This paper reports the calculated relaxed lattice configurations and corresponding electronic and magnetic structures, and Raman frequencies of two divacancies in diamond, V2 and VC=CV, in which the vacancies are first and third neighbours, respectively. The calculations are formulated within a supercell approach to local defects in crystalline solids, here 64- and 128-atom unit cells and based largely on the B3LYP one-electron approximation constructed from an all-electron Gaussian basis set. Three important findings are first, that, of the four possible spin states, Sz= 0, 1, 2, 3, the singlet is predicted to be lowest in energy for both divacancies; second, that the singlet state of V2 is ∼ 1.7 eV lower in energy than that in VC=CV; and third, that the Raman peak at 1628 cm- 1 in defective diamond can be ascribed to the presence of a C=C double bond, as in the singlet state of VC=CV. © 2018, Springer-Verlag GmbH Germany, part of Springer Nature.

Looking for sp2carbon atoms in diamond: a quantum mechanical study of interacting vacancies

Sansone, Giuseppe;Salustro, Simone;Maschio, Lorenzo;Dovesi, Roberto
2018-01-01

Abstract

This paper reports the calculated relaxed lattice configurations and corresponding electronic and magnetic structures, and Raman frequencies of two divacancies in diamond, V2 and VC=CV, in which the vacancies are first and third neighbours, respectively. The calculations are formulated within a supercell approach to local defects in crystalline solids, here 64- and 128-atom unit cells and based largely on the B3LYP one-electron approximation constructed from an all-electron Gaussian basis set. Three important findings are first, that, of the four possible spin states, Sz= 0, 1, 2, 3, the singlet is predicted to be lowest in energy for both divacancies; second, that the singlet state of V2 is ∼ 1.7 eV lower in energy than that in VC=CV; and third, that the Raman peak at 1628 cm- 1 in defective diamond can be ascribed to the presence of a C=C double bond, as in the singlet state of VC=CV. © 2018, Springer-Verlag GmbH Germany, part of Springer Nature.
2018
137
29
1
9
http://link.springer-ny.com/link/service/journals/00214/index.htm
Defects; Diamond; Raman; Simulation; Vibrations; Physical and Theoretical Chemistry
Sansone, Giuseppe; Salustro, Simone*; Noël, Yves; Maschio, Lorenzo; Mackrodt, William C.; Dovesi, Roberto
File in questo prodotto:
File Dimensione Formato  
Sansone_Divacancies.pdf

Accesso aperto

Descrizione: Articolo
Tipo di file: POSTPRINT (VERSIONE FINALE DELL’AUTORE)
Dimensione 8.24 MB
Formato Adobe PDF
8.24 MB Adobe PDF Visualizza/Apri

I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/2318/1664267
Citazioni
  • ???jsp.display-item.citation.pmc??? ND
  • Scopus 9
  • ???jsp.display-item.citation.isi??? 9
social impact