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Physical Review Letters

Temperature Dependence of Photoluminescence Intensity and Spin Contrast in Nitrogen-Vacancy Centers

S. Ernst, Patrick Scheidegger, S. Diesch, Luca Lorenzelli, Christian L. Degen

Published Aug 24, 2023• 24 citations
Publisher

Abstract

Two photoluminescence experiments and models of nitrogen-vacancy centers in diamond over broad temperature ranges improve our understanding of the photodynamics of vacancy centers and other spin defects.
DOI
10.1103/physrevlett.131.086903

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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.
Nitrogen-vacancy (NV) centers in single-crystal CVD diamond are promising candidates for quantum sensing due to their remarkable optical and spin properties [1]. These defects exhibit stable photoluminescence (PL), long spin coherence times, and high sensitivity to external fields [2]. In this study, we present a room-temperature PL characterization of NV centers excited with a 532 nm laser. The setup was optimized for high signal-to-noise ratio and spectral resolution. Key parameters analyzed include emission intensity, zero-phonon line (ZPL) at ~637 nm, phonon sidebands, and the charge state distribution between NV⁰ and NV⁻. The NV⁻ state, crucial for spin-based sensing, is evaluated to understand its stability under different nitrogen doping conditions [3]. The relative intensities of NV⁰ and NV⁻ provide insights into nitrogen incorporation and vacancy formation. These results contribute to optimizing synthesis conditions for enhanced NV⁻ concentration, supporting the advancement of diamond-based quantum sensing technologies.
The photodynamics of diamond nitrogen-vacancy (NV) centers limits their performance in many quantum technologies. Quenching of photoluminescence, which degrades NV readout, is commonly ascribed to a dark state that is not fully understood. Using a nanoscale cavity to generate intense infrared fields that quench NV emission nonlinearly with field intensity, we show that the dark state is accessed by two-photon pumping into the 4 ⁣A2^4\!A_24A2​ quartet state of the neutrally charged NV (NV0^00). We constrain this state's energy relative to the NV0^00 ground-state (2 ⁣E^2\!E2E) to <0.58{<}0.58<0.58\,eV and the recombination energy threshold to the NV−^-− ground state (3 ⁣A2^3\!A_23A2​) to ≤2.33 eV\leq2.33\,\text{eV}≤2.33eV. Furthermore, we estimate the intrinsic lifetime of 4 ⁣A2^4\!A_24A2​ state to be 1.78−6.06 μs1.78-6.06\,μ\text{s}1.78−6.06μs and show that accessing this state allows sensing of local infrared fields. This new understanding will allow predictions of the limits of NV technologies reliant upon intense fields, including levitated systems, spin--optomechanical devices, and absorption--based magnetometers.