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arXiv:1206.0852 · Physical Review Letters

Measurement of the Ultrafast Spectral Diffusion of the Optical Transition of Nitrogen Vacancy Centers in Nano-Size Diamond Using Correlation Interferometry

Janik Wolters, Nikola Sadzak, Andreas Wolfgang Schell, Tim Schröder, Oliver J. Benson

Published Jan 9, 2013• 121 citations

Abstract

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.

DOI: 10.1103/physrevlett.110.027401

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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.

The zero-phonon transition rate of a nitrogen-vacancy center is enhanced by a factor of ∼70 by coupling to a photonic crystal resonator fabricated in monocrystalline diamond using standard semiconductor fabrication techniques. Photon correlation measurements on the spectrally filtered zero-phonon line show antibunching, a signature that the collected photoluminescence is emitted primarily by a single nitrogen-vacancy center. The linewidth of the coupled nitrogen-vacancy center and the spectral diffusion are characterized using high-resolution photoluminescence and photoluminescence excitation spectroscopy.

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.

Photoluminescence excitation spectroscopy of nitrogen vacancy (NV) centers in type Ib diamond nanocrystals shows that in spite of spectral diffusion and spin-nonconserving transitions, zero-phonon linewidth as small as

16\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}

, which is nearly lifetime limited, can be observed at low temperature. Relatively small effects of spectral diffusion have also been observed in a small fraction of NV centers.

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.

In many quantum architectures the solid-state qubits, such as quantum dots or color centers, are interfaced via emitted photons. However, the frequency of photons emitted by solid-state systems exhibits slow uncontrollable fluctuations over time (spectral diffusion), creating a serious problem for implementation of the photon-mediated protocols. Here we show that a sequence of optical pulses applied to the solid-state emitter can stabilize the emission line at the desired frequency. We demonstrate efficiency, robustness, and feasibility of the method analytically and numerically. Taking nitrogen-vacancy center in diamond as an example, we show that only several pulses, with the width of 1 ns, separated by few ns (which is not difficult to achieve) can suppress spectral diffusion. Our method provides a simple and robust way to greatly improve the efficiency of photon-mediated entanglement and/or coupling to photonic cavities for solid-state qubits.