Terahertz Probe of Photoexcited Carrier Dynamics in Dirac Semimetal Cd3As2

TL;DR

This study investigates the ultrafast relaxation dynamics of photoexcited carriers in the 3D Dirac semimetal Cd3As2 using transient terahertz spectroscopy, revealing biexponential decay processes and phonon interactions relevant for optoelectronic applications.

Contribution

The paper provides the first detailed analysis of carrier relaxation and phonon interactions in Cd3As2 using transient terahertz spectroscopy, highlighting unique electron-phonon coupling behaviors.

Findings

Biexponential decay with electron-phonon and phonon anharmonic processes

Observation of phonon-assisted intraband absorption in THz spectra

Intensity-dependent electron-phonon coupling modifications

Abstract

The relaxation dynamics of photoexcited quasiparticles of three-dimensional (3D) Dirac semimetals are vital towards their application in high performance electronic and optoelectronic devices. In this work, the relaxation dynamics of photoexcited carriers of 3D Dirac semimetal Cd3As2 are investigated by transient terahertz spectroscopy. The visible pump-THz probe spectroscopy measurement shows clear biexponential decays with two characteristic time constants. According to the pump-power and temperature dependence, these two characteristic time constants are attributed to the electron phonon coupling (1-4 ps) and anharmonic decay of hot coupled phonons to electronic uncoupled phonons (2-9 ps), respectively. An anomalous electron-optical phonon coupling reduction and a bottleneck slowing of hot optical phonons relaxation are observed with higher excitation intensities similar to that in graphene. On the other hand, the electron-optical phonon coupling can be enhanced due to the phonon frequency broadening and softening at elevated lattice temperature. Furthermore, the transient THz spectrum response is strongly modified by the phonon assisted intraband absorption of hot carriers from a pure electronic Drude model, which is evidenced by a characteristic THz absorption dip in the transient THz absorption spectrum. This absorption dip is pinned by the discrete optical phonon energy that assists the intraband transition enabled by photoexcitation of hot carriers.