Abstract

Employing time-resolved photoelectron spectroscopy we analyze the relaxation dynamics of hot electrons in the charge density wave / Mott material 1T-TaS_2. At 1.2 eV above the Fermi level we observe a hot electron lifetime of 12 +- 5 fs in the metallic state and of 60 +- 10 fs in the broken symmetry ground state - a direct consequence of the reduced phase space for electron-electron scattering determined by the Mott gap. Boltzmann equation calculations which account for the interaction of hot electrons in a Bloch band with a doublon-holon excitation in the Mott state provide insight into the unoccupied electronic structure in the correlated state.

Highlights

  • Employing time-resolved photoelectron spectroscopy we analyze the relaxation dynamics of hot electrons in the charge density wave/Mott material 1T -TaS2

  • At 1.2 eV above the Fermi level we observe a hot electron lifetime of 12 ± 5 fs in the metallic state and of 60 ± 10 fs in the broken symmetry ground state—a direct consequence of the reduced phase space for electron-electron scattering determined by the Mott gap

  • Boltzmann equation calculations which account for the interaction of hot electrons in a Bloch band with a doublon-holon excitation in the Mott state provide insight into the unoccupied electronic structure in the correlated state

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Summary

Rapid Communications

Doublon bottleneck in the ultrafast relaxation dynamics of hot electrons in 1T -TaS2. Employing time-resolved photoelectron spectroscopy we analyze the relaxation dynamics of hot electrons in the charge density wave/Mott material 1T -TaS2. Boltzmann equation calculations which account for the interaction of hot electrons in a Bloch band with a doublon-holon excitation in the Mott state provide insight into the unoccupied electronic structure in the correlated state. We investigate hot electron relaxation in the charge density wave/Mott material 1T -TaS2 by fs time-resolved photoelectron spectroscopy measurements and Boltzmann equation calculations, which treat the interaction of delocalized, propagating electrons in a Bloch band with the correlated electron system. The absence of electronic states in the Mott gap up to an excitation energy set by the Coulomb repulsion U reduces the phase space for electron-electron scattering considerably and increases the hot electron lifetime in the Bloch band. Photoelectrons are created by probe pulses at 6.1 eV photon energy and 100 fs pulse duration, which are obtained by frequency quadrupling in β-barium borate crystals and analyzed in normal

Published by the American Physical Society
Photoelectron intensity
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