Search for: All records

Abstract Above‐band gap optical excitation of non‐centrosymmetric semiconductors can lead to the spatial shift of the center of electron charge in a process known as shift current. Shift current is investigated in single‐crystal SnS₂, a layered semiconductor with the band gap of ≈2.3 eV, by THz emission spectroscopy and first principles density functional theory (DFT). It is observed that normal incidence excitation with above gap (400 nm; 3.1 eV) pulses results in THz emission from 2H SnS₂() polytype, where such emission is nominally forbidden by symmetry. It is argued that the underlying symmetry breaking arises due to the presence of stacking faults that are known to be ubiquitous in SnS₂single crystals and construct a possible structural model of a stacking fault with symmetry properties consistent with the experimental observations. In addition to shift current, it is observed THz emission by optical rectification excited by below band gap (800 nm; 1.55 eV) pulses but it requires excitation fluence more than two orders of magnitude higher to produce same signal amplitude. These results suggest that ultrafast shift current in which can be excited with visible light in blue–green portion of the spectrum makes SnS₂a promising source material for THz photonics. 

Computational spectrometry is an emerging field that uses photodetection in conjunction with numerical algorithms for spectroscopic measurements. Compact single photodetectors made from layered materials are particularly attractive since they eliminate the need for bulky mechanical and optical components used in traditional spectrometers and can easily be engineered as heterostructures to optimize device performance. However, such photodetectors are typically nonlinear devices, which adds complexity to extracting optical spectra from their response. Here, we train an artificial neural network to recover the full nonlinear spectral photoresponse of a single GeSe-InSe p-n heterojunction device. The device has a spectral range of 400 to 1100 nm, a small footprint of ~25 × 25 square micrometers, and a mean reconstruction error of 2 × 10⁻⁴for the power spectrum at 0.35 nanometers. Using our device, we demonstrate a solution to metamerism, an apparent matching of colors with different power spectral distributions, which is a fundamental problem in optical imaging.