X-ray induced Coulomb explosion imaging of transient excited-state structural rearrangements in CS2

被引：7

作者：

Unwin, James ^{[1
]}

Allum, Felix ^{[1
,2
,3
]}

Britton, Mathew ^{[2
,3
]}

Gabalski, Ian ^{[3
,4
]}

Bromberger, Hubertus ^{[5
]}

Brouard, Mark ^{[1
]}

Bucksbaum, Philip H. ^{[3
,4
,6
]}

Driver, Taran ^{[2
,3
]}

Ekanayake, Nagitha ^{[5
]}

Garg, Diksha ^{[5
]}

Gougoula, Eva ^{[5
]}

Heathcote, David ^{[1
]}

Howard, Andrew J. ^{[3
,4
]}

Hockett, Paul ^{[7
]}

Holland, David M. P. ^{[8
]}

Kumar, Sonu ^{[5
,9
]}

Lam, Chow-shing ^{[1
]}

Lee, Jason W. L. ^{[5
]}

Mcmanus, Joseph ^{[1
]}

Mikosch, Jochen ^{[10
]}

Milesevic, Dennis ^{[1
]}

Minns, Russell S. ^{[11
]}

Papadopoulou, Christina C. ^{[5
]}

Passow, Christopher ^{[5
]}

Razmus, Weronika O. ^{[11
]}

Roeder, Anja ^{[12
]}

Rouzee, Arnaud ^{[12
]}

Schuurman, Michael ^{[7
,13
]}

Simao, Alcides ^{[14
]}

Stolow, Albert ^{[7
,13
,15
,16
]}

Tul-Noor, Atia ^{[5
]}

Vallance, Claire ^{[1
]}

Walmsley, Tiffany ^{[1
]}

Rolles, Daniel ^{[17
]}

Erk, Benjamin ^{[5
]}

Burt, Michael ^{[1
]}

Forbes, Ruaridh ^{[2
]}

机构：

[1] Univ Oxford, Dept Chem, Chem Res Lab, Oxford OX1 3TA, England

[2] SLAC Natl Accelerator Lab, Linac Coherent Light Source, Menlo Pk, CA 94025 USA

[3] Stanford PULSE Inst, SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA

[4] Stanford Univ, Dept Appl Phys, Stanford, CA 94305 USA

[5] Deutsch Elektronen Synchrotron DESY, Notkestr 85, D-22607 Hamburg, Germany

[6] Stanford Univ, Dept Phys, Stanford, CA 94305 USA

[7] Natl Res Council Canada, Ottawa, ON K1A 0R6, Canada

[8] Daresbury Lab, Warrington WA4 4AD, Cheshire, England

[9] Univ Hamburg, Dept Phys, Jungiusstr 9, D-20355 Hamburg, Germany

[10] Univ Kassel, Inst Phys, Heinrich Plett Str 40, D-34132 Kassel, Germany

[11] Univ Southampton, Sch Chem, Southampton SO17 1BJ, England

[12] Max Born Inst, Max Born Str 2A, D-12489 Berlin, Germany

[13] Univ Ottawa, Dept Chem & Biomol Sci, 150 Louis Pasteur, Ottawa, ON K1N 6N5, Canada

[14] Ruhr Univ Bochum, Fak Chem & Biochem, Organ Chem 2, Univ Str 150, D-44801 Bochum, Germany

[15] Univ Ottawa, Dept Phys, 150 Louis Pasteur, Ottawa, ON K1N 6N5, Canada

[16] NRC uOttawa Joint Ctr Extreme Photon, Ottawa, ON K1A 0R6, Canada

[17] Kansas State Univ, Dept Phys, JR Macdonald Lab, Manhattan, KS 66506 USA

来源：

COMMUNICATIONS PHYSICS | 2023年 / 6卷 / 01期

基金：

欧洲研究理事会; 英国工程与自然科学研究理事会; 加拿大自然科学与工程研究理事会; 英国科学技术设施理事会;

关键词：

COVARIANCE DATA-ACQUISITION; PHOTOELECTRON-SPECTROSCOPY; ABSORPTION-SPECTROSCOPY; EXTREME-ULTRAVIOLET; DYNAMICS; LASER; TIME; ELECTRON; COINCIDENCE; PHOTODISSOCIATION;

D O I：

10.1038/s42005-023-01414-7

中图分类号：

O4 [物理学];

学科分类号：

0702 ;

摘要：

Structural imaging of transient excited-state species is a key goal of molecular physics, promising to unveil rich information about the dynamics underpinning photochemical transformations. However, separating the electronic and nuclear contributions to the spectroscopic observables is challenging, and typically requires the application of high-level theory. Here, we employ site-selective ionisation via ultrashort soft X-ray pulses and time-resolved Coulomb explosion imaging to interrogate structural dynamics of the ultraviolet photochemistry of carbon disulfide. This prototypical system exhibits the complex motifs of polyatomic photochemistry, including strong non-adiabatic couplings, vibrational mode couplings, and intersystem crossing. Immediately following photoexcitation, we observe Coulomb explosion signatures of highly bent and stretched excited-state geometries involved in the photodissociation. Aided by a model to interpret such changes, we build a comprehensive picture of the photoinduced nuclear dynamics that follows initial bending and stretching motions, as the reaction proceeds towards photodissociation.

引用

页数：11

共 81 条

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