---
OA_place: publisher
OA_type: hybrid
_id: '9666'
abstract:
- lang: eng
text: Predicting phase stabilities of crystal polymorphs is central to computational
materials science and chemistry. Such predictions are challenging because they
first require searching for potential energy minima and then performing arduous
free-energy calculations to account for entropic effects at finite temperatures.
Here, we develop a framework that facilitates such predictions by exploiting all
the information obtained from random searches of crystal structures. This framework
combines automated clustering, classification and visualisation of crystal structures
with machine-learning estimation of their enthalpy and entropy. We demonstrate
the framework on the technologically important system of TiO2, which has many
polymorphs, without relying on prior knowledge of known phases. We find a number
of new phases and predict the phase diagram and metastabilities of crystal polymorphs
at 1600 K, benchmarking the results against full free-energy calculations.
article_processing_charge: No
article_type: original
arxiv: 1
author:
- first_name: Aleks
full_name: Reinhardt, Aleks
last_name: Reinhardt
- first_name: Chris J.
full_name: Pickard, Chris J.
last_name: Pickard
- first_name: Bingqing
full_name: Cheng, Bingqing
id: cbe3cda4-d82c-11eb-8dc7-8ff94289fcc9
last_name: Cheng
orcid: 0000-0002-3584-9632
citation:
ama: Reinhardt A, Pickard CJ, Cheng B. Predicting the phase diagram of titanium
dioxide with random search and pattern recognition. Physical Chemistry Chemical
Physics. 2020;22(22):12697-12705. doi:10.1039/d0cp02513e
apa: Reinhardt, A., Pickard, C. J., & Cheng, B. (2020). Predicting the phase
diagram of titanium dioxide with random search and pattern recognition. Physical
Chemistry Chemical Physics. Royal Society of Chemistry. https://doi.org/10.1039/d0cp02513e
chicago: Reinhardt, Aleks, Chris J. Pickard, and Bingqing Cheng. “Predicting the
Phase Diagram of Titanium Dioxide with Random Search and Pattern Recognition.”
Physical Chemistry Chemical Physics. Royal Society of Chemistry, 2020.
https://doi.org/10.1039/d0cp02513e.
ieee: A. Reinhardt, C. J. Pickard, and B. Cheng, “Predicting the phase diagram of
titanium dioxide with random search and pattern recognition,” Physical Chemistry
Chemical Physics, vol. 22, no. 22. Royal Society of Chemistry, pp. 12697–12705,
2020.
ista: Reinhardt A, Pickard CJ, Cheng B. 2020. Predicting the phase diagram of titanium
dioxide with random search and pattern recognition. Physical Chemistry Chemical
Physics. 22(22), 12697–12705.
mla: Reinhardt, Aleks, et al. “Predicting the Phase Diagram of Titanium Dioxide
with Random Search and Pattern Recognition.” Physical Chemistry Chemical Physics,
vol. 22, no. 22, Royal Society of Chemistry, 2020, pp. 12697–705, doi:10.1039/d0cp02513e.
short: A. Reinhardt, C.J. Pickard, B. Cheng, Physical Chemistry Chemical Physics
22 (2020) 12697–12705.
date_created: 2021-07-15T12:37:27Z
date_published: 2020-06-14T00:00:00Z
date_updated: 2024-10-16T12:29:54Z
day: '14'
ddc:
- '530'
doi: 10.1039/d0cp02513e
extern: '1'
external_id:
arxiv:
- '1909.08934'
pmid:
- '32459228'
file:
- access_level: open_access
checksum: 0a6872972b1b2e60f9095d39b01753fa
content_type: application/pdf
creator: asandaue
date_created: 2021-07-15T12:43:51Z
date_updated: 2021-07-15T12:43:51Z
file_id: '9667'
file_name: 202_PhysicalChemistryChemicalPhysics_Reinhardt.pdf
file_size: 3151206
relation: main_file
success: 1
file_date_updated: 2021-07-15T12:43:51Z
has_accepted_license: '1'
intvolume: ' 22'
issue: '22'
language:
- iso: eng
license: https://creativecommons.org/licenses/by/3.0/
month: '06'
oa: 1
oa_version: Published Version
page: 12697-12705
pmid: 1
publication: Physical Chemistry Chemical Physics
publication_identifier:
eissn:
- 1463-9084
issn:
- 1463-9076
publication_status: published
publisher: Royal Society of Chemistry
quality_controlled: '1'
scopus_import: '1'
status: public
title: Predicting the phase diagram of titanium dioxide with random search and pattern
recognition
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/3.0/legalcode
name: Creative Commons Attribution 3.0 Unported (CC BY 3.0)
short: CC BY (3.0)
type: journal_article
user_id: 0043cee0-e5fc-11ee-9736-f83bc23afbf0
volume: 22
year: '2020'
...
---
_id: '9668'
abstract:
- lang: eng
text: Estimating the homogeneous ice nucleation rate from undercooled liquid water
is crucial for understanding many important physical phenomena and technological
applications, and challenging for both experiments and theory. From a theoretical
point of view, difficulties arise due to the long time scales required, as well
as the numerous nucleation pathways involved to form ice nuclei with different
stacking disorders. We computed the homogeneous ice nucleation rate at a physically
relevant undercooling for a single-site water model, taking into account the diffuse
nature of ice–water interfaces, stacking disorders in ice nuclei, and the addition
rate of particles to the critical nucleus. We disentangled and investigated the
relative importance of all the terms, including interfacial free energy, entropic
contributions and the kinetic prefactor, that contribute to the overall nucleation
rate. Breaking down the problem into pieces not only provides physical insights
into ice nucleation, but also sheds light on the long-standing discrepancy between
different theoretical predictions, as well as between theoretical and experimental
determinations of the nucleation rate. Moreover, we pinpoint the main shortcomings
and suggest strategies to systematically improve the existing simulation methods.
article_processing_charge: No
article_type: original
arxiv: 1
author:
- first_name: Bingqing
full_name: Cheng, Bingqing
id: cbe3cda4-d82c-11eb-8dc7-8ff94289fcc9
last_name: Cheng
orcid: 0000-0002-3584-9632
- first_name: Christoph
full_name: Dellago, Christoph
last_name: Dellago
- first_name: Michele
full_name: Ceriotti, Michele
last_name: Ceriotti
citation:
ama: 'Cheng B, Dellago C, Ceriotti M. Theoretical prediction of the homogeneous
ice nucleation rate: Disentangling thermodynamics and kinetics. Physical Chemistry
Chemical Physics. 2018;20(45):28732-28740. doi:10.1039/c8cp04561e'
apa: 'Cheng, B., Dellago, C., & Ceriotti, M. (2018). Theoretical prediction
of the homogeneous ice nucleation rate: Disentangling thermodynamics and kinetics.
Physical Chemistry Chemical Physics. Royal Society of Chemistry. https://doi.org/10.1039/c8cp04561e'
chicago: 'Cheng, Bingqing, Christoph Dellago, and Michele Ceriotti. “Theoretical
Prediction of the Homogeneous Ice Nucleation Rate: Disentangling Thermodynamics
and Kinetics.” Physical Chemistry Chemical Physics. Royal Society of Chemistry,
2018. https://doi.org/10.1039/c8cp04561e.'
ieee: 'B. Cheng, C. Dellago, and M. Ceriotti, “Theoretical prediction of the homogeneous
ice nucleation rate: Disentangling thermodynamics and kinetics,” Physical Chemistry
Chemical Physics, vol. 20, no. 45. Royal Society of Chemistry, pp. 28732–28740,
2018.'
ista: 'Cheng B, Dellago C, Ceriotti M. 2018. Theoretical prediction of the homogeneous
ice nucleation rate: Disentangling thermodynamics and kinetics. Physical Chemistry
Chemical Physics. 20(45), 28732–28740.'
mla: 'Cheng, Bingqing, et al. “Theoretical Prediction of the Homogeneous Ice Nucleation
Rate: Disentangling Thermodynamics and Kinetics.” Physical Chemistry Chemical
Physics, vol. 20, no. 45, Royal Society of Chemistry, 2018, pp. 28732–40,
doi:10.1039/c8cp04561e.'
short: B. Cheng, C. Dellago, M. Ceriotti, Physical Chemistry Chemical Physics 20
(2018) 28732–28740.
date_created: 2021-07-15T12:51:44Z
date_published: 2018-12-07T00:00:00Z
date_updated: 2021-08-09T12:36:47Z
day: '07'
doi: 10.1039/c8cp04561e
extern: '1'
external_id:
arxiv:
- '1807.05551'
pmid:
- '30412211'
intvolume: ' 20'
issue: '45'
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://arxiv.org/abs/1807.05551
month: '12'
oa: 1
oa_version: Preprint
page: 28732-28740
pmid: 1
publication: Physical Chemistry Chemical Physics
publication_identifier:
eissn:
- 1463-9084
issn:
- 1463-9076
publication_status: published
publisher: Royal Society of Chemistry
quality_controlled: '1'
scopus_import: '1'
status: public
title: 'Theoretical prediction of the homogeneous ice nucleation rate: Disentangling
thermodynamics and kinetics'
type: journal_article
user_id: 6785fbc1-c503-11eb-8a32-93094b40e1cf
volume: 20
year: '2018'
...
---
OA_place: publisher
OA_type: hybrid
_id: '17964'
abstract:
- lang: eng
text: Charge transfer rates at metal/organic interfaces affect the efficiencies
of devices for organic based electronics and photovoltaics. A quantitative study
of electron transfer rates, which take place on the femtosecond timescale, is
often difficult, especially since in most systems the molecular adsorption geometry
is unknown. Here, we use X-ray resonant photoemission spectroscopy to measure
ultrafast charge transfer rates across pyridine/Au(111) interfaces while also
controlling the molecular orientation on the metal. We demonstrate that a bi-directional
charge transfer across the molecule/metal interface is enabled upon creation of
a core-exciton on the molecule with a rate that has a strong dependence on the
molecular adsorption angle. Through density functional theory calculations, we
show that the alignment of molecular levels relative to the metal Fermi level
is dramatically altered when a core-hole is created on the molecule, allowing
the lowest unoccupied molecular orbital to fall partially below the metal Fermi
level. We also calculate charge transfer rates as a function of molecular adsorption
geometry and find a trend that agrees with the experiment. These findings thus
give insight into the charge transfer dynamics of a photo-excited molecule on
a metal surface.
article_processing_charge: Yes (in subscription journal)
article_type: original
author:
- first_name: Dean
full_name: Cvetko, Dean
last_name: Cvetko
- first_name: Guido
full_name: Fratesi, Guido
last_name: Fratesi
- first_name: Gregor
full_name: Kladnik, Gregor
last_name: Kladnik
- first_name: Albano
full_name: Cossaro, Albano
last_name: Cossaro
- first_name: Gian Paolo
full_name: Brivio, Gian Paolo
last_name: Brivio
- first_name: Latha
full_name: Venkataraman, Latha
id: 9ebb78a5-cc0d-11ee-8322-fae086a32caf
last_name: Venkataraman
orcid: 0000-0002-6957-6089
- first_name: Alberto
full_name: Morgante, Alberto
last_name: Morgante
citation:
ama: Cvetko D, Fratesi G, Kladnik G, et al. Ultrafast electron injection into photo-excited
organic molecules. Physical Chemistry Chemical Physics. 2016;18(32):22140-22145.
doi:10.1039/c6cp04099c
apa: Cvetko, D., Fratesi, G., Kladnik, G., Cossaro, A., Brivio, G. P., Venkataraman,
L., & Morgante, A. (2016). Ultrafast electron injection into photo-excited
organic molecules. Physical Chemistry Chemical Physics. Royal Society of
Chemistry. https://doi.org/10.1039/c6cp04099c
chicago: Cvetko, Dean, Guido Fratesi, Gregor Kladnik, Albano Cossaro, Gian Paolo
Brivio, Latha Venkataraman, and Alberto Morgante. “Ultrafast Electron Injection
into Photo-Excited Organic Molecules.” Physical Chemistry Chemical Physics.
Royal Society of Chemistry, 2016. https://doi.org/10.1039/c6cp04099c.
ieee: D. Cvetko et al., “Ultrafast electron injection into photo-excited
organic molecules,” Physical Chemistry Chemical Physics, vol. 18, no. 32.
Royal Society of Chemistry, pp. 22140–22145, 2016.
ista: Cvetko D, Fratesi G, Kladnik G, Cossaro A, Brivio GP, Venkataraman L, Morgante
A. 2016. Ultrafast electron injection into photo-excited organic molecules. Physical
Chemistry Chemical Physics. 18(32), 22140–22145.
mla: Cvetko, Dean, et al. “Ultrafast Electron Injection into Photo-Excited Organic
Molecules.” Physical Chemistry Chemical Physics, vol. 18, no. 32, Royal
Society of Chemistry, 2016, pp. 22140–45, doi:10.1039/c6cp04099c.
short: D. Cvetko, G. Fratesi, G. Kladnik, A. Cossaro, G.P. Brivio, L. Venkataraman,
A. Morgante, Physical Chemistry Chemical Physics 18 (2016) 22140–22145.
date_created: 2024-09-09T09:39:29Z
date_published: 2016-07-14T00:00:00Z
date_updated: 2024-12-18T10:17:35Z
day: '14'
doi: 10.1039/c6cp04099c
extern: '1'
external_id:
pmid:
- '27444572'
intvolume: ' 18'
issue: '32'
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.1039/C6CP04099C
month: '07'
oa: 1
oa_version: Published Version
page: 22140-22145
pmid: 1
publication: Physical Chemistry Chemical Physics
publication_identifier:
eissn:
- 1463-9084
issn:
- 1463-9076
publication_status: published
publisher: Royal Society of Chemistry
quality_controlled: '1'
scopus_import: '1'
status: public
title: Ultrafast electron injection into photo-excited organic molecules
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 18
year: '2016'
...
---
OA_type: closed access
_id: '18004'
abstract:
- lang: eng
text: We characterize electron transport across Au–molecule–Au junctions of heterogeneous
carboxyl and methyl sulfide terminated saturated and conjugated molecules. Low-bias
conductance measurements are performed using the scanning tunneling microscopy
based break-junction technique in the presence of solvents and at room temperature.
For a series of alkanes with 1–4 carbon atoms in the hydrocarbon chain, our results
show an exponential decrease in conductance with increasing molecule length characterized
by a decay constant of 0.9 ± 0.1 per methylene group. Control measurements in
pH 11 solutions and with COOMe terminations suggest that the carboxylic acid group
binds through the formation of a COO−–Au bond. Simultaneous measurements of conductance
and force across these junctions yield a rupture force of 0.6 ± 0.1 nN, comparable
to that required to rupture a Au–SMe bond. By establishing reliable, in situ junction
formation, these experiments provide a new approach to probe electronic properties
of carboxyl groups at the single molecule level.
article_number: '13841'
article_processing_charge: No
article_type: original
author:
- first_name: Seokhoon
full_name: Ahn, Seokhoon
last_name: Ahn
- first_name: Sriharsha V.
full_name: Aradhya, Sriharsha V.
last_name: Aradhya
- first_name: Rebekka S.
full_name: Klausen, Rebekka S.
last_name: Klausen
- first_name: Brian
full_name: Capozzi, Brian
last_name: Capozzi
- first_name: Xavier
full_name: Roy, Xavier
last_name: Roy
- first_name: Michael L.
full_name: Steigerwald, Michael L.
last_name: Steigerwald
- first_name: Colin
full_name: Nuckolls, Colin
last_name: Nuckolls
- first_name: Latha
full_name: Venkataraman, Latha
id: 9ebb78a5-cc0d-11ee-8322-fae086a32caf
last_name: Venkataraman
orcid: 0000-0002-6957-6089
citation:
ama: Ahn S, Aradhya SV, Klausen RS, et al. Electronic transport and mechanical stability
of carboxyl linked single-molecule junctions. Physical Chemistry Chemical Physics.
2012;14(40). doi:10.1039/c2cp41578j
apa: Ahn, S., Aradhya, S. V., Klausen, R. S., Capozzi, B., Roy, X., Steigerwald,
M. L., … Venkataraman, L. (2012). Electronic transport and mechanical stability
of carboxyl linked single-molecule junctions. Physical Chemistry Chemical Physics.
Royal Society of Chemistry. https://doi.org/10.1039/c2cp41578j
chicago: Ahn, Seokhoon, Sriharsha V. Aradhya, Rebekka S. Klausen, Brian Capozzi,
Xavier Roy, Michael L. Steigerwald, Colin Nuckolls, and Latha Venkataraman. “Electronic
Transport and Mechanical Stability of Carboxyl Linked Single-Molecule Junctions.”
Physical Chemistry Chemical Physics. Royal Society of Chemistry, 2012.
https://doi.org/10.1039/c2cp41578j.
ieee: S. Ahn et al., “Electronic transport and mechanical stability of carboxyl
linked single-molecule junctions,” Physical Chemistry Chemical Physics,
vol. 14, no. 40. Royal Society of Chemistry, 2012.
ista: Ahn S, Aradhya SV, Klausen RS, Capozzi B, Roy X, Steigerwald ML, Nuckolls
C, Venkataraman L. 2012. Electronic transport and mechanical stability of carboxyl
linked single-molecule junctions. Physical Chemistry Chemical Physics. 14(40),
13841.
mla: Ahn, Seokhoon, et al. “Electronic Transport and Mechanical Stability of Carboxyl
Linked Single-Molecule Junctions.” Physical Chemistry Chemical Physics,
vol. 14, no. 40, 13841, Royal Society of Chemistry, 2012, doi:10.1039/c2cp41578j.
short: S. Ahn, S.V. Aradhya, R.S. Klausen, B. Capozzi, X. Roy, M.L. Steigerwald,
C. Nuckolls, L. Venkataraman, Physical Chemistry Chemical Physics 14 (2012).
date_created: 2024-09-09T12:00:50Z
date_published: 2012-07-09T00:00:00Z
date_updated: 2025-01-03T09:01:38Z
day: '09'
doi: 10.1039/c2cp41578j
extern: '1'
external_id:
pmid:
- '22850823'
intvolume: ' 14'
issue: '40'
language:
- iso: eng
month: '07'
oa_version: None
pmid: 1
publication: Physical Chemistry Chemical Physics
publication_identifier:
eissn:
- 1463-9084
issn:
- 1463-9076
publication_status: published
publisher: Royal Society of Chemistry
quality_controlled: '1'
scopus_import: '1'
status: public
title: Electronic transport and mechanical stability of carboxyl linked single-molecule
junctions
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 14
year: '2012'
...