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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, ƁdƔm Gali, Sheng Meng, Zhi-Heng Loh
InstitutionsHUN-REN Wigner Research Centre for Physics, Budapest University of Technology and Economics
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 (NVāˆ’) 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 NVāˆ’ center occur primarily in the lowest vibronic level of the 3E state.