Observation of femtosecond molecular dynamics via pump-probe gas phase x-ray scattering

被引：55
|
作者：
Budarz, J. M. [1 ,2 ]
Minitti, M. P. [2 ]
Cofer-Shabica, D. V. [1 ]
Stankus, B. [1 ]
Kirrander, A. [3 ]
Hastings, J. B. [2 ]
Weber, P. M. [1 ]
机构：
[1] Brown Univ, Dept Chem, Providence, RI 02912 USA
[2] SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA
[3] Univ Edinburgh, Sch Chem, Edinburgh EH9 3JJ, Midlothian, Scotland
来源：
JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS | 2016年 / 49卷 / 03期
基金：
美国国家科学基金会;
关键词：
femtosecond; x-ray scattering; x-ray free electron lasers; molecular dynamics; ULTRAFAST STRUCTURAL DYNAMICS; ELECTRON-DIFFRACTION; FEMTOCHEMISTRY; TRANSMISSION; PATHWAY; MATTER; SPACE;
D O I：
10.1088/0953-4075/49/3/034001
中图分类号：
O43 [光学];
学科分类号：
070207 ; 0803 ;
摘要：
We describe a gas-phase x-ray scattering experiment capable of capturing molecular motions with atomic spatial resolution and femtosecond time resolution. X-ray free electron lasers can deliver intense x-ray pulses of ultrashort duration, making them suitable to study ultrafast chemical reaction dynamics in an ultraviolet pump, x-ray probe scheme. A cell diffractometer balances sample flow with gas density and laser focusing conditions to provide adequate scattering vector resolution with high signal intensity and near-uniform excitation probability. Images from a pixel-array x-ray detector, spatially and electronically calibrated, allow for detection of scattering intensity changes below 1%. First experiments on the ring-opening reaction of 1,3-cyclohexadiene to form 1, 3, 5-hexatriene show a rapid initial reaction on an 80 fs time scale.
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页数：11
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