Theory of subcycle time-resolved photoemission: Application to terahertz photodressing in 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 fight-binding (TB) models, the Peierls substitution is the commonly employed scheme for single-band models. Mull-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.

Automated summary

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. We introduce the theory of time-resolved photoemission within both gauges from the perspective of nonequilibrium Green's functions, we investigate the gauge invariance, and discuss typical effects observed in subcycle time-resolved photoemission. The formalism presented is an ideal starting point for realistic trARPES simulations including scattering effects.