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arXiv:2206.11362

Quantifying NV-center Spectral Diffusion by Symmetry

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

Published Jun 22, 2022• 2 citations
arXivHTMLPDF

Abstract

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.

DOI
10.48550/arxiv.2206.11362

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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.
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.
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.
Abstract Nitrogen-vacancy (NV) defect centers in diamond are key to applications in quantum sensing and quantum computing. They create localized electronic states in the diamond lattice with distinct population relaxation pathways following photoexcitation that ultimately enable its unique properties. The defect is known to exist in two charge states: neutral and negative, with respectively one and two known optically-active electronic transitions. Here, we report on the observation of a large number of hitherto undiscovered excited electronic states in both charge states as evidenced by distinct optical transitions in the infrared to ultraviolet part of the spectrum. These transitions are observed by monitoring the electronic relaxation of NV centers after photoexcitation using transient absorption spectroscopy, directly probing transient phenomena occurring on timescales from femtoseconds to microseconds. We also for the first time probed the electron transfer dynamics from the 3 E state of NV− to nearby single-substitutional nitrogen defects (N s ) that leads to the well-known effect of NV photoluminescence quenching.
Abstract Many applications of nitrogen-vacancy (NV) centers in diamond crucially rely on a spectrally narrow and stable optical zero-phonon line transition. Though many impressive proof-of-principle experiments have been demonstrated, much work remains in engineering NV centers with spectral properties that are sufficiently robust for practical implementation. To elucidate the mechanisms underlying their interactions with the environment, we apply multi-dimensional coherent spectroscopy to an NV center ensemble in bulk diamond at cryogenic temperatures. Our spectra reveal thermal dephasing due to quasi-localized vibrational modes as well as ultrafast spectral diffusion on the picosecond timescale. The intrinsic, ensemble-averaged homogeneous linewidth is found to be in the tens of GHz range by extrapolating to zero temperature. We also observe a temperature-dependent Stark splitting of the excited state manifold, relevant to NV sensing protocols.
Silicon has turned from a niche laboratory-scale material into the backbone of modern electronics. Diamond functionalized with color centers could follow a similar path and grow from proof-of-concepts experiments to application-oriented quantum technologies. Quantum sensing, communication, and information processing with color centers has been proven to work in scientific experiments and enhanced sensitivities as well as novel functionalities have been reported. While the first generation of diamond quantum devices relied on color centers formed uncontrolled in natural diamond with a high statistical variation in composition and crystallinity, the situation has changed nowadays. With the emergence of high purity monocrystals and the option for isotopic purification of the carbon matrix, technological progress in materials science on the atomic-scale enabled tailoring the spin properties in diamond. But, since many color centers typically require vacancies to combine with impurities in the carbon lattice via diffusion, the generation of color centers underlies a statistical process providing only little control on the center's final position in the crystal lattice. The negatively charged nitrogen-vacancy (NV−^-−) center is the most studied optically active defect in diamond and exhibits remarkable spin properties and sensing capabilities, even on the nanoscale and at room temperature. The spin properties of NV−^-− centers close to the surface (1\,nm - 30\,nm) have been thoroughly studied and the deeper the spins are located in diamond the less decoherence from surface defects is observed. Creating NV−^-− centers at the surface by nitrogen ion implantation and burying them beneath a thin diamond layer via chemical vapor deposition (CVD) of diamond is reported to enhance the coherence times significantly. By separating the color center generation from controlling the resulting depth by an additional diamond layer, narrow depth profiles can be achieved by reducing the ion energy during implantation. Although the coherence properties improve, many of the implanted NV−^-− center are reported to vanish in the hydrogen-rich plasma of growth CVD chambers. The mechanism responsible for the instability of NV−^-− centers towards the plasma remains unclear, though. One hypothesis is the formation of nitrogen-vacancy-hydrogen centers from diffusing hydrogen and implanted NV−^-− centers but is has not been proven, yet. Here, we demonstrate the fabrication of depth confined NV−^-− centers by combining low energy (1\,keV - 5\,keV) ion implantation and CVD overgrowth. By increasing the thickness of the overgrown layer (6\,nm - 100\,nm) the influence of surface noise is shown to decrease leading to bulk-like coherence properties of up to $450\,\upmu$s (Hahn-echo) and T2∗T_2^*T2∗​ dephasing times around $20\,\upmu$s. Monitoring the NV−^-− density as a function of the overgrowth time, we analyze the kinetics of the passivation in case of implanting ion doses of 1011^{11}11 15^{15}15N +^{+}+/cm2^22 and 1012^{12}12 15^{15}15N +^{+}+/cm2^22. The passivation turns out to occur faster for lower doses offering insights into sub-surface hydrogen diffusion in diamond. Analyzing the spin bath before and after overgrowth reveals a drastic reduction in paramagnetic spins after the CVD process but no NVH−^-− is found around the surviving NV−^-− centers. Checking the chemical composition in overgrown implantation sites with secondary-ion-mass-specrometry (SIMS), however, confirms significant amounts of hydrogen in the 15^{15}15N-implanted layers. Since the concentration found for hydrogen exceeds the one for nitrogen by far, we suggest that diffusing hydrogen interacts also with vacancies forming probably mostly diamagnetic defects. In the last part of this dissertation, NV−^-− centers are generated with sub-nanometer precision below a thin 13^{13}13C-enriched layer for quantum simulation. For fabricating the spin architecture starting from a 12^{12}12C base layer, we overgrow implanted nitrogen with a 13^{13}13C layer and bury the spins beneath a 30\,nm-thick 12^{12}12C capping layer. By measuring the coupling strength between the electron and nuclear spins, we deduce a NV−^-− placement accuracy reaching below one nanometer with respect to the 13^{13}13C-layer. Regarding the spin properties of the electron spins, no reduction in T2T_2T2​ is observed despite of the proximity to the dense 13^{13}13C-bath. As a consequence, the overgrowth of NV−^-− centers is demonstrated as a bottom-up approach to produce buried spin architectures with sharp isotopic transitions and efficient 13^{13}13C-NV−^-− coupling. Together with the potential for bulk-like coherence properties the synergy of implantation and overgrowth is a powerful tool to fabricate reproducible quantum systems with tailored properties and high depth confinement.