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arXiv:2302.00011 · Physical Review Letters

Temperature-Dependent Photophysics of Single NV Centers in Diamond

Jodok Happacher, Juanita Bocquel, Hossein T. Dinani, Märta A. Tschudin, Patrick Reiser, David A. Broadway, Jeronimo R. Maze, Patrick Maletinsky

Published Aug 24, 2023• 26 citations
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Abstract

We present a comprehensive study of the temperature- and magnetic-field-dependent photoluminescence (PL) of individual NV centers in diamond, spanning the temperature-range from cryogenic to ambient conditions. We directly observe the emergence of the NV's room-temperature effective excited-state structure and provide a clear explanation for a previously poorly understood broad quenching of NV PL at intermediate temperatures around 50 K, as well as the subsequent revival of NV PL. We develop a model based on two-phonon orbital averaging that quantitatively explains all of our findings, including the strong impact that strain has on the temperature dependence of the NV's PL. These results complete our understanding of orbital averaging in the NV excited state and have significant implications for the fundamental understanding of the NV center and its applications in quantum sensing.

DOI
10.1103/physrevlett.131.086904

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We present a comprehensive study of the temperature- and magnetic-field-dependent photoluminescence (PL) of individual NV centers in diamond, spanning the temperature-range from cryogenic to ambient conditions. We directly observe the emergence of the NV's room-temperature effective excited-state structure and provide a clear explanation for a previously poorly understood broad quenching of NV PL at intermediate temperatures around 50 K, as well as the subsequent revival of NV PL. We develop a model based on two-phonon orbital averaging that quantitatively explains all of our findings, including the strong impact that strain has on the temperature dependence of the NV's PL. These results complete our understanding of orbital averaging in the NV excited state and have significant implications for the fundamental understanding of the NV center and its applications in quantum sensing.
We investigate the magnetic field dependent photophysics of individual nitrogen-vacancy (NV) color centers in diamond under cryogenic conditions. At distinct magnetic fields, we observe significant reductions in the NV photoluminescence rate, which indicate a marked decrease in the optical readout efficiency of the NV's ground state spin. We assign these dips to excited state level anticrossings, which occur at magnetic fields that strongly depend on the effective, local strain environment of the NV center. Our results offer new insights into the structure of the NVs' excited states and a new tool for their effective characterization. Using this tool, we observe strong indications for strain-dependent variations of the NV's orbital g factor, obtain new insights into NV charge state dynamics, and draw important conclusions regarding the applicability of NV centers for low-temperature quantum sensing.
We report on measurements of the photoluminescence properties of single nitrogen-vacancy centers in diamond at temperatures between 4 K and 300 K. We observe a strong reduction of the PL intensity and spin contrast between ca. 10 K and 100 K that recovers to high levels below and above. Further, we find a rich dependence on magnetic bias field and crystal strain. We develop a comprehensive model based on spin mixing and orbital hopping in the electronic excited state that quantitatively explains the observations. Beyond a more complete understanding of the excited-state dynamics, our work provides a novel approach for probing electron-phonon interactions and a predictive tool for optimizing experimental conditions for quantum applications.
The nitrogen vacancy (NV) center in diamond is well known for its outstanding optical and spin properties, enabling various applications in quantum sensing and quantum information at both cryogenic and ambient temperatures. Despite a large body of work, however, the NV center's dynamics at intermediate temperatures are incompletely understood. This paper describes a basic rate model able to explain the NV population dynamics over the full parameter space of temperature, crystallographic strain, and magnetic field. Numerical simulations of the model are in excellent agreement with experiments discussed in the accompanying PRL.
The emission intensity of diamond samples containing negatively charged nitrogen-vacancy centres are measured as a function of magnetic field along the ⟨111⟩ direction for various temperatures. At low temperatures the responses are sample and stress dependent and can be modelled in terms of the previous understanding of the 3 E excited state fine structure which is strain dependent. At room temperature the responses are largely sample and stress independent, and modelling involves invoking a strain independent excited state with a single zero field spin-level splitting of 1.42 GHz. The change in behaviour is attributed to a temperature dependent averaging process over the components of the excited state orbital doublet. It decouples orbit and spin and at high temperature the spin levels become independent of any orbit splitting. One significant implication of this averaging is that it simplifies the development of room temperature applications.
Abstract Transverse-magnetic-field-induced spin mixing in nitrogen-vacancy (NV) centers hybridizes the |0⟩ and | ± 1⟩ manifolds, degrading optical spin polarization and spin-dependent fluorescence and thereby limiting optically detected magnetic resonance (ODMR) contrast and quantum-sensor fidelity. While recent work has clarified key elements of NV photophysics, how spin mixing evolves with temperature under device-relevant operating conditions─and how it intertwines with charge-state dynamics─remains insufficiently quantified. Here we perform systematic magnetic-field-temperature (B-T) mapping of transverse-field-induced photoluminescence (PL) quenching in an ensemble of NV centers. By spectrally resolving the NV– and NV0 zero-phonon-line emission, we disentangle spin-mixing-driven contrast loss within NV– from correlated changes in charge-state-resolved fluorescence. We introduce an operational critical field Bc extracted from the PL-contrast line shape, which provides a compact, reproducible figure-of-merit for transverse-field robustness and enables straightforward comparison across temperatures and field geometries. The measured temperature dependence of Bc is captured by a concise model incorporating phonon-mediated excited-state orbital dynamics, establishing a predictive framework for optimizing operating conditions and benchmarking ensemble NV sensing platforms.
We report a study of the 3E excited-state structure of single negatively charged nitrogen-vacancy (NV) defects in diamond, combining resonant excitation at cryogenic temperatures and optically detected magnetic resonance. A theoretical model is developed and shows excellent agreement with experimental observations. In addition, we show that the two orbital branches associated with the 3E excited state are averaged when operating at room temperature. This study leads to an improved physical understanding of the NV defect electronic structure, which is invaluable for the development of diamond-based quantum information processing.