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Title: Jahn-Teller-induced femtosecond electronic depolarization dynamics of the nitrogen-vacancy defect in diamond
Authors: Ulbricht, Ronald
Dong, Shuo
Chang, I-Ya
Mariserla, Bala Murali Krishna
Dani, Keshav M.
Hyeon-Deuk, Kim
Loh, Zhi-Heng
Keywords: Chemical Physics
Optical Properties of Diamond
Issue Date: 2016
Source: Ulbricht, R., Dong, S., Chang, I.-Y., Mariserla, B. M. K., Dani, K. M., Hyeon-Deuk, K., et al. (2016). Jahn-Teller-induced femtosecond electronic depolarization dynamics of the nitrogen-vacancy defect in diamond. Nature Communications, 7, 13510-.
Series/Report no.: Nature Communications
Abstract: Single-photon emission from the nitrogen-vacancy defect in diamond constitutes one of its many proposed applications. Owing to its doubly degenerate 3E electronic excited state, photons from this defect can be emitted by two optical transitions with perpendicular polarization. Previous measurements have indicated that orbital-selective photoexcitation does not, however, yield photoluminescence with well-defined polarizations, thus hinting at orbital-averaging dynamics even at cryogenic temperatures. Here we employ femtosecond polarization anisotropy spectroscopy to investigate the ultrafast electronic dynamics of the 3E state. We observe subpicosecond electronic dephasing dynamics even at cryogenic temperatures, up to five orders of magnitude faster than dephasing rates suggested by previous frequency- and time-domain measurements. Ab initio molecular dynamics simulations assign the ultrafast depolarization dynamics to nonadiabatic transitions and phonon-induced electronic dephasing between the two components of the 3E state. Our results provide an explanation for the ultrafast orbital averaging that exists even at cryogenic temperatures.
ISSN: 2041-1723
DOI: 10.1038/ncomms13510
Schools: School of Physical and Mathematical Sciences 
Rights: © 2016 The Author(s). This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit
Fulltext Permission: open
Fulltext Availability: With Fulltext
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