Nanothermometry with Enhanced Sensitivity and Enlarged Working Range Using Diamond Sensors.

Nanothermometry is increasingly demanded in frontier research in physics, chemistry, materials science and engineering, and biomedicine. An ideal thermometer should have features of reliable temperature interpretation, high sensitivity, fast response, minimum disturbance of the target's temperature, applicability in a variety of environments, and a large working temperature range. For applications in nanosystems, high spatial resolution is also desirable. Such requirements impose great challenges in nanothermometry since the shrinking of the sensor volume usually leads to a reduction in sensitivity.Diamond with nitrogen-vacancy (NV) centers provides opportunities for nanothermometry. NV center spins have sharp resonances due to their superb coherence. NV centers are multimodal sensors. They can directly sense magnetic fields, electric fields, temperature, pressure, and nuclear spins and, through proper transduction, measure other quantities such as the pH and deformation. In particular, their spin resonance frequencies vary with temperature, making them a promising thermometer. The high thermal conductivity, high hardness, chemical stability, and biocompatibility of diamond enable reliable and fast temperature sensing in complex environments ranging from erosive liquids to live systems. Chemical processing of diamond surfaces allows various functionalities such as targeting. The small size and the targeting capability of nanodiamonds then enable site-specific temperature sensing with nanoscale spatial resolution. However, the sensitivity of NV-based nanothermometry is yet to meet the requirement of practical systems with a large gap of a few orders of magnitude. On the other hand, although NV-based quantum sensing works well from 0.3 to 600 K, extending the sensing scheme to high temperature remains challenging due to uncertainty in identifying the exact physical limits and possible solution at elevated temperatures.This Account focuses on our efforts to enhance the temperature sensitivity and widen the working temperature range of diamond-based nanothermometry. We start with explaining the working principle and features of NV-based thermometry with examples of applications. Then a transducer-based concept is introduced with practical schemes to improve the sensitivity of the nanodiamond thermometer. Specifically, we show that the temperature signal can be transduced and amplified by adopting hybrid structures of nanodiamond and magnetic nanoparticles, which results in a record temperature sensitivity of 76 µK/√Hz. We also demonstrate quantum sensing with NV at high temperatures of up to 1000 K by adopting a pulsed heating-cooling scheme to carry out the spin polarization and readout at room temperature and the spin manipulation (sensing) at high temperatures. Finally, unsolved problems and future endeavors of diamond nanothermometry are discussed.

Braiding Lateral Morphotropic Grain Boundaries in Homogenetic Oxides.

Interfaces formed by correlated oxides offer a critical avenue for discovering emergent phenomena and quantum states. However, the fabrication of oxide interfaces with variable crystallographic orientations and strain states integrated along a film plane is extremely challenging by conventional layer-by-layer stacking or self-assembling. Here, the creation of morphotropic grain boundaries (GBs) in laterally interconnected cobaltite homostructures is reported. Single-crystalline substrates and suspended ultrathin freestanding membranes provide independent templates for coherent epitaxy and constraint on the growth orientation, resulting in seamless and atomically sharp GBs. Electronic states and magnetic behavior in hybrid structures are laterally modulated and isolated by GBs, enabling artificially engineered functionalities in the planar matrix. This work offers a simple and scalable method for fabricating unprecedented innovative interfaces through controlled synthesis routes as well as providing a platform for exploring potential applications in neuromorphics, solid-state batteries, and catalysis.

Room-Temperature Ferromagnetism at an Oxide-Nitride Interface.

Heterointerfaces have led to the discovery of novel electronic and magnetic states because of their strongly entangled electronic degrees of freedom. Single-phase chromium compounds always exhibit antiferromagnetism following the prediction of the Goodenough-Kanamori rules. So far, exchange coupling between chromium ions via heteroanions has not been explored and the associated quantum states are unknown. Here, we report the successful epitaxial synthesis and characterization of chromium oxide (Cr_{2}O_{3})-chromium nitride (CrN) superlattices. Room-temperature ferromagnetic spin ordering is achieved at the interfaces between these two antiferromagnets, and the magnitude of the effect decays with increasing layer thickness. First-principles calculations indicate that robust ferromagnetic spin interaction between Cr^{3+} ions via anion-hybridization across the interface yields the lowest total energy. This work opens the door to fundamental understanding of the unexpected and exceptional properties of oxide-nitride interfaces and provides access to hidden phases at low-dimensional quantum heterostructures.

Association of Nanodiamond Rotation Dynamics with Cell Activities by Translation-Rotation Tracking.

Correlated translation-orientation tracking of single particles can provide important information for understanding the dynamics of live systems and their interaction with the probes. However, full six-dimensional (6D) motion tracking has yet to be achieved. Here, we developed synchronized 3D translation and 3D rotation tracking of single diamond particles based on nitrogen-vacancy center sensing. We first performed 6D tracking of diamond particles attached to a giant plasma membrane vesicle to demonstrate the method. Quantitative analysis of diamond particles' motion allowed elimination of the geometric effect and revealed the net rotation on the vesicle. 6D tracking was then applied to measure live cell dynamics. Motion characteristics of nanodiamonds on cell membranes under various controlled physiological conditions suggest that the nanodiamonds' rotation is associated with cell metabolic activities. Our technique extends the toolbox of single particle tracking and provides a unique solution to problems where correlated analysis of translation and rotation is critical.

Observing Information Backflow from Controllable Non-Markovian Multichannels in Diamond.

The unavoidable interaction of a quantum open system with its environment leads to the dissipation of quantum coherence and correlations, making its dynamical behavior a key role in many quantum technologies. In this Letter, we demonstrate the engineering of multiple dissipative channels by controlling the adjacent nuclear spins of a nitrogen-vacancy center in diamond. With a controllable non-Markovian dynamics of this open system, we observe that the quantum Fisher information flows to and from the environment using different noisy channels. Our work contributes to the developments of both noisy quantum metrology and quantum open systems from the viewpoints of metrologically useful entanglement.

Coherent quantum control of nitrogen-vacancy center spins near 1000 kelvin.

Quantum coherence control usually requires low temperature environments. Even for nitrogen-vacancy center spins in diamond, a remarkable exception, the coherence signal is limited to about 700 K due to the quench of the spin-dependent fluorescence at a higher temperature. Here we overcome this limit and demonstrate quantum coherence control of the electron spins of nitrogen-vacancy centers in nanodiamonds at temperatures near 1000 K. The scheme is based on initialization and readout of the spins at room temperature and control at high temperature, which is enabled by pulse laser heating and rapid diffusion cooling of nanodiamonds on amorphous carbon films. Using the diamond magnetometry based on optically detected magnetic resonance up to 800 K, we observe the magnetic phase transition of a single nickel nanoparticle at about 615 K. This work enables nano-thermometry and nano-magnetometry in the high-temperature regime.

Hybrid nanodiamond quantum sensors enabled by volume phase transitions of hydrogels.

Diamond nitrogen-vacancy (NV) center-based magnetometry provides a unique opportunity for quantum bio-sensing. However, NV centers are not sensitive to parameters such as temperature and pressure, and immune to many biochemical parameters such as pH and non-magnetic biomolecules. Here, we propose a scheme that can potentially enable the measurement of various biochemical parameters using diamond quantum sensing, by employing stimulus-responsive hydrogels as a spacing transducer in-between a nanodiamond (ND, with NV centers) and magnetic nanoparticles (MNPs). The volume phase transition of hydrogel upon stimulation leads to sharp variation in the separation distance between the MNPs and the ND. This in turn changes the magnetic field that the NV centers can detect sensitively. We construct a temperature sensor under this hybrid scheme and show the proof-of-the-principle demonstration of reversible temperature sensing. Applications in the detection of other bio-relevant parameters are envisioned if appropriate types of hydrogels can be engineered.

Single-Shot Readout of a Nuclear Spin Weakly Coupled to a Nitrogen-Vacancy Center at Room Temperature.

Single-shot readout of qubits is required for scalable quantum computing. Nuclear spins are superb quantum memories due to their long coherence time, but are difficult to be read out in a single shot due to their weak interaction with probes. Here we demonstrate single-shot readout of a weakly coupled ^{13}C nuclear spin at room temperature, which is unresolvable in traditional protocols. States of the weakly coupled nuclear spin are trapped and read out projectively by sequential weak measurements, which are implemented by dynamical decoupling pulses. A nuclear spin coupled to the nitrogen-vacancy (NV) center with strength 330 kHz is read out in 200 ms with a fidelity of 95.5%. This work provides a general protocol for single-shot readout of weakly coupled qubits at room temperature and therefore largely extends the range of physical systems for scalable quantum computing.

Demonstration of entanglement-enhanced phase estimation in solid.

Precise parameter estimation plays a central role in science and technology. The statistical error in estimation can be decreased by repeating measurement, leading to that the resultant uncertainty of the estimated parameter is proportional to the square root of the number of repetitions in accordance with the central limit theorem. Quantum parameter estimation, an emerging field of quantum technology, aims to use quantum resources to yield higher statistical precision than classical approaches. Here we report the first room-temperature implementation of entanglement-enhanced phase estimation in a solid-state system: the nitrogen-vacancy centre in pure diamond. We demonstrate a super-resolving phase measurement with two entangled qubits of different physical realizations: an nitrogen-vacancy centre electron spin and a proximal (13)C nuclear spin. The experimental data shows clearly the uncertainty reduction when entanglement resource is used, confirming the theoretical expectation. Our results represent an elemental demonstration of enhancement of quantum metrology against classical procedure.

Protection of centre spin coherence by dynamic nuclear spin polarization in diamond.

We experimentally investigate the protection of electron spin coherence of a nitrogen-vacancy (NV) centre in diamond by dynamic nuclear spin polarization (DNP). The electron spin decoherence of an NV centre is caused by the magnetic field fluctuation of the (13)C nuclear spin bath, which contributes large thermal fluctuation to the centre electron spin when it is in an equilibrium state at room temperature. To address this issue, we continuously transfer the angular momentum from electron spin to nuclear spins, and pump the nuclear spin bath to a polarized state under the Hartmann-Hahn condition. The bath polarization effect is verified by the observation of prolongation of the electron spin coherence time (T). Optimal conditions for the DNP process, including the pumping pulse duration and repeat numbers, are proposed by numerical simulation and confirmed by experiment. We also studied the depolarization effect of laser pulses. Our results provide a new route for quantum information processing and quantum simulation using the polarized nuclear spin bath.

Noise-resilient quantum evolution steered by dynamical decoupling.

Realistic quantum computing is subject to noise. Therefore, an important frontier in quantum computing is to implement noise-resilient quantum control over qubits. At the same time, dynamical decoupling can protect the coherence of qubits. Here we demonstrate non-trivial quantum evolution steered by dynamical decoupling control, which simultaneously suppresses noise effects. We design and implement a self-protected controlled-NOT gate on the electron spin of a nitrogen-vacancy centre and a nearby carbon-13 nuclear spin in diamond at room temperature, by employing an engineered dynamical decoupling control on the electron spin. Final state fidelity of 0.91(1) is observed in preparation of a Bell state using the gate. At the same time, the qubit coherence time is elongated at least 30 fold. The design scheme does not require the dynamical decoupling control to commute with the qubit interaction and therefore works for general qubit systems. This work marks a step towards implementing realistic quantum computing systems.

Room-temperature quantum cloning machine with full coherent phase control in nanodiamond.

In contrast to the classical world, an unknown quantum state cannot be cloned ideally, as stated by the no-cloning theorem. However, it is expected that approximate or probabilistic quantum cloning will be necessary for different applications, and thus various quantum cloning machines have been designed. Phase quantum cloning is of particular interest because it can be used to attack the Bennett-Brassard 1984 (BB84) states used in quantum key distribution for secure communications. Here, we report the first room-temperature implementation of quantum phase cloning with a controllable phase in a solid-state system: the nitrogen-vacancy centre of a nanodiamond. The phase cloner works well for all qubits located on the equator of the Bloch sphere. The phase is controlled and can be measured with high accuracy, and the experimental results are consistent with theoretical expectations. This experiment provides a basis for phase-controllable quantum information devices.

Controllable effects of quantum fluctuations on spin free-induction decay at room temperature.

Fluctuations of local fields cause decoherence of quantum objects. Usually at high temperatures, thermal noises are much stronger than quantum fluctuations unless the thermal effects are suppressed by certain techniques such as spin echo. Here we report the discovery of strong quantum-fluctuation effects of nuclear spin baths on free-induction decay of single electron spins in solids at room temperature. We find that the competition between the quantum and thermal fluctuations is controllable by an external magnetic field. These findings are based on Ramsey interference measurement of single nitrogen-vacancy center spins in diamond and numerical simulation of the decoherence, which are in excellent agreement.