Conformer-specific photochemistry imaged in real space and time

被引：28

作者：

Champenois, E. G. ^{[1
]}

Sanchez, D. M. ^{[1
,2
,9
]}

Yang, J. ^{[1
,3
,4
]}

Nunes, J. P. Figueira ^{[5
]}

Attar, A. ^{[3
]}

Centurion, M. ^{[5
]}

Forbes, R. ^{[3
]}

Guhr, M. ^{[6
]}

Hegazy, K. ^{[1
,7
]}

Ji, F. ^{[3
]}

Saha, S. K. ^{[5
]}

Liu, Y. ^{[8
]}

Lin, M-F ^{[3
]}

Luo, D. ^{[3
]}

Moore, B. ^{[5
]}

Shen, X. ^{[3
]}

Ware, M. R. ^{[1
]}

Wang, X. J. ^{[3
]}

Martinez, T. J. ^{[1
,2
]}

Wolf, T. J. A. ^{[1
]}

机构：

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

[2] Stanford Univ, Dept Chem, Stanford, CA 94305 USA

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

[4] Tsinghua Univ, Ctr Basic Mol Sci, Dept Chem, Beijing, Peoples R China

[5] Univ Nebraska, Dept Phys & Astron, Lincoln, NE 68588 USA

[6] Univ Potsdam, Inst Phys & Astron, Potsdam, Germany

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

[8] SUNY Stony Brook, Dept Phys & Astron, Stony Brook, NY USA

[9] Lawrence Livermore Natl Lab, Design Phys Div, Livermore, CA USA

来源：

SCIENCE | 2021年 / 374卷 / 6564期

关键词：

ALPHA-PHELLANDRENE; DYNAMICS; SPECTROSCOPY; MOLECULES;

D O I：

10.1126/science.abk3132

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Conformational isomers (conformers) of molecules play a decisive role in biology and organic chemistry. However, experimental methods for investigating chemical reaction dynamics are typically not conformer-sensitive. We report on a gas-phase megaelectronvolt ultrafast electron diffraction investigation of a-phellandrene undergoing an electrocyclic ring-opening reaction. We directly imaged the evolution of a specific set of a-phellandrene conformers into the product isomer predicted by the Woodward-Hoffmann rules in real space and time. Our experimental results are in quantitative agreement with nonadiabatic quantum molecular dynamics simulations, which provide considerable detail of how conformation influences the time scale and quantum efficiency of photoinduced ring-opening reactions.

引用

页码：178 / 182

页数：5

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