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Nature Communications

The phonon-modulated Jahn–Teller distortion of the nitrogen vacancy center in diamond

William P. Carbery, Camille A. Farfan, Ronald Ulbricht, Daniel B. Turner

Published Oct 5, 2024• 15 citations
Publisher

Abstract

The negatively charged nitrogen vacancy (NV) center in diamond is an optically accessible material defect with a unique combination of spin and optical properties that has attracted interest in quantum-information sciences and as a design candidate for nanoscale quantum sensors. Here, we present time-resolved nonlinear optical spectroscopy measurements, conducted with ultrabroadband laser pulses, that reveal strong modulation of the excited-state by the longitudinal optical (LO) phonon of the diamond lattice. The LO phonon and its overtones geometrically distort neighboring NV centers, driving long lived (3.5 ps) excited state relaxation of coupled NV centers after the initial excitation and ultrafast (<150 fs) decay of the Jahn-Teller distortion. These observations elevate the LO phonon to an important tuning mode of the Jahn-Teller conical intersection and help resolve previous spectroscopy experiments that noted longer-lived excited-state dynamics.

DOI
10.1038/s41467-024-52712-9

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The negatively charged nitrogen vacancy (NV) center in diamond is an optically accessible material defect with a unique combination of spin and optical properties that has attracted interest in quantum-information sciences and as a design candidate for nanoscale quantum sensors. Here, we present time-resolved nonlinear optical spectroscopy measurements, conducted with ultrabroadband laser pulses, that reveal strong modulation of the excited-state by the longitudinal optical (LO) phonon of the diamond lattice. The LO phonon and its overtones geometrically distort neighboring NV centers, driving long lived (3.5 ps) excited state relaxation of coupled NV centers after the initial excitation and ultrafast (<150 fs) decay of the Jahn-Teller distortion. These observations elevate the LO phonon to an important tuning mode of the Jahn-Teller conical intersection and help resolve previous spectroscopy experiments that noted longer-lived excited-state dynamics.
Applications of the negatively charged nitrogen-vacancy center in diamond exploit the center's unique optical and spin properties, which at ambient temperature are predominately governed by electron-phonon interactions. Here, we investigate these interactions at ambient and elevated temperatures by observing the motional narrowing of the center's excited-state spin resonances. We determine that the center's Jahn-Teller dynamics are much slower than currently believed and that they do not solely account for the broadening of the center's optical resonance above cryogenic temperatures. We show that the inclusion of interactions with symmetric phonon modes can explain the observed broadening and resolve the current inconsistencies in the literature. However, our model also reveals unexpected features of the electron-phonon processes that coincide with other poorly understood vibronic features of the center and require further investigation.
We present a first-principles study of the multimode Jahn-Teller (JT) effect in the exctied 3E^{3}E3E state of the negatively charged nitrogen-vacancy (NV) center in diamond. Using density functional theory combined with an intrinsic distortion path (IDP) analysis, we resolve the full activation pathways of the JT distortion and quantitatively decompose the distortion into contributions from individual vibrational modes. We find that multiple vibrational modes participate cooperatively in the JT dynamics, giving rise to a shallow adiabatic potential energy surface with low barriers, consistent with thermally activated pseudorotation. The dominant JT-active modes are found to closely correspond to vibrational features observed in two-dimensional electronic spectroscopy (2DES), in agreement with recent ab initio molecular dynamics simulations. Our results establish a microscopic, mode-resolved picture of vibronic coupling in the excited-state NV center and provide new insight into dephasing, relaxation, and optically driven dynamics relevant to solid-state quantum technologies.
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.
The understanding of the coherence properties of photons emitted from negatively charged nitrogen-vacancy (NV) centers in diamond is essential for the success of quantum information applications based on indistinguishable photons. Here we study both the polarization of photons emitted from and the linewidth of photons absorbed by single NV centers as a function of temperature T. We find that for T < 100 K the main dephasing mechanism contributing to the linewidth broadening is phonon-mediated population transfer between the two excited orbital states. The observed T5 temperature dependence of the population transfer rate and linewidth is experimental evidence of a dynamic Jahn-Teller effect in the excited states.
The negatively charged nitrogen-vacancy (NV(-)) center in diamond is considered to be one of the most promising solid state systems for quantum information applications. Excited states of the NV(-) center play a center role in the proposed applications. Using a combination of first-principles calculations and vibronic interaction model analysis, we establish the presence of a dynamic Jahn-Teller effect in the (3)E excited state. The calculated temperature-dependent dephasing rate for the zero phonon line as well as the splitting of the first two vibronic states are in good agreement with experiment.
Anti-Stokes optical cooling in diamond nitrogen-vacancy (NV) centers is investigated using photoluminescence (PL) spectroscopy, time-resolved measurements, and rate-equation modeling. Under excitation below the zero-phonon line, anti-Stokes emission from the negatively charged NV- state appears, but optical excitation also induces charge-state conversion between NV- and neutral NV0. Excitation-dependent PL dynamics reveal a reduction of the NV- population under strong excitation. A minimal rate-equation model constrained by nanosecond and millisecond PL measurements predicts that photoionization suppresses the NV--mediated cooling contribution and leads to self-limiting cooling behavior. The calculations further show that net cooling requires exceptionally high quantum efficiency and does not increase monotonically with excitation density. These results highlight photoinduced charge-state conversion as a key photophysical bottleneck for defect-based anti-Stokes optical cooling.