Pump-Flow-Probe X-ray Absorption Spectroscopy as a Tool for Studying Intermediate States of Photocatalytic Systems

被引：33

作者：

Smolentsev, Grigory ^{[1
,2
]}

Guda, Alexander ^{[3
]}

Zhang, Xiaoyi ^{[4
]}

Haldrup, Kristoffer ^{[5
]}

Andreiadis, Eugen S. ^{[6
]}

Chayarot-Kerlidou, Murielle ^{[6
]}

Canton, Sophie E. ^{[1
]}

Nachtegaal, Maarten ^{[2
]}

Artero, Vincent ^{[6
]}

Sundstrom, Villy ^{[1
]}

机构：

[1] Lund Univ, S-22100 Lund, Sweden

[2] Paul Scherrer Inst, CH-5232 Villigen, Switzerland

[3] Southern Fed Univ, Res Ctr Nanoscale Struct Matter, Rostov Na Donu 344090, Russia

[4] Argonne Natl Lab, Xray Sci Div, Argonne, IL 60439 USA

[5] Tech Univ Denmark, NEXMAP Sect, Dept Phys, Ctr Mol Movies, DK-2800 Lyngby, Denmark

[6] Univ Grenoble 1, CNRS, CEA, Lab Chem & Biol Met, Grenoble, France

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2013年 / 117卷 / 34期

基金：

瑞士国家科学基金会; 欧洲研究理事会; 瑞典研究理事会;

关键词：

FINE-STRUCTURE; EXCITED-STATE; WATER; COBALT; SCATTERING; COMPLEXES; CATALYSTS; TRANSITION; DYNAMICS; DETECTOR;

D O I：

10.1021/jp4010554

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

A new setup for pump-flow-probe X-ray absorption spectroscopy has been implemented at the SuperXAS beamline of the Swiss Light Source. It allows recording X-ray absorption spectra with a time resolution of tens of microseconds and high detection efficiency for samples with sub-millimolar concentrations. A continuous wave laser is used for the photoexcitation, with the distance between laser and X-ray beams and velocity of liquid flow determining the time delay, while the focusing of both beams and the flow speed profile define the time resolution. This method is compared with the alternative measurement technique that utilizes a 1 kHz repetition rate laser and multiple X-ray probe pulses. Such an experiment was performed at beamline 11ID-D of the Advanced Photon Source. Advantages, limitations, and potential for improvement of the pump-flow-probe setup are discussed by analyzing the photon statistics. Both methods with Co K-edge probing were applied to the investigation of a cobaloxime-based photocatalytic reaction. The interplay between optimizing for efficient photoexcitation and time resolution as well and the effect of sample degradation for these two setups are discussed.

引用

页码：17367 / 17375

页数：9

共 49 条

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