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At least 595 records · Page 33
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Explorations of the nonheme high-valent iron-oxo landscape: crystal structure of a synthetic complex with an [Fe IV 2 (μ-O) 2 ] diamond core relevant to the chemistry of sMMOH

Methanotrophic bacteria utilize methane monooxygenase (MMO) to carry out the first step in metabolizing methane. The soluble enzymes employ a hydroxylase component (sMMOH) with a nonheme diiron active site that activates O 2 and generates a powerful oxidant capable of converting methane to methanol. It is proposed that the diiron(II) center in the reduced enzyme reacts with O 2 to generate a diferric-peroxo intermediate called P that then undergoes O–O cleavage to convert into a diiron(IV) derivative called Q, which carries out methane hydroxylation. Most (but not all) of the spectroscopic data of Q accumulated by various groups to date favor the presence of an Fe IV 2 (μ-O) 2 unit with a diamond core. The Que lab has had a long-term interest in making synthetic analogs of iron enzyme intermediates. To this end, the first crystal structure of a complex with a Fe III Fe IV (μ-O) 2 diamond core was reported in 1999, which exhibited an Fe∙∙∙Fe distance of 2.683(1) Å. Now more than 20 years later, a complex with an Fe IV 2 (μ-O) 2 diamond core has been synthesized in sufficient purity to allow diffraction-quality crystals to be grown. Finally, its crystal structure has been solved, revealing an Fe∙∙∙Fe distance of 2.711(4) Å for comparison with structural data for related complexes with lower iron oxidation states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

Effects of high energy Au-ion irradiation on the microstructure of diamond films

The effects of 2.245 GeV Au-ion irradiation and subsequent annealing processes on the evolution of microstructure of diamond films with microcrystalline (MCD) or ultra-nanocrystalline (UNCD) granular structure were investigated, using near edge x-ray absorption fine structure and electron energy loss spectroscopy in transmission electron microscopy. For MCD films, the Au-ion irradiation disintegrated some of the diamond grains, resulting in the formation of nano-sized carbon clusters embedded in a matrix of amorphous carbon (a-C). The annealing process recrystallized the diamond grains and converted the a-C into nano-sized graphite particulates and, at the same time, induced the formation of nano-sized i-carbon clusters, the bcc structured carbon with a{sub 0} = 0.432 nm. In contrast, for UNCD films, the Au-ion irradiation transformed the grain boundary phase into nano-sized graphite, but insignificantly altered the crystallinity of the grains of the UNCD films. The annealing process recrystallized the materials. In some of the regions, the residual a-C phases were transformed into nano-sized graphites, whereas in other regions i-carbon nanoclusters were formed. The difference in irradiation-induced microstructural transformation behavior between the MCD and the UNCD films is ascribed to the different granular structures of the two types of films.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Research Update: Direct conversion of amorphous carbon into diamond at ambient pressures and temperatures in air

We report on fundamental discovery of conversion of amorphous carbon into diamond by irradiating amorphous carbon films with nanosecond lasers at room-temperature in air at atmospheric pressure. We can create diamond in the form of nanodiamond (size range <100 nm) and microdiamond (>100 nm). Nanosecond laser pulses are used to melt amorphous diamondlike carbon and create a highly undercooled state, from which various forms of diamond can be formed upon cooling. The quenching from the super undercooled state results in nucleation of nanodiamond. It is found that microdiamonds grow out of highly undercooled state of carbon, with nanodiamond acting as seed crystals.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Curved diamond-crystal spectrographs for x-ray free-electron laser noninvasive diagnostics

Here, we report on the manufacturing and X-ray tests of bent diamond-crystal X-ray spectrographs, designed for noninvasive diagnostics of the X-ray free-electron laser (XFEL) spectra in the spectral range from 5 to 15 keV. The key component is a curved, 20-µm thin, single crystalline diamond triangular plate in the (110) orientation. The radius of curvature can be varied between R = 0.6 m and R = 0.1 m in a controlled fashion, ensuring imaging in a spectral window of up to 60 eV for ' 8 keV X-rays. All of the components of the bending mechanism (about 10 parts) are manufactured from diamond, thus ensuring safe operations in intense XFEL beams. The spectrograph is transparent to 88% for 5-keV photons, and to 98% for 15-keV photons. Therefore, it can be used for noninvasive diagnostics of the X-ray spectra during XFEL operations.

47 OTHER INSTRUMENTATION↗
DOE OSTI2017

Analysis of the reverse I-V characteristics of diamond-based PIN diodes

Diamond is one of the most promising candidates for high power and high temperature applications, due to its large bandgap and high thermal conductivity. As a result of the growth and fabrication process of diamond-based devices, structural defects such as threading dislocations (TDs) may degrade the electrical properties of such devices. Understanding and control of such defects are important for improving device technology, particularly the reverse breakdown characteristics. Here, we show that the reverse bias current-voltage characteristics in diamond PIN diodes can be described by hopping conduction and Poole-Frenkel emission through TDs over the temperature (T) range of 323 K < T < 423 K, for typical values of the TD density found in epitaxially grown materials.

Saremi, Mehdi (ORCID:0000000150415886)↗
DOE OSTI2018

Micro-architecture embedding ultra-thin interlayer to bond diamond and silicon via direct fusion

The continuous demand on miniaturized electronic circuits bearing high power density illuminates the need to modify the silicon-on-insulator-based chip architecture. This is due to the low thermal conductivity of the few hundred nanometer-thick insulator present between the silicon substrate and active layers. The thick insulator is notorious for releasing the heat generated from the active layers during the operation of devices, leading to degradation in their performance and thus reducing their lifetime. To avoid the heat accumulation, we propose a method to fabricate the silicon-on-diamond (SOD) microstructure featured by an exceptionally thin silicon oxycarbide interlayer (~3 nm). While exploiting the diamond as an insulator, we employ spark plasma sintering to render the silicon directly fused to the diamond. Importantly, this process can manufacture the SOD microarchitecture via a simple/rapid way and incorporates the ultra-thin interlayer for minute thermal resistance. The approach invented herein expects to minimize the thermal interfacial resistance of the devices and is thus deemed as a breakthrough appealing to the current chip industry.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Graphite to diamond transformation under shock compression: Role of orientational order

To gain insight into the role of orientational order on the shock-induced graphite to diamond phase transformation, three pyrolytic graphite types having different orientational orders were shock-compressed along the average c -axis to peak stresses between 35 and 69 GPa. The materials studied were ZYB-grade highly oriented pyrolytic graphite (HOPG), ZYH-grade HOPG, and as-deposited pyrolytic graphite (PG) having mosaic spreads of 0.8° ± 0.2°, 3.5° ± 1.5°, and ~45°, respectively. Wave profiles, obtained using laser interferometry, show a multiple-wave structure with a distinct, rapid (<10 ns) rise to the high-pressure phase for each graphite type. Multiple-wave profiles, first observed in this study for the less ordered ZYH-grade HOPG and PG samples, show that somewhat poorly oriented pyrolytic graphites also undergo a well-defined phase transformation. Previously, rapid transformation was reported for ZYB-grade but not ZYH-grade HOPG. The measured wave profiles for both HOPG grades are very similar and both grades show a ~22 GPa transformation stress. In contrast, the PG wave profiles are quite different and show a ~46 GPa transformation stress. The continuum results (stress-density states) presented here cannot distinguish between the different high-pressure phases [hexagonal diamond (HD) or cubic diamond] reported in recent x-ray studies. Because ZYB-grade HOPG was recently shown to transform to HD and due to the similar peak states for both HOPG grades, it seems likely that ZYH-grade also transforms into HD. In conclusion, the very different shock responses of PG and HOPG suggest different transformation mechanisms for PG and HOPG, but the high-pressure PG phase remains unclear in the present work.

58 GEOSCIENCES↗
DOE OSTI2019

How carbon vacancies can affect the properties of group IV color centers in diamond: A study of thermodynamics and kinetics

Recently, there has been much interest in using Group IV elements from the periodic table to fabricate and study XV color centers in diamond, where X=Si, Ge, Sn, or Pb and V is a carbon vacancy. These Group IV color centers have a number of interesting spin and optical properties, which could potentially make them better candidates than NV− centers for important applications in quantum computing and quantum information processing. Unfortunately, the very same ion implantation process that is required to create these XV color centers in diamond necessarily also produces many carbon vacancies (VC), which can form complexes with these color centers (VC−XV) that can dramatically affect the properties of the isolated XV color centers. The main focus of this work is to use density-functional theory to study the thermodynamics and kinetics of the formation of these VC−XV complexes and to suggest experimental ways to impede this process such as varying the Fermi level of the host diamond material through chemical doping or applying an external electrical bias. We also include a discussion of how the simple presence of many VC can negatively impact the spin coherence times (T2) of Group IV color centers through the presence of acoustic phonons.

Kuate Defo, Rodrick↗
DOE OSTI2021

Large microwave inductance of granular boron-doped diamond superconducting films

Boron-doped diamond granular thin films are known to exhibit superconductivity with an optimal critical temperature of T c =7.2 K. Here, we report the measured in-plane complex surface impedance of boron-doped diamond films in the microwave frequency range using a resonant technique. Experimentally measured inductance values are in good agreement with estimates obtained from the normal state sheet resistance of the material. Additionally, the magnetic penetration depth temperature dependence is consistent with that of a fully gapped s-wave superconductor. Boron-doped diamond films should find application where high kinetic inductance is needed, such as microwave kinetic inductance detectors and quantum impedance devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Quantum networks based on color centers in diamond

With the ability to transfer and process quantum information, large-scale quantum networks will enable a suite of fundamentally new applications, from quantum communications to distributed sensing, metrology, and computing. This Perspective reviews requirements for quantum network nodes and color centers in diamond as suitable node candidates. We give a brief overview of state-of-the-art quantum network experiments employing color centers in diamond and discuss future research directions, focusing, in particular, on the control and coherence of qubits that distribute and store entangled states, and on efficient spin–photon interfaces. We discuss a route toward large-scale integrated devices combining color centers in diamond with other photonic materials and give an outlook toward realistic future quantum network protocol implementations and applications.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2022

Nanoscale solid-state nuclear quadrupole resonance spectroscopy using depth-optimized nitrogen-vacancy ensembles in diamond

Nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) spectroscopy of bulk quantum materials have provided insight into phenomena, such as quantum phase criticality, magnetism, and superconductivity. With the emergence of nanoscale 2D materials with magnetic phenomena, inductively detected NMR and NQR spectroscopy are not sensitive enough to detect the smaller number of spins in nanomaterials. The nitrogen-vacancy (NV) center in diamond has shown promise in bringing the analytic power of NMR and NQR spectroscopy to the nanoscale. However, due to depth-dependent formation efficiency of the defect centers, noise from surface spins, band bending effects, and the depth dependence of the nuclear magnetic field, there is ambiguity regarding the ideal NV depth for surface NMR of statistically polarized spins. In this work, we prepared a range of shallow NV ensemble layer depths and determined the ideal NV depth by performing NMR spectroscopy on statistically polarized 19 F in Fomblin oil on the diamond surface. We found that the measurement time needed to achieve a signal-to-noise ratio of 3 using XY8-N noise spectroscopy has a minimum at an NV ensemble depth of 5.5 ± 1.5 nm for ensembles activated from 100 ppm nitrogen concentration. To demonstrate the sensing capabilities of NV ensembles, we perform NQR spectroscopy on the 11 B of hexagonal boron nitride flakes. We compare our best diamond to previous work with a single NV and find that this ensemble provides a shorter measurement time with excitation diameters as small as 4 μm. Furthermore, this analysis provides ideal conditions for further experiments involving NMR/NQR spectroscopy of 2D materials with magnetic properties.

2D materials↗
DOE OSTI2023

Externally Heated Diamond ANvil Cell Experimentation (EH-DANCE) for studying materials and processes under extreme conditions

Externally heated diamond anvil cells provide a stable and uniform thermal environment, making them a versatile device to simultaneously generate high-pressure and high-temperature conditions in various fields of research, such as condensed matter physics, materials science, chemistry, and geosciences. The present study features the Externally Heated Diamond ANvil Cell Experimentation (EH-DANCE) system, a versatile configuration consisting of a diamond anvil cell with a customized microheater for stable resistive heating, bidirectional pressure control facilitated by compression and decompression membranes, and a water-cooled enclosure suitable for vacuum and controlled atmospheres. This integrated system excels with its precise control of both pressure and temperature for mineral and materials science research under extreme conditions. Here, we showcase the capabilities of the system through its successful application in the investigation of the melting temperature and thermal equation of state of high-pressure ice-VII at temperatures up to 1400 K. The system was also used to measure the elastic properties of solid ice-VII and liquid H 2 O using Brillouin scattering and Raman spectra of carbonates using Raman spectroscopy, highlighting the potential of the EH-DANCE system in high-pressure research.

Instruments & Instrumentation↗
DOE OSTI2024

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↗
DOE OSTI2024

Multi-microscopy characterization of threading dislocations in CVD-grown diamond films

We present site-coincident imaging of a high dislocation density boron-doped chemical vapor deposition-grown homoepitaxial (001) diamond film using electron channeling contrast imaging (ECCI), cathodoluminescence, transmission electron microscopy (TEM), and scanning secondary ion mass spectroscopy (SIMS). With growing interest in large area heteroepitaxial substrates, we show that ECCI is a promising technique to accurately evaluate dislocations in diamond films. We find the electron backscatter yield is sufficient to distinguish individual threading dislocations in ECCI despite the low atomic number of carbon, and we have generally good agreement between dislocations observed in ECCI and TEM of the same region. Importantly, relying on luminescence in the 430 nm dislocation-related A-band alone results in an underestimation of the defect density as we find only 20%–40% of the threading dislocations luminesce. Here, we further show that dislocations do not perturb the spatial uniformity of boron doping measured by SIMS, even when the dislocations are clustered with high density, and we can tentatively rule out strong segregation effects at the dislocations. Our results establish the complementary use of microscopy and microanalysis methods to rapidly characterize and understand the impact of dislocations in diamond thin films.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Integrated phononic waveguide on thin-film lithium niobate on diamond

Here, we demonstrate wavelength-scale phononic waveguides formed by transfer-printed thin-film lithium niobate (LN) on bulk diamond, a material stack that combines the strong piezoelectricity of LN with the high acoustic velocity and color-center compatibility of diamond. We characterize a delay line based on a 100 μm long phononic waveguide at room and cryogenic temperatures. The total insertion loss through the device at 4 K is −5.8 dB, corresponding to a $>$ 50 % transducer efficiency, at a frequency of 2.8 GHz. Our work represents a step toward phonon-mediated hybrid quantum systems consisting of strain-sensitive color centers in diamond.

Malik, Sultan [Stanford Univ., CA (United States)]↗
DOE OSTI2026

Design of a double-sided laser heating compatible piezoelectrically driven dynamic diamond anvil cell

Piezoelectrically driven dynamic diamond anvil cells are generally limited to use at room temperature due to spatial conflicts with the optical components necessary for double-sided laser heating. Here, this work describes the design of a double-sided laser-heating-compatible, piezoelectrically driven dynamic diamond anvil cell (LH-dDAC) that expands the range of experimentally accessible compression rate/temperature space. By developing a spatially in-parallel design, in which the diamond anvils and the piezo actuators lie alongside each other, the total length of the apparatus is reduced to 66.5 mm. The new LH-dDAC is capable of probing both overpressure and compression-rate effects on the kinetics of phase transitions. We illustrate the capability of the new LH-dDAC using the following cases: (1) a simultaneous pressure and temperature jump from 19.5 GPa and room temperature to 40 GPa and ≈1550 K and (2) a controlled compression ramp at ≈1850 K and ≈100 GPa/s. By pairing rapid compression with laser heating, the new LH-dDAC opens the door to studies of diffusionally controlled transformations at high pressures and temperatures.

Copley, J. A. [Princeton Univ., NJ (United States)↗
DOE OSTI2025

Engineering spin coherence in core-shell diamond nanocrystals

Fluorescent diamond nanocrystals can host spin qubit sensors capable of probing the physical properties of biological systems with nanoscale spatial resolution. Sub-100 nm diamond nanosensors can readily be delivered into intact cells and even living organisms. However, applications beyond current proof-of-principle experiments require a substantial increase in sensitivity, which is limited by surface induced charge instability and electron-spin dephasing. In this work, we utilize engineered core-shell structures to achieve a drastic increase in qubit coherence times (T 2 ) from 1.1 to 35 μs in bare nanodiamonds to upward of 52 to 87 μs. We use electron-paramagnetic-resonance results to present a band bending model and connect silica encapsulation to the removal of deleterious mid-gap surface states that are negatively affecting the qubit’s spin properties. Combined with a 1.9-fold increase in particle luminescence these advances correspond to up to two-order-of-magnitude reduction in integration time. Probing qubit dynamics at a single particle level further reveals that the noise characteristics fundamentally change from a bath with spins that rearrange their spatial configuration during the course of an experiment to a more dilute static bath. The observed results shed light on the underlying mechanisms governing fluorescence and spin properties in diamond nanocrystals and offer an effective noise mitigation strategy based on engineered core-shell structures.

core-shell↗
DOE OSTI2025

Design, fabrication, and testing of diamond axicons for X-ray microscopy applications

This work presents the design, fabrication, and experimental validation of a refractive diamond axicon for X-ray beam shaping. The diamond axicon was developed to overcome the limitations of polymer-based axicons particularly for application in Transmission X-ray Microscopy (TXM) systems, offering superior mechanical strength, thermal stability, and radiation resistance, making it ideal for synchrotron applications. The axicon was fabricated using femtosecond laser ablation and tested at 11 keV under various coherence conditions. Results demonstrated that the axicon efficiently transformed the X-ray beam into a ring-shaped profile with over 80% transmission. Simulations confirmed the experimental findings and highlighted the potential for further improvements. This work paves the way for the use of diamond axicons in next-generation synchrotron facilities, with future efforts focusing on optimizing fabrication and testing the axicon in full TXM systems.

Samadi, Nazanin↗