AI Insight
This study applies the aperiodic defect model (ADM) to calculate the properties of a negatively charged monovacancy in phosphorene, a two-dimensional material consisting of a single layer of phosphorus atoms. Unlike conventional supercell methods, the ADM embeds a single defect in the true crystalline environment without artificial defect-defect interactions, and reduces the problem to a manageable fragment that allows the use of high-level quantum chemistry methods such as CCSD(T) and EOM-CCSD. The calculations yield a formation energy of 0.81 eV for the vacancy in the (5|9) configuration and an excitation energy of 1.95 eV to the lowest singlet excited state.
Why it matters
Accurate modeling of point defects in two-dimensional materials like phosphorene is critical for the development of semiconductor devices, quantum emitters, and sensors, and the ADM offers a systematically improvable framework that could improve the reliability of defect property predictions across a wide range of solid-state and surface systems.
arXiv:2603.23761v3 Announce Type: replace
Abstract: We apply the recently introduced aperiodic defect model (ADM) to a negatively charged monovacancy in a phosphorene monolayer. In contrast to conventional supercell approaches, the ADM treats a single defect embedded in the true non-defective crystalline mean field thereby avoiding spurious defect-defect interactions and the need for charge corrections. At the same time, it effectively reduces the calculation to a fragment, enabling the use of high-level molecular electronic-structure methods. Converging the Hartree-Fock and correlation contributions to the thermodynamic limit yields a benchmark CCSD(T)/POB-TZVP-rev2 formation energy of 0.81 eV for the negatively charged monovacancy in the (5|9) configuration. The excitation energy to the lowest singlet excited state of this defect at the EOM-CCSD/POB-TZVP-rev2 level is found to be 1.95 eV. Overall, the ADM provides a highly promising route towards quantitatively accurate and systematically improvable descriptions of defects in solids and on surfaces, bridging the gap between solid-state physics and molecular quantum chemistry.
Source: Application of the aperiodic defect model to a negatively charged monovacancy in phosphorene