Quantum-optical theory of the few femtosecond nonlinear optical response of Drude metals with a non-parabolic conduction band

TL;DR

This paper introduces an energy-space density matrix framework to analyze the ultrafast nonlinear optical response of Drude metals with non-parabolic conduction bands, capturing quantum coherence effects and simplifying computations.

Contribution

It develops a novel energy-space density matrix approach that extends previous models, enabling detailed analysis of quantum coherence and nonlinear dynamics in ultrafast optical interactions with metals.

Findings

Quantum coherence signatures in absorption dynamics

Emergence of strong excited-state absorption under intense excitation

Spontaneous emission can be neglected in this regime

Abstract

We develop an energy-space density matrix framework to investigate the interaction of extremely short optical pulses (ESPs) with transparent conducting oxides (TCOs). This approach captures not only electron populations, material polarization, and the permittivity, but also the quantum coherences between states. Compared to traditional momentum-space models, the energy-space formulation offers substantial computational simplification while retaining accuracy. Building on but going beyond the scope of Ref.~\cite{single_cycle_nlty_Letter}, we focus on dynamical features previously unexplored. Our formulation reveals clear signatures of quantum coherence in the net absorption dynamics and highlights the emergence of strong excited-state absorption under intense excitation. It also clarifies that spontaneous emission can be neglected in this regime. Furthermore, we investigate the influence of pump pulse intensity on the local field's duration, spectral broadening and shift, and phase induced by carrier dynamics, highlighting the absorptive nature of the nonlinear response. Our results provide a unified framework for understanding nonlinear light-matter interaction in dispersive, low-density electron systems driven far from equilibrium by intense broadband excitation.