Interpreting pulse-shape effects in pump-probe spectroscopies

Abstract

The effect of the pulse-shape on pump-probe spectroscopies is examined for the simplest model of noninteracting fermions on an infinite-dimensional hypercubic lattice. The probe-modified density of states follows the time evolution of the pump and displays narrowing and Floquet-like sidebands at the pump maximum, whereas the photoelectron spectra are also strongly affected by the nonequilibrium occupation of the single-particle states due to the excitation from the pump. The nonequilibrium Raman cross section is derived, and the nonresonant one in both the $A_{1\mathrm{g}}$ and $B_{1\mathrm{g}}$ symmetries contains a number of peaks at the pump maximum, which can be attributed to an interference effect or Brillouin scattering off the time variations of the stress tensor. Both the "measured" occupation of single-particle states and the ratio of Stokes to anti-Stokes peaks are strongly modified by the probe-pulse width, which must be included in the interpretation of experimental results.

18 pages, 7 figures

References in corpus (5)

• Theoretical description of time-resolved photoemission spectroscopy: application to pump-probe experiments
• Novel Electron-Phonon Relaxation Pathway in Graphite Revealed by Time-Resolved Raman Scattering and Angle-Resolved Photoemission Spectroscopy
• Emergence of Floquet Behavior for Lattice Fermions Driven by Light Pulses
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• Detection of squeezed phonons in pump-probe spectroscopy
• Ultrafast Raman probe of the photoinduced superconducting to normal state transition in the cuprate Bi${}_2$Sr${}_2$CaCu${}_2$O${}_{8+\delta }$