Quantum nonlinear spectroscopy of single nuclear spins.

Conventional nonlinear spectroscopy, which use classical probes, can only access a limited set of correlations in a quantum system. Here we demonstrate that quantum nonlinear spectroscopy, in which a quantum sensor and a quantum object are first entangled and the sensor is measured along a chosen basis, can extract arbitrary types and orders of correlations in a quantum system. We measured fourth-order correlations of single nuclear spins that cannot be measured in conventional nonlinear spectroscopy, using sequential weak measurement via a nitrogen-vacancy center in diamond.

Quantum-assisted distortion-free audio signal sensing.

Quantum sensors are known for their high sensitivity in sensing applications. However, this sensitivity often comes with severe restrictions on other parameters which are also important. Examples are that in measurements of arbitrary signals, limitation in linear dynamic range could introduce distortions in magnitude and phase of the signal.

Heterodyne sensing of microwaves with a quantum sensor.

Diamond quantum sensors are sensitive to weak microwave magnetic fields resonant to the spin transitions. However, the spectral resolution in such protocols is ultimately limited by the sensor lifetime. Here, we demonstrate a heterodyne detection method for microwaves (MW) leading to a lifetime independent spectral resolution in the GHz range.

Coherent electrical readout of defect spins in silicon carbide by photo-ionization at ambient conditions.

Quantum technology relies on proper hardware, enabling coherent quantum state control as well as efficient quantum state readout. In this regard, wide-bandgap semiconductors are an emerging material platform with scalable wafer fabrication methods, hosting several promising spin-active point defects. Conventional readout protocols for defect spins rely on fluorescence detection and are limited by a low photon collection efficiency.

Robust and Accurate Electric Field Sensing with Solid State Spin Ensembles.

Electron spins in solids constitute remarkable quantum sensors. Individual defect centers in diamond were used to detect individual nuclear spins with a nanometer scale resolution, and ensemble magnetometers rival SQUID and vapor cell magnetometers when taking into account room-temperature operation and size. NV center spins can also detect electric field vectors, despite their weak coupling to electric fields.

Triple nitrogen-vacancy centre fabrication by CNH ion implantation.

Quantum information processing requires quantum registers based on coherently interacting quantum bits. The dipolar couplings between nitrogen vacancy (NV) centres with nanometre separation makes them a potential platform for room-temperature quantum registers. The fabrication of quantum registers that consist of NV centre arrays has not advanced beyond NV pairs for several years.

Probing Quantum Thermalization of a Disordered Dipolar Spin Ensemble with Discrete Time-Crystalline Order.

We investigate thermalization dynamics of a driven dipolar many-body quantum system through the stability of discrete time crystalline order. Using periodic driving of electronic spin impurities in diamond, we realize different types of interactions between spins and demonstrate experimentally that the interplay of disorder, driving, and interactions leads to several qualitatively distinct regimes of thermalization. For short driving periods, the observed dynamics are well described by an effective Hamiltonian which sensitively depends on interaction details.

Photoelectrical imaging and coherent spin-state readout of single nitrogen-vacancy centers in diamond.

Nitrogen-vacancy (NV) centers in diamond have become an important instrument for quantum sensing and quantum information science. However, the readout of NV spin state requires bulky optical setups, limiting fabrication of miniaturized compact devices for practical use. Here we realized photoelectrical detection of magnetic resonance as well as Rabi oscillations on a single-defect level.

High-resolution spectroscopy of single nuclear spins via sequential weak measurements.

Nuclear magnetic resonance (NMR) of single spins have recently been detected by quantum sensors. However, the spectral resolution has been limited by the sensor's relaxation to a few kHz at room temperature. This can be improved by using quantum memories, at the expense of sensitivity.

Nonvolatile nuclear spin memory enables sensor-unlimited nanoscale spectroscopy of small spin clusters.

In nanoscale metrology, dissipation of the sensor limits its performance. Strong dissipation has a negative impact on sensitivity, and sensor-target interaction even causes relaxation or dephasing of the latter. The weak dissipation of nitrogen-vacancy (NV) sensors in room temperature diamond enables detection of individual target nuclear spins, yet limits the spectral resolution of nuclear magnetic resonance (NMR) spectroscopy to several hundred Hertz, which typically prevents molecular recognition.

Nanoscale nuclear magnetic resonance with chemical resolution.

Nuclear magnetic resonance (NMR) spectroscopy is a key analytical technique in chemistry, biology, and medicine. However, conventional NMR spectroscopy requires an at least nanoliter-sized sample volume to achieve sufficient signal. We combined the use of a quantum memory and high magnetic fields with a dedicated quantum sensor based on nitrogen vacancy centers in diamond to achieve chemical shift resolution in H and F NMR spectroscopy of 20-zeptoliter sample volumes.

Depolarization Dynamics in a Strongly Interacting Solid-State Spin Ensemble.

We study the depolarization dynamics of a dense ensemble of dipolar interacting spins, associated with nitrogen-vacancy centers in diamond. We observe anomalously fast, density-dependent, and nonexponential spin relaxation. To explain these observations, we propose a microscopic model where an interplay of long-range interactions, disorder, and dissipation leads to predictions that are in quantitative agreement with both current and prior experimental results.

Observation of discrete time-crystalline order in a disordered dipolar many-body system.

Understanding quantum dynamics away from equilibrium is an outstanding challenge in the modern physical sciences. Out-of-equilibrium systems can display a rich variety of phenomena, including self-organized synchronization and dynamical phase transitions. More recently, advances in the controlled manipulation of isolated many-body systems have enabled detailed studies of non-equilibrium phases in strongly interacting quantum matter; for example, the interplay between periodic driving, disorder and strong interactions has been predicted to result in exotic 'time-crystalline' phases, in which a system exhibits temporal correlations at integer multiples of the fundamental driving period, breaking the discrete time-translational symmetry of the underlying drive.

Investigation of the silicon vacancy color center for quantum key distribution.

Single photon sources (SPS) are crucial for quantum key distribution. Here we demonstrate a stable triggered SPS at 738 nm with linewidth less than 5 nm at room temperature based on a negatively charged single silicon vacancy color center. Thanks to the short photon duration of about 1.

Local and bulk (13)C hyperpolarization in nitrogen-vacancy-centred diamonds at variable fields and orientations.

Polarizing nuclear spins is of fundamental importance in biology, chemistry and physics. Methods for hyperpolarizing (13)C nuclei from free electrons in bulk usually demand operation at cryogenic temperatures. Room temperature approaches targeting diamonds with nitrogen-vacancy centres could alleviate this need; however, hitherto proposed strategies lack generality as they demand stringent conditions on the strength and/or alignment of the magnetic field.

Fluorescence Polarization Switching from a Single Silicon Vacancy Colour Centre in Diamond.

Single-photon emitters with stable and uniform photoluminescence properties are important for quantum technology. However, in many cases, colour centres in diamond exhibit spectral diffusion and photoluminescence intensity fluctuation. It is therefore essential to investigate the dynamics of colour centres at the single defect level in order to enable the on-demand manipulation and improved applications in quantum technology.

Single spin optically detected magnetic resonance with 60-90 GHz (E-band) microwave resonators.

Magnetic resonance with ensembles of electron spins is commonly performed around 10 GHz, but also at frequencies above 240 GHz and in corresponding magnetic fields of over 9 T. However, experiments with single electron and nuclear spins so far only reach into frequency ranges of several 10 GHz, where existing coplanar waveguide structures for microwave (MW) delivery are compatible with single spin readout techniques (e.g.

All-optical initialization, readout, and coherent preparation of single silicon-vacancy spins in diamond.

The silicon-vacancy (SiV-) color center in diamond has attracted attention because of its unique optical properties. It exhibits spectral stability and indistinguishability that facilitate efficient generation of photons capable of demonstrating quantum interference. Here we show optical initialization and readout of electronic spin in a single SiV- center with a spin relaxation time of T1=2.

Magnetic resonance identification of hydrogen at a zinc vacancy in ZnO.

Hydrogen (H) at a zinc vacancy (VZn) in ZnO is identified by electron paramagnetic resonance (EPR) and electron spin echo envelope modulation (ESEEM). In ZnO irradiated by 2 MeV electrons, a doublet EPR spectrum, labelled S1, is observed. The doublet structure and the accompanying weak satellites are shown to be the allowed and forbidden lines of the hyperfine structure due to the dipolar interaction between an electron spin S = 1/2 and a nuclear spin I = 1/2 of (1)H located at a VZn.

Sensing single remote nuclear spins.

The detection of single nuclear spins would be useful for fields ranging from basic science to quantum information technology. However, although sensing based on diamond defects and other methods have shown high sensitivity, they have not been capable of detecting single nuclear spins, and defect-based techniques further require strong defect-spin coupling. Here, we present the detection and identification of single and remote (13)C nuclear spins embedded in nuclear spin baths surrounding a single electron spin of a nitrogen-vacancy centre in diamond.

Ultralong spin coherence time in isotopically engineered diamond.

As quantum mechanics ventures into the world of applications and engineering, materials science faces the necessity to design matter to quantum grade purity. For such materials, quantum effects define their physical behaviour and open completely new (quantum) perspectives for applications. Carbon-based materials are particularly good examples, highlighted by the fascinating quantum properties of, for example, nanotubes or graphene.