Wafer-Scale Black Arsenic–Phosphorus Thin-Film Synthesis Validated with Density Functional Perturbation Theory Predictions

Abstract

Herein we report the wafer-scale synthesis of thin-film black arsenic–phosphorus (b-AsP) alloys via two-step solid-source molecular beam deposition (MBD) and subsequent hermetic thermal annealing. We characterize our thin films with a variety of compositional and structural metrology techniques. X-ray photoelectron spectroscopy and energy dispersive spectroscopy determine compositions of As0.78P0.22 for our thin films, while X-ray reflectivity measurements indicate film thicknesses of 6–9 nm. High-resolution transmission electron spectroscopy images reveal a nanocrystalline morphology with orthorhombic b-AsP grains on the order of ∼5 nm. Raman scattering spectroscopy is employed to characterize the vibrational spectra of our thin films, and the results obtained are in agreement with previously reported b-AsP spectra. Evidence of uniform wafer-scale growth is substantiated by Raman mapping. We simulate crystal structure, band gaps, and Raman spectra from first-principles DFT-based computations and find exc...