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Decomposing electronic and lattice contributions in optical pump – X-ray probe transient inner-shell absorption spectroscopy of CuO

Journal Article · · Faraday Discussions
DOI:https://doi.org/10.1039/c8fd00236c· OSTI ID:1594925
 [1];  [1];  [2];  [1];  [1];  [1];  [3];  [1];  [4];  [4];  [4];  [2];  [5];  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany). Center for Free-Electron Laser Science
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany). Center for Free-Electron Laser Science
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Electronic and lattice contributions to picosecond time-resolved X-ray absorption spectra (trXAS) of CuO at the oxygen K-edge are analyzed by comparing trXAS spectra, recorded using excitation wavelengths of 355 nm and 532 nm, to steady-state, temperature-dependent XAS measurements. The trXAS spectra at pump-probe time-delays ≥150 ps are dominated by lattice heating effects. Insight into the temporal evolution of lattice temperature profiles on timescales up to 100s of nanoseconds after laser excitation are reported, on an absolute temperature scale, with a temporal sensitivity and a spatial selectivity on the order of 10s of picoseconds and 10s of nanometers, respectively, effectively establishing an "ultrafast thermometer". In particular, for the 532 nm experiment at ~5 mJ cm-2 fluence, both the initial sample temperature and its dynamic evolution are well captured by a one-dimensional thermal energy deposition and diffusion model. The thermal conductivity k = (1.3 ± 0.4) W m-1 K-1 derived from this model is in good agreement with the literature value for CuO powder, kpowder = 1.013 W m-1 K-1. For 355 nm excitation, a quantitative analysis of the experiments is hampered by the large temperature gradients within the probed sample volume owing to the small UV penetration depth. The impact of the findings on mitigating or utilizing photoinduced lattice temperature changes in future X-ray free electron laser (XFEL) experiments is discussed.
Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1594925
Alternate ID(s):
OSTI ID: 1508862
Journal Information:
Faraday Discussions, Journal Name: Faraday Discussions Journal Issue: 0 Vol. 216; ISSN 1359-6640; ISSN FDISE6
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

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