4.2 Article

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

Journal

FARADAY DISCUSSIONS
Volume 216, Issue -, Pages 414-433

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/c8fd00236c

Keywords

-

Funding

  1. U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division [DE-AC02-05CH11231]
  2. DOE Office of Science User Facility [DE-AC02-05CH11231]
  3. ALS
  4. Alexander von Humboldt foundation
  5. Helmholtz Association [VI 419]
  6. Helmholtz Research Association (Germany)

Ask authors/readers for more resources

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 similar to 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, k(powder) = 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.

Authors

I am an author on this paper
Click your name to claim this paper and add it to your profile.

Reviews

Primary Rating

4.2
Not enough ratings

Secondary Ratings

Novelty
-
Significance
-
Scientific rigor
-
Rate this paper

Recommended

No Data Available
No Data Available