Excitation-Energy-Selective Control of Hot-Carrier Cooling via a Resonant Optical-Phonon Bottleneck in Graphene

TL;DR

This study reveals how excitation energy controls hot-carrier cooling in graphene, showing a resonant phonon bottleneck that significantly prolongs carrier lifetime within a specific spectral window.

Contribution

It demonstrates excitation-energy-selective control of carrier relaxation in graphene through a resonant optical-phonon bottleneck, advancing understanding of non-equilibrium carrier-phonon interactions.

Findings

Carrier lifetime increases by an order of magnitude within 0.42-0.48 eV.

Resonant enhancement of optical-phonon lifetime causes hot phonon accumulation.

A unified energy-balance model captures the observed cooling dynamics.

Abstract

Understanding and controlling hot-carrier relaxation in graphene is crucial for advancing ultrafast optoelectronic and terahertz technologies. Here, we investigate carrier cooling dynamics in monolayer and bilayer graphene using mid-infrared pump pulses (0.22-0.73 eV) and terahertz probe pulses. We uncover a pronounced, reproducible, and non-monotonic dependence of the carrier relaxation time on excitation photon energy. Remarkably, within a narrow spectral window (0.42 to 0.48 eV), the carrier lifetime increases by an order of magnitude compared to a few picosecond-scale cooling observed at other energies. We show that this anomalous slowdown originates from a resonant enhancement of the optical-phonon lifetime, causing accumulation and reabsorption of hot optical phonons that suppress energy transfer to the lattice. All observed behaviors are captured within a unified carrier-phonon energy-balance framework, where excitation-energy-dependent variations of the effective optical-phonon decay pathway govern the cooling dynamics. These findings demonstrate excitation-energy-selective control of hot-carrier relaxation in graphene and provide new insight into non-equilibrium carrier-phonon interactions near the optical-phonon bottleneck.