Jahn-Teller-induced femtosecond electronic depolarization dynamics of the nitrogen-vacancy defect in diamond

Ronald Ulbricht (), Shuo Dong, I-Ya Chang, Bala Murali Krishna Mariserla, Keshav M. Dani, Kim Hyeon-Deuk () and Zhi-Heng Loh ()
Additional contact information
Ronald Ulbricht: School of Physical and Mathematical Sciences, Nanyang Technological University
Shuo Dong: School of Physical and Mathematical Sciences, Nanyang Technological University
I-Ya Chang: Kyoto University
Bala Murali Krishna Mariserla: Femtosecond Spectroscopy Unit, Okinawa Institute of Science and Technology Graduate University
Keshav M. Dani: Femtosecond Spectroscopy Unit, Okinawa Institute of Science and Technology Graduate University
Kim Hyeon-Deuk: Kyoto University
Zhi-Heng Loh: School of Physical and Mathematical Sciences, Nanyang Technological University

Nature Communications, 2016, vol. 7, issue 1, 1-6

Abstract: 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.

Date: 2016
References: Add references at CitEc
Citations: View citations in EconPapers (3)

Downloads: (external link)
https://www.nature.com/articles/ncomms13510 Abstract (text/html)

Related works:
This item may be available elsewhere in EconPapers: Search for items with the same title.

Export reference: BibTeX RIS (EndNote, ProCite, RefMan) HTML/Text

Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms13510

Ordering information: This journal article can be ordered from
https://www.nature.com/ncomms/

DOI: 10.1038/ncomms13510

Access Statistics for this article

Nature Communications is currently edited by Nathalie Le Bot, Enda Bergin and Fiona Gillespie

More articles in Nature Communications from Nature
Bibliographic data for series maintained by Sonal Shukla () and Springer Nature Abstracting and Indexing ().