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.
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.
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.
Quantum sensing has witnessed rapid development and transition from laboratories to practical applications in the past decade. Applications of quantum sensors, ranging from nanotechnologies to biosensing, are expected to benefit from quantum sensors' unprecedented spatial resolution and sensitivity. Solid-state spin systems are particularly attractive platforms for quantum sensing technologies because room temperature operation is viable while reaching the quantum limits of sensitivity. Among various solid-state spin systems, nitrogen-vacancy (NV) centers in diamond demonstrated high-fidelity initialization, coherent control, and high contrast readout of the electron spin state. However, electron spin coherence due to noise from the surrounding spin bath and this environment effect limits the sensitivity of NV centers. Thus, a critical task in NV center-based quantum sensing is sensitivity enhancement through coherence protection. Several strategies, such as dynamical decoupling techniques, feedback control, and nuclear spin-assisted sensing protocols, have been developed and realized for this task. Among these strategies, nuclear spin-assisted protocols have demonstrated greater enhancement of electron spin coherence. In addition, the electron and nuclear spin pair of an NV center in diamond naturally allows the application of the nuclear spin-assisted sensitivity enhancement protocol. Owing to long nuclear coherence times, further enhancement of sensitivity can be achieved by exploiting active nuclear spins (e.g., 14N, 13C) in the proximity of an NV center as memory ancillas when coupled with the NV center. Here, we review the spin properties of NV centers, mechanisms of the nuclear spin-assisted protocol and its gate variation, and the status of quantum sensing applications in high-resolution nuclear spin spectroscopy, atomic imaging, and magnetic field sensing. We discuss the potential for commercialization, current challenges in sensitivity enhancement, and conclude with future research directions for promoting the development of nuclear spin-assisted protocol and its integration into industrial applications.
Laser-induced fluorescence quenching in nitrogen-vacancy (NV) centers in diamond is studied simultaneously with in situ measurements of the heating-induced shift of the electron spin resonance of NV centers in the presence of a microwave field. These experiments reveal a strong correlation between fluorescence suppression in NV centers and the rise of the local temperature inside the diamond crystal. This finding sheds light on quantum pathways behind stimulated fluorescence quenching in NV centers of diamond and may imply significant limitations on the applications of this effect as a method of superresolving imaging in biological systems.
The Nitrogen-Vacancy (NV) center is becoming a promising qubit for quantum information processing. The defect has a long coherence time at room temperature and it allows spin state initialized and read out by laser and manipulated by microwave pulses. It has been utilized as a ultra sensitive probe for magnetic fields and remote spins as well. Here, we review the recent progresses in experimental demonstrations based on NV centers. We first introduce our work on implementation of the Deutsch-Jozsa algorithm with a single electronic spin in diamond. Then the quantum nature of the bath around the center spin is revealed and continuous wave dynamical decoupling has been demonstrated. By applying dynamical decoupling, a multi-pass quantum metrology protocol is realized to enhance phase estimation. In the final, we demonstrated NV center can be regarded as a ultra-sensitive sensor spin to implement nuclear magnetic resonance (NMR) imaging at nanoscale.
Nitrogen vacancy centers in diamond are among the leading solid state quantum platforms, offering exceptional spatial resolution and sensitivity for applications such as magnetic field sensing, thermometry, and bioimaging. However, in high background environments,such as those encountered in in vitro diagnostics, the performance of NV based sensors can be compromised by strong background fluorescence, particularly from substrates such as nitrocellulose. In this work, we analytically and experimentally investigate the use of pulsed laser excitation combined with time gating techniques to suppress background fluorescence and enhance the signal to noise ratio in NV based quantum sensing, with an emphasis on spin enhanced biosensing. Through experimental studies using mixed ensembles of silicon vacancy and NV centers in bulk diamond, as well as fluorescent nanodiamonds on NC substrates, we demonstrate significant improvements in NV spin resonance visibility, demonstrated by an increase of the SNR by up to 4x, and a resulting measurement time reduction by 16x. The presented technique and results here can help significantly increase the readout efficiency and speed in future applications of NV centers in high background environments, such as in IVD, where the NV centers are used as a fluorescent label for biomolecules.
We study the spin and orbital dynamics of single nitrogen vacancy (NV) centers in diamond between room temperature and 700 K. We find that the ability to optically address and coherently control single spins above room temperature is limited by nonradiative processes that quench the NV center’s fluorescence-based spin readout between 550 K and 700 K. Combined with electronic structure calculations, our measurements indicate that the energy difference between the E and A1 electronic states is ∼0.8 eV. We also find that the inhomogeneous spin lifetime (T ∗ 2 ) is independent of temperature up to at least 625 K, suggesting that single NV centers could be applied as nanoscale thermometers over a broad temperature range.