Work

Application of the aperiodic defect model to a negatively charged monovacancy in phosphorene

Year: 2026

Type: article

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 toward 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: The Journal of Chemical Physics

DOI: 10.1063/5.0335485

Authors: Charlotte Rickert, Lily Barta, Ernst-Christian Flach, Daniel Kats, Denis Usvyat

Institutions: Humboldt-Universität zu Berlin, Max Planck Institute for Solid State Research

Language: English

Topic: Advanced Chemical Physics Studies

Subfield: Atomic and Molecular Physics, and Optics

Field: Physics and Astronomy

Domain: Physical Sciences

Open Access status: hybrid

Estimated APC paid: $3,500

Funder: Studienstiftung des Deutschen Volkes