Abstract

We present a numerical study on the intraband optical conductivity of hot carriers at quasi-equilibria in photoexcited graphene based on the semiclassical Boltzmann transport equations (BTE) with the aim of understanding the effects of intrinsic optical phonon and extrinsic coulomb scattering caused by charged impurities at the graphene--substrate interface. Instead of using full-BTE solutions, we employ iterative solutions of the BTE and the comprehensive model for the temporal evolutions of hot-carrier temperature and hot-optical-phonon occupations to reduce computational costs. Undoped graphene exhibits large positive photoconductivity owing to the increase in thermally excited carriers and the reduction in charged impurity scattering. The frequency dependencies of the photoconductivity in undoped graphene having high concentrations of charged impurities significantly deviate from those observed in the simple Drude model, which can be attributed to temporally varying charged impurity scattering during terahertz (THz) probing in the hot-carrier cooling process. Heavily doped graphene exhibits small negative photoconductivity similar to that of the Drude model. In this case, charged impurity scattering is substantially suppressed by the carrier-screening effect, and the temperature dependencies of the Drude weight and optical phonon scattering governs the negative photoconductivity. In lightly doped graphene, the appearance of negative and positive photoconductivity depends on the frequency and the crossover from negative photoconductivity to positive emerges from increasing the charged impurity concentration. This indicates the change of the dominant scattering mechanism from optical phonons to charged impurities. Our approach provides a quantitative understanding of non-Drude behaviors and the temporal evolution of photoconductivity in graphene.

Highlights

  • In many optoelectronic graphene applications (e.g., photodetection [1], plasmonics [2], light harvesting [3], data communication [4,5], ultrafast laser [6,7,8], and terahertz (THz) technologies [9,10,11,12,13]), it is crucial to understand the carrier dynamics that occur following photoexcitation and their influence on electrical and optical conductivities

  • III, we presented the numerical results of the intraband optical conductivity of hot carriers in undoped and heavily doped graphene after photoexcitation, considering the intrinsic and extrinsic carrier scattering mechanisms that exhibits positive and negative photoconductivity, depending on the Fermi energy

  • The large positive photoconductivity arises from the positive change of the hot carrier population surpassing the negative contribution by the enhanced carrier scattering by the optical phonon

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Summary

INTRODUCTION

In many optoelectronic graphene applications (e.g., photodetection [1], plasmonics [2], light harvesting [3], data communication [4,5], ultrafast laser [6,7,8], and terahertz (THz) technologies [9,10,11,12,13]), it is crucial to understand the carrier dynamics that occur following photoexcitation and their influence on electrical and optical conductivities. We calculate the frequency-dependent intraband optical conductivity of hot carriers in photoexcited graphene based on the Boltzmann transport equation (BTE), including the intrinsic and extrinsic interactions in the collision term. Because the intraband transition is dominant in the THz-frequency region of 0.1–10 THz, the microscopic polarization for interband transition in the semiconductor Bloch equation may be negligible in the calculation of optical conductivity at the quasiequilibrium carrier distribution in graphene after photoexcitation [16,18,22] Under such conditions, the semiclassical BTE may offer an alternative [40,41]. We present numerical simulations of the intraband optical conductivity of hot carriers in photoexcited graphene with different Fermi energies, considering the intrinsic and extrinsic carrier scatterings and the temporal variations of the carrier distribution and momentum relaxation rate during THz probing.

Iterative solutions of BTE in steady state
Iterative solutions of BTE under time-dependent electric field
NUMERICAL RESULTS
Undoped graphene
Heavily doped graphene
DISCUSSION AND CONCLUSION
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