Complexes of silicon, vacancy, and hydrogen in diamond: A density functional study

Gergo Thiering, A. Gali

Research output: Contribution to journalArticle

11 Citations (Scopus)

Abstract

Paramagnetic luminescent point defects in diamond are increasingly important candidates for quantum information processing applications. Recently, the coherent manipulation of single silicon-vacancy defect spins has been demonstrated in chemical vapor deposited diamond samples where silicon may be introduced as a contamination in the growth process. Hydrogen impurity may simultaneously enter diamond too and form complexes with silicon-vacancy defects. However, relatively little is known about these complexes in diamond. Here we report plane-wave supercell density functional theory results on various complexes of silicon vacancy and hydrogen in diamond. We found a family of complexes of silicon, vacancies, and hydrogen atoms that are thermally stable in diamond with relatively low formation energies that might form yet unobserved or unidentified silicon-related defects. These complexes often show infrared optical transitions and are paramagnetic. We tentatively assign one of these complexes to a recently reported but yet unidentified infrared absorber center. We show that this center has a metastable triplet state and might exhibit a spin-selective decay to the ground state, thus it is an interesting candidate for quantum information processing applications. We also discuss here methodology aspects of calculating hyperfine parameters and intradefect level excitations in systems with notoriously complex electron states within hybrid density functional approach. We also demonstrate that a simplified approach using ab initio data can be very powerful to predict the relative intensities of the phonon replica associated with quasilocal vibration modes in the photoexcitation spectrum.

Original languageEnglish
Article number165203
JournalPhysical Review B - Condensed Matter and Materials Physics
Volume92
Issue number16
DOIs
Publication statusPublished - Oct 20 2015

Fingerprint

Diamond
Silicon
Vacancies
Hydrogen
Diamonds
diamonds
silicon
hydrogen
Defects
defects
Infrared radiation
Optical transitions
Photoexcitation
energy of formation
Point defects
electron states
photoexcitation
replicas
optical transition
point defects

ASJC Scopus subject areas

  • Condensed Matter Physics
  • Electronic, Optical and Magnetic Materials

Cite this

Complexes of silicon, vacancy, and hydrogen in diamond : A density functional study. / Thiering, Gergo; Gali, A.

In: Physical Review B - Condensed Matter and Materials Physics, Vol. 92, No. 16, 165203, 20.10.2015.

Research output: Contribution to journalArticle

@article{b391681ebd344883940e7b2f9625f798,
title = "Complexes of silicon, vacancy, and hydrogen in diamond: A density functional study",
abstract = "Paramagnetic luminescent point defects in diamond are increasingly important candidates for quantum information processing applications. Recently, the coherent manipulation of single silicon-vacancy defect spins has been demonstrated in chemical vapor deposited diamond samples where silicon may be introduced as a contamination in the growth process. Hydrogen impurity may simultaneously enter diamond too and form complexes with silicon-vacancy defects. However, relatively little is known about these complexes in diamond. Here we report plane-wave supercell density functional theory results on various complexes of silicon vacancy and hydrogen in diamond. We found a family of complexes of silicon, vacancies, and hydrogen atoms that are thermally stable in diamond with relatively low formation energies that might form yet unobserved or unidentified silicon-related defects. These complexes often show infrared optical transitions and are paramagnetic. We tentatively assign one of these complexes to a recently reported but yet unidentified infrared absorber center. We show that this center has a metastable triplet state and might exhibit a spin-selective decay to the ground state, thus it is an interesting candidate for quantum information processing applications. We also discuss here methodology aspects of calculating hyperfine parameters and intradefect level excitations in systems with notoriously complex electron states within hybrid density functional approach. We also demonstrate that a simplified approach using ab initio data can be very powerful to predict the relative intensities of the phonon replica associated with quasilocal vibration modes in the photoexcitation spectrum.",
author = "Gergo Thiering and A. Gali",
year = "2015",
month = "10",
day = "20",
doi = "10.1103/PhysRevB.92.165203",
language = "English",
volume = "92",
journal = "Physical Review B-Condensed Matter",
issn = "0163-1829",
publisher = "American Physical Society",
number = "16",

}

TY - JOUR

T1 - Complexes of silicon, vacancy, and hydrogen in diamond

T2 - A density functional study

AU - Thiering, Gergo

AU - Gali, A.

PY - 2015/10/20

Y1 - 2015/10/20

N2 - Paramagnetic luminescent point defects in diamond are increasingly important candidates for quantum information processing applications. Recently, the coherent manipulation of single silicon-vacancy defect spins has been demonstrated in chemical vapor deposited diamond samples where silicon may be introduced as a contamination in the growth process. Hydrogen impurity may simultaneously enter diamond too and form complexes with silicon-vacancy defects. However, relatively little is known about these complexes in diamond. Here we report plane-wave supercell density functional theory results on various complexes of silicon vacancy and hydrogen in diamond. We found a family of complexes of silicon, vacancies, and hydrogen atoms that are thermally stable in diamond with relatively low formation energies that might form yet unobserved or unidentified silicon-related defects. These complexes often show infrared optical transitions and are paramagnetic. We tentatively assign one of these complexes to a recently reported but yet unidentified infrared absorber center. We show that this center has a metastable triplet state and might exhibit a spin-selective decay to the ground state, thus it is an interesting candidate for quantum information processing applications. We also discuss here methodology aspects of calculating hyperfine parameters and intradefect level excitations in systems with notoriously complex electron states within hybrid density functional approach. We also demonstrate that a simplified approach using ab initio data can be very powerful to predict the relative intensities of the phonon replica associated with quasilocal vibration modes in the photoexcitation spectrum.

AB - Paramagnetic luminescent point defects in diamond are increasingly important candidates for quantum information processing applications. Recently, the coherent manipulation of single silicon-vacancy defect spins has been demonstrated in chemical vapor deposited diamond samples where silicon may be introduced as a contamination in the growth process. Hydrogen impurity may simultaneously enter diamond too and form complexes with silicon-vacancy defects. However, relatively little is known about these complexes in diamond. Here we report plane-wave supercell density functional theory results on various complexes of silicon vacancy and hydrogen in diamond. We found a family of complexes of silicon, vacancies, and hydrogen atoms that are thermally stable in diamond with relatively low formation energies that might form yet unobserved or unidentified silicon-related defects. These complexes often show infrared optical transitions and are paramagnetic. We tentatively assign one of these complexes to a recently reported but yet unidentified infrared absorber center. We show that this center has a metastable triplet state and might exhibit a spin-selective decay to the ground state, thus it is an interesting candidate for quantum information processing applications. We also discuss here methodology aspects of calculating hyperfine parameters and intradefect level excitations in systems with notoriously complex electron states within hybrid density functional approach. We also demonstrate that a simplified approach using ab initio data can be very powerful to predict the relative intensities of the phonon replica associated with quasilocal vibration modes in the photoexcitation spectrum.

UR - http://www.scopus.com/inward/record.url?scp=84944726070&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84944726070&partnerID=8YFLogxK

U2 - 10.1103/PhysRevB.92.165203

DO - 10.1103/PhysRevB.92.165203

M3 - Article

AN - SCOPUS:84944726070

VL - 92

JO - Physical Review B-Condensed Matter

JF - Physical Review B-Condensed Matter

SN - 0163-1829

IS - 16

M1 - 165203

ER -