Dataset for "Many-body Theory Calculations of Positron Binding to Halogenated Hydrocarbons"

The dataset includes the input files for EXCITON+ that include the Gaussian basis parameters and molecular geometries used. A zip of the input files (bse.inp and INPUT) required to run the EXCITON+ code for each molecule considered in related publication. The zip consists of subdirectories named after each molecule. Each molecule's subdirectory contains the two input files bse.inp and INPUT.

Abstract for "Many-body Theory Calculations of Positron Binding to Halogenated Hydrocarbons":
Positron binding energies in halogenated hydrocarbons are calculated \emph{ab initio} using many-body theory. For chlorinated molecules, including planars for which the interaction is highly anisotropic, very good to excellent agreement with experiment and recent DFT-based model-potential calculations is found. Predictions for fluorinated and brominated molecules are presented. The comparative effect of fluorination, chlorination and bromination is elucidated by identifying trends within molecular families including dihaloethylenes and halomethanes based on global molecular properties (dipole moment, polarizability, ionization energy). It is shown that relative to brominated and chlorinated molecules, fluorinated molecules generate a less attractive positron-molecule potential due to larger ionization energies and smaller density of molecular orbitals close to the HOMO, resulting in very weak, or in most cases loss of, positron binding. Overall, however, it is shown that the global molecular properties are not universal predictors of binding energies, exemplified by consideration of CH3Cl vs.~\emph{cis.}-C2H2F2: despite the latter having a larger dipole moment, lower ionization energy and similar polarizability its binding energy is significantly smaller (25 meV vs.~3 meV, respectively), owing to the important contribution of multiple molecular orbitals to, and the anisotropy of, the positron-molecule correlation potential.