Spectral measurement of the breakdown limit of $\beta-Ga_{2}O_{3}$ and tunnel ionization of self-trapped excitons and holes

TL;DR

This study investigates the strong-field exciton and hole dynamics in $eta-Ga_{2}O_{3}$ using spectral measurements, revealing field-induced effects, breakdown detection, and tunnel ionization processes with novel quantitative models.

Contribution

It introduces a quantum mechanical model for tunnel ionization of self-trapped excitons and holes, providing new insights into high-field carrier transport in $eta-Ga_{2}O_{3}$.

Findings

Spectral red-shift saturates at dielectric breakdown threshold.

Field-dependent photocurrent explained by tunnel ionization of STH and STX.

Estimated ultrafast hole self-trapping time of 0.045 fs.

Abstract

$\beta-Ga_{2}O_{3}$ is an unusual semiconductor where large electric fields (~1-6 MV/cm) can be applied while still maintaining a dominant excitonic absorption peak below its ultra-wide bandgap. This provides a rare opportunity in the solid-state to examine exciton and carrier self-trapping dynamics in the strong-field limit at steady-state. Under sub-bandgap photon excitation, we observe a field-induced red-shift of the spectral photocurrent peak associated with exciton absorption and threshold-like increase in peak amplitude at high-field associated with self-trapped hole ionization. The field-dependent spectral response is quantitatively fit with an eXciton-modified Franz-Keldysh (XFK) effect model, which includes the electric-field dependent exciton binding energy due to the quadratic Stark effect. A saturation of the spectral red-shift with reverse bias is observed exactly at the onset of dielectric breakdown providing a spectral means to detect and quantify the local electric field and dielectric breakdown behavior. Additionally, the field-dependent responsivity provides insight to the photocurrent production pathway revealing the photocurrent contributions of self-trapped excitons (STXs) and self-trapped holes (STHs). Photocurrent and p-type transport in $\beta-Ga_{2}O_{3}$ are quantitatively explained by field-dependent tunnel ionization of excitons and self-trapped holes. We employ a quantum mechanical model of the field-dependent tunnel ionization of STX and STH to model the non-linear field-dependence of the photocurrent amplitude. Fitting to the data, we estimate an effective mass of valence band holes $(18.8 m_{0})$ and an ultrafast self-trapping time of holes (0.045 fs). This indicates that minority-hole transport in $\beta-Ga_{2}O_{3}$ can only arise through tunnel ionization of STH under strong fields.