First-principles interpretation of attosecond time-resolved XUV absorption spectroscopy of laser excited Silicon

C. D. Pemmaraju, S. Sato, K. Yabana, Krupa Ramasesha, M. Schultze, Stephen R. Leone, David Prendergast

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Abstract

The availability of ultrafast x-ray pulses both from powerful free electron laser light-sources as well as table top high-harmonic generation, has significantly enhanced the utility of core-level spectroscopies as probes for investigating dynamical processes in functional materials. Theoretical approaches to complement these time-domain experiments are therefore actively being developed. In this study we employ a combination of real-time time-dependent density functional theory (TDDFT), occupancy-constrained density functional theory and many-body perturbation theory approaches to help interpret spectral signatures observed in attosecond time-resolved core-level spectroscopic measurements on laser-excited silicon. Using non-equilibrium electron-hole densities obtained from real-time TDDFT simulations of the valence electronic structure we estimate the transient modulation of L-edge absorption in femtosecond infrared pump - attosecond XUV probe experiments. We further estimate the contribution of electron-phonon and electron-electron scattering mechanisms to the lifetime broadening observed in measured L-edge spectra using occupation-constrained density functional theory and GW calculations respectively.
Original languageEnglish
Title of host publicationAPS March Meeting 2015
PagesA15.001
Publication statusPublished - Mar 2015
Externally publishedYes
EventAPS March Meeting 2015 - San Antonio, Texas, United States
Duration: 2 Mar 20156 Mar 2015

Conference

ConferenceAPS March Meeting 2015
CountryUnited States
CitySan Antonio, Texas
Period2/03/156/03/15

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Keywords

  • Energy transfer
  • Fused silica
  • Phase shift
  • Pump probe spectroscopy
  • Refractive index
  • Ultrashort pulses

Fields of Expertise

  • Advanced Materials Science

Cite this

Pemmaraju, C. D., Sato, S., Yabana, K., Ramasesha, K., Schultze, M., Leone, S. R., & Prendergast, D. (2015). First-principles interpretation of attosecond time-resolved XUV absorption spectroscopy of laser excited Silicon. In APS March Meeting 2015 (pp. A15.001)