Coupled Electronic and Nuclear Motions during Azobenzene Photoisomerization Monitored by Ultrafast Electron Diffraction

Rouxel, Jérémy R.; Keefer, Daniel; Aleotti, Flavia; Nenov, Artur; Garavelli, Marco; Mukamel, Shaul

doi:10.1021/acs.jctc.1c00792

Title: Coupled Electronic and Nuclear Motions during Azobenzene Photoisomerization Monitored by Ultrafast Electron Diffraction

Journal Article · 24 January 2022 · Journal of Chemical Theory and Computation

DOI: https://doi.org/10.1021/acs.jctc.1c00792 · OSTI ID:1922848

^[1];

^[2]; Aleotti, Flavia ^[3];

^[3];

^[2]

Univ. of California, Irvine, CA (United States); Univ. Lyon, Saint-Etienne (France); Regents, University of California, Irivne
Univ. of California, Irvine, CA (United States)
Univ. degli Studi di Bologna (Italy)

Ultrafast electron diffraction is a powerful technique that can resolve molecular structures with femtosecond and angstrom resolutions. We demonstrate theoretically how it can be used to monitor conical intersection dynamics in molecules. Specific contributions to the signal are identified which vanish in the absence of vibronic coherence and offer a direct window into conical intersection paths. A special focus is on hybrid scattering from nuclei and electrons, a process that is unique to electron (rather than X-ray) diffraction and monitors the strongly coupled nuclear and electronic motions in the vicinity of conical intersections. Furthermore, an application is made to the cis to trans isomerization of azobenzene, computed with exact quantum dynamics wavepacket propagation in a reactive two-dimensional nuclear space.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Univ. of California, Irvine, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: SC0019484

OSTI ID:: 1922848

Journal Information:: Journal of Chemical Theory and Computation, Journal Name: Journal of Chemical Theory and Computation Journal Issue: 2 Vol. 18; ISSN 1549-9618

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (35)

Enlightening Materials with Photoswitches Goulet‐Hanssens, Alexis; Eisenreich, Fabian; Hecht, Stefan Advanced Materials, Vol. 32, Issue 20 https://doi.org/10.1002/adma.201905966	journal	January 2020
Ultrafast Electron Diffraction (UED): A New Development for the 4D Determination of Transient Molecular Structures Srinivasan, Ramesh; Lobastov, Vladimir A.; Ruan, Chong-Yu Helvetica Chimica Acta, Vol. 86, Issue 6 https://doi.org/10.1002/hlca.200390147	journal	June 2003
Molcas 8: New capabilities for multiconfigurational quantum chemical calculations across the periodic table : Molcas 8 Aquilante, Francesco; Autschbach, Jochen; Carlson, Rebecca K. Journal of Computational Chemistry, Vol. 37, Issue 5 https://doi.org/10.1002/jcc.24221	journal	November 2015
Density matrix averaged atomic natural orbital (ANO) basis sets for correlated molecular wave functions: I. First row atoms Widmark, Per-Olof; Malmqvist, Per-�ke; Roos, Bj�rn O. Theoretica Chimica Acta, Vol. 77, Issue 5 https://doi.org/10.1007/BF01120130	journal	January 1990
Femtosecond photoisomerization of cis-azobenzene Nägele, T.; Hoche, R.; Zinth, W. Chemical Physics Letters, Vol. 272, Issue 5-6 https://doi.org/10.1016/S0009-2614(97)00531-9	journal	July 1997
Capturing Chemistry in Action with Electrons: Realization of Atomically Resolved Reaction Dynamics Ischenko, Anatoly A.; Weber, Peter M.; Miller, R. J. Dwayne Chemical Reviews, Vol. 117, Issue 16 https://doi.org/10.1021/acs.chemrev.6b00770	journal	May 2017
Ab Initio Computation of Rotationally-Averaged Pump–Probe X-ray and Electron Diffraction Signals Parrish, Robert M.; Martínez, Todd J. Journal of Chemical Theory and Computation, Vol. 15, Issue 3 https://doi.org/10.1021/acs.jctc.8b01051	journal	January 2019
Multidimensional Potential Energy Surfaces Resolved at the RASPT2 Level for Accurate Photoinduced Isomerization Dynamics of Azobenzene Aleotti, Flavia; Soprani, Lorenzo; Nenov, Artur Journal of Chemical Theory and Computation, Vol. 15, Issue 12 https://doi.org/10.1021/acs.jctc.9b00561	journal	October 2019
A Red-Shifted, Fast-Relaxing Azobenzene Photoswitch for Visible Light Control of an Ionotropic Glutamate Receptor Kienzler, Michael A.; Reiner, Andreas; Trautman, Eric Journal of the American Chemical Society, Vol. 135, Issue 47 https://doi.org/10.1021/ja408104w	journal	November 2013
Photoisomerization Dynamics and Pathways of trans - and cis -Azobenzene in Solution from Broadband Femtosecond Spectroscopies and Calculations Quick, M.; Dobryakov, A. L.; Gerecke, M. The Journal of Physical Chemistry B, Vol. 118, Issue 29 https://doi.org/10.1021/jp504999f	journal	July 2014
Three-dimensional view of ultrafast dynamics in photoexcited bacteriorhodopsin Nass Kovacs, Gabriela; Colletier, Jacques-Philippe; Grünbein, Marie Luise Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-10758-0	journal	July 2019
Observation of the molecular response to light upon photoexcitation Yong, Haiwang; Zotev, Nikola; Ruddock, Jennifer M. Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15680-4	journal	May 2020
The photochemical ring-opening of 1,3-cyclohexadiene imaged by ultrafast electron diffraction Wolf, T. J. A.; Sanchez, D. M.; Yang, J. Nature Chemistry, Vol. 11, Issue 6 https://doi.org/10.1038/s41557-019-0252-7	journal	April 2019
Towards jitter-free ultrafast electron diffraction technology Kim, Hyun Woo; Vinokurov, Nikolay A.; Baek, In Hyung Nature Photonics, Vol. 14, Issue 4 https://doi.org/10.1038/s41566-019-0566-4	journal	December 2019
Using azobenzene photocontrol to set proteins in motion Bozovic, Olga; Jankovic, Brankica; Hamm, Peter Nature Reviews Chemistry https://doi.org/10.1038/s41570-021-00338-6	journal	December 2021
Ultrafast electron optics: Propagation dynamics of femtosecond electron packets Siwick, Bradley J.; Dwyer, Jason R.; Jordan, Robert E. Journal of Applied Physics, Vol. 92, Issue 3 https://doi.org/10.1063/1.1487437	journal	August 2002
Molecular dynamics and spectra. I. Diatomic rotation and vibration Berens, Peter H.; Wilson, Kent R. The Journal of Chemical Physics, Vol. 74, Issue 9 https://doi.org/10.1063/1.441739	journal	May 1981
An accurate and efficient scheme for propagating the time dependent Schrödinger equation Tal‐Ezer, H.; Kosloff, R. The Journal of Chemical Physics, Vol. 81, Issue 9 https://doi.org/10.1063/1.448136	journal	November 1984
Design of specially adapted reactive coordinates to economically compute potential and kinetic energy operators including geometry relaxation Thallmair, Sebastian; Roos, Matthias K.; de Vivie-Riedle, Regina The Journal of Chemical Physics, Vol. 144, Issue 23 https://doi.org/10.1063/1.4953667	journal	June 2016
Monitoring nonadiabatic avoided crossing dynamics in molecules by ultrafast X-ray diffraction Kowalewski, Markus; Bennett, Kochise; Mukamel, Shaul Structural Dynamics, Vol. 4, Issue 5 https://doi.org/10.1063/1.4984241	journal	September 2017
Ultrafast x-ray and electron scattering of free molecules: A comparative evaluation Ma, Lingyu; Yong, Haiwang; Geiser, Joseph D. Structural Dynamics, Vol. 7, Issue 3 https://doi.org/10.1063/4.0000010	journal	May 2020
Signatures of electronic and nuclear coherences in ultrafast molecular x-ray and electron diffraction Rouxel, Jérémy R.; Keefer, Daniel; Mukamel, Shaul Structural Dynamics, Vol. 8, Issue 1 https://doi.org/10.1063/4.0000043	journal	January 2021
Determining the radial distribution function of water using electron scattering: A key to solution phase chemistry de Kock, M. B.; Azim, S.; Kassier, G. H. The Journal of Chemical Physics, Vol. 153, Issue 19 https://doi.org/10.1063/5.0024127	journal	November 2020
Monitoring molecular nonadiabatic dynamics with femtosecond X-ray diffraction Bennett, Kochise; Kowalewski, Markus; Rouxel, Jérémy R. Proceedings of the National Academy of Sciences, Vol. 115, Issue 26 https://doi.org/10.1073/pnas.1805335115	journal	June 2018
Imaging conical intersection dynamics during azobenzene photoisomerization by ultrafast X-ray diffraction Keefer, Daniel; Aleotti, Flavia; Rouxel, Jérémy R. Proceedings of the National Academy of Sciences, Vol. 118, Issue 3 https://doi.org/10.1073/pnas.2022037118	journal	January 2021
Femtosecond electron diffraction: heralding the era of atomically resolved dynamics Sciaini, Germán; Miller, R. J. Dwayne Reports on Progress in Physics, Vol. 74, Issue 9 https://doi.org/10.1088/0034-4885/74/9/096101	journal	August 2011
Coherent and Incoherent Electron-Phonon Coupling in Graphite Observed with Radio-Frequency Compressed Ultrafast Electron Diffraction Chatelain, Robert P.; Morrison, Vance R.; Klarenaar, Bart L. M. Physical Review Letters, Vol. 113, Issue 23 https://doi.org/10.1103/PhysRevLett.113.235502	journal	December 2014
X-Ray Sum Frequency Diffraction for Direct Imaging of Ultrafast Electron Dynamics Rouxel, Jérémy R.; Kowalewski, Markus; Bennett, Kochise Physical Review Letters, Vol. 120, Issue 24 https://doi.org/10.1103/PhysRevLett.120.243902	journal	June 2018
Spectroscopic and Structural Probing of Excited-State Molecular Dynamics with Time-Resolved Photoelectron Spectroscopy and Ultrafast Electron Diffraction Liu, Yusong; Horton, Spencer L.; Yang, Jie Physical Review X, Vol. 10, Issue 2 https://doi.org/10.1103/PhysRevX.10.021016	journal	April 2020
On the sensitivity of electron and X-ray scattering factors to valence charge distributions Zheng, Jin-Cheng; Zhu, Yimei; Wu, Lijun Journal of Applied Crystallography, Vol. 38, Issue 4 https://doi.org/10.1107/S0021889805016109	journal	July 2005
Imaging CF ₃ I conical intersection and photodissociation dynamics with ultrafast electron diffraction Yang, Jie; Zhu, Xiaolei; Wolf, Thomas J. A. Science, Vol. 361, Issue 6397 https://doi.org/10.1126/science.aat0049	journal	July 2018
Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction Yang, Jie; Zhu, Xiaolei; F. Nunes, J. Pedro Science, Vol. 368, Issue 6493 https://doi.org/10.1126/science.abb2235	journal	May 2020
Mapping Atomic Motions with Ultrabright Electrons: The Chemists' Gedanken Experiment Enters the Lab Frame Miller, R. J. Dwayne Annual Review of Physical Chemistry, Vol. 65, Issue 1 https://doi.org/10.1146/annurev-physchem-040412-110117	journal	April 2014
4d Ultrafast Electron Diffraction, Crystallography, and Microscopy Zewail, Ahmed H. Annual Review of Physical Chemistry, Vol. 57, Issue 1 https://doi.org/10.1146/annurev.physchem.57.032905.104748	journal	May 2006
Femtosecond/Picosecond Time-Resolved Spectroscopy of trans - Azobenzene: Isomerization Mechanism Following S ₂ (ππ*) ← S ₀ Photoexcitation Fujino, Tatsuya; Arzhantsev, Sergei Yu.; Tahara, Tahei Bulletin of the Chemical Society of Japan, Vol. 75, Issue 5 https://doi.org/10.1246/bcsj.75.1031	journal	May 2002

Similar Records

Imaging conical intersection dynamics during azobenzene photoisomerization by ultrafast X-ray diffraction

Journal Article · 2021 · Proceedings of the National Academy of Sciences of the United States of America · OSTI ID:1759080

Keefer, Daniel; Aleotti, Flavia; Rouxel, Jérémy R.; +5 more

Nonadiabatic ab initio molecular dynamics of photoisomerization in bridged azobenzene

Journal Article · 2012 · Journal of Chemical Physics · OSTI ID:22099119

Aihua, Gao; Bin, Li; Peiyu, Zhang; +1 more

Nonadiabatic simulation study of photoisomerization of azobenzene: Detailed mechanism and load-resisting capacity

Journal Article · 2008 · Journal of Chemical Physics · OSTI ID:21254780

Junfeng, Shao; Yibo, Lei; Zhenyi, Wen; +2 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Title: Coupled Electronic and Nuclear Motions during Azobenzene Photoisomerization Monitored by Ultrafast Electron Diffraction

Citation Formats

References (35)

Similar Records

Related Subjects