Vibrational relaxation dynamics of the nitrogen-vacancy center in diamond

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...

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Bibliographic Details
Main Authors: Ulbricht, Ronald, Dong, Shuo, Gali, Adam, Meng, Sheng, Loh, Zhi-Heng
Other Authors: School of Physical and Mathematical Sciences
Format: Article
Language:English
Published: 2018
Subjects:
Vibrational Energy Relaxation
Nitrogen Vacancy
DRNTU::Science::Physics
Online Access:https://hdl.handle.net/10356/80429
http://hdl.handle.net/10220/46490
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Institution: Nanyang Technological University
Language: English
Description
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.

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