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Disentangling the electronic and lattice contributions to the dielectric response of photoexcited bismuth

F. Thiemann1,*, G. Sciaini2, A. Kassen1, T. S. Lott2, and M. Horn-von Hoegen1,3

  • 1Department of Physics, University of Duisburg-Essen, Lotharstrasse 1, 47057 Duisburg, Germany
  • 2Department of Chemistry, The Ultrafast Electron Imaging Lab, and Waterloo Institute for Nanotechnology, University of Waterloo, Waterloo, Ontario, Canada N2L 3G1
  • 3Center for Nanointegration (CENIDE), University of Duisburg-Essen, Carl-Benz-Strasse 199, 47057 Duisburg, Germany

  • *fabian.thiemann@uni-due.de

Phys. Rev. B 109, L041105 – Published 16 January, 2024

DOI: https://doi.org/10.1103/PhysRevB.109.L041105

Abstract

Elucidating the interplay between nuclear and electronic degrees of freedom that govern the complex dielectric behavior of materials under intense photoexcitation is essential for tailoring optical properties on demand. However, conventional transient reflectivity experiments have been unable to differentiate between real and imaginary components of the dielectric response, omitting crucial electron-lattice interactions. Utilizing thin film interference we unambiguously determine the photoinduced change in the complex dielectric function in the Peierls semimetal bismuth and examine its dependence on the excitation density and nuclear motion of the A1g phonon. Our modeled transient reflectivity data reveal a progressive broadening and redshift of Lorentz oscillators with increasing excitation density and underscores the importance of both electronic and nuclear coordinates in the renormalization of interband transitions.

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