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At least 19 records

Electric field sensitivity of molecular color centers

Molecular color centers with S=1 ground states are promising candidates for quantum sensing of electric fields. These molecules have an electronic structure similar to solid state color centers, but they allow for processing modalities that permit direct interfacing with an analyte. Currently, it is unknown how sensitive these molecules are to electric fields and what molecular properties affect their sensitivity. We perform density functional theory calculations to understand the impact of electric fields on the electronic structure of five nominally tetrahedral molecular color centers exhibiting variable transition metal chemistry and ligand densities. We then extract the Stark parameters from each of these molecules and compare them to molecular properties such as the dipole moment and inner shell stiffness and find that the dipole moment of the molecule largely governs sensitivity. We predict that polar heteroleptic molecules may have electric field sensitivities comparable to solid state color centers such as nitrogen-vacancy centers in diamond.

Physics↗

High-Performance Near-Infrared Quantum Emission from Color Centers in hBN

Color centers hosted in hexagonal boron nitride (hBN) have emerged as a highly promising platform for single-photon emission and spin-photon technologies relevant to quantum communication and quantum networking. As a wide bandgap van der Waals material, hBN can host optically active quantum defects across a broad spectral range. Here, we demonstrate a simple and scalable oxygen-plasma process that reproducibly creates single quantum emitters in hBN with blinking-free zero-phonon lines (ZPLs) spanning near-infrared (NIR) from 700 up to 971 nm. These emitters combine MHz-level brightness, single-photon purity up to 99.9%, and ultranarrow cryogenic line widths down to 2.7 GHz under quasi-resonant excitation, placing them in a particularly attractive regime for quantum photonics. Photostability measurements further reveal resistance to photobleaching, subnanometer spectral stability over long time scales, and near-shot-noise-limited intensity fluctuations. Analysis of the phonon sidebands shows weak vibronic coupling and ZPL-dominated emission, with Debye–Waller factors approaching 50%. Control experiments together with elemental mapping support oxygen incorporation as a necessary ingredient in activating the NIR emitter population, while first-principles calculations identify O N V N and O N V N H as the leading defect candidates. These results establish a high-performance NIR quantum-emitter platform in hBN for free-space quantum networking and future integrated quantum-photonic architectures.

2D materials↗

Photophysics of O-band and transition metal color centers in monolithic silicon for quantum communications

Color centers in the O-band (1260–1360 nm) are crucial for realizing long-coherence quantum network nodes in memory-assisted quantum communications. However, only a limited number of O-band color centers have been thoroughly explored in silicon hosts as spin-photon interfaces. This study explores and compares two promising O-band color centers in silicon for high-fidelity spin-photon interfaces: T and *Cu (transition metal) centers. During T center generation process, we observed the formation and dissolution of other color centers, including the copper-silver related centers with a doublet line around 1312 nm (*Cu$^0_n$), near the optical fiber zero dispersion wavelength (around 1310 nm). We then investigated the photophysics of both T and *Cu centers, focusing on their emission spectra and spin properties. The *Cu$^0_0$ line under a 0.5 T magnetic field demonstrated a 25% broadening, potentially due to spin degeneracy, suggesting that this center can be a promising alternative to T centers.

42 ENGINEERING↗

Unraveling sources of emission heterogeneity in Silicon Vacancy color centers with cryo-cathodoluminescence microscopy

Diamond color centers have proven to be versatile quantum emitters and exquisite sensors of stress, temperature, electric and magnetic fields, and biochemical processes. Among color centers, the silicon-vacancy (SiV - ) defect exhibits high brightness, minimal phonon coupling, narrow optical linewidths, and high degrees of photon indistinguishability. Yet the creation of reliable and scalable SiV - -based color centers has been hampered by heterogeneous emission, theorized to originate from surface imperfections, crystal lattice strain, defect symmetry, or other lattice impurities. Here, we advance high-resolution cryo-electron microscopy combined with cathodolumines cence spectroscopy and 4D scanning transmission electron microscopy (STEM) to elucidate the structural sources of heterogeneity in SiV - emission from nanodiamond with sub-nanometer-scale resolution. Our diamond nanoparticles are grown directly on TEM membranes from molecular-level seedings, representing the natural formation conditions of color centers in diamond. We show that individual subcrystallites within a single nanodiamond exhibit distinct zero-phonon line (ZPL) energies and differences in brightness that can vary by 0.1 meV in energy and over 70% in brightness. These changes are correlated with the atomic-scale lattice structure. We find that ZPL blue shifts result from tensile strain, while ZPL red shifts are due to compressive strain. We also find that distinct crystallites host distinct densities of SiV - emitters and that grain boundaries impact SiV - emission significantly. Finally, we interrogate nanodiamonds as small as 40 nm in diameter and show that these diamonds exhibit no spatial change to their ZPL energy. Our work provides a foundation for atomic-scale structure-emission correlation, e.g., of single atomic defects in a range of quantum and two-dimensional materials.

36 MATERIALS SCIENCE↗

Fabrication of single color centers in sub-50 nm nanodiamonds using ion implantation

Diamond color centers have been widely studied in the field of quantum optics. The negatively charged silicon vacancy (SiV – ) center exhibits a narrow emission linewidth at the wavelength of 738 nm, a high Debye–Waller factor, and unique spin properties, making it a promising emitter for quantum information technologies, biological imaging, and sensing. In particular, nanodiamond (ND)-based SiV – centers can be heterogeneously integrated with plasmonic and photonic nanostructures and serve as in vivo biomarkers and intracellular thermometers. Out of all methods to produce NDs with SiV – centers, ion implantation offers the unique potential to create controllable numbers of color centers in preselected individual NDs. However, the formation of single color centers in NDs with this technique has not been realized. We report the creation of single SiV– centers featuring stable high-purity single-photon emission through Si implantation into NDs with an average size of ~20 nm. We observe room temperature emission, with zero-phonon line wavelengths in the range of 730–800 nm and linewidths below 10 nm. Our results offer new opportunities for the controlled production of group-IV diamond color centers with applications in quantum photonics, sensing, and biomedicine.

36 MATERIALS SCIENCE↗

Purcell-Enhanced Emissions from Diamond Color Centers in Slow Light Photonic Crystal Waveguides

Diamond color centers are promising candidates for optically addressable quantum memories, which motivates the development of efficient photonic interfaces, often using nanophotonic cavities with narrow spectral line widths and small mode volumes. However, they require perfect spectral and spatial overlap between the cavity mode and quantum emitter, which is challenging. This is especially true for solid-state quantum emitters that are often randomly positioned and suffer from inhomogeneous broadening. Another approach to enhance light-matter interaction across large optical bandwidths and areas is using slow light waveguides. Here, in this study, we demonstrate diamond slow light photonic crystal (PhC) waveguides optically coupled to embedded silicon-vacancy (SiV) color centers. We use the recently developed thin-film diamond approach to fabricate fully suspended two-dimensional PhC waveguides. We demonstrate waveguide modes with high group indices up to 70 and observe Purcell-enhanced emissions of the SiVs. Our approach represents a practical diamond platform for robust spin-photon interfaces with color centers.

2D photonic crystal waveguide↗

Hybrid quantum nanophotonic devices with color centers in nanodiamonds [Invited]

Optically active color centers in nanodiamonds offer unique opportunities for generating and manipulating quantum states of light. These mechanically, chemically, and optically robust emitters can be produced in mass quantities, deterministically manipulated, and integrated with a variety of quantum device geometries and photonic material platforms. Nanodiamonds with deeply sub-wavelength sizes coupled to nanophotonic structures feature a giant enhancement of light-matter interaction, promising high bitrates in quantum photonic systems. We review the recent advances in controlled techniques for synthesizing, selecting, and manipulating nanodiamond-based color centers for their integration with quantum nanophotonic devices.

Sahoo, Swetapadma (ORCID:0000000179281391)↗

Measuring Two Key Parameters of H3 Color Centers in Diamond

A method of measuring two key parameters of H3 color centers in diamond has been created as part of a continuing effort to develop tunable, continuous-wave, visible lasers that would utilize diamond as the lasing medium. (An H3 color center in a diamond crystal lattice comprises two nitrogen atoms substituted for two carbon atoms bonded to a third carbon atom. H3 color centers can be induced artificially; they also occur naturally. If present in sufficient density, they impart a yellow hue.) The method may also be applicable to the corresponding parameters of other candidate lasing media. One of the parameters is the number density of color centers, which is needed for designing an efficient laser. The other parameter is an optical-absorption cross section, which, as explained below, is needed for determining the number density. The present method represents an improvement over prior methods in which optical-absorption measurements have been used to determine absorption cross sections or number densities. Heretofore, in order to determine a number density from such measurements, it has been necessary to know the applicable absorption cross section; alternatively, to determine the absorption cross section from such measurements, it has been necessary to know the number density. If, as in this case, both the number density and the absorption cross section are initially unknown, then it is impossible to determine either parameter in the absence of additional information.

Roberts, W. Thomas↗

Combining femtosecond laser annealing and shallow ion implantation for local color center creation in diamond

A common technique for color center creation in wideband gap semiconductors employs ion implantation and a subsequent thermal annealing. In general, this annealing process is conducted in a vacuum oven. Here, we exploit the annealing based on femtosecond laser pulses. For that purpose, we implant fluorine ions at 54 keV and chlorine ions at 74 keV in diamond and perform micrometer precise annealing using focused femtosecond laser pulses at 800 ± (30) nm with different pulse numbers and repetition rates. In this way, we were able to create shallow spots with color centers of varying brightness.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

A Chemist’s Guide to Solid-State Qubits: Diamond Color Centers as Embedded Vacancy-Centered Molecules

Diamond point defects or color centers are at the crux of solid-state quantum technology applications, from computing to sensing. Modeling molecular qubits has advanced by leaps and bounds mainly due to the advanced quantum mechanical (QM) tools in the arsenal of quantum chemists for modeling (isolated) molecular systems, which should be easily translatable for analogous systems in the solid state. Here, we simulate a series of diamond defects: a carbon vacancy (V C ) and second row substitutions that are adjacent to a V C or D C V C , with D = B, N, and O, to evaluate their magnetic and optical properties. We applied molecular orbital principles, an embedded cluster method, and a multiconfigurational QM theory to computationally characterize the above-mentioned defects for a multitude of spin, charge, and excited states. Our computational approach delivered high-quality QM insights that compare well with experiments. Furthermore, with this framework, we confirm the spin-triplets B C V C – and O C V C 0 to be analogous to N C V C – , with calculated bright transitions that respectively correspond to UV (3.80 eV) and blue (2.65 eV) light absorption and emission lifetimes (τ) of 2.3 and 5.6 ns, which are higher in energy and more short-lived (and thus brighter) than that for N C V C – : green (2.26 eV), τ = 9.5 ns.

Martirez, John Mark P. [Princeton Plasma Physics L↗

Multiplexed color centers in a silicon photonic cavity array

Entanglement distribution is central to the modular scaling of quantum processors and establishing quantum networks. Color centers with telecom-band transitions and long spin coherence times are suitable candidates for long-distance entanglement distribution. However, high-bandwidth memory-enhanced quantum communication is limited by high-yield, scalable creation of efficient spin-photon interfaces. Here, we develop a silicon photonics platform consisting of arrays of bus-coupled cavities. The coupling to a common bus waveguide enables simultaneous access to individually addressable cavity-enhanced T center arrays. We demonstrate frequency-multiplexed operation of two T centers in separate photonic crystal cavities. In addition, we investigate the cavity enhancement of a T center through hybridized modes formed between physically distant cavities. Our results show that bus-coupled arrays of cavity-enhanced color centers could enable efficient on-chip and long-distance entanglement distribution.

Komza, Lukasz↗

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.↗