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At least 37 records · Page 2

Passive Low-Energy Nuclear-Recoil Detection with Color Centers

Crystal-damage events such as tracks and point defects have been used to record and detect radiation for a long time and recently they have been proposed as a means for dark-matter detection. Color centers can be read out optically and we propose a scheme based on selective plane illumination microscopy for micrometer-scale imaging of large volumes corresponding to kilogram mass detectors. This class of detectors would be passive and would operate at room temperature and we call this the passive low-energy optical color-center nuclear-recoil (PALEOCCENE) detection method. We apply these concepts to the detection of reactor neutrinos using coherent elastic neutrino nucleus scattering (CE ν NS). Crystal-damage formation energies are intrinsically on the order of 25 eV, resulting in similarly low nuclear-recoil thresholds. Furthermore, this would enable the observation of reactor-neutrino CE ν NS with detectors as small as 10 g. Additionally, a competitive search for spin-dependent dark-matter scattering down to a dark-matter mass of 0.3 GeV could be possible. Passive crystal detectors might also be attractive for nuclear-nonproliferation safeguards if used to monitor reactor power and to put limits on plutonium production. The passive nature and small footprint of the proposed detectors implies that these might fit well within accepted reactor-safeguards operations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Exploration of Defect Dynamics and Color Center Qubit Synthesis with Pulsed Ion Beams

Short-pulse ion beams have been developed in recent years and now enable applications in materials science. A tunable flux of selected ions delivered in pulses of a few nanoseconds can affect the balance of defect formation and dynamic annealing in materials. We report results from color center formation in silicon with pulses of 900 keV protons. G-centers in silicon are near-infrared photon emitters with emerging applications as single-photon sources and for spin-photon qubit integration. G-centers consist of a pair of substitutional carbon atoms and one silicon interstitial atom and are often formed by carbon ion implantation and thermal annealing. Here, we report on G-center formation with proton pulses in silicon samples that already contained carbon, without carbon ion implantation or thermal annealing. The number of G-centers formed per proton increased when we increased the pulse intensity from 6.9 × 10 9 to 7.9 × 10 10 protons/cm 2 /pulse, demonstrating a flux effect on G-center formation efficiency. We observe a G-center ensemble linewidth of 0.1 nm (full width half maximum), narrower than previously reported. Pulsed ion beams can extend the parameter range available for fundamental studies of radiation-induced defects and the formation of color centers for spin-photon qubit applications.

43 PARTICLE ACCELERATORS↗

Many-Electron System on Helium and Color Center Spectroscopy

Electrons on the helium surface display sharp resonant absorption lines related to the transitions between the subbands of quantized motion transverse to the surface. A magnetic field parallel to the surface strongly affects the absorption spectrum.We show that the effect results from admixing the intersubband transitions to the in-plane quantum dynamics of the strongly correlated electron liquid or a Wigner crystal. This is similar to the admixing of electron transitions in color centers to phonons. Furthermore, the spectrum permits a direct characterization of the many-electron dynamics and also enables testing the theory of color centers in a system with controllable coupling.

36 MATERIALS SCIENCE↗

Methods for Color Center Preserving Hydrogen‐Termination of Diamond

Abstract Chemical functionalization of diamond surfaces by hydrogen is an important method for controlling the charge state of near‐surface fluorescent color centers, an essential process in fabricating devices such as diamond field‐effect transistors and chemical sensors, and a required first step for realizing families of more complex terminations through subsequent chemical processing. In all these cases, termination is typically achieved using hydrogen plasma sources that can etch or damage the diamond, as well as deposited materials or embedded color centers. This work explores alternative methods for lower‐damage hydrogenation of diamond surfaces, specifically the annealing of diamond samples in high‐purity, non‐explosive mixtures of nitrogen and hydrogen gas, and the exposure of samples to microwave hydrogen plasmas in the absence of intentional stage heating. The effectiveness of these methods are characterized by x‐ray photoelectron spectroscopy (XPS), and comparison of the results to density‐functional modelling of the surface hydrogenation energetics implicates surface oxygen ligands as the primary factor limiting the termination quality of annealed samples. Finally, photoluminescence (PL) spectroscopy is used to verify that both the annealing and reduced sample temperature plasma methods are non‐destructive to near‐surface ensembles of nitrogen‐vacancy (NV) centers, in stark contrast to plasma treatments that use heated sample stages.

36 MATERIALS SCIENCE↗

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↗

Color center in β -Ga 2 O 3 emitting at the telecom range

Transition metal (TM) ions incorporated into a host from a wide bandgap semiconductor are recognized as a promising system for quantum technologies with enormous potential. In this work, we report on a TM color center in β-Ga 2 O 3 with physical properties attractive for quantum information applications. The center is found to emit at 1.316 μm and exhibits weak coupling to phonons, with optically addressable higher-lying excited states, beneficial for single-photon emission within the telecom range (O-band). Using magneto-photoluminescence (PL) complemented by time-resolved PL measurements, we identify the monitored emission to be internal 1 E→ 3 A 2 spin-forbidden transitions of a 3d 8 TM ion with a spin-triplet ground state—a possible candidate for a spin qubit. We tentatively attribute this color center to a complex involving a sixfold coordinated Cu 3+ ion.

36 MATERIALS SCIENCE↗

Detecting fractionalization in critical spin liquids using color centers

Quantum spin liquids are highly entangled ground states of insulating spin systems, in which magnetic ordering is prevented down to the lowest temperatures due to quantum fluctuations. One of the most extraordinary characteristics of quantum spin liquid phases is their ability to support fractionalized, low-energy quasiparticles known as spinons, which carry spin-1/2 but bear no charge. Relaxometry based on color centers in crystalline materials—of which nitrogen-vacancy (NV) centers in diamond are a well-explored example—provides an exciting new platform to probe the spin spectral functions of magnetic materials with both energy and momentum resolution and to search for signatures of these elusive, fractionalized excitations. In this work, we theoretically investigate the color-center relaxometry of two archetypal quantum spin liquids: the two-dimensional U(1) quantum spin liquid with a spinon Fermi surface and the spin-1/2 antiferromagnetic spin chain. The former is characterized by a metallic, spin-split ground state of mobile, interacting spinons, which closely resembles a spin-polarized Fermi liquid ground state but with neutral quasiparticles. We show that the observation of the Stoner continuum and the collective spin wave mode in the spin spectral function would provide a strong evidence for the existence of spinons and fractionalization. In one dimension, mobile spinons form a Luttinger liquid ground state. We show that the spin spectral function exhibits strong features representing the collective density and spin-wave modes, which are broadened in an algebraic fashion with an exponent characterized by the Luttinger parameter. The possibilities of measuring these collective modes and detecting the power-law decay of the spectral weight using NV relaxometry are discussed. We also examine how the transition rates are modified by marginally irrelevant operators in the Heisenberg limit. Published by the American Physical Society 2024

Takei, So (ORCID:0000000191771895)↗

[2 + 2] Cycloaddition Produces Divalent Organic Color-Centers with Reduced Heterogeneity in Single-Walled Carbon Nanotubes

Organic color centers (OCCs), generated by the covalent functionalization of single-walled carbon nanotubes, have been exploited for chemical sensing, bioimaging, and quantum technologies. However, monovalent OCCs can assume at least 6 different bonding configurations on the sp 2 carbon lattice of a chiral nanotube, resulting in heterogeneous OCC photoluminescence emissions. Herein, we show that a heat-activated [2 + 2] cycloaddition reaction enables the synthesis of divalent OCCs with a reduced number of atomic bonding configurations. The chemistry occurs by simply mixing enophile molecules (e.g., methylmaleimide, maleic anhydride, and 4-cyclopentene-1,3-dione) with an ethylene glycol suspension of SWCNTs at elevated temperature (70–140 °C). Unlike monovalent OCC chemistries, we observe just three OCC emission peaks that can be assigned to the three possible bonding configurations of the divalent OCCs based on density functional theory calculations. Notably, these OCC photoluminescence peaks can be controlled by temperature to decrease the emission heterogeneity even further. Furthermore, this divalent chemistry provides a scalable way to synthesize OCCs with tightly controlled emissions for emerging applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Studies on color-center formation in glass utilizing measurements made during 1 to 3 MeV electron irradiation

The coloring of NBS 710 glass was studied using a facility for making optical absorption measurements during and after electron irradiation. The induced absorption contains three Gaussian shaped bands. The color center growth curves contain two saturating exponential and one linear components. After irradiation the coloring decays can be described by three decreasing exponentials. At room temperature both the coloring curve plateau and coloring rate increases with increasing dose rate. Coloring measurements made at fixed dose rate but at increasing temperature indicate: (1) The coloring curve plateau decreases with increasing temperature and coloring is barely measurable near 400 C. (2) The plateau is reached more rapidly as the temperature increases. (3) The decay occurring after irradiation cannot be described by Arrhenius kinetics. At each temperature the coloring can be explained by simple kinetics. The temperature dependence of the decay can be explained if it is assumed that the thermal untrapping is controlled by a distribution of activation energies.

Swyler, K. J.↗

Multi-energy ion irradiation effects and distinctive features of color center generation in yttria-stabilized zirconia driven by structural discrepancy

Regarding a requirement for inert matrix fuel (IMF) to burn minor actinides and plutonium and high-level waste immobilization, Yttria-stabilized zirconia (ZrO 2 -6.5 wt% Y 2 O 3 ) (YSZ) crystals with cubic phase are selected to comprehensively evaluate the irradiation resistance by irradiation-induced structural discrepancies across multiple energy conditions. Electronic excitation and nuclear collisions reveal distinct color centers, influenced by varying component ratios that reflect their formation mechanisms. Key factors driving ultra-fast structural transitions include collision cascades, pressure waves, and energy dissipation from electronic excitation. In this work, we find that in the electronic energy loss (E ele )-dominant region, internal latent tracks with unique surface nanostructures emerge, distinct from the defect clusters seen in the nuclear energy loss (E nuc )-dominant region, while the threshold for latent track formation and melting are identified. In conclusion, structural discrepancies driven by different energy-loss mechanisms promote the generation of singly ionized and nearest-neighbor doubly ionized oxygen vacancies, which respectively dominate the formation of F⁺ and T-centers, resulting in bandgap narrowing (4.80 eV → 4.73 eV), and furthermore triggering visible light emission (2.17 eV → 2.20 eV) in irradiated YSZ crystals, thus, enabling the design of novel irradiation-tailored material functionalities.

36 MATERIALS SCIENCE↗

Modeling of Radiative Emission from Shallow Color Centers in Single Crystalline Diamond

Optically active defects in diamond are widely used as bright single-photon sources for quantum sensing, computing, and communication. For many applications, it is useful to place the emitter close to the diamond surface, where the radiative properties of the emitter are strongly modified by its dielectric environment. It is well-known that the radiative power from an electric dipole decreases as the emitter approaches an interface with a lower-index dielectric, leading to an increase in the radiative lifetime. For emitters in crystalline solids, modeling of this effect needs to take into account the crystal orientation and direction of the surface cut, which can greatly impact the emission characteristics. In this paper, a framework for analyzing the emission rates of shallow (<100 nm) defects is provided, in which optical transitions are derived from electric dipoles in a plane perpendicular to their spin axis. The calculations for the depth-dependent radiative lifetime for color centers in (100)-, (110)-, and (111)-cut diamond are presented, which can be extended to other vacancy defects in diamond.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Photochemical spin-state control of binding configuration for tailoring organic color center emission in carbon nanotubes

Abstract Incorporating fluorescent quantum defects in the sidewalls of semiconducting single-wall carbon nanotubes (SWCNTs) through chemical reaction is an emerging route to predictably modify nanotube electronic structures and develop advanced photonic functionality. Applications such as room-temperature single-photon emission and high-contrast bio-imaging have been advanced through aryl-functionalized SWCNTs, in which the binding configurations of the aryl group define the energies of the emitting states. However, the chemistry of binding with atomic precision at the single-bond level and tunable control over the binding configurations are yet to be achieved. Here, we explore recently reported photosynthetic protocol and find that it can control chemical binding configurations of quantum defects, which are often referred to as organic color centers, through the spin multiplicity of photoexcited intermediates. Specifically, photoexcited aromatics react with SWCNT sidewalls to undergo a singlet-state pathway in the presence of dissolved oxygen, leading to ortho binding configurations of the aryl group on the nanotube. In contrast, the oxygen-free photoreaction activates previously inaccessible para configurations through a triplet-state mechanism. These experimental results are corroborated by first principles simulations. Such spin-selective photochemistry diversifies SWCNT emission tunability by controlling the morphology of the emitting sites.

36 MATERIALS SCIENCE↗

Nuclear recoil detection with color centers in bulk lithium fluoride

We present initial results on the detection of nuclear recoils in lithium fluoride (LiF) through the fluorescence of color centers created by particle interactions in the crystal lattice. Using light-sheet fluorescence microscopy, we image nuclear recoil tracks from both fast and thermal neutron interactions deep within a cubic-centimeter-scale sample. Automated three-dimensional feature extraction based on machine-learning tools enables the identification and classification of individual events. We observe that the fluorescence response of LiF to gamma irradiation is strongly suppressed, by a factor of 30–50 compared to neutron exposure, demonstrating intrinsic insensitivity to electromagnetic backgrounds. The observed and simulated event characteristics are consistent, including their number, size, and topology. These results establish the feasibility of LiF as a scalable detection medium for rare nuclear-recoil events and constitute a first step toward 10–1000 g scale detectors with single-event sensitivity for applications in reactor-neutrino detection, neutron spectroscopy, and dark matter searches.

Aroujo, G R [University of Zurich]↗