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arXiv:1112.5490 · Physical Review Letters

Dynamic Stabilization of the Optical Resonances of Single Nitrogen-Vacancy Centers in Diamond

Víctor M. Acosta, Charles Santori, Andrei Faraon, Zhihong Huang, Kai‐Mei C. Fu, Alastair D. Stacey, David Simpson, Kumaravelu Ganesan, Snjezana Tomljenovic‐Hanic, Andrew D. Greentree, Steven Prawer, Raymond G. Beausoleil

Published May 14, 2012• 147 citations
arXivHTMLPDF

Abstract

We report electrical tuning by the Stark effect of the excited-state structure of single nitrogen-vacancy (NV) centers located ≲100 nm from the diamond surface. The zero-phonon line (ZPL) emission frequency is controllably varied over a range of 300 GHz. Using high-resolution emission spectroscopy, we observe electrical tuning of the strengths of both cycling and spin-altering transitions. Under resonant excitation, we apply dynamic feedback to stabilize the ZPL frequency. The transition is locked over several minutes and drifts of the peak position on timescales ≳100 ms are reduced to a fraction of the single-scan linewidth, with standard deviation as low as 16 MHz (obtained for an NV in bulk, ultrapure diamond). These techniques should improve the entanglement success probability in quantum communications protocols.

DOI
10.1103/physrevlett.108.206401

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Bulletin of the American Physical Society•Feb 29, 2012•0 citations
We report electrical tuning by the Stark effect of the excited-state structure of single nitrogen-vacancy (NV) centers located ≲100 nm from the diamond surface. The zero-phonon line (ZPL) emission frequency is controllably varied over a range of 300 GHz. Using high-resolution emission spectroscopy, we observe electrical tuning of the strengths of both cycling and spin-altering transitions. Under resonant excitation, we apply dynamic feedback to stabilize the ZPL frequency. The transition is locked over several minutes and drifts of the peak position on timescales ≳100 ms are reduced to a fraction of the single-scan linewidth, with standard deviation as low as 16 MHz (obtained for an NV in bulk, ultrapure diamond). These techniques should improve the entanglement success probability in quantum communications protocols.
We demonstrate precise control over the zero-phonon optical transition energies of individual nitrogen-vacancy (NV) centers in diamond by applying multiaxis electric fields, via the dc Stark effect. The Stark shifts display surprising asymmetries that we attribute to an enhancement and rectification of the local electric field by photoionized charge traps in the diamond. Using this effect, we tune the excited-state orbitals of strained NV centers to degeneracy and vary the resulting degenerate optical transition frequency by >10 GHz, a scale comparable to the inhomogeneous frequency distribution. This technique will facilitate the integration of NV-center spins within photonic networks.
Photoluminescence (PL) spectra of single nitrogen vacancy (NV) centers in 50-nm diamond nanocrystals at the zero-phonon line (ZPL) were directly observed using a Fabry-Perot interferometer at cryogenic temperatures. The narrowest linewidth of ZPL was 1.2 GHz (1.9 ± 0.7 GHz on average), comparable to ZPL linewidths in PL spectra reported for NV centers in pure bulk diamond. This observation is important to the application of NV centers for use in quantum communication and computation devices, and in nano-sensing.
Lifetime-limited optical excitation lines of single nitrogen-vacancy (NV) defect centers in diamond have been observed at liquid helium temperature. They display unprecedented spectral stability over many seconds and excitation cycles. Spectral tuning of the spin-selective optical resonances was performed via the application of an external electric field (i.e., the Stark shift). A rich variety of Stark shifts were observed including linear as well as quadratic components. The ability to tune the excitation lines of single NV centers has potential applications in quantum information processing.
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.
Nitrogen-vacancy (NV) centers in diamond can be read out optically or electrically. To better understand the physics of their internal electronic transitions as well as ionization and recharging, we study the spin contrast observed in both readout methods as a function of the excitation wavelength for both single NV centers and ensembles. While the optical readout works best between 525 and 550 nm, the highest electrical spin contrast is achieved by resonantly exciting the NV0 zero-phonon line at 575 nm. Additional spectral features attributed to a further excited state of NV−, phonon sidebands and tunnel coupling to nitrogen donors are observed and discussed.
For quantum information applications, nitrogen-vacancy (NV) centers in diamond combine many of the advantages of atomic systems (optical access, millisecond spin-coherence times) with the engineering flexibility of solid-state devices. Recent demonstrations of coherent coupling between photons and individual NV-center spins [1,2] provide a route to integrating NV-center qubits within photonic networks and for on-demand generation of entangled single-spin/single-photon pairs. Such applications require the ability to tune the NV-center zero-phonon optical transitions, to compensate for natural sample inhomogeneities which perturb the electronic orbital states. Here we demonstrate the ability to electrically control the orbitals of individual NV centers by applying voltages to micron-scale surface gates [3]. Surprisingly, the local electric field experienced by an NV center is significantly enhanced by a photoinduced space charge resulting from photoionization of deep donor impurities within the diamond, even in high-purity single-crystal material (< 5 ppb nitrogen content). Since the photoinduced electric fields are reproducible as a function of gate voltage and are predominantly directed perpendicular to the diamond surface, we can harness them to obtain three-dimensional control of the local electric field vector with surface gates alone. To demonstrate this technique, we tune the excited-state orbital doublet of a strained NV center to degeneracy, as required for some spin-photon entanglement protocols [2], and then adjust the optical transition frequency, showing that we can tune multiple NV centers to have the same degenerate transition energy. This method should enable the coherent coupling of multiple NV center spins to indistinguishable photons within a scalable photonic network.