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arXiv:2405.16280 · Physical Review Letters

Probing Electric-Dipole-Enabled Transitions in the Excited State of the Nitrogen-Vacancy Center in Diamond

Tom Delord, Richard Monge, Gabriel I. López‐Morales, Olaf Bach, Cyrus E. Dreyer, Johannes Flick, Carlos A. Meriles

Published Nov 6, 2025• 5 citations
arXivHTMLPDF

Abstract

The excited orbitals of color centers often show strong electric dipoles, which can serve as a resource for entanglement, emission tuning, or electric field sensing. Here, we use resonant laser excitation to examine the electric transitions in the excited state (ES) orbitals of the negatively charged nitrogen vacancy center in diamond. By applying microwave electric fields, we perform Rabi driving between ES orbitals, and show that the dressed states can be tuned in frequency and are protected against fluctuations of the transverse electric field. In contrast with previous results, we observe sharp microwave resonances between magnetic states of the ES orbitals, and find that they are broadened due to simultaneous electric dipole driving.

DOI
10.1103/hp9c-rh23

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The excited orbitals of color centers often show strong electric dipoles, which can serve as a resource for entanglement, emission tuning, or electric field sensing. Here, we use resonant laser excitation to examine the electric transitions in the excited state (ES) orbitals of the negatively charged nitrogen vacancy center in diamond. By applying microwave electric fields, we perform Rabi driving between ES orbitals, and show that the dressed states can be tuned in frequency and are protected against fluctuations of the transverse electric field. In contrast with previous results, we observe sharp microwave resonances between magnetic states of the ES orbitals, and find that they are broadened due to simultaneous electric dipole driving.
We study the resonant optical transitions of a single nitrogen-vacancy (NV) center that is coherently dressed by a strong mechanical drive. Using a gigahertz-frequency diamond mechanical resonator that is strain coupled to a NV center's orbital states, we demonstrate coherent Raman sidebands out to the ninth order and orbital-phonon interactions that mix the two excited-state orbital branches. These interactions are spectroscopically revealed through a multiphonon Rabi splitting of the orbital branches which scales as a function of resonator driving amplitude and is successfully reproduced in a quantum model. Finally, we discuss the application of mechanical driving to engineering NV-center orbital states.
The negatively charged nitrogen vacancy (NV${}^{\ensuremath{-}}$) center in diamond is a well-known color center with interesting applications in nanoscale sensing and quantum metrology, due to its high sensitivity to minute local electric, magnetic, and strain fields. Motivated by these applications of the this center, the authors employ here first-principles calculations based on quantum embedding to derive a many-body description of its excited-state dipole couplings and strain susceptibilities, which underlie the electric field and strain induced Stark effects.
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.
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.
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 present results of our research on two-field (two-frequency) microwave spectroscopy in nitrogen-vacancy ($\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$) color centers in a diamond. Both fields are tuned to transitions between the spin sublevels of the $\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$ ensemble in the 3A2{}^{3}{A}_{2}3A2​ ground state (one field has a fixed frequency while the second one is scanned). Particular attention is focused on the case where two microwave fields drive the same transition between two $\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$ ground state sublevels (${m}_{\mathrm{s}}=0\ensuremath{\leftrightarrow}{m}_{\mathrm{s}}=+1$). In this case, the observed spectra exhibit a complex narrow structure composed of three Lorentzian resonances positioned at the pump-field frequency. The resonance widths and amplitudes depend on the lifetimes of the levels involved in the transition. We attribute the spectra to coherent population oscillations induced by the two nearly degenerate microwave fields, which we have also observed in real time. The observations agree well with a theoretical model and can be useful for investigation of the NV relaxation mechanisms.