Pump-flow-probe x-ray absorption spectroscopy as a tool for studying aintermediate states of photocatalytic systems

Research output: Contribution to journalJournal article – Annual report year: 2013Researchpeer-review

  • Author: Smolentsev, Grigory

    Lund University, Sweden

  • Author: Guda, Alexander

    Southern Federal University, Russian Federation

  • Author: Zhang, Xiaoyi

    Argonne National Laboratory, United States

  • Author: Haldrup, Kristoffer

    Department of Physics, Technical University of Denmark, Fysikvej, 2800, Kgs. Lyngby, Denmark

  • Author: Andreiadis, Eugen S.

    French Alternative Energies and Atomic Energy Commission, France

  • Author: Chavarot-Kerlidou, Murielle

    French Alternative Energies and Atomic Energy Commission, France

  • Author: Canton, Sophie E.

    Lund University, Sweden

  • Author: Nachtegaal, Maarten

    Paul Scherrer Institute, Switzerland

  • Author: Artero, Vincent

    French Alternative Energies and Atomic Energy Commission, France

  • Author: Sundstrom, Villy

    Lund University, Sweden

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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. © 2013 American Chemical Society.
Original languageEnglish
JournalThe Journal of Physical Chemistry Part C
Volume117
Issue number34
Pages (from-to)17367-17375
ISSN1932-7447
DOIs
Publication statusPublished - 2013
CitationsWeb of Science® Times Cited: No match on DOI

    Research areas

  • Continuous wave lasers, Photoexcitation, X ray absorption spectroscopy, Probes

ID: 61145371