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Physical Review Applied

Quantifying the Spectral Diffusion of N- V Centers by Symmetry

Brendan McCullian, Hil Fung Harry Cheung, H. Y. Chen, Gregory D. Fuchs

Published Dec 5, 2022• 23 citations
Publisher

Abstract

The spectrally narrow, spin-dependent optical transitions of nitrogen-vacancy (N-$V$) center defects in diamond can be harnessed for quantum networking applications. Key to such networking schemes is the generation of indistinguishable photons. Two challenges limit scalability in such systems: defect-to-defect variations of the optical transition frequencies caused by local strain variation, and spectral diffusion of the optical frequencies on repeated measurement caused by photoexcitation of nearby charge traps. In this experimental study we undertake a group-theoretic approach to quantifying spectral diffusion and strain, decomposing each into components corresponding to Jahn-Teller symmetries of the N-$V$ center. We investigate correlations between the components of strain, spectral diffusion, and depth from the surface, finding that strain and spectral diffusion are each dominated by longitudinal perturbations. We also find a weak negative correlation between transverse static strain and total spectral diffusion, suggesting that transverse strain provides some degree of protection from spectral diffusion. Additionally, we find that spectral diffusion becomes more pronounced with increasing depth in the diamond bulk. Our symmetry-decomposed technique for quantifying spectral diffusion can be valuable for understanding how a given nanoscale charge trap environment influences spectral diffusion and for developing strategies of mitigation.

DOI
10.1103/physrevapplied.18.064011

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The spectrally narrow, spin-dependent optical transitions of nitrogen-vacancy (N-VVV) center defects in diamond can be harnessed for quantum networking applications. Key to such networking schemes is the generation of indistinguishable photons. Two challenges limit scalability in such systems: defect-to-defect variations of the optical transition frequencies caused by local strain variation, and spectral diffusion of the optical frequencies on repeated measurement caused by photoexcitation of nearby charge traps. In this experimental study we undertake a group-theoretic approach to quantifying spectral diffusion and strain, decomposing each into components corresponding to Jahn-Teller symmetries of the N-VVV center. We investigate correlations between the components of strain, spectral diffusion, and depth from the surface, finding that strain and spectral diffusion are each dominated by longitudinal perturbations. We also find a weak negative correlation between transverse static strain and total spectral diffusion, suggesting that transverse strain provides some degree of protection from spectral diffusion. Additionally, we find that spectral diffusion becomes more pronounced with increasing depth in the diamond bulk. Our symmetry-decomposed technique for quantifying spectral diffusion can be valuable for understanding how a given nanoscale charge trap environment influences spectral diffusion and for developing strategies of mitigation.
The spectrally narrow, spin-dependent optical transitions of nitrogen vacancy (NV) center defects in diamond can be harnessed for quantum networking applications. Key to such networking schemes is the generation of indistinguishable photons. Two challenges limit scalability in such systems: defect-to-defect variations of the optical transition frequencies caused by local strain variation, and spectral diffusion of the optical frequencies on repeated measurement caused by photoexcitation of nearby charge traps. In this experimental study we undertake a group theoretic approach to quantifying spectral diffusion and strain, decomposing each into components corresponding to Jahn-Teller symmetries of the NV center. We investigate correlations between the components of strain, spectral diffusion, and depth from surface, finding that strain and spectral diffusion are each dominated by longitudinal perturbations. We also find a weak negative correlation between transverse static strain and total spectral diffusion suggesting that transverse strain provides some degree of protection from spectral diffusion. Additionally, we find that spectral diffusion becomes more pronounced with increasing depth in the diamond bulk. Our symmetry-decomposed technique for quantifying spectral diffusion can be valuable for understanding how a given nanoscale charge trap environment influences spectral diffusion and for developing strategies of mitigation.
Spectral diffusion is the phenomenon of random jumps in the emission wavelength of narrow lines. This phenomenon is a major hurdle for applications of solid state quantum emitters like quantum dots, molecules, or diamond defect centers in an integrated quantum optical technology. Here, we provide further insight into the underlying processes of spectral diffusion of the zero-phonon line of single nitrogen vacancy centers in nano-size diamond by using a novel method based on photon correlation interferometry. The method works although the spectral diffusion rate is several orders of magnitude higher than the photon detection rate and thereby improves the time resolution of previous experiments with nano-size diamond by 6 orders of magnitude. We study the dependency of the spectral diffusion rate on the excitation power, temperature, and excitation wavelength under off-resonant excitation. Our results bring insight into the mechanism of spectral diffusion and suggest a strategy to increase the number of spectrally indistinguishable photons emitted by diamond nanocrystals.
Quantum emitters in diamond are leading optically accessible solid-state qubits. Among these, Group IV-vacancy defect centers have attracted great interest as coherent and stable optical interfaces to long-lived spin states. Theory indicates that their inversion symmetry provides first-order insensitivity to stray electric fields, a common limitation for optical coherence in any host material. Here we experimentally quantify this electric field dependence via an external electric field applied to individual tin-vacancy (SnV) centers in diamond. These measurements reveal that the permanent electric dipole moment and polarizability are at least 4 orders of magnitude smaller than for the diamond nitrogen vacancy (NV) centers, representing the first direct measurement of the inversion symmetry protection of a Group IV defect in diamond. Moreover, we show that by modulating the electric-field-induced dipole we can use the SnV as a nanoscale probe of local electric field noise, and we employ this technique to highlight the effect of spectral diffusion on the SnV.
The negatively charged nitrogen-vacancy $({\mathrm{NV}}^{\ensuremath{-}})$ center in diamond is a promising candidate for many quantum applications. Here, we examine the splitting and broadening of the center's infrared (IR) zero-phonon line (ZPL). We develop a model for these effects that accounts for the strain induced by photodependent microscopic distributions of defects. We apply this model to interpret observed variations of the IR ZPL shape with temperature and photoexcitation conditions. We identify an anomalous temperature-dependent broadening mechanism and that defects other than the substitutional nitrogen center significantly contribute to strain broadening. The former conclusion suggests the presence of a strong Jahn-Teller effect in the center's singlet levels and the latter indicates that major sources of broadening are yet to be identified. These conclusions have important implications for the understanding of the center and the engineering of diamond quantum devices. Finally, we propose that, once the major sources of broadening are identified, the IR ZPL has the potential to be a sensitive spectroscopic tool for probing microscopic strain fields and performing defect tomography.
Point defects in semiconductors are becoming central to quantum technologies. They can be used as spin qubits interfacing with photons, which are fundamental for building quantum networks. Currently, the most prominent quantum defect in diamond is the nitrogen-vacancy (NV) center. However, it suffers from spectral diffusion that negatively impacts optical coherence and is due to the coupling of the emission energy with uncontrolled electric fields. The group IV vacancy complexes on the other hand have shown to be significantly more spectrally-stable as they are centrosymmetric and thus immune to the linear Stark shift. They however suffer from several issues ranging from low operation temperature to low optical efficiency due to dark states and difficulty in stabilizing the right defect charge state. Here we search for alternative to the group IV vacancy complex in diamond by systematically evaluating all possible vacancy complex using high-throughput first-principles computational screening. We identify the defects that combine centrosymmetry, emission in the visible range, as well as favorable and achievable electronic structure promoting higher operation temperature and defect levels well within the band gap. We find ZnV−2V^{-2}V−2 to be especially appealing.
Silicon-vacancy (SiV) centers in diamond are promising systems for quantum information applications due to their bright single-photon emission and optically accessible spin states. Furthermore, SiV centers in low-strain diamond are insensitive to perturbations of the dielectric environment; i.e., they show very weak spectral diffusion. This property renders ensembles of SiV centers interesting for sensing applications. We here report on photoluminescence excitation (PLE) spectroscopy on an SiV ensemble in a low strain, chemical vapor deposition-grown high-quality diamond layer, where we measure the fine structure with high resolution and obtain the line widths and splittings of the SiV centers. We investigate the temperature dependence of the width and position of the fine structure peaks. Our measurements reveal line widths of about 10 GHz as compared to a lifetime limited width on the order of 0.1 GHz. This difference arises from the inhomogeneous broadening of the transitions caused by residual strain. To overcome inhomogeneous broadening we use spectral hole burning spectroscopy, which enables us to measure a nearly lifetime limited homogeneous line width of 279 MHz. Furthermore, we demonstrate evidence of coherent interaction in the system by driving a $\mathrm{\ensuremath{\Lambda}}$ scheme. Additional measurements on single emitters created by ion implantation confirm the homogeneous line widths seen in the spectral hole burning experiments and relate the ground-state splitting to the decoherence rate.