Published December 2021 | Version v1
Journal article

Theory of subcycle time-resolved photoemission: Application to terahertz photodressing in graphene

  • 1. Stanford Institute for Materials and Energy Sciences (SIMES), SLAC National Accelerator Laboratory, Menlo Park, CA 94025 (United States)
  • 2. Max Planck Institute for the Structure and Dynamics of Matter, Center for Free Electron Laser Science (CFEL), Luruper Chaussee 149, 22761 Hamburg (Germany)

Description

Highlights: • We develop the theoretical description of trARPES in the subcycle regime. • Light-matter coupling is included in the theory in a gauge-invariant way. • The theory is applied to THz pump-probe photoemission from graphene. Motivated by recent experimental progress we revisit the theory of pump–probe time- and angle-resolved photoemission spectroscopy (trARPES), which is one of the most powerful techniques to trace transient pump-driven modifications of the electronic properties. The pump-induced dynamics can be described in different gauges for the light–matter interaction. Standard minimal coupling leads to the velocity gauge, defined by linear coupling to the vector potential. In the context of tight-binding (TB) models, the Peierls substitution is the commonly employed scheme for single-band models. Multi-orbital extensions – including the coupling of the dipole moments to the electric field – have been introduced and tested recently. In this work, we derive the theory of time-resolved photoemission within both gauges from the perspective of nonequilibrium Green's functions. This approach naturally incorporates the photoelectron continuum, which allows for a direct calculation of the observable photocurrent. Following this route we introduce gauge-invariant expressions for the time-resolved photoemission signal. The theory is applied to graphene pumped with short terahertz pulses, which we treat within a first-principles TB model. We investigate the gauge invariance and discuss typical effects observed in subcycle time-resolved photoemission. Our formalism is an ideal starting point for realistic trARPES simulations including scattering effects.

Availability note (English)

Available from http://dx.doi.org/10.1016/j.elspec.2021.147121

Additional details

Identifiers

DOI
10.1016/j.elspec.2021.147121;
PII
S0368204821000736;

Publishing Information

Journal Title
Journal of Electron Spectroscopy and Related Phenomena
Journal Volume
253
Journal Page Range
vp.
ISSN
0368-2048
CODEN
JESRAW

Optional Information

Copyright
Copyright (c) 2021 Elsevier B.V. All rights reserved.