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Vibrational relaxation dynamics of the nitrogen-vacancy center in diamond

MetadataDetails
Publication Date2018-06-08
JournalPhysical review. B./Physical review. B
AuthorsRonald Ulbricht, Shuo Dong, Ádåm Gali, Sheng Meng, Zhi-Heng Loh
InstitutionsChinese Academy of Sciences, Hungarian Academy of Sciences
Citations26

We employ a combination of spectrally resolved optical pump-probe spectroscopy and excited-state ab initio molecular dynamics (ESAIMD) simulations to study the ultrafast vibrational relaxation dynamics of the 3E excited state of negatively charged nitrogen vacancy (NV−) defects. The experimental results reveal vibrational relaxation in the phonon sideband with a time constant of approximately 50 fs, in excellent agreement with the ∼40-fs structural equilibration timescale predicted by ESAIMD simulations. The observed ultrafast vibrational energy relaxation implies that dynamical processes triggered by photoexcitation into the phonon sideband of the NV− center occur primarily in the lowest vibronic level of the 3E state.