Towards efficient time-resolved X-ray absorption studies of electron dynamics at photocatalytic interfaces

Neppl, Stefan; Mahl, Johannes; Tremsin, Anton S; Rude, Bruce; Qiao, Ruimin; Yang, Wanli; Guo, Jinghua; Gessner, Oliver

doi:10.1039/c6fd00125d

Title: Towards efficient time-resolved X-ray absorption studies of electron dynamics at photocatalytic interfaces

Journal Article · Wed May 18 00:00:00 EDT 2016 · Faraday Discussions

DOI:https://doi.org/10.1039/c6fd00125d· OSTI ID:1845090

Neppl, Stefan ^[1]; Mahl, Johannes ^[1]; Tremsin, Anton S ^[2]; Rude, Bruce ^[1]; Qiao, Ruimin ^[1]; Yang, Wanli ^[1]; Guo, Jinghua ^[1]; Gessner, Oliver ^[1]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States)

We present a picosecond time-resolved X-ray absorption spectroscopy (tr-XAS) setup designed for synchrotron-based studies of interfacial photochemical dynamics. The apparatus combines a high power, variable repetition rate picosecond laser system with a time-resolved X-ray fluorescence yield detection technique. Time-tagging of the detected fluorescence signals enables the parallel acquisition of X-ray absorption spectra at a variety of pump–probe delays employing the well-defined time structure of the X-ray pulse trains. The viability of the setup is demonstrated by resolving dynamic changes in the fine structure near the O1s X-ray absorption edge of cuprous oxide (Cu₂O) after photo-excitation with a 355 nm laser pulse. Two distinct responses are detected. A pronounced, quasi-static, reversible change of the Cu₂O O1s X-ray absorption spectrum by up to ~30% compared to its static line shape corresponds to a redshift of the absorption edge by ~1 eV. This value is small compared to the 2.2 eV band gap of Cu₂O but in agreement with previously published results. Here, the lifetime of this effect exceeds the laser pulse-to-pulse period of 8 μs, resulting in a quasi-static spectral change that persists as long as the sample is exposed to the laser light, and completely vanishes once the laser is blocked. Additionally, a short-lived response corresponding to a laser-induced shift of the main absorption line by ~2 eV to lower energies appears within <200 ps and decays with a characteristic timescale of 43 ± 5 ns. Both the picosecond rise and nanosecond decay of this X-ray response are simultaneously captured by making use of a time-tagging approach – highlighting the prospects of the experimental setup for efficient probing of the electronic and structural dynamics in photocatalytic systems on multiple timescales.

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Research Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1845090

Journal Information:: Faraday Discussions, Vol. 194; ISSN 1359-6640

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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