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arXiv:2006.02323 · Physical Review Letters

Hidden Silicon-Vacancy Centers in Diamond

Christopher L. Smallwood, Ronald Ulbricht, Matthew W. Day, Tim Schröder, Kelsey M. Bates, Travis M. Autry, Geoffrey Diederich, Edward S. Bielejec, Mark E. Siemens, Steven T. Cundiff

Published May 24, 2021• 41 citations
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Abstract

We characterize a high-density sample of negatively charged silicon-vacancy (SiV^{-}) centers in diamond using collinear optical multidimensional coherent spectroscopy. By comparing the results of complementary signal detection schemes, we identify a hidden population of SiV^{-} centers that is not typically observed in photoluminescence and which exhibits significant spectral inhomogeneity and extended electronic T_{2} times. The phenomenon is likely caused by strain, indicating a potential mechanism for controlling electric coherence in color-center-based quantum devices.

DOI
10.1103/physrevlett.126.213601

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We characterize a high-density sample of negatively charged silicon-vacancy (SiV^{-}) centers in diamond using collinear optical multidimensional coherent spectroscopy. By comparing the results of complementary signal detection schemes, we identify a hidden population of SiV^{-} centers that is not typically observed in photoluminescence and which exhibits significant spectral inhomogeneity and extended electronic T_{2} times. The phenomenon is likely caused by strain, indicating a potential mechanism for controlling electric coherence in color-center-based quantum devices.
Color centers in diamond are point defects within the diamond host lattice that absorb and emit light at optical frequencies. Besides contributing to the striking visual characteristics of "fancy colored" diamonds as gemstones, the centers--particularly the negatively charged nitrogen-vacancy (NV) center and silicon-vacancy (SiV-) center--offer a number of possibilities for quantum computation and quantum information processing. In this talk, I will summarize recent progress made in characterizing negatively charged silicon-vacancy centers in diamond using the technique of optical multidimensional coherent spectroscopy (MDCS). By comparing photoluminescence-based and heterodyne-detection based signal collection schemes in a high-density SiV- center sample, we have selectively identified a population of long-lived and nonradiative silicon-vacancy centers in diamond with more than 40 times as much inhomogeneous spectral broadening as the radiative silicon-vacancy center states that are more commonly observed using photoluminescence. Estimates of the degree of inhomogeneity and overall sample characteristics indicate that strain is likely to play a large role in the formation of these nonradiative states. The findings open possibilities for being able to actively tune the degree of radiative coupling in silicon-vacancy center systems, opening possibilities for new types of quantum-optical devices.
Negatively charged silicon-vacancy (SiV−^-−) centers in diamond offer an attractive platform for the development of many forms of quantum technology. However, questions remain in connection to how large ensembles of SiV−^-− centers behave in concert. Here, we develop a computational model designed to simulate recent experiments where optical multidimensional coherent spectroscopy (MDCS) was used to examine a high-concentration sample of SiV−^-− centers in diamond, revealing significant variations in spectral signature depending on the detection scheme. Simulation results reveal that strain effects are highly random in this system, with a characteristic axial strain of 2.8×10−42.8 \times 10^{-4}2.8×10−4 and a shear strain of 3.5×10−53.5 \times 10^{-5}3.5×10−5. They suggest in addition that highly strained centers (with values exceeding 1.5×10−51.5 \times 10^{-5}1.5×10−5) may become significantly decoupled from optical emission. The results have implications for the use of SiV−^-− centers as quantum sensors.
An ensemble of silicon vacancy (SiV−) centers in diamond is probed using two-pulse correlation spectroscopy and multidimensional coherent spectroscopy. Two main distinct families of SiV− centers are identified, and these families are paired with two orientation groups by comparing spectra from different linear polarizations of the incident laser. By tracking the peak centers in the measured spectra, the full diamond strain tensor is calculated local to the laser spot. Measurements are made at multiple points on the sample surface, and variations in the strain tensor are observed.
Electrically driven emission from negatively charged silicon-vacancy (SiV)− centers in single crystal diamond is demonstrated. The SiV centers were generated using ion implantation into an i region of a p-i-n single crystal diamond diode. Both electroluminescence and the photoluminescence signals exhibit the typical emission that is attributed to the (SiV)− centers. Under forward and reversed biased PL measurements, no signal from the neutral (SiV)0 defect could be observed. The realization of electrically driven (SiV)− emission is promising for scalable nanophotonics devices employing color centers in single crystal diamond.