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At least 955 records · Page 53

Hollow-cathode chemical vapor deposition of thick, low-stress diamond-like carbon films

A radio-frequency (RF), hollow-cathode plasma source with confining magnetic field is described for the chemical vapor deposition of thick ( > 10 µm), amorphous diamond-like carbon ablator films for inertial confinement fusion applications. Plasma is characterized by optical emission spectroscopy, while properties of the resultant films are measured by a combination of profilometry, Rutherford backscattering spectrometry, elastic recoil detection analysis, X-ray diffraction, Raman spectroscopy, and atomic force microscopy. The dependence of the deposition rate, film density, elemental composition, self-bias and residual stress is reported as a function of RF power. Higher density films were found when using Ar plasma, than N 2 or H 2 plasma. The coatings produced are x-ray amorphous, exhibit low compressive stress ( ~ 100 MPa), high density ( < 1.7 g/cm 3 ), hydrogen content of ~ 30 at.%, and a low average roughness of 0.75 nm. Finally, applications of these films as tunable-density ablators for inertial confinement fusion experiments are discussed.

36 MATERIALS SCIENCE↗

Experimental Approach to Controllably Vary Protein Oxidation While Minimizing Electrode Adsorption for Boron-Doped Diamond Electrochemical Surface Mapping Applications

Oxidative protein surface mapping has become a powerful approach for measuring the solvent accessibility of folded protein structures. A variety of techniques exist for generating the key reagent hydroxyl radicals for these measurements; however, many of these approaches require use of radioactive sources or caustic oxidizing chemicals. The purpose of this research was to evaluate and optimize the use of boron-doped diamond (BDD) electrochemistry as a highly accessible tool for producing hydroxyl radicals as a means to induce a controllable level of oxidation on a range of intact proteins. These experiments utilize a relatively high flow rates to reduce protein residence time inside the electrochemical flow chamber, along with a unique cell activation approach to improve control over the intact protein oxidation yield. Studies were conducted to evaluate the level of protein adsorption onto the electrode surface. This report demonstrates a robust protocol for the use of BDD electrochemistry and high performance LC-MS/MS as a high-throughput experimental pipeline for probing higher order protein structure, and illustrates how it is complementary to predictive computational modeling efforts.

boron-doped diamond electrochemistry↗

A Free-Standing Boron-Doped Diamond Grid Electrode for Fundamental Spectroelectrochemistry

Spectroelectrochemistry (SEC) is a powerful technique that enables a variety of redox properties to be studied, including formal potential (E o ), thermodynamic values (ΔG, ΔH, ΔS), diffusion coefficient (D), electron transfer stoichiometry (n), and others. SEC requires an electrode which light can pass through while maintaining sufficient electrical conductivity. This has been traditionally composed of metal or metal oxide films atop transparent substrates like glass, quartz, or metallic mesh. Robust electrode materials like boron-doped diamond (BDD) could help expand the environments in which SEC can be performed, but most designs are limited to thin films (~100–200 nm) on transparent substrates less resilient than free-standing BDD. Here, this work presents a free-standing BDD grid electrode (G-BDD) for fundamental SEC measurements, using the well-characterized Fe(CN) 6 3–/4– redox couple as proof-of-concept. With a combination of cyclic voltammetry (CV), thin-layer SEC, and chronoabsorptometry, several of the redox properties mentioned above were calculated and compared. For E o' , n, and D, similar results were obtained when comparing the CV [E o' = +0.279 (±0.002) V vs Ag/AgCl; n = 0.97; D = 4.1 × 10 –6 cm 2 ·s –1 ] and SEC [E o' = +0.278 (±0.001) V vs Ag/AgCl; n = 0.91; D = 5.2 × 10 –6 cm 2 ·s –1 ] techniques. Both values align with what has been previously reported. To calculate D from the SEC data, modification of the classical equation used in chronoabsorptometry was required to accommodate the G-BDD electrode geometry. Overall, this work expands on the applicability of SEC techniques and BDD as a versatile electrode material.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Interplay of Mechanochemistry and Material Processes in the Graphite to Diamond Phase Transformation

The manifestation of intramolecular strains in covalent systems is widely known to accelerate chemical reactions and open alternative reaction paths. This process is moderately well understood for isolated molecules and unimolecular processes. However, in condensed matter processes such as phase transformations, material properties and structure may influence typical mechanochemical effects. Therefore, we utilize steered molecular dynamics to induce out of plane strains in graphite and compress the system under a constant strain rate to induce phase transformation. We show that the out of plane strain allows phase transformations to initiate at small amounts of compressive strain. Yet, in contrast to typical mechanochemical results, the sum of compressive and out of plane work needed to form a diamond has a local minimum due to altered defect formation processes during phase transformation. Additionally, these altered processes slow the kinetics of the phase transformation, taking longer from initiation to total material transformation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Strongly Cavity-Enhanced Spontaneous Emission from Silicon-Vacancy Centers in Diamond

Quantum emitters are an integral component for a broad range of quantum technologies, including quantum communication, quantum repeaters, and linear optical quantum computation. Solid-state color centers are promising candidates for scalable quantum optics due to their long coherence time and small inhomogeneous broadening. However, once excited, color centers often decay through phonon-assisted processes, limiting the efficiency of single-photon generation and photon-mediated entanglement generation. Herein, we demonstrate strong enhancement of spontaneous emission rate of a single silicon-vacancy center in diamond embedded within a monolithic optical cavity, reaching a regime in which the excited-state lifetime is dominated by spontaneous emission into the cavity mode. We observe 10-fold lifetime reduction and 42-fold enhancement in emission intensity when the cavity is tuned into resonance with the optical transition of a single silicon-vacancy center, corresponding to 90% of the excited-state energy decay occurring through spontaneous emission into the cavity mode. Here, we also demonstrate the largest coupling strength ( g /2π = 4.9 ± 0.3 GHz) and cooperativity ( C = 1.4) to date for color-center-based cavity quantum electrodynamics systems, bringing the system closer to the strong coupling regime.

36 MATERIALS SCIENCE↗

Radiation-Induced Damage and Recovery of Ultra-Nanocrystalline Diamond: Toward Applications in Harsh Environments

Ultra-nanocrystalline diamond (UNCD) is increasingly being used in the fabrication of devices and coatings due to its excellent tribological properties, corrosion resistance, and biocompatibility. Here in this work, we study its response to irradiation with kiloelectronvolt electrons as a controlled model for extreme ionizing environments. Real time Raman spectroscopy reveals that the radiation-damage mechanism entails dehydrogenation of UNCD grain boundaries, and we show that the damage can be recovered by annealing at 883 K. Lastly, our results have significant practical implications for the implementation of UNCD in extreme environment applications, and indicate that the films can be used as radiation sensors.

36 MATERIALS SCIENCE↗

Super-Resolution Airy Disk Microscopy of Individual Color Centers in Diamond

Super-resolution imaging techniques enable nanoscale microscopy in fields such as physics, biology, and chemistry. However, many super-resolution techniques require specialized optical components, such as a helical-phase mask. In this work, we present a novel technique, super-resolution Airy disk microscopy, that can be used in a standard confocal microscope without any specialized optics. We demonstrate this technique, in combination with ground state depletion, to image and control nitrogen-vacancy (NV) centers in bulk diamond below the diffraction limit. A greater than 14-fold improvement in resolution compared to the diffraction limit is achieved, corresponding to a spatial resolution of 16.9(8) nm for a 1.3 NA microscope with 589 nm light. We make use of our enhanced spatial resolution to control the spins states of individual NV centers separated from each other by less than the diffraction limit, including pairs sharing the same orientation that are indistinguishable with a conventional electron spin resonance measurement.

36 MATERIALS SCIENCE↗

All-optical reconfiguration of single silicon-vacancy centers in diamond for non-volatile memories

Strain engineering is vital for tuning the optical and spin properties of solid-state color centers, enhancing spin coherence and compensating emission wavelength shift. Here, we develop an all-optical approach to directly modify the local strain of color centers at the nanoscale by migrating the nearby defect. High-power pulsed optical irradiation triggers defect migration, which subsequently leads to the redistribution of the local crystal lattice of the host material. This redistribution alters the strain experienced by nearby color centers. Using silicon-vacancy centers in diamond, we validate this method and demonstrate a ground state splitting enhancement of up to 1.8 THz. Unlike conventional methods, our approach requires no external fields or nanostructure modifications, enabling non-volatile strain control and optical memory functionality across wide temperature ranges. Its local, permanent nature offers a scalable path for enhancing spin coherence in large-scale quantum systems and has potential applications in photonic machine learning.

Nanoscale devices↗

Characterization of single crystal chemical vapor deposition diamond detectors for neutron spectrometry

Detectors made from artificial chemical vapor deposition single crystal diamond have shown great potential for fast neutron spectrometry. In this paper, we present the results of measurements made at the Physikalisch-Technische Bundesanstalt accelerator using neutron fields in the energy range from 7 MeV to 16 MeV. This study presents the first results of the characterization of the detector in this energy range.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Effect of high-intensity x-ray radiation on Bragg diffraction in silicon and diamond

We simulated the Bragg reflection of high-intensity short x-ray pulses from single-crystal silicon and diamond by coupling tight-binding-molecular dynamics with a simple atomic kinetics model. We found that even when the pulse-averaged Bragg intensity degrades significantly, the reflectivity drops only slightly at the beginning of the pulse until the lattice is disordered by non-thermal melting. These results suggest that Bragg reflectors could produce shortened x-ray pulses through temporal slicing.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Note: Measurements of fast electrons in the TORE-SUPRA tokamak by means of modified Cherenkov-type diamond detector

The Note reports on experimental studies of ripple born fast electrons within the TORE-SUPRA facility, which were performed by means of a modified measuring head equipped with diamond detectors designed especially for recording the electron-induced Cherenkov radiation. There are presented signals produced by fast electrons in the TORE-SUPRA machine, which were recorded during two experimental campaigns performed in 2010. Shapes of these electron-induced signals are considerably different from those observed during the first measurements carried out by the prototype Cherenkov probe in 2008. An explanation of the observed differences is given.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Nonlinear ionization mechanism dependence of energy absorption in diamond under femtosecond laser irradiation

We present first-principles calculations for nonlinear photoionization of diamond induced by the intense femtosecond laser field. A real-time and real-space time-dependent density functional theory with the adiabatic local-density approximation is applied to describe the laser-material interactions in the Kohn-Sham formalism with the self-interaction correction. For a certain laser wavelength, the intensity dependence of energy absorption on multiphoton and/or tunnel ionization mechanisms is investigated, where laser intensity regions vary from 10{sup 12} W/cm{sup 2} to 10{sup 16} W/cm{sup 2}. In addition, the effect of laser wavelength on energy absorption at certain ionization mechanism is discussed when the Keldysh parameter is fixed. Theoretical results show that: (1) at the fixed laser wavelength, the relationship between the energy absorption and laser intensity shows a good fit of E = c{sub M}I{sup N} (N is the number of photons absorbed to free from the valence band) when multiphoton ionization dominates; (2) while when tunnel ionization becomes significant, the relationship coincides with the expression of E = c{sub T}I{sup n} (n < N).

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

The potential application of ultra-nanocrystalline diamond films for heavy ion irradiation detection

The potential of utilizing the ultra-nanocrystalline (UNCD) films for detecting the Au-ion irradiation was investigated. When the fluence for Au-ion irradiation is lower than the critical value (f{sub c}= 5.0 Multiplication-Sign 10{sup 12} ions/cm{sup 2}) the turn-on field for electron field emission (EFE) process of the UNCD films decreased systematically with the increase in fluence that is correlated with the increase in sp{sup 2}-bonded phase ({pi}{sup *}-band in EELS) due to the Au-ion irradiation. The EFE properties changed irregularly, when the fluence for Au-ion irradiation exceeds this critical value. The transmission electron microscopic microstructural examinations, in conjunction with EELS spectroscopic studies, reveal that the structural change preferentially occurred in the diamond-to-Si interface for the samples experienced over critical fluence of Au-ion irradiation, viz. the crystalline SiC phase was induced in the interfacial region and the thickness of the interface decreased. These observations implied that the UNCD films could be used as irradiation detectors when the fluence for Au-ion irradiation does not exceed such a critical value.

36 MATERIALS SCIENCE↗

Laser-driven 1 GeV carbon ions from preheated diamond targets in the break-out afterburner regime

Experimental data are presented for laser-driven carbon C{sup 6+} ion-acceleration, verifying 2D-PIC studies for multi-species targets in the Break-Out Afterburner regime. With Trident's ultra-high contrast at relativistic intensities of 5 × 10{sup 20} W/cm{sup 2} and nm-scale diamond targets, acceleration of carbon ions has been optimized by using target laser-preheating for removal of surface proton contaminants. Using a high-resolution wide angle spectrometer, carbon C{sup 6+} ion energies exceeding 1 GeV or 83 MeV/amu have been measured, which is a 40% increase in maximum ion energy over uncleaned targets. These results are consistent with kinetic plasma modeling and analytic theory.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Increased negatively charged nitrogen-vacancy centers in fluorinated diamond

We investigated the effect of fluorine-terminated diamond surface on the charged state of shallow nitrogen vacancy defect centers (NVs). Fluorination is achieved with CF{sub 4} plasma, and the surface chemistry is confirmed with x-ray photoemission spectroscopy. Photoluminescence of these ensemble NVs reveals that fluorine-treated surfaces lead to a higher and more stable negatively charged nitrogen vacancy (NV{sup −}) population than oxygen-terminated surfaces. NV{sup −} population is estimated by the ratio of negative to neutral charged NV zero-phonon lines. Surface chemistry control of NV{sup −} density is an important step towards improving the optical and spin properties of NVs for quantum information processing and magnetic sensing.

36 MATERIALS SCIENCE↗

Radiation-assisted Frenkel-Poole transport in single-crystal diamond

The measurement of the density of occupied states as a function of the applied electric field, performed on single-crystal chemical vapour deposition diamond by x-ray modulated photocurrent technique, is reported. Two regimes of non-linear charge transport were observed: a classical Frenkel-Poole (FP) process at high electric fields (>6800 V/cm), and a radiation-assisted transport mechanism at intermediate electric fields (2000 to 6800 V/cm), consisting of a double-step process in which the direct re-emission into the extended band occurs following multiple photo-induced FP-like hopping transitions.

36 MATERIALS SCIENCE↗

Three-dimensional diamond detectors: Charge collection efficiency of graphitic electrodes

Implementation of 3D-architectures in diamond detectors promises to achieve unreached performances in the radiation-harsh environment of future high-energy physics experiments. This work reports on the collection efficiency under β-irradiation of graphitic 3D-electrodes, created by laser pulses in the domains of nanoseconds (ns-made-sensors) and femtoseconds (fs-made-sensors). Full collection is achieved with the fs-made-sensors, while a loss of 25%–30% is found for the ns-made-sensors. The peculiar behaviour of ns-made sensors has been explained by the presence of a nano-structured sp{sup 3}-carbon layer around the graphitic electrodes, evidenced by micro-Raman imaging, by means of a numerical model of the charge transport near the electrodes.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

High stability electron field emitters made of nanocrystalline diamond coated carbon nanotubes

We report enhanced life-time stability for the electron field emitters prepared by coating nanocrystalline diamond (NCD) on carbon nanotubes (CNTs). Upon overcoming the problem of poor stability in CNTs, the NCD-CNTs exhibit excellent life-time stability of 250 min tested at different applied voltages of 600 and 900 V. In contrast, the life-time stability of CNTs is only 33 min even at relatively low voltage of 360 V and starts arcing at 400 V. Hence, the NCD-CNTs with improved life-time stability have great potential for the applications as cathodes in flat panel displays and microplasma display devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗