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

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• 作者：Grigory Smolentsev ; Alexander Guda ; Xiaoyi Zhang ; Kristoffer Haldrup ; Eugen S. Andreiadis ; Murielle Chavarot-Kerlidou ; Sophie E. Canton ; Maarten Nachtegaal ; Vincent Artero ; Villy Sundstrom
• 刊名：Journal of Physical Chemistry C
• 出版年：2013
• 出版时间：August 29, 2013
• 年：2013
• 卷：117
• 期：34
• 页码：17367-17375
• 全文大小：346K
• 年卷期：v.117,no.34(August 29, 2013)
• ISSN：1932-7455

文摘

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.