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 μK, experimental sensitivities below 50 mK/√Hz and a shot-noise limited sensitivity of 9.6 mK/√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.

High-fidelity multiqubit initialization is vital for quantum simulation, quantum information processing, and quantum sensing. In diamond platforms, nuclear spin registers can be initialized through polarization transfer from a nearby electronic spin whose high gyromagnetic ratio enables efficient dynamical nuclear polarization (DNP). These hybrid systems are typically controlled using diabatic spin rotations, which require precise knowledge of all system parameters. Adiabatic DNP protocols, on the other hand, have less strict requirements and could enable robust and high-fidelity spin transfer. However, due to the slow adiabatic sweeps and limited electron spin coherence times, this approach has remained inaccessible. Here, we demonstrate adiabatic pulsed nuclear spin polarization at room temperature in diamond. We achieve enhanced polarization efficiency, a broad resonance window, and improved tolerance to hyperfine coupling uncertainties relative to conventional diabatic pulsed protocols. We also show how this approach can benefit the initialization of spin clusters. These results set the scene for enhanced qubit initialization in solid state through adiabatic pulsed driving, with applications in solid-state quantum sensor and quantum memory technologies.

Optically addressable spin-based quantum sensors enable nanoscale measurements of temperature, magnetic field, pH, and other physical properties of a system. Advancing the sensors beyond proof-of-principle demonstrations in living cells and multicellular organisms towards reliable, damage-free quantum sensing poses three distinct technical challenges. First, spin-based quantum sensing requires optical accessibility and microwave delivery. Second, any microelectronics must be biocompatible and designed for imaging living specimens. Third, efficient microwave delivery and temperature control are essential to reduce unwanted heating and to maintain an optimal biological environment. Here, we present the Quantum Biosensing Chip (Q-BiC), which facilitates microfluidic-compatible microwave delivery and includes on-chip temperature control. We demonstrate the use of Q-BiC in conjunction with nanodiamonds containing nitrogen vacancy centers to perform optically detected magnetic resonance in living systems. We quantify the biocompatibility of microwave excitation required for optically detected magnetic resonance both in vitro in HeLa cells and in vivo in the nematode Caenorhabditis elegans for temperature measurements and determine the microwave-exposure range allowed before detrimental effects are observed. In addition, we show that nanoscale quantum thermometry can be performed in immobilised but non-anaesthetised adult nematodes with minimal stress. These results enable the use of spin-based quantum sensors without damaging the biological system under study, facilitating the investigation of the local thermodynamic and viscoelastic properties of intracellular processes.

Whirling topological textures play a key role in exotic phases of magnetic materials and are promising for logic and memory applications. In antiferromagnets, these textures exhibit enhanced stability and faster dynamics with respect to their ferromagnetic counterparts, but they are also difficult to study due to their vanishing net magnetic moment. One technique that meets the demand of highly sensitive vectorial magnetic field sensing with negligible backaction is diamond quantum magnetometry. Here we show that an archetypal antiferromagnet-haematite-hosts a rich tapestry of monopolar, dipolar and quadrupolar emergent magnetic charge distributions. The direct read-out of the previously inaccessible vorticity of an antiferromagnetic spin texture provides the crucial connection to its magnetic charge through a duality relation. Our work defines a paradigmatic class of magnetic systems to explore two-dimensional monopolar physics, and highlights the transformative role that diamond quantum magnetometry could play in exploring emergent phenomena in quantum materials.

Nitrogen-vacancy centres in diamond nanocrystals are among the leading candidates for realising nanoscale quantum sensing under ambient conditions. Due to their exceptional electronic spin coherence at room temperature and optical addressability, these solid state spin-based sensors can achieve a wide selection of sensing modalities, including probing temperature, external magnetic and electric field, as well as the detection of nearby electronic and nuclear spins. In this article, we discuss recent progress made utilizing nanodiamond quantum sensors in living systems and explore both opportunities for future advances and challenges that lie ahead.

Next-generation biological sensors and diagnostic tools require high sensitivity and spatial resolution to be able to identify emergent biological behaviour. Correlating multiple interdependent parameters at the nanoscale could help uncover details of cellular response to external perturbations. Temperature and viscosity are key parameters of interest that relate to cellular energetics and metabolism, morphological changes, cell division and active transport. Cells respond to temperature through viscoadaptation, and a change in viscosity may in turn affect the local temperature profile. Diamond nanocrystals containing nitrogen-vacancy colour centres can harness quantum phenomena to perform a variety of sensing tasks such as measuring temperature, viscosity and external magnetic and electric field, at the nanoscale inside live cells. These quantum sensors can operate without suffering from bleaching and are unaffected by changes in local pH and local refractive index, remaining robust to fluctuations in background fluorescence. In this talk, I will present our latest results on performing nanoscale quantum sensing in living cells for reporting two parameters simultaneously: temperature and rheology. We implement a fast orbital tracking scheme on a quantum sensor formed of a 50-nm diamond nanocrystal containing an ensemble of ~200 nitrogen-vacancy centres. This enables 3D-localization beyond the diffraction limit in a dynamic intracellular environment, opening the door to quantum measurements using highly mobile nanoparticles. We demonstrate the operation of the quantum sensor in a living human cancer cell, extracting simultaneously information about the nanoscale temperature environment, the thermal and stochastic forces acting on the nanodiamond, and properties of its viscoelastic environment.

Sensors that harness quantum mechanical effects can enable high sensitivity and high spatial resolution probing of their environment. The nitrogen-vacancy defect in diamond, a single, optically accessible electronic spin, is a promising quantum sensor that can operate in soft and living systems and provides nanoscale spatial resolution when hosted inside a diamond nanoparticle. Nanodiamond quantum sensors are nontoxic, amenable to surface functionalization, and can be introduced into a variety of living systems. The optical readout of the spin provides detailed information about the local electromagnetic and thermal environment in a noninvasive way. In this Perspective, we introduce the different modalities that nanodiamond quantum sensors offer, highlight recent progress in quantum sensing of biological systems, and discuss remaining challenges and directions for future efforts.

The viscoelasticity of the cytoplasm plays a critical role in cell morphology, cell division, and intracellular transport. Viscoelasticity is also interconnected with other biophysical properties, such as temperature, which is known to influence cellular bioenergetics. Probing the connections between intracellular temperature and cytoplasmic viscoelasticity provides an exciting opportunity for the study of biological phenomena, such as metabolism and disease progression. The small length scales and transient nature of changes in these parameters combined with their complex interdependencies pose a challenge for biosensing tools, which are often limited to a single readout modality. Here, we present a dual-mode quantum sensor capable of performing simultaneous nanoscale thermometry and rheometry in dynamic cellular environments. We use nitrogen-vacancy centers in diamond nanocrystals as biocompatible sensors for in vitro measurements. We combine subdiffraction resolution single-particle tracking in a fluidic environment with optically detected magnetic resonance spectroscopy to perform simultaneous sensing of viscoelasticity and temperature. We use our sensor to demonstrate probing of the temperature-dependent viscoelasticity in complex media at the nanoscale. We then investigate the interplay between intracellular forces and the cytoplasmic rheology in live cells. Finally, we identify different rheological regimes and reveal evidence of active trafficking and details of the nanoscale viscoelasticity of the cytoplasm.

We demonstrate a dual-modal quantum sensor capable of simultaneously sensing nanoscale temperature and rheology in a dynamic cellular environment. We illustrate intracellular nanothermometry and nanorheology by studying the intracellular temperature response to external thermal modulations.

Understanding the dynamics of a quantum bit's environment is essential for the realization of practical systems for quantum information processing and metrology. We use single nitrogen-vacancy (NV) centers in diamond to study the dynamics of a disordered spin ensemble at the diamond surface. Specifically, we tune the density of "dark" surface spins to interrogate their contribution to the decoherence of shallow NV center spin qubits. When the average surface spin spacing exceeds the NV center depth, we find that the surface spin contribution to the NV center free induction decay can be described by a stretched exponential with variable power n. We show that these observations are consistent with a model in which the spatial positions of the surface spins are fixed for each measurement, but some of them reconfigure between measurements. In particular, we observe a depth-dependent critical time associated with a dynamical transition from Gaussian (n=2) decay to n=2/3, and show that this transition arises from the competition between the small decay contributions of many distant spins and strong coupling to a few proximal spins at the surface. These observations demonstrate the potential of a local sensor for understanding complex systems and elucidate pathways for improving and controlling spin qubits at the surface.

Scanning diamond magnetometers based on the optically detected magnetic resonance of the nitrogen-vacancy centre offer very high sensitivity and non-invasive imaging capabilities when the stray fields emanating from ultrathin magnetic materials are sufficiently low (< 10 mT). Beyond this low-field regime, the optical signal quenches and a quantitative measurement is challenging. While the field-dependent NV photoluminescence can still provide qualitative information on magnetic morphology, this operation regime remains unexplored particularly for surface magnetisation larger than $\sim$ 3 mA. Here, we introduce a multi-angle reconstruction technique (MARe) that captures the full nanoscale domain morphology in all magnetic-field regimes leading to NV photoluminescence quench. To demonstrate this, we use [Ir/Co/Pt]$_{14}$ multilayer films with surface magnetisation an order of magnitude larger than previous reports. Our approach brings non-invasive nanoscale magnetic field imaging capability to the study of a wider pool of magnetic materials and phenomena.

Quantum metrology is a powerful tool for explorations of fundamental physical phenomena and applications in material science and biochemical analysis. While in principle the sensitivity can be improved by increasing the density of sensing particles, in practice this improvement is severely hindered by interactions between them. Here, using a dense ensemble of interacting electronic spins in diamond, we demonstrate a novel approach to quantum metrology to surpass such limitations. It is based on a new method of robust quantum control, which allows us to simultaneously suppress the undesired effects associated with spin-spin interactions, disorder, and control imperfections, enabling a fivefold enhancement in coherence time compared to state-of-the-art control sequences. Combined with optimal spin state initialization and readout directions, this allows us to achieve an ac magnetic field sensitivity well beyond the previous limit imposed by interactions, opening a new regime of high-sensitivity solid-state ensemble magnetometers.

While conventional nuclear magnetic resonance (NMR) spectroscopy is widely used for chemical analysis of macroscopic sample volumes, quantum NMR sensors based on nitrogen-vacancy (N-V) centers in bulk diamond have brought NMR spectroscopy to the nanoscale, demonstrating single-nucleus sensitivity and chemical structure determination. However, the detection volume for existing nanoscale N-V NMR devices extends only nanometers above a bulk diamond chip, which prevents measurements in thicker structures, such as cells. Here, we introduce N-V NMR devices based on nanodiamonds and use them to detect and distinguish multiple nuclear species in a sample volume of about 20(3) nm(3). We describe how analyte concentrations can be measured in situ using nuclear spins on the nanodiamond surface for calibration. The nanodiamond host provides a small size (similar to 30 nm diameter), low toxicity, and opportunities for surface functionalization, which makes these devices promising for intracellular applications. These results mark an important step toward feasible and reliable nanoscale NMR measurements inside living cells.

We introduce a new approach for the robust control of quantum dynamics of strongly interacting many-body systems. Our approach involves the design of periodic global control pulse sequences to engineer desired target Hamiltonians that are robust against disorder, unwanted interactions, and pulse imperfections. It utilizes a matrix representation of the Hamiltonian engineering protocol based on time-domain transformations of the Pauli spin operator along the quantization axis. This representation allows us to derive a concise set of algebraic conditions on the sequence matrix to engineer robust target Hamiltonians, enabling the simple yet systematic design of pulse sequences. We show that this approach provides an efficient framework to (i) treat any secular many-body Hamiltonian and engineer it into a desired form, (ii) target dominant disorder and interaction characteristics of a given system, (iii) achieve robustness against imperfections, (iv) provide optimal sequence length within given constraints, and (v) substantially accelerate numerical searches of pulse sequences. Using this systematic approach, we develop novel sets of pulse sequences for the protection of quantum coherence, optimal quantum sensing, and quantum simulation. Finally, we experimentally demonstrate the robust operation of these sequences in a system with the most general interaction form.

Conventional nuclear magnetic resonance (NMR) spectroscopy relies on acquiring signal from a macroscopic ensemble of molecules to gain information about molecular structure and dynamics. Transferring this technique to nanoscale sample sizes would enable molecular analysis without the effects of averaging over spatial and temporal inhomogeneities and without the need for macroscopic volumes of analyte, both inherent to large ensemble measurements. Nanoscale NMR based on nitrogen vacancy (NV) centers inside bulk diamond chips achieves single nuclear spin sensitivity and the resolution required to determine chemical structure, but their detection volume is limited to a few nanometers above the diamond surface for the most sensitive devices. This precludes them from use for nuclear spin sensing with nanoscale resolution inside thicker structures, such as cells. Here, we demonstrate the detection of NMR signals from multiple nuclear species in a (19 nm)3 volume using versatile NV-NMR devices inside nanodiamonds that have a typical 30 nm diameter. The devices detect a signal generated by a small number of analyte molecules on the order of 1000. To use these devices in situ, the detected signal must be corrected for the unknown geometry of each nanodiamond device. We show that such a calibration could be performed by exploiting the signal from a thin layer of nuclei on the diamond surface. These results, combined with the low toxicity of nanodiamonds and their amenability to surface functionalization, indicate that nanodiamond NV-NMR devices could become a useful tool for nanoscale NMR-based sensing inside living cells.

Quantum state readout is a key component of quantum technologies, including applications in sensing, computation, and secure communication. Readout fidelity can be enhanced by repeating readouts. However, the number of repeated readouts is limited by measurement backaction, which changes the quantum state that is measured. This detrimental effect can be overcome by storing the quantum state in an ancilla qubit, chosen to be robust against measurement backaction and to allow error correction. Here, we protect the electronic-spin state of a diamond nitrogen-vacancy center from measurement backaction using a robust multilevel 14 N nuclear-spin memory and perform repetitive readout, as demonstrated in previous work on bulk diamond devices. We achieve additional protection using error correction based on the quantum logic of coherent feedback to reverse measurement backaction. The repetitive spin readout scheme provides a 13-fold enhancement of readout fidelity over conventional readout and the error correction a 2-fold improvement in the signal. These experiments demonstrate full quantum control of a nitrogen-vacancy center electronic-spin coupled to its host 14 N nuclear spin inside a ~25 nm nanodiamond, creating a sensitive and biologically compatible platform for nanoscale quantum sensing. Our error-corrected repetitive readout scheme is particularly useful for quadrupolar nuclear magnetic resonance imaging in the low magnetic field regime where conventional repetitive readout suffers from strong measurement backaction. More broadly, methods for correcting longitudinal (bit-flip) errors described here could be used to improve quantum algorithms that require non-volatile local memory, such as correlation spectroscopy measurements for high resolution sensing.

We show here that oxidised nanodiamonds show improved biocompatibility compared to graphitic nanodiamonds when applied in living cells.