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The vacancy–hydrogen defect in diamond: A computational study
Author(s) -
Peaker C. V.,
Goss J. P.,
Briddon P. R.,
Horsfall A. B.,
Rayson M. J.
Publication year - 2015
Publication title -
physica status solidi (a)
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.532
H-Index - 104
eISSN - 1862-6319
pISSN - 1862-6300
DOI - 10.1002/pssa.201532215
Subject(s) - vacancy defect , lone pair , diamond , spectroscopy , atomic physics , chemistry , degenerate energy levels , crystallographic defect , electron paramagnetic resonance , atom (system on chip) , hydrogen , charge (physics) , hydrogen atom , condensed matter physics , molecular physics , crystallography , physics , nuclear magnetic resonance , molecule , group (periodic table) , organic chemistry , quantum mechanics , computer science , embedded system
Hydrogen is grown into CVD diamond and occurs in point defects also involving a lattice vacancy, V . Complexes involving V , H and nitrogen, or silicon have been identified by experiment, and in some cases the microscopic structure has been identified with the use of quantum‐chemical simulations. In this study, we present the results of density functional simulations of the primitive vacancy‐hydrogen defect in diamond. We find that the symmetry of the VH defect is C 3 v , with the H atom strongly bonded to one of the four C radicals that are formed when the vacancy is created. The defect is expected to occur in both the neutral and negatively charged forms, with the possibility of both positive and − 2 charge states. For VH 0 , S = 3 / 2 and S = 1 / 2 spin states are found to be indistinguishable in energy, with the quartet not expected to yield sharp optical transitions, unlike the doublet. V H− 1in the S = 1 ground‐state is predicted to have an optical transition that is broadly similar to that of N V − ( S = 1 ), although it is important to note that the non‐degenerate band involved in the transitions arises from a different origin in V H− 1as there are no lone‐pairs present in this case. We have also made predictions for the C–H stretch mode frequencies, noting a general trend with charge state. Combinations of optical spectroscopy, paramagnetic resonance and vibrational mode spectroscopy are therefore required to fully experimentally resolve VH in its various charge and spin states.