An Ultrafast Shakedown Reveals the Energy Landscape, Relaxation Dynamics, and Concentration of the N3VH0 Defect in Diamond
- 17 July 2020
- journal article
- research article
- Published by American Chemical Society (ACS) in The Journal of Physical Chemistry Letters
- Vol. 11 (16), 6677-6683
- https://doi.org/10.1021/acs.jpclett.0c01806
Abstract
Atomic-scale defects can control the exploitable optoelectronic performance of crystalline materials, and several point defects in diamond are emerging functional components for a range of quantum technologies. Nitrogen and hydrogen are common impurities incorporated into diamond, and there is a family of defects that includes both. The N3VH0 defect is a lattice vacancy where three nearest neighbor carbon atoms are replaced with nitrogen atoms and a hydrogen is bonded to the remaining carbon. It is regularly observed in natural and high-temperature annealed synthetic diamond, and gives rise to prominent absorption features in the mid-infrared. Here, we combine time- and spectrally-resolved infrared absorption spectroscopy to yield unprecedented insight into the N3VH0 defect’s vibrational dynamics following infrared excitation of the C–H stretch. In doing so, we gain fundamental information about the energies of quantized vibrational states, and corroborate our results with theory. We map out, for the first time, energy relaxation pathways, which include multiphonon relaxation processes and anharmonic coupling to the C–H bend mode. These advances provide new routes to quantify and probe atomic-scale defects.Funding Information
- Engineering and Physical Sciences Research Council (EP/N010825/1)
- Royal Society
- Leverhulme Trust
- Office of Naval Research (N62909-16-1-2111-P00002)
This publication has 26 references indexed in Scilit:
- Nitrogen in DiamondChemical Reviews, 2020
- Quantum technologies with optically interfaced solid-state spinsNature Photonics, 2018
- The nitrogen-vacancy colour centre in diamondPhysics Reports, 2013
- Colour-causing defects and their related optoelectronic transitions in single crystal CVD diamondJournal of Physics: Condensed Matter, 2013
- Charge transfer effects, thermo and photochromism in single crystal CVD synthetic diamondJournal of Physics: Condensed Matter, 2009
- Single defect centres in diamond: A reviewPhysica Status Solidi (a), 2006
- Hydrogen Incorporation in Diamond: The Vacancy-Hydrogen ComplexPhysical Review Letters, 2004
- Hydrogen Incorporation in Diamond: The Nitrogen-Vacancy-Hydrogen ComplexPhysical Review Letters, 2003
- High Carrier Mobility in Single-Crystal Plasma-Deposited DiamondScience, 2002
- Origin of Surface Conductivity in DiamondPhysical Review Letters, 2000