Transform-Limited Photon Emission from a Lead-Vacancy Center in Diamond above 10 K.

Transform-limited photon emission from quantum emitters is essential for high-fidelity entanglement generation. In this Letter, we report the coherent optical property of a single negatively charged lead-vacancy (PbV) center in diamond. Photoluminescence excitation measurements reveal stable fluorescence with a linewidth of 39 MHz at 6 K, close to the transform limit estimated from the lifetime measurement. We observe 4 orders of magnitude different linewidths of the two zero-phonon lines, and find that the phonon-induced relaxation in the ground state contributes to this huge difference in the linewidth. Because of the suppressed phonon absorption in the PbV center, we observe nearly transform-limited photon emission up to 16 K, demonstrating its high temperature robustness compared to other color centers in diamond.

High-precision robust monitoring of charge/discharge current over a wide dynamic range for electric vehicle batteries using diamond quantum sensors.

Accurate prediction of the remaining driving range of electric vehicles is difficult because the state-of-the-art sensors for measuring battery current are not accurate enough to estimate the state of charge. This is because the battery current of EVs can reach a maximum of several hundred amperes while the average current is only approximately 10 A, and ordinary sensors do not have an accuracy of several tens of milliamperes while maintaining a dynamic range of several hundred amperes. Therefore, the state of charge has to be estimated with an ambiguity of approximately 10%, which makes the battery usage inefficient. This study resolves this limitation by developing a diamond quantum sensor with an inherently wide dynamic range and high sensitivity for measuring the battery current. The design uses the differential detection of two sensors to eliminate in-vehicle common-mode environmental noise, and a mixed analog-digital control to trace the magnetic resonance microwave frequencies of the quantum sensor without deviation over a wide dynamic range. The prototype battery monitor was fabricated and tested. The battery module current was measured up to 130 A covering WLTC driving pattern, and the accuracy of the current sensor to estimate battery state of charge was analyzed to be 10 mA, which will lead to 0.2% CO2 reduction emitted in the 2030 WW transportation field. Moreover, an operating temperature range of - 40 to + 85 °C and a maximum current dynamic range of ± 1000 A were confirmed.

Gradiometer Using Separated Diamond Quantum Magnetometers.

The negatively charged nitrogen-vacancy (NV) center in diamonds is known as the spin defect and using its electron spin, magnetometry can be realized even at room temperature with extremely high sensitivity as well as a high dynamic range. However, a magnetically shielded enclosure is usually required to sense weak magnetic fields because environmental magnetic field noises can disturb high sensitivity measurements. Here, we fabricated a gradiometer with variable sensor length that works at room temperature using a pair of diamond samples containing negatively charged NV centers. Each diamond is attached to an optical fiber to enable free sensor placement. Without any magnetically shielding, our gradiometer realizes a magnetic noise spectrum comparable to that of a three-layer magnetically shielded enclosure, reducing the noises at the low-frequency range below 1 Hz as well as at the frequency of 50 Hz (power line frequency) and its harmonics. These results indicate the potential of highly sensitive magnetic sensing by the gradiometer using the NV center for applications in noisy environments such as outdoor and in vehicles.

Simultaneous wide-field imaging of phase and magnitude of AC magnetic signal using diamond quantum magnetometry.

Spectroscopic analysis of AC magnetic signal using diamond quantum magnetometry is a promising technique for inductive imaging. Conventional dynamic decoupling like XY8 provides a high sensitivity of an oscillating magnetic signal with intricate dependence on magnitude and phase, complicating high throughput detection of each parameter. In this study, a simple measurement scheme for independent and simultaneous detection of magnitude and phase is demonstrated by a sequential measurement protocol. Wide-field imaging experiment was performed for an oscillating magnetic field with approximately [Formula: see text]-squared observation area. Single pixel phase precision was [Formula: see text] for [Formula: see text] AC magnetic signal. Our method enables potential applications including inductive inspection and impedance imaging.

Magnetometer with nitrogen-vacancy center in a bulk diamond for detecting magnetic nanoparticles in biomedical applications.

We developed a novel magnetometer that employs negatively charged nitrogen-vacancy (NV-) centers in diamond, to detect the magnetic field generated by magnetic nanoparticles (MNPs) for biomedical applications. The compact probe system is integrated into a fiber-optics platform allowing for a compact design. To detect signals from the MNPs effectively, we demonstrated, for the first time, the application of an alternating current (AC) magnetic field generated by the excitation coil of several hundred microteslas for the magnetization of MNPs in diamond quantum sensing. In the lock-in detection system, the minimum detectable AC magnetic field (at a frequency of 1.025 kHz) was approximately 57.6 nT for one second measurement time. We were able to detect the micromolar concentration of MNPs at distances of a few millimeters. These results indicate that the magnetometer with the NV- centers can detect the tiny amounts of MNPs, thereby offering potential for future biomedical applications.

A quantum thermometric sensing and analysis system using fluorescent nanodiamonds for the evaluation of living stem cell functions according to intracellular temperature.

Intracellular thermometry techniques play an important role in elucidating the relationship between the intracellular temperature and stem cell functions. However, there have been few reports on thermometry techniques that can detect the intracellular temperature of cells during several days of incubation. In this study, we developed a novel quantum thermometric sensing and analysis system (QTAS) using fluorescent nanodiamonds (FNDs). FNDs could label adipose tissue-derived stem cells (ASCs) at high efficiency with 24 h of incubation, and no cytotoxicity was observed in ASCs labeled with less than 500 µg mL-1 of FNDs. The peak of FNDs was confirmed at approximately 2.87 GHz with the characteristic fluorescence spectra of NV centers that could be optically detected (optically detected magnetic resonance [ODMR]). The ODMR peak clearly shifted to the high-frequency side as the temperature decreased and gave a mean temperature dependence of -(77.6 ± 11.0) kHz °C-1, thus the intracellular temperature of living ASCs during several days of culturing could be precisely measured using the QTAS. Moreover, the intracellular temperature was found to influence the production of growth factors and the degree of differentiation into adipocytes and osteocytes. These data suggest that the QTAS can be used to investigate the relationship between intracellular temperature and cellular functions.

Direct Nanoscale Sensing of the Internal Electric Field in Operating Semiconductor Devices Using Single Electron Spins.

The electric field inside semiconductor devices is a key physical parameter that determines the properties of the devices. However, techniques based on scanning probe microscopy are limited to sensing at the surface only. Here, we demonstrate the direct sensing of the internal electric field in diamond power devices using single nitrogen-vacancy (NV) centers. The NV center embedded inside the device acts as a nanoscale electric field sensor. We fabricated vertical diamond p-i-n diodes containing the single NV centers. By performing optically detected magnetic resonance measurements under reverse-biased conditions with an applied voltage of up to 150 V, we found a large splitting in the magnetic resonance frequencies. This indicated that the NV center senses the transverse electric field in the space-charge region formed in the i-layer. The experimentally obtained electric field values are in good agreement with those calculated by a device simulator. Furthermore, we demonstrate the sensing of the electric field in different directions by utilizing NV centers with different N-V axes. This direct and quantitative sensing method using an electron spin in a wide-band-gap material provides a way to monitor the electric field in operating semiconductor devices.

Tin-Vacancy Quantum Emitters in Diamond.

Tin-vacancy (Sn-V) color centers were created in diamond via ion implantation and subsequent high-temperature annealing up to 2100 °C at 7.7 GPa. The first-principles calculation suggested that a large atom of tin can be incorporated into a diamond lattice with a split-vacancy configuration, in which a tin atom sits on an interstitial site with two neighboring vacancies. The Sn-V center showed a sharp zero phonon line at 619 nm at room temperature. This line split into four peaks at cryogenic temperatures, with a larger ground state splitting (∼850 GHz) than that of color centers based on other group-IV elements, i.e., silicon-vacancy (Si-V) and germanium-vacancy (Ge-V) centers. The excited state lifetime was estimated, via Hanbury Brown-Twiss interferometry measurements on single Sn-V quantum emitters, to be ∼5 ns. The order of the experimentally obtained optical transition energies, compared with those of Si-V and Ge-V centers, was in good agreement with the theoretical calculations.

Germanium-Vacancy Single Color Centers in Diamond.

Atomic-sized fluorescent defects in diamond are widely recognized as a promising solid state platform for quantum cryptography and quantum information processing. For these applications, single photon sources with a high intensity and reproducible fabrication methods are required. In this study, we report a novel color center in diamond, composed of a germanium (Ge) and a vacancy (V) and named the GeV center, which has a sharp and strong photoluminescence band with a zero-phonon line at 602 nm at room temperature. We demonstrate this new color center works as a single photon source. Both ion implantation and chemical vapor deposition techniques enabled fabrication of GeV centers in diamond. A first-principles calculation revealed the atomic crystal structure and energy levels of the GeV center.

Experimental analysis of charge redistribution due to chemical bonding by high-resolution transmission electron microscopy.

The electronic charge density distribution or the electrostatic atomic potential of a solid or molecule contains information not only on the atomic structure, but also on the electronic properties, such as the nature of the chemical bonds or the degree of ionization of atoms. However, the redistribution of charge due to chemical bonding is small compared with the total charge density, and therefore difficult to measure. Here, we demonstrate an experimental analysis of charge redistribution due to chemical bonding by means of high-resolution transmission electron microscopy (HRTEM). We analyse charge transfer on the single-atom level for nitrogen-substitution point defects in graphene, and confirm the ionicity of single-layer hexagonal boron nitride. Our combination of HRTEM experiments and first-principles electronic structure calculations opens a new way to investigate electronic configurations of point defects, other non-periodic arrangements or nanoscale objects that cannot be studied by an electron or X-ray diffraction analysis.

Long-range ordered single-crystal graphene on high-quality heteroepitaxial Ni thin films grown on MgO(111).

Large-area single crystal monolayer graphene is synthesized on Ni(111) thin films, which have flat terraces and no grain boundaries. The flat single-crystal Ni films are heteroepitaxially grown on MgO(111) substrates using a buffer layer technique. Low-energy electron diffraction and various spectroscopic methods reveal the long-range single crystallinity and uniform monolayer thickness of the graphene. When transferred onto an insulating wafer, continuous millimeter-scale single domain graphene is obtained.

Detection of mismatched DNA on partially negatively charged diamond surfaces by optical and potentiometric methods.

The effects of surface charge density on DNA hybridization have been investigated on a mixture of hydrogen-, oxygen-, and amine-terminated diamond surfaces. A difference in the hybridization efficiencies of complementary and mismatched DNA was clearly observed by fluorescence and potentiometric observations at a particular coverage of oxygen. In the fluorescence observation, singly mismatched DNA was detected with high contrast after appropriate hybridization on the surface with 10-20% oxygen coverage. The amount of oxygen in the form of C-O(-) (deprotonated C-OH) producing the surface negative-charge density was estimated by X-ray photoelectron spectroscopy. Electrolyte solution gate field-effect transistors (SGFETs) were used for potentiometric observations. The signal difference (change in gate potential) on the SGFET, which was as large as approximately 20 mV, was caused by the difference in the hybridization efficiencies of complementary target DNA (cDNA) and singly mismatched (1MM) target DNA with a common probe DNA immobilized on the same SGFET. The reversible change in gate potential caused by the hybridization and denaturation cycles and discriminating between the complementary and 1MM DNA targets was very stable throughout the cyclical detections. Moreover, the ratio of signals caused by hybridization of the cDNA and 1MM DNA targets with the probe DNA immobilized on the SGFET was determined to be 3:1 when hybridization had occurred (after 15 min on SGFET), as determined by real-time measurements. From the viewpoint of hybridization kinetics, the rate constant for hybridization of singly mismatched DNA was a factor of approximately 3 smaller than that of cDNA on this functionalized (oxidized and aminated) diamond surface.

Mechanism analysis of interrupted growth of single-walled carbon nanotube arrays.

We investigated the growth mechanism of layered single-walled carbon nanotube (SWNT) mats by a cutting method. Transmission electron microscope observations revealed that new SWNTs grown below first grown SWNTs also have caps at their tips. Raman spectroscopy suggests that the SWNTs in each layer have the same chirality distribution. This growth method might be a way to prove a factor of chirality selection of SWNTs.

Enhanced field emission properties of vertically aligned double-walled carbon nanotube arrays.

Vertically aligned double-walled carbon nanotube (VA-DWCNT) arrays were synthesized by point-arc microwave plasma chemical vapor deposition on Cr/n-Si and SiO(2)/n-Si substrates. The outer tube diameters of VA-DWCNTs are in the range of 2.5-3.8 nm, and the average interlayer spacing is approximately 0.42 nm. The field emission properties of these VA-DWCNTs were studied. It was found that a VA-DWCNT array grown on a Cr/n-Si substrate had better field emission properties as compared with a VA-DWCNT array grown on a SiO(2)/n-Si substrate and randomly oriented DWCNTs, showing a turn-on field of about 0.85 V µm(-1) at the emission current density of 0.1 µA cm(-2) and a threshold field of 1.67 V µm(-1) at the emission current density of 1.0 mA cm(-2). The better field emission performance of the VA-DWCNT array was mainly attributed to the vertical alignment of DWCNTs on the Cr/n-Si substrate and the low contact resistance between CNTs and the Cr/n-Si substrate.

Growth kinetics of 0.5 cm vertically aligned single-walled carbon nanotubes.

Half-centimeter-high mats of vertically aligned single-walled carbon nanotubes were grown at 600 degrees C by point-arc microwave plasma chemical vapor deposition. The mats were produced from 0.5 nm of an Fe catalyst layer, thus showing one of the highest catalytic yields of approximately 105 times. The growth process shows a lack of poisoning of the catalyst, in contrast to other reports. The experimental results confirm that the growth rate is ultimately limited by the gas phase diffusion of hydrocarbon radicals.

Direct evidence for root growth of vertically aligned single-walled carbon nanotubes by microwave plasma chemical vapor deposition.

The root growth mode of extremely dense and vertically aligned single-walled carbon nanotubes (SWNTs) synthesized by microwave plasma chemical vapor deposition was clarified by a new method, marker growth, which does not require transmission electron microscopy. SWNT layers were grown intermittently on a substrate, and a line between the layers was used as a marker to identify the growth mode. Micro-Raman spectroscopy revealed that the SWNT layers have the same diameter distribution.