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Physical Review Applied

Magnetic-Field-Assisted Spectral Decomposition and Imaging of Charge States of N - V Centers in Diamond

Tanmoy Chakraborty, R. Bhattacharya, V. S. Anjusha, Miloš Nesládek, Dieter Suter, T. S. Mahesh

Published Feb 16, 2022• 5 citations
Publisher

Abstract

With the advent of quantum technology, nitrogen vacancy ($\mathrm{N}$-$V$) centers in diamond turn out to be a frontier that provides an efficient platform for quantum computation, communication, and sensing applications. Due to the coupled spin-charge dynamics of the $\mathrm{N}$-$V$ system, knowledge of $\mathrm{N}$-$V$ charge-state dynamics can help to formulate efficient spin-control sequences strategically. Here, we report two spectroscopy-based deconvolution methods to create charge-state mapping images of ensembles of $\mathrm{N}$-$V$ centers in diamond. First, relying on the fact that an off-axis external magnetic field mixes the electronic spins and selectively modifies the photoluminescence (PL) of $\mathrm{N}$-${V}^{\ensuremath{-}}$, we perform decomposition of the optical spectrum for an ensemble of $\mathrm{N}$-$V$ and extract the spectra for $\mathrm{N}$-${V}^{\ensuremath{-}}$ and $\mathrm{N}$-${V}^{0}$ states. Next, we introduce an optical-filter-based decomposition protocol and perform PL imaging for $\mathrm{N}$-${V}^{\ensuremath{-}}$ and $\mathrm{N}$-${V}^{0}$. Previously obtained spectra for $\mathrm{N}$-${V}^{\ensuremath{-}}$ and $\mathrm{N}$-${V}^{0}$ states are used to calculate their transmissivities through a long-pass optical filter. These results help us to determine the spatial distribution of the $\mathrm{N}$-$V$ charge states in a diamond sample.

DOI
10.1103/physrevapplied.17.024046

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With the advent of quantum technology, nitrogen vacancy (N\mathrm{N}N-VVV) centers in diamond turn out to be a frontier that provides an efficient platform for quantum computation, communication, and sensing applications. Due to the coupled spin-charge dynamics of the N\mathrm{N}N-VVV system, knowledge of N\mathrm{N}N-VVV charge-state dynamics can help to formulate efficient spin-control sequences strategically. Here, we report two spectroscopy-based deconvolution methods to create charge-state mapping images of ensembles of N\mathrm{N}N-VVV centers in diamond. First, relying on the fact that an off-axis external magnetic field mixes the electronic spins and selectively modifies the photoluminescence (PL) of N\mathrm{N}N-V\ensuremath−{V}^{\ensuremath{-}}V\ensuremath−, we perform decomposition of the optical spectrum for an ensemble of N\mathrm{N}N-VVV and extract the spectra for N\mathrm{N}N-V\ensuremath−{V}^{\ensuremath{-}}V\ensuremath− and N\mathrm{N}N-V0{V}^{0}V0 states. Next, we introduce an optical-filter-based decomposition protocol and perform PL imaging for N\mathrm{N}N-V\ensuremath−{V}^{\ensuremath{-}}V\ensuremath− and N\mathrm{N}N-V0{V}^{0}V0. Previously obtained spectra for N\mathrm{N}N-V\ensuremath−{V}^{\ensuremath{-}}V\ensuremath− and N\mathrm{N}N-V0{V}^{0}V0 states are used to calculate their transmissivities through a long-pass optical filter. These results help us to determine the spatial distribution of the N\mathrm{N}N-VVV charge states in a diamond sample.
With the advent of quantum technology, nitrogen vacancy (NVNVNV) centers in diamond turn out to be a frontier which provides an efficient platform for quantum computation, communication and sensing applications. Due to the coupled spin-charge dynamics of the NVNVNV system, knowledge about NVNVNV charge state dynamics can help to formulate efficient spin control sequences strategically. Through this paper we report two spectroscopy-based deconvolution methods to create charge state mapping images of ensembles of NVNVNV centers in diamond. First, relying on the fact that an off axis external magnetic field mixes the electronic spins and selectively modifies the photoluminescence (PL) of NV−NV^-NV−, we perform decomposition of the optical spectrum for an ensemble of NVNVNVs and extract the spectra for NV−NV^-NV− and NV0NV^0NV0 states. Next, we introduce an optical filter based decomposition protocol and perform PL imaging for NV−NV^-NV− and NV0NV^0NV0. Earlier obtained spectra for NV−NV^-NV− and NV0NV^0NV0 states are used to calculate their transmissivities through a long pass optical filter. These results help us to determine the spatial distribution of the NVNVNV charge states in a diamond sample.
Magnetic sensing and imaging using ensembles of nitrogen-vacancy (N-VVV) centers in diamond recently have found application in disciplines as wide-ranging as condensed matter physics, biology, and paleomagnetism. However, distinguishing the signals from the four inequivalent N-VVV orientations requires an external magnetic field, which can hinder the study of some magnetic samples. The authors present an $a\phantom{\rule{0}{0ex}}l\phantom{\rule{0}{0ex}}l-o\phantom{\rule{0}{0ex}}p\phantom{\rule{0}{0ex}}t\phantom{\rule{0}{0ex}}i\phantom{\rule{0}{0ex}}c\phantom{\rule{0}{0ex}}a\phantom{\rule{0}{0ex}}l$ method to tease apart the signals at arbitrary bias fields, by exploiting the distribution of photoluminescence at the Fourier plane of a microscope. Their technique will help N-VVV-based magnetic sensing reach its full potential.
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.
Nitrogen vacancy (NV) centers in diamond are at the heart of many emerging quantum technologies, all of which require control over the NV charge state. Hence, methods for quantification of the relative photoluminescence intensities of the NV0 and NV− charge states, i.e., a charge state ratio, are vital. Several approaches to quantify NV charge state ratios have been reported but are either limited to bulk-like NV diamond samples or yield qualitative results. We propose an NV charge state quantification protocol based on the determination of sample- and experimental setup-specific NV0 and NV− reference spectra. The approach employs blue (400–470 nm) and green (480–570 nm) excitation to infer pure NV0 and NV− spectra, which are then used to quantify NV charge state ratios in subsequent experiments via least squares fitting. We test our dual excitation protocol (DEP) for a bulk diamond NV sample and 20 and 100 nm nanodiamond particles and compare results with those obtained via other commonly used techniques such as zero-phonon line fitting and non-negative matrix factorization. We find that DEP can be employed across different samples and experimental setups and yields consistent and quantitative results for NV charge state ratios that are in agreement with our understanding of NV photophysics. By providing robust NV charge state quantification across sample types and measurement platforms, DEP will support the development of NV-based quantum technologies.
Characterizing the local internal environment surrounding solid-state spin defects is crucial to harnessing them as nanoscale sensors of external fields. This is especially germane to the case of defect ensembles which can exhibit a complex interplay between interactions, internal fields, and lattice strain. Working with the nitrogen-vacancy (NV) center in diamond, we demonstrate that local electric fields dominate the magnetic resonance behavior of NV ensembles at a low magnetic field. We introduce a simple microscopic model that quantitatively captures the observed spectra for samples with NV concentrations spanning more than two orders of magnitude. Motivated by this understanding, we propose and implement a novel method for the nanoscale localization of individual charges within the diamond lattice; our approach relies upon the fact that the charge induces a NV dark state which depends on the electric field orientation.
The nitrogen vacancy (NV) center in diamond is promising as an electron spin qubit due to its long-lived coherence and optical addressability. The ground state is a spin triplet with two levels $({m}_{s}=\ifmmode\pm\else\textpm\fi{}1)$ degenerate at zero magnetic field. Polarization-selective microwave excitation is an attractive method to address the spin transitions independently since this allows operation down to zero magnetic field. Using a resonator designed to produce circularly polarized microwaves, we have investigated the polarization selection rules of the NV center. We first apply this technique to NV ensembles in [100]- and [111]-oriented samples. Next, we demonstrate an imaging technique, based on optical polarization dependence, which allows rapid identification of the orientations of many single NV centers. Finally, we test the microwave polarization selection rules of individual NV centers of known orientation.