Hunting the elusive shallow n-type donor – An ab initio study of Li and N co-doped diamond

Sergio Conejeros, Muhammad Zamir Othman, Alex Croot, Judy Hart, Kane M O'Donnell, Paul W May*, Neil L Allan*

*Corresponding author for this work

Research output: Contribution to journalArticle (Academic Journal)peer-review

Abstract

We report calculated energetics (at the GGA, and at the B3LYP, HSE06 hybrid density functional levels of theory) and electronic properties (B3LYP, HSE06) of Li and N co-doped diamond containing LiNx clusters (x = 1–4). Defect energies and structural properties at the GGA and hybrid (B3LYP, HSE06) levels of theory are very similar. Our results for isolated Li and N dopants agree with previous work in that they are not suitable candidates for shallow n-type donors. Here, we investigate the effects of addition of N atoms as a co-dopant with Li, which vary with the Li:N ratio and whether Li is interstitial or substitutional. Reaction energies, geometries, bonding and densities of states (DOS) are examined. Nitrogen stabilises substitutional rather than interstitial lithium. Atom-projected DOS show that the chief contributions to the defect states are not from orbitals on the dopant atoms themselves but from states associated with neighbouring carbon atoms. Only the tetrahedral 1:4 cluster, LiCN4, with substitutional Li is likely to behave as a shallow donor. We propose a non-molecular synthetic route for preparation of the LiCN4-doped material via prior generation of the N4V centre at temperatures at which Li is mobile but LiCN4 clusters are not.
Original languageEnglish
Pages (from-to)857-868
Number of pages12
JournalCarbon
Volume171
Early online date25 Sep 2020
DOIs
Publication statusPublished - 1 Jan 2021

Bibliographical note

Funding Information:
The authors are grateful to the Public Service Department, Government of Malaysia, EPSRC grant EP/K030302/1 for financial support and Ben Truscott for his help with the software. S.C. gratefully acknowledges the Becas Chile program (CONICYT PAI/INDUSTRIA 74150058 ) for a postdoctoral grant at the University of Bristol , and FONDECYT Grant 11171063 . This work was carried out using the computational facilities of the Advanced Computing Research Centre, University of Bristol http://www.bris.ac.uk/acrc . The raw data for these calculations can be found on the University of Bristol data repository with d.o.i. 10.5523/bris.2ypb34qlp93ox2spy3k3ql4trd.

Funding Information:
The authors are grateful to the Public Service Department, Government of Malaysia, EPSRC grant EP/K030302/1 for financial support and Ben Truscott for his help with the software. S.C. gratefully acknowledges the Becas Chile program (CONICYT PAI/INDUSTRIA 74150058) for a postdoctoral grant at the University of Bristol, and FONDECYT Grant 11171063. This work was carried out using the computational facilities of the Advanced Computing Research Centre, University of Bristol http://www.bris.ac.uk/acrc. The raw data for these calculations can be found on the University of Bristol data repository with d.o.i. 10.5523/bris.2ypb34qlp93ox2spy3k3ql4trd.

Publisher Copyright:
© 2020 Elsevier Ltd

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