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

• Published in: Journal of electron spectroscopy and related phenomena 2021-12, Vol.253 (C), p.147121, Article 147121
• Main Authors: Schüler, Michael, Sentef, Michael A.
• Format: Article
• Language: English
• Subjects: Graphene; Nonequilibrium Green’s functions; Time- and angle-resolved photoemission
• ISSN: 0368-2048; 1873-2526
• DOI: 10.1016/j.elspec.2021.147121

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. •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.