Abstract
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 excited state of negatively charged nitrogen vacancy () defects. The experimental results reveal vibrational relaxation in the phonon sideband with a time constant of approximately 50 fs, in excellent agreement with the -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 center occur primarily in the lowest vibronic level of the state.
- Received 13 April 2018
- Revised 21 May 2018
DOI:https://doi.org/10.1103/PhysRevB.97.220302
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