Spectral measurement of the breakdown limit of and tunnel ionization of self-trapped excitons and holes
arXiv:2011.00375 · doi:10.1103/PhysRevApplied.16.034011
Abstract
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 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 and an ultrafast self-trapping time of holes (0.045 fs). This indicates that minority-hole transport in can only arise through tunnel ionization of STH under strong fields.
arXiv comment47 pages, 12 figures
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