Vibrational relaxation dynamics of the nitrogen-vacancy center in diamond
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 res...
| Main Authors: | , , , , |
|---|---|
| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2018
|
| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/80429 http://hdl.handle.net/10220/46490 |
| Summary: | 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. |
|---|