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arXiv:2303.00073 · Advanced Sensor Research

Cross‐Correlated Quantum Thermometry Using Diamond Containing Dual‐Defect Centers

Madhav Gupta, Tongtong Zhang, Lambert Yeung, Jiahua Zhang, Yayin Tan, Yau Chuen Yiu, Shuxiang Zhang, Qi Wang, Zhongqiang Wang, Zhiqin Chu

Published Sep 10, 2023• 5 citations
arXivHTMLPDF

Abstract

Abstract The contactless temperature measurement at micro/nanoscale is vital to a broad range of fields in modern science and technology. The nitrogen‐vacancy (NV) center, a kind of diamond defect with unique spin‐dependent photoluminescence, is recognized as one of the most promising nanothermometers. However, this quantum thermometry technique is prone to a number of possible perturbations, which will unavoidably degrade its actual temperature sensitivity. Here, for the first time, a cross‐validated optical thermometry method is developed using a bulk diamond sample containing both NV centers and silicon‐vacancy (SiV) centers, achieving a sensitivity of 22 and 86 mK (√Hz) −1 respectively. Particularly, the latter has been intrinsically immune to those influencing perturbations for the NV‐based quantum thermometry, hence serving as a real‐time cross‐validation system. As a proof‐of‐concept demonstration, a trustworthy temperature measurement is shown under the influence of varying magnetic fields, which is a common artefact present in practical systems. This multi‐modality approach allows synchronized cross‐validation of the measured temperature, which is required for micro/nanoscale quantum thermometry in complicated environments such as a living cell.

DOI
10.1002/adsr.202300103

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Journal of the Chinese Chemical Society•Dec 19, 2022•8 citations
Abstract The contactless temperature measurement at micro/nanoscale is vital to a broad range of fields in modern science and technology. The nitrogen‐vacancy (NV) center, a kind of diamond defect with unique spin‐dependent photoluminescence, is recognized as one of the most promising nanothermometers. However, this quantum thermometry technique is prone to a number of possible perturbations, which will unavoidably degrade its actual temperature sensitivity. Here, for the first time, a cross‐validated optical thermometry method is developed using a bulk diamond sample containing both NV centers and silicon‐vacancy (SiV) centers, achieving a sensitivity of 22 and 86 mK (√Hz) −1 respectively. Particularly, the latter has been intrinsically immune to those influencing perturbations for the NV‐based quantum thermometry, hence serving as a real‐time cross‐validation system. As a proof‐of‐concept demonstration, a trustworthy temperature measurement is shown under the influence of varying magnetic fields, which is a common artefact present in practical systems. This multi‐modality approach allows synchronized cross‐validation of the measured temperature, which is required for micro/nanoscale quantum thermometry in complicated environments such as a living cell.
We demonstrate fluorescence thermometry techniques with sensitivities approaching 10 mK · Hz(-1/2) based on the spin-dependent photoluminescence of nitrogen vacancy (NV) centers in diamond. These techniques use dynamical decoupling protocols to convert thermally induced shifts in the NV center's spin resonance frequencies into large changes in its fluorescence. By mitigating interactions with nearby nuclear spins and facilitating selective thermal measurements, these protocols enhance the spin coherence times accessible for thermometry by 45-fold, corresponding to a 7-fold improvement in the NV center's temperature sensitivity. Moreover, we demonstrate these techniques can be applied over a broad temperature range and in both finite and near-zero magnetic field environments. This versatility suggests that the quantum coherence of single spins could be practically leveraged for sensitive thermometry in a wide variety of biological and microscale systems.
Accurate temperature readings of transient events at the nanometer scale are challenging due to the low sensitivity of available sensors. Nanodiamonds containing nitrogen-vacancy (NV) centers have been used for nanoscale thermometry in complex environments, including inside living cells. However, their performance has been limited by short coherence times and low photon counts. In this work, we use isotopically-purified dual-NV nanodiamonds and a bespoke quantum sensing chip to showcase an order of magnitude improvement in temperature measurement sensitivity compared with previous reports. We demonstrate robust temperature measurements with an error of 682 μμμK, experimental sensitivities below 50 mK/√Hz\surd \text{Hz}√Hz and a shot-noise limited sensitivity of 9.6 mK/√Hz\surd \text{Hz}√Hz. To confirm the utility of these high-performance nanothermometers, we quantify the temperature change induced by the thermometry measurement itself, specifically the optical excitation laser used to probe the NV spin state. In addition, we observe directly at the nanometre scale the transient heating caused by the exothermic mixing of dimethyl sulfoxide in water. Sub-millikelvin resolution and millikelvin sensitivity thermometry unlock the possibility of monitoring minute thermal fluctuations in living systems and assessing catalyst performance at the nanometre scale.
Modern sensing applications increasingly require the simultaneous measurement of multiple physical parameters with high sensitivity. However, traditional sensors often suffer from cross-sensitivity to different variables, making it difficult to separate overlapping effects, such as those caused by temperature and magnetic fields, in complex environments. This challenge highlights the need for robust multiparametric sensors capable of independently and accurately monitoring diverse conditions in real time. In this context, nitrogen-vacancy (NV) centers in diamond present a promising solution. These atomic-scale defects can be optically initialized, manipulated, and read out via laser excitation using optically detected magnetic resonance (ODMR), and they can operate under ambient and harsh conditions. In this work, we demonstrate a simultaneous and internally cross-validated sensing platform capable of detecting both magnetic fields and temperature with a sensitivity of around 500 nT/Hz and 10 mK/Hz, respectively. Our method integrates ODMR, zero-phonon line spectral shifts, and linewidth broadening, each providing independent spectral signatures sensitive to distinct physical effects. This approach enhances measurement precision, enables internal consistency checks, and decouples intertwined phenomena such as temperature-induced variations in magnetization. The demonstrated technique significantly expands the functional capabilities of NV-based sensors, advancing their potential for high-precision metrology in complex environments.
Abstract We demonstrate a method for thermal detection that is the sensitivity 6.2 mK Hz −1 2 , which uses the frequency lock closed-loop scheme to track Zeeman-split resonance of nitrogen-vacancy (NV) centers in diamond. The NV diamond surface acts as a temperature measurement sensor to transfer the temperature variation as D ( T ) parameter change to lead to the movement of the energy levels to detect the temperature. By frequency modulation technology and closed-loop feedback locking technology, automatic temperature detection and step signal reading are realized, with a resolution of 7.6 mK. It is found that the closed-loop output is basically unchanged, while the open-loop output has an error signal proportional to the laser fluctuation. The closed-loop feedback technique can improve the stability and resolution of the system and provides a method for measuring the actual temperature detection. Such a demonstration marks a vital advance in transitioning the NV thermometer from a laboratory system to a functional device for detecting temperature fields in a practical environment.
In modern-day quantum metrology, quantum sensors are widely employed to detect weak magnetic fields or nanoscale signals. Quantum devices, exploiting quantum coherence, are inevitably connected to physical constants and can achieve accuracy, repeatability, and precision approaching fundamental limits. As a result, these sensors have shown utility in a wide range of research domains spanning both science and technology. A rapidly emerging quantum sensing platform employs atomic-scale defects in crystals. In particular, magnetometry using nitrogen-vacancy (NV) color centers in diamond has garnered increasing interest. NV systems possess a combination of remarkable properties, optical addressability, long coherence times, and biocompatibility. Sensors based on NV centers excel in spatial resolution and magnetic sensitivity. These diamond-based sensors promise comparable combination of high spatial resolution and magnetic sensitivity without cryogenic operation. The above properties of NV magnetometers promise increasingly integrated quantum measurement technology, as a result, they have been extensively developed with various protocols and find use in numerous applications spanning materials characterization, nuclear magnetic resonance (NMR), condensed matter physics, paleomagnetism, neuroscience and living systems biology, and industrial vector magnetometry. In this chapter, NV centers are explored for magnetic sensing in a number of contexts. In general, we introduce novel regimes for magnetic-field probes with NV ensembles. Specifically, NV centers are developed for sensitive magnetometers for applications where microwaves (MWs) are prohibitively invasive and operations need to be carried out under zero ambient magnetic field. The primary goal of our discussion is to improve the utility of these NV center-based magnetometers.
Abstract The neutral nitrogen‐vacancy (NV0) defects in diamond are photostable color centers, suitable for a wide range of applications in science and engineering. However, the photophysical properties of the centers have not yet been fully characterized. This work measured the stimulated emission cross sections of NV0 in a single‐crystal diamond by two‐photon excitation of its matrix at 344 nm. From the measured photoluminescence spectrum and the fluorescence lifetime of 20 ± 1 ns, we determined a peak stimulated emission cross section of 1.43 ± 0.07 × 10−17 cm2 at 650 nm for the NV0 centers. In addition, we have also examined the thermal shifts of the zero‐phonon line of NV0 centers in nanoscale diamonds (~100 nm in diameter) over the temperature range of 30–120°C. A temperature measurement sensitivity of 0.2 K·Hz−1/2 was achieved, which is about two‐fold better than that of NV−, despite that the fluorescence intensity of NV0 is about six‐fold lower than that of NV− in the same nanoparticles. The result is attributed to the smaller electron–phonon coupling strength of the neutral center, compared with its negatively charged counterpart.