Highly Sensitive Broadband Polarized Photodetector Based on the As0.6P0.4/WSe2 Heterostructure toward Imaging and Optical Communication Application.

Polarization-sensitive photodetectors based on two-dimensional anisotropic materials still encounter the issues of narrow spectral coverage and low polarization sensitivity. To address these obstacles, anisotropic As0.6P0.4 with a narrow band gap has been integrated with WSe2 to construct a type-II heterostructure, realizing a high-performance polarization-sensitive photodetector with broad spectral range from 405 to 2200 nm. By operating in photovoltaic mode at zero bias, the device shows a very low dark current of ∼0.02 picoampere, high responsivity of 492 m A/W, and high photoswitching ratio of 6 × 104, yielding a high specific detectivity of 1.4 × 1012 Jones. The strong in-plane anisotropy of As0.6P0.4 endows the device with a capability of polarization-sensitive detection with a high polarization ratio of 6.85 under a bias voltage. As an image sensor and signal receiver, the device shows great potential in imaging and optical communication applications. This work develops an anisotropic vdW heterojunction to realize polarization-sensitive photodetectors with wide spectral coverage, fast response, and high sensitivity, providing a new candidate for potential applications of polarization-resolved electronics and photonics.

Developing correlation-consistent numeric atom-centered orbital basis sets for krypton: Applications in RPA-based correlated calculations.

Localized atomic orbitals are the preferred basis set choice for large-scale explicit correlated calculations, and high-quality hierarchical correlation-consistent basis sets are a prerequisite for correlated methods to deliver numerically reliable results. At present, numeric atom-centered orbital (NAO) basis sets with valence correlation consistency (VCC), designated as NAO-VCC-nZ, are only available for light elements from hydrogen (H) to argon (Ar) [Zhang et al., New J. Phys. 15, 123033 (2013)]. In this work, we extend this series by developing NAO-VCC-nZ basis sets for krypton (Kr), a prototypical element in the fourth row of the periodic table. We demonstrate that NAO-VCC-nZ basis sets facilitate the convergence of electronic total-energy calculations using the Random Phase Approximation (RPA), which can be used together with a two-point extrapolation scheme to approach the complete basis set limit. Notably, the Basis Set Superposition Error (BSSE) associated with the newly generated NAO basis sets is minimal, making them suitable for applications where BSSE correction is either cumbersome or impractical to do. After confirming the reliability of NAO basis sets for Kr, we proceed to calculate the Helmholtz free energy for Kr crystal at the theoretical level of RPA plus renormalized single excitation correction. From this, we derive the pressure-volume (P-V) diagram, which shows excellent agreement with the latest experimental data. Our work demonstrates the capability of correlation-consistent NAO basis sets for heavy elements, paving the way toward numerically reliable correlated calculations for bulk materials.

Basis-Set-Error-Free Random-Phase Approximation Correlation Energies for Atoms Based on the Sternheimer Equation.

The finite basis set errors for all-electron random-phase approximation (RPA) correlation energy calculations are analyzed for isolated atomic systems. We show that, within the resolution-of-identity (RI) RPA framework, the major source of the basis set errors is the incompleteness of the single-particle atomic orbitals used to expand the Kohn-Sham eigenstates, instead of the auxiliary basis set (ABS) to represent the density response function χ0 and the bare Coulomb operator v. By solving the Sternheimer equation for the first-order wave function on a dense radial grid, we are able to eliminate the major error─the incompleteness error of the single-particle atomic basis set─for atomic RPA calculations. The error stemming from a finite ABS can be readily rendered vanishingly small by increasing the size of the ABS, or by iteratively determining the eigenmodes of the χ0v operator. The variational property of the RI-RPA correlation energy can be further exploited to optimize the ABS in order to achieve fast convergence of the RI-RPA correlation energy. These numerical techniques enable us to obtain basis-set-error-free RPA correlation energies for atoms, and in this work, such energies for atoms from H to Kr are presented. The implications of the numerical techniques developed in the present work for addressing the basis set issue for molecules and solids are discussed.