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At least 199 records · Page 11

Quantum sensing of paramagnetic analytes by nanodiamonds in levitated microdroplets and aqueous solutions

Nanodiamonds (ND) hosting negatively charged nitrogen-vacancy (NV-) color centers have received attention for applications in magnetic field, electric field, chemical, and bio-sensing. The versatility of these probes is their excellent room-temperature optical and spin properties, along with their small size, functionalized surfaces and resistance to bleaching, making them ideal as nanoscopic sensors in picoliter volumes (e.g. single cells, but also microcompartments and aerosols). For quantitative ND-NV- sensing of paramagnetic analytes in such contexts, however, there remains an incomplete understanding of how factors related to the aqueous phase environment control detection efficiency. To address this, optically detected magnetic resonance (ODMR) is measured in bulk macroscale solutions and single levitated microdroplets as a function of Gd+3 concentration (340 nM to 1.5 mM), nanodiamond size, pH, competitor ions, and ligands. The ODMR response to [Gd+3] is found to be nonlinear, and pH, ND and sample volume dependent; indicating the detection of Gd+3 requires efficient adsorption of the analyte to the diamond surface. Langmuir adsorption isotherms embedded in a quantitative photophysical model links the ODMR response to adsorption thermodynamics of Gd+3. The equilibrium constant for Gd+3 adsorption to a carboxylated ND surface is determined to be (1 ± 0.5) x 105 M-1 corresponding to a free energy of adsorption of (-28 ± 1) kJ mol-1. These results provide general insight into how complex aqueous and microscale environments impact nanodiamond based quantum sensing modalities, and portend their application as quantitative chemical sensors in microenvironments.

Brown, Emily K↗

Perfect preferential orientation of nitrogen-vacancy defects in a synthetic diamond sample

We show that the orientation of nitrogen-vacancy (NV) defects in diamond can be efficiently controlled through chemical vapor deposition growth on a (111)-oriented diamond substrate. More precisely, we demonstrate that spontaneously generated NV defects are oriented with a ∼97% probability along the [111] axis, corresponding to the most appealing orientation among the four possible crystallographic axes. Such a nearly perfect preferential orientation is explained by analyzing the diamond growth mechanism on a (111)-oriented substrate and could be extended to other types of defects. This work is a significant step towards the design of optimized diamond samples for quantum information and sensing applications.

36 MATERIALS SCIENCE↗

Localized chemical switching of the charge state of nitrogen-vacancy luminescence centers in diamond

We present a direct-write chemical technique for controlling the charge state of near-surface nitrogen vacancy centers (NVs) in diamond by surface fluorination. Fluorination of H-terminated diamond is realized by electron beam stimulated desorption of H{sub 2}O in the presence of NF{sub 3} and verified with environmental photoyield spectroscopy (EPYS) and photoluminescence (PL) spectroscopy. PL spectra of shallow NVs in H- and F-terminated nanodiamonds show the expected dependence of the NV charge state on their energetic position with respect to the Fermi-level. EPYS reveals a corresponding difference between the ionization potential of H- and F-terminated diamond. The electron beam fluorination process is highly localized and can be used to fluorinate H-terminated diamond, and to increase the population of negatively charged NV centers.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Boron-doped superlattices and Bragg mirrors in diamond

A periodic modulation of the boron doping level of single crystal diamond multilayers over more than three orders of magnitude during epitaxial growth by microwave plasma-enhanced chemical vapor deposition is shown to yield Bragg mirrors in the visible. The thicknesses and doping level of the individual layers were controlled by in situ spectroscopic ellipsometry, enabling to tune the reflectance peak to the wavelength range of diamond color centers, such as NV{sup 0} or NV{sup −}. The crystalline quality, periodicity, and sharpness of the doping transitions in these doping superlattices over tens of periods were confirmed by high resolution X-ray diffraction.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Microscopic diamond solid-immersion-lenses fabricated around single defect centers by focused ion beam milling

Recent efforts to define microscopic solid-immersion-lenses (SIL) by focused ion beam milling into diamond substrates that are registered to a preselected single photon emitter are summarized. We show how we determine the position of a single emitter with at least 100 nm lateral and 500 nm axial accuracy, and how the milling procedure is optimized. The characteristics of a single emitter, a Nitrogen Vacancy (NV) center in diamond, are measured before and after producing the SIL and compared with each other. A count rate of 1.0 × 10{sup 6} counts/s is achieved with a [111] oriented NV center.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Inhomogeneous broadening of optically detected magnetic resonance of the ensembles of nitrogen-vacancy centers in diamond by interstitial carbon atoms

We study the impact of the negatively charged nitrogen-vacancy (NV{sup –}) center density on the lattice strain resulting in the splitting of the optically detected magnetic resonance of HPHT diamond. A simple model, taking into account the presence of the interstitial carbon atoms, acting like a wedge force on the crystal lattice, explains the broadening and splitting of the optically detected magnetic resonance of the ensemble of NV{sup –} centers at densities within the range of 10{sup 13} ÷ 10{sup 14 }cm{sup −3}. This model uses a complete generalized spin Hamiltonian, takes into account the strain-effect of each center in the ensemble and gives good agreement with experimental data.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Towards achieving strong coupling in three-dimensional-cavity with solid state spin resonance

We investigate the microwave magnetic field confinement in several microwave three-dimensional (3D)-cavities, using a 3D finite-element analysis to determine the best design and achieve a strong coupling between microwave resonant cavity photons and solid state spins. Specifically, we design cavities for achieving strong coupling of electromagnetic modes with an ensemble of nitrogen vacancy (NV) defects in diamond. We report here a novel and practical cavity design with a magnetic filling factor of up to 4 times (2 times higher collective coupling) than previously achieved using one-dimensional superconducting cavities with a small mode volume. In addition, we show that by using a double-split resonator cavity, it is possible to achieve up to 200 times better cooperative factor than the currently demonstrated with NV in diamond. These designs open up further opportunities for studying strong and ultra-strong coupling effects on spins in solids using alternative systems with a wider range of design parameters. The strong coupling of paramagnetic spin defects with a photonic cavity is used in quantum computer architecture, to interface electrons spins with photons, facilitating their read-out and processing of quantum information. To achieve this, the combination of collective coupling of spins and cavity mode is more feasible and offers a promising method. This is a relevant milestone to develop advanced quantum technology and to test fundamental physics principles.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Broadband, large-area microwave antenna for optically detected magnetic resonance of nitrogen-vacancy centers in diamond

We report on a microwave planar ring antenna specifically designed for optically detected magnetic resonance (ODMR) of nitrogen-vacancy (NV) centers in diamond. It has the resonance frequency at around 2.87 GHz with the bandwidth of 400 MHz, ensuring that ODMR can be observed under external magnetic fields up to 100 G without the need of adjustment of the resonance frequency. It is also spatially uniform within the 1-mm-diameter center hole, enabling the magnetic-field imaging in the wide spatial range. These features facilitate the experiments on quantum sensing and imaging using NV centers at room temperature.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Enhanced room-temperature spin Seebeck effect in a YIG/C 60 /Pt layered heterostructure

We report on large enhancement of the longitudinal spin Seebeck effect (LSSE) in the Y 3 Fe 5 O 12 (YIG)/Pt system at room temperature due to the addition of a thin layer of organic semiconductor (C 60 ) in between the YIG and the Pt. LSSE measurements show that the LSSE voltage increases significantly, from the initial value of 150 nV for the YIG/Pt structure to 240 nV for the YIG/C 60 (5nm)/Pt structure. Radio-frequency transverse susceptibility experiments reveal a significant decrease in the surface perpendicular magnetic anisotropy (PMA) of the YIG film when C 60 is deposited on it. These results suggest that the LSSE enhancement may be attributed to increased spin mixing conductance, the decreased PMA, and the large spin diffusion length of C 60 .

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Reduced photothermal heating in diamonds enriched with H3 point defects

Solid-state laser refrigeration of semiconductors remains an outstanding experimental challenge. In this work, we show that, following excitation with a laser wavelength of 532 nm, bulk diamond crystals doped with H3 centers both emit efficient up-conversion (anti-Stokes) photoluminescence and also show significantly reduced photothermal heating relative to crystals doped with nitrogen–vacancy (NV) centers. The H3 center in diamond is a highly photostable defect that avoids bleaching at high laser irradiances of 10–70 MW/cm 2 and has been shown to exhibit laser action, tunable over the visible band of 500–600 nm. Here, the observed reduction of photothermal heating arises due to a decrease in the concentration of absorbing point defects, including NV-centers. These results encourage future exploration of techniques for H3 enrichment in diamonds under high-pressure, high-temperature conditions for the simultaneous anti-Stokes fluorescence cooling and radiation balanced lasing in semiconductor materials. Reducing photothermal heating in diamond through the formation of H3 centers also opens up new possibilities in quantum sensing via optically detected magnetic resonance spectroscopy at ambient conditions.

42 ENGINEERING↗

Probing itinerant carrier dynamics at the diamond surface using single nitrogen vacancy centers

Color centers in diamond are widely explored for applications in quantum sensing, computing, and networking. Their optical, spin, and charge properties have extensively been studied, while their interactions with itinerant carriers are relatively unexplored. Here, we show that NV centers situated 10 ± 5 nm of the diamond surface can be converted to the neutral charge state via hole capture. By measuring the hole capture rate, we extract the capture cross section, which is suppressed by proximity to the diamond surface. The distance dependence is consistent with a carrier diffusion model, indicating that the itinerant carrier lifetime can be long, even at the diamond surface. Measuring dynamics of near-surface NV centers offers a tool for characterizing the diamond surface and investigating charge transport in diamond devices.

Physics↗

Creation of color centers in diamond by recoil implantation through dielectric films

The need of near-surface color centers in diamond for quantum technologies motivates the controlled doping of specific extrinsic impurities into the crystal lattice. Further, recent experiments have shown that this can be achieved by momentum transfer from a surface precursor via ion implantation, an approach known as “recoil implantation.” Here, we extend this technique to incorporate dielectric precursors for creating nitrogen-vacancy (NV) and silicon-vacancy (SiV) centers in diamond. Specifically, we demonstrate that gallium focused-ion-beam exposure to a thin layer of silicon nitride or silicon dioxide on the diamond surface results in the introduction of both extrinsic impurities and carbon vacancies. These defects subsequently give rise to near-surface NV and SiV centers with desirable properties after annealing.

42 ENGINEERING↗

Magnetometry in a diamond anvil cell using nitrogen vacancy centers in a nanodiamond ensemble

The emerging field of optical magnetometry utilizing negative-charged nitrogen vacancy (NV – ) centers provides a highly sensitive lab bench technique for spatially resolved physical property measurements. Their implementation in high pressure diamond anvil cell (DAC) environments will become common as other techniques are often limited due to the spatial constraints of the sample chamber. Apparatus and techniques are described here permitting for more general use of magnetic field measurements inside a DAC using continuous wave optical detected magnetic resonance in NV – centers in a layer of nanodiamonds. A microstrip antenna delivers a uniform microwave field to the DAC and is compatible with simple metal gaskets, and the sensor layer of deposited nanodiamonds allows for simple determination of the magnetic field magnitude for B in the 1–100 G range. The ferromagnetic transition in iron at 18 GPa is measured with the apparatus, along with its hysteretic response.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Triangular cross-section grating couplers for integrated quantum nanophotonic hardware in silicon carbide

We design, fabricate, and characterize fishbone grating couplers for triangular cross-section photonics in silicon carbide compatible with color center integration. The periodic and aperiodic grating coupler designs are optimized to outcouple up to 31% of light in the fundamental TE mode of a triangular waveguide. The devices are fabricated using an ion beam etching process in a 4H–SiC sample implanted with NV center ensembles. The room-temperature transmission and the cryogenic NV center photoluminescence collection measurements indicate experimental grating coupler efficiency of up to 24%. This result provides a scalable method to efficiently extract color center light from SiC quantum nanophotonic devices to free-space optics.

Saha, Pranta↗

Microwave-photonic control of optically accessible spin defects in diamond

A growing variety of optically accessible spin qubits have emerged in recent years as key components for quantum sensors, computers, and memories. However, the scalability of conventional spin-based quantum architectures remains limited by direct microwave delivery, which introduces thermal noise, electromagnetic crosstalk, and design constraints for cryogenic, high-field, and distributed systems. In this work, we present a unified framework for RF-over-fiber (RFoF) control of spins accessible through optically detected magnetic resonance (ODMR) spectroscopy of nitrogen-vacancy (NV) centers in diamond. The RFoF platform relies on an intensity-modulated 1310 nm laser carrying microwave signals over fiber and a high-speed photodiode for optical-to-electrical conversion to drive NV spin transitions. We report an RFoF power-conversion efficiency of 3.42% for an RF output PRF,out=-5.5 dBm at 2.87 GHz, enabling clear resolution of Zeeman splitting in

Rahman, M Reefaz [ORNL] (ORCID:0000000323541611)↗

Morphogenesis of spin cycloids in a noncollinear antiferromagnet

Pattern formation in spin systems with continuous-rotational symmetry (CRS) provides a powerful platform to study emergent complex magnetic phases and topological defects in condensed-matter physics. However, its understanding and correlation with unconventional magnetic order along with high-resolution nanoscale imaging are challenging. Here, we employ scanning nitrogen vacancy (NV) magnetometry to unveil the morphogenesis of spin cycloids at both the local and global scales within a single ferroelectric domain of (111)-oriented BiFeO 3 , which is a noncollinear antiferromagnet, resulting in formation of a glassy labyrinthine pattern. We find that the domains of locally oriented cycloids are interconnected by an array of topological defects and exhibit isotropic energy landscape predicted by first-principles calculations. We propose that the CRS of spin-cycloid propagation directions within the (111) drives the formation of the labyrinthine pattern and the associated topological defects such as antiferromagnetic skyrmions. Unexpectedly, reversing the as-grown ferroelectric polarization from [$\overline{1}$ $\overline{1}$ $\overline{1}$] to [111] produces a noncycloidal NV image contrast which ¯ could be attributed to either the emergence of a uniformly magnetized state or a reversal of the cycloid polarity. These findings highlight that (111)-oriented BiFeO 3 is not only important for studying the fascinating subject of pattern formation but could also be utilized as an ideal platform for integrating novel topological defects in the field of antiferromagnetic spintronics.

magnetoelectric↗

Dressed-State Hamiltonian Engineering in a Strongly Interacting Solid-State Spin Ensemble

In quantum science applications, ranging from many-body physics to quantum metrology, dipolar interactions in spin ensembles are often controlled via Floquet engineering. However, this technique typically reduces the interaction strength between spins and effectively weakens the coupling to a target sensing field, limiting the metrological sensitivity. In this Letter, we develop and demonstrate an alternative method that directly tunes the native dipolar interaction in an ensemble of nitrogen-vacancy (NV) centers in diamond, thereby overcoming these limitations inherent to Floquet engineering. Our approach utilizes dressed-state qubit encoding under a bias magnetic field applied perpendicular to the crystal lattice orientation. This method leads to a 3.2× enhancement of the dimensionless coherence parameter JT 2 compared to state-of-the-art Floquet engineering and a 2.6× (8.3 dB) enhanced sensitivity in ac magnetometry. Furthermore, our results provide a powerful Hamiltonian engineering tool for future studies with NV ensembles and other interacting higher-spin (S > $\frac{1}{2}$) systems.

Quantum control↗

Aluminum vacancy/sulfur complex in wurtzite AlN as an optically controllable spin qubit

Using our rational methodology, we reveal a defect in wurtzite AlN that can serve as an optically controllable spin qubit. It combines an Al vacancy and a S atom substituting the neighboring N atom (V Al⁢ S N ). Linear response GW and Bethe-Salpeter equation calculations guide us to find suitable ground and excited triplet and singlet states of V Al⁢ S N . The obtained optical spin-polarization cycle is similar to that observed in the negative nitrogen-vacancy (NV – ) center in diamond. Furthermore, the calculated optical oscillator strengths for V Al⁢ S N suggest that, in contrast to the NV – center, the optical emission in the singlet and triplet states have comparable rates, which is favorable for the qubit functionality.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗