Y, Lee S-C, Clays K, Kwon O-P. 2013. Molecular origins of the high-performance
nonlinear optical susceptibility in a phenolic polyene chromophore: Electron density
distributions, hydrogen bonding, and ab initio calculations. The Journal of Physical
Chemistry C. 117(18), 9416–9430.'
mla: 'Lin, Tze-Chia, et al. “Molecular Origins of the High-Performance Nonlinear
Optical Susceptibility in a Phenolic Polyene Chromophore: Electron Density Distributions,
Hydrogen Bonding, and Ab Initio Calculations.” The Journal of Physical Chemistry
C, vol. 117, no. 18, American Chemical Society (ACS), 2013, pp. 9416–30, doi:10.1021/jp400648q.'
short: T.-C. Lin, J.M. Cole, A.P. Higginbotham, A.J. Edwards, R.O. Piltz, J. Pérez-Moreno,
J.-Y. Seo, S.-C. Lee, K. Clays, O.-P. Kwon, The Journal of Physical Chemistry
C 117 (2013) 9416–9430.
date_created: 2019-05-03T09:40:31Z
date_published: 2013-05-09T00:00:00Z
date_updated: 2021-01-12T08:07:17Z
day: '09'
doi: 10.1021/jp400648q
extern: '1'
intvolume: ' 117'
issue: '18'
language:
- iso: eng
month: '05'
oa_version: None
page: 9416-9430
publication: The Journal of Physical Chemistry C
publication_identifier:
issn:
- 1932-7447
- 1932-7455
publication_status: published
publisher: American Chemical Society (ACS)
quality_controlled: '1'
status: public
title: 'Molecular origins of the high-performance nonlinear optical susceptibility
in a phenolic polyene chromophore: Electron density distributions, hydrogen bonding,
and ab initio calculations'
type: journal_article
user_id: 3E5EF7F0-F248-11E8-B48F-1D18A9856A87
volume: 117
year: '2013'
...