arXiv subjects

Rhonda M. Stroud

Publications and source records attributed to Rhonda M. Stroud.

At least 19 recordsLinked to original sources

arXiv2026

Calorimetric Measurement of the Surface Energy of Enstatite, MgSiO$_3$

Surface thermodynamics of minerals influence their properties and occurrence in both terrestrial and planetary systems. Using high-temperature oxide melt solution calorimetry, we report the first direct measurement of the surface energy of enstatite, MgSiO$_3$. Enstatite nanoparticles of different sizes were synthesized using the sol-gel method, characterized with X-ray diffraction, thermal analysis, infrared spectroscopy, surface area measurements, and electron microscopy. The materials consist of crystallites with sizes of $\sim $10 - 20 nm, which are agglomerated into larger nanoparticles. Thus, both surface and interface terms contribute to the measured enthalpies. Analysis based on calorimetry and calculated surface and interface areas gives the surface enthalpy of enstatite as 4.79 $\pm$ 0.45 J m$^{-2}$. This value is comparable to that of forsterite (Mg$_2$SiO$_4$) and larger than those of many nonsilicate oxide materials. This large surface energy may present a barrier to the nucleation of enstatite in planetary atmospheres and other geochemical and planetary environments. The interfacial energy of enstatite appears to be close to zero. The transition enthalpy from bulk orthoenstatite to bulk clinoenstatite is 0.34 $\pm$ 0.93 kJ mol$^{-1}$, which is in agreement with earlier reports. The methodology developed here can be extended to other materials having complex structures and morphologies to separate surface and interfacial contributions to energetics.

cond-mat.mtrl-sci↗

arXiv2023

Explosive Nucleosynthesis in Core-Collapse Type II Supernovae: Insights from new C, N, Si, and Al-Mg isotopic compositions of presolar grains

We report C, N, Si, and Al-Mg isotope data for 39 presolar X silicon carbide (SiC) and four silicon nitride grains - a group of presolar grains that condensed in the remnants of core-collapse Type II supernovae (CCSNe) - isolated from the Murchison meteorite. Energy dispersive X-ray (EDX) data were used to determine the Mg and Al contents of the X SiC grains for comparison with the Mg/Al ratios determined by secondary ion mass spectroscopy (SIMS). Previous SIMS studies have used O-rich standards in the absence of alternatives. In this study, the correlated isotopic and elemental data of the X SiC grains enabled accurate determination of the initial 26Al/27Al ratios for the grains. Our new grain data suggest that (i) the literature data for X grains are affected to varying degrees by asteroidal/terrestrial contamination, and (ii) the Al/Mg ratios in SiC are a factor of two (with +/-6% 1 sigma uncertainties) lower than estimated based on the SIMS analyses that used O-rich standards. The lowered Al/Mg ratios result in proportionally higher inferred initial 26Al/27Al ratios for presolar SiC grains. In addition, the suppression of asteroidal/terrestrial contamination in this study leads to the observation of negative trends for 12C/13C-30Si/28Si and 26Al/27Al-30Si/28Si among our CCSN grains. We discuss these isotope trends in the light of explosive CCSN nucleosynthesis models, based on which we provide new insights into several non-traditional CCSN nucleosynthesis processes, including explosive H burning, the existence of a C/Si zone in the outer regions of CCSNe, and neutrino-nucleus reactions in deep CCSN regions.

astro-ph.SR↗

arXiv2023

Tracing the history of an unusual compound presolar grain from progenitor star to asteroid parent body host

We conducted a TEM study of an unusual oxide-silicate composite presolar grain (F2-8) from the unequilibrated ordinary chondrite Semarkona. The presolar composite grain is relatively large, has an amoeboidal shape, and contains Mg-rich olivine, Mg-Al spinel, and Ca-rich pyroxene. The shape and phase assemblage are reminiscent of amoeboid-olivine-aggregates and add to the growing number of TEM observations of presolar refractory inclusion-like (CAIs and AOAs) grains. In addition to the dominant components, F2-8 also contains multiple subgrains, including an alabandite-oldhamite composite grain within the olivine and several magnetite subgrains within the Mg-Al spinel. We argue that the olivine, Mg-Al spinel, and alabandite-oldhamite formed by equilibrium condensation, whereas the Ca-rich pyroxene formed by non-equilibrium condensation, all in an M-type AGB star envelope. On the other hand, the magnetite subgrains are likely the result of aqueous alteration on the Semarkona asteroidal parent body. Additional evidence of secondary processing includes Fe-enrichment in the Mg-Al spinel and olivine, elevated Al contents in the olivine, and beam sensitivity and a modulated structure for the olivine. Compound presolar grains record condensation conditions over a wide range of temperatures. Additionally, the presence of several different presolar phases in a composite grain can impart information on the relative rates and effects of post-condensation processing in a range of environments, including the interstellar medium, solar nebula, and the host asteroid parent body. The TEM observations of F2-8 provide insights across the lifetime of the grain from its formation by condensation in an M-type AGB star envelope, its transit through the interstellar medium, and aqueous alteration during its residence on Semarkona's asteroidal parent body.

astro-ph.EP↗

arXiv2022

Presolar stardust in asteroid Ryugu

We have conducted a NanoSIMS-based search for presolar material in samples recently returned from C-type asteroid Ryugu as part of JAXA's Hayabusa2 mission. We report the detection of all major presolar grain types with O- and C-anomalous isotopic compositions typically identified in carbonaceous chondrite meteorites: 1 silicate, 1 oxide, 1 O-anomalous supernova grain of ambiguous phase, 38 SiC, and 16 carbonaceous grains. At least two of the carbonaceous grains are presolar graphites, whereas several grains with moderate C isotopic anomalies are probably organics. The presolar silicate was located in a clast with a less altered lithology than the typical extensively aqueously altered Ryugu matrix. The matrix-normalized presolar grain abundances in Ryugu are 4.8$^{+4.7}_{-2.6}$ ppm for O-anomalous grains, 25$^{+6}_{-5}$ ppm for SiC grains and 11$^{+5}_{-3}$ ppm for carbonaceous grains. Ryugu is isotopically and petrologically similar to carbonaceous Ivuna-type (CI) chondrites. To compare the in situ presolar grain abundances of Ryugu with CI chondrites, we also mapped Ivuna and Orgueil samples and found a total of SiC grains and 6 carbonaceous grains. No O-anomalous grains were detected. The matrix-normalized presolar grain abundances in the CI chondrites are similar to those in Ryugu: 23 $^{+7}_{-6}$ ppm SiC and 9.0$^{+5.3}_{-4.6}$ ppm carbonaceous grains. Thus, our results provide further evidence in support of the Ryugu-CI connection. They also reveal intriguing hints of small-scale heterogeneities in the Ryugu samples, such as locally distinct degrees of alteration that allowed the preservation of delicate presolar material.

astro-ph.EP↗

arXiv2022

TEM analyses of in situ presolar grains from unequilibrated ordinary chondrite LL3.0 Semarkona

We investigated six presolar grains from very primitive regions of the matrix in the unequilibrated ordinary chondrite Semarkona with TEM. These grains include one SiC, one oxide (Mg-Al spinel), and four silicates. Structural and elemental compositional studies of presolar grains located within their meteorite hosts have the potential to provide information on conditions and processes throughout the grains' histories. Our analyses show that the SiC and spinel grains are stoichiometric and well crystallized. In contrast, the majority of the silicate grains are non-stoichiometric and poorly crystallized. These findings are consistent with previous TEM studies of presolar grains from interplanetary dust particles and chondritic meteorites. We interpret the poorly crystalline nature, non-stoichiometry, more Fe- rather than Mg-rich compositions, and/or compositional heterogeneities as features of the formation by condensation under non-equilibrium conditions. Evidence for parent body alteration includes rims with mobile elements (S or Fe) on the SiC grain and one silicate grain. Other features characteristic of secondary processing in the interstellar medium, the solar nebula, and/or on parent bodies, were not observed or are better explained by processes operating in circumstellar envelopes. In general, there was very little overprinting of primary features of the presolar grains by secondary processes (e.g., ion irradiation, grain-grain collisions, thermal metamorphism, aqueous alteration). This finding underlines the need for additional TEM studies of presolar grains located in the primitive matrix regions of Semarkona, to address gaps in our knowledge of presolar grain populations accreted to ordinary chondrites.

astro-ph.EP↗

arXiv2022

Room-temperature oxygen transport in nano-thin BixOySez enables precision modulation of 2D materials

Oxygen conductors and transporters are important to several consequential renewable energy technologies, including fuel cells and syngas production. Separately, monolayer transition metal dichalcogenides (TMDs) have demonstrated significant promise for a range of applications, including quantum computing, advanced sensors, valleytronics, and next-gen optoelectronics. Here, we synthesize a few nanometer-thick BixOySez compound that strongly resembles a rare R3m bismuth oxide (Bi2O3) phase, and combine it with monolayer TMDs, which are highly sensitive to their environment. We use the resulting 2D heterostructure to study oxygen transport through BixOySez into the interlayer region, whereby the 2D material properties are modulated, finding extraordinarily fast diffusion at room temperature under laser exposure. The oxygen diffusion enables reversible and precise modification of the 2D material properties by controllably intercalating and deintercalating oxygen. Changes are spatially confined, enabling submicron features (e.g. pixels), and are long-term stable for more than 221 days. Our work suggests few nanometer-thick BixOySez is a promising unexplored room-temperature oxygen transporter. Additionally, our findings suggest the mechanism can be applied to other 2D materials as a generalized method to manipulate their properties with high precision and submicron spatial resolution.

cond-mat.mtrl-sci↗

arXiv2022

Laser-patterned submicron Bi2Se3-WS2 pixels with tunable circular polarization at room temperature

Characterizing and manipulating the circular polarization of light is central to numerous emerging technologies, including spintronics and quantum computing. Separately, monolayer tungsten disulfide (WS2) is a versatile material that has demonstrated promise in a variety of applications, including single photon emitters and valleytronics. Here, we demonstrate a method to tune the photoluminescence (PL) intensity (factor of x161), peak position (38.4meV range), circular polarization (39.4% range), and valley polarization of a Bi2Se3-WS2 2D heterostructure using a low-power laser (0.762uW) in ambient. Changes are spatially confined to the laser spot, enabling submicron (814nm) features, and are long-term stable (>334 days). PL and valley polarization changes can be controllably reversed through laser exposure in vacuum, allowing the material to be erased and reused. Atmospheric experiments and first-principles calculations indicate oxygen diffusion modulates the exciton radiative vs. non-radiative recombination pathways, where oxygen absorption leads to brightening, and desorption to darkening.

cond-mat.mtrl-sci↗

arXiv2021

TEM analyses of unusual presolar silicon carbide: Insights into the range of circumstellar dust condensation conditions

Presolar silicon carbide (SiC) grains in meteoritic samples can help constrain circumstellar condensation processes and conditions in C-rich stars and core-collapse supernovae. This study presents our findings on eight presolar SiC grains from AGB stars (four mainstream and one Y grain) and core-collapse supernovae (three X grains), chosen on the basis of μ-Raman spectral features that were indicative of their having unusual non-3C polytypes and/or high degrees of crystal disorder. Analytical transmission electron microscopy (TEM), which provides elemental compositional and structural information, shows evidence for complex histories for the grains. Our TEM results confirm the presence of non-3C,2H crystal domains. Minor element heterogeneities and/or subgrains were observed in all grains analyzed for their compositions. The C/O ratios inferred for the parent stars varied from 0.98 to greater than or equal to 1.03. Our data show that SiC condensation can occur under a wide range of conditions, in which environmental factors other than temperature (e.g., pressure, gas composition, heterogeneous nucleation on pre-condensed phases) play a significant role. Based on previous μ-Raman studies, about 10% of SiC grains may have infrared (IR) spectral features that are influenced by crystal defects, porosity, and/or subgrains. Future sub-diffraction limited IR measurements of complex SiC grains might shed further light on the relative contributions of each of these features to the shape and position of the characteristic IR 11-μm SiC feature and thus improve the interpretation of IR spectra of AGB stars like those that produced the presolar SiC grains.

astro-ph.SR↗

arXiv2021

Automatic detection of impact craters on Al foils from the Stardust interstellar dust collector using convolutional neural networks

NASA's Stardust mission utilized a sample collector composed of aerogel and aluminum foil to return cometary and interstellar particles to Earth. Analysis of the aluminum foil begins with locating craters produced by hypervelocity impacts of cometary and interstellar dust. Interstellar dust craters are typically less than one micrometer in size and are sparsely distributed, making them difficult to find. In this paper, we describe a convolutional neural network based on the VGG16 architecture that achieves high specificity and sensitivity in locating impact craters in the Stardust interstellar collector foils. We evaluate its implications for current and future analyses of Stardust samples.

astro-ph.IM↗

arXiv2020

Epitaxial bulk acoustic wave resonators as highly coherent multi-phonon sources for quantum acoustodynamics

Solid-state quantum acoustodynamic (QAD) systems provide a compact platform for quantum information storage and processing by coupling acoustic phonon sources with superconducting or spin qubits. The multi-mode composite high-overtone bulk acoustic wave resonator (HBAR) is a popular phonon source well suited for QAD. However, scattering from defects, grain boundaries, and interfacial/surface roughness in the composite transducer severely limits the phonon relaxation time in sputter-deposited devices. Here, we grow an epitaxial-HBAR, consisting of a metallic NbN bottom electrode and a piezoelectric GaN film on a SiC substrate. The acoustic impedance-matched epi-HBAR has a power injection efficiency > 99% from transducer to phonon cavity. The smooth interfaces and low defect density reduce phonon losses, yielding fxQ products and phonon lifetimes up to 1.36 x 10^17 Hz and 500 microseconds respectively. The GaN/NbN/SiC epi-HBAR is an electrically actuated, multi-mode phonon source that can be directly interfaced with NbN-based superconducting qubits or SiC-based spin qubits.

physics.app-ph↗

arXiv2019

Enabling remote quantum emission in 2D semiconductors via porous metallic networks

The interaction between two-dimensional crystals (2DCs) and metals is ubiquitous in 2D material research. Here we report how 2DC overlayers influence the recrystallization of relatively thick metal films and the subsequent synergetic benefits this provides for coupling surface plasmon-polaritons (SPPs) to photon emission in 2D semiconductors. We show that annealing 2DC/Au films on SiO2 results in a 'reverse epitaxial' process where initially nanocrystalline Au films become highly textured and in close crystallographic registry to the 2D crystal overlayer. With continued annealing, the metal underlayer dewets to form an oriented pore enabled network (OPEN) film in which the 2DC overlayer remains suspended above or coats the inside of the metal pores. This OPEN film geometry supports SPPs launched by either direct laser excitation or by light emitted from the TMD semiconductor itself, where energy in-coupling and out-coupling occurs at the metal pore sites such that dielectric spacers between the metal and 2DC layer are unnecessary. At low temperatures a high density of single-photon emitters (SPEs) is present across an OPEN-WSe2 film, and we demonstrate non-local excitation of SPEs at a distance of 17 μm with minimal loss of photon purity. Our results suggest the OPEN film geometry is a versatile platform that could facilitate the use of layered materials in quantum optics systems.

cond-mat.mes-hall↗

arXiv2019

Presolar Grains in Primitive Ungrouped Carbonaceous Chondrite Northwest Africa 5958

We report a correlated NanoSIMS-transmission electron microscopy study of the ungrouped carbonaceous chondrite Northwest Africa (NWA) 5958. We identified 10 presolar SiC grains, 2 likely presolar graphite grains, and 20 presolar silicate and/or oxide grains in NWA 5958. We suggest a slight modification of the commonly used classification system for presolar oxides and silicates that better reflects the grains' likely stellar origins. The matrix-normalized presolar SiC abundance in NWA 5958 is $18_{-10}^{+15}$ ppm (2$σ$), similar to that seen in many classes of unmetamorphosed chondrites. In contrast, the matrix-normalized abundance of presolar O-rich phases (silicates and oxides) is $30.9_{-13.1}^{+17.8}$ ppm (2$σ$), much lower than seen in interplanetary dust particles and the least altered CR, CO and ungrouped C chondrites, but close to that reported for CM chondrites. NanoSIMS mapping also revealed an unusual $^{13}$C-enriched ($δ^{13}$C$\sim$ 100--200 permil) carbonaceous rim surrounding a 1.4 $μ$m diameter phyllosilicate grain. TEM analysis of two presolar grains with a likely origin in asymptotic giant branch stars identified one as enstatite and one as Al-Mg spinel with minor Cr. The enstatite grain amorphized rapidly under the electron beam, suggesting partial hydration. TEM data of NWA 5958 matrix confirm that it has experienced aqueous alteration and support the suggestion of Jacquet et al. (2016) that this meteorite has affinities to CM2 chondrites.

astro-ph.EP↗

arXiv2018

High-temperature Dust Condensation around an AGB Star: Evidence from a Highly Pristine Presolar Corundum

Corundum ($α$-Al$_{2}$O$_{3}$) and amorphous or metastable Al$_{2}$O$_{3}$ are common components of circumstellar dust observed around O-rich asymptotic giant branch (AGB) stars and found in primitive meteorites. We report a detailed isotopic and microstructural investigation of a unique presolar corundum grain, QUE060, identified in an acid residue of the Queen Alexandra Range 97008 (LL3.05) meteorite. Based on its O and Mg isotopic compositions, this 1.4 $μ$m diameter grain formed in a low- or intermediate-mass AGB star. It has four developed rhombohedral $\{$011$\}$ faces of corundum and a rough, rounded face with cavities. High Mg contents (Mg/Al $>$ 0.004) are due to the decay of radioactive $^{26}$Al. No spinel (MgAl$_{2}$O$_{4}$) inclusions that might have exsolved from the corundum are observed, but there are several high-Mg domains with modulated structures. The subhedral shape of grain QUE060 is the first clear evidence that corundum condenses and grows to micrometer sizes in the extended atmospheres around AGB stars. The flat faces indicate that grain QUE060 experienced little modification by gas-grain and grain-grain collisions in the interstellar medium (ISM) and solar nebula. The Mg distribution in its structure indicates that grain QUE060 has not experienced any severe heating events since the exhaustion of $^{26}$Al. However, it underwent at least one very transient heating event to form the high-Mg domains. A possible mechanism for producing this transient event, as well as the one rough surface and cavity, is a single grain-grain collision in the ISM. These results indicate that grain QUE060 is the most pristine circumstellar corundum studied to date.

astro-ph.EP↗

arXiv2018

Controlling the Infrared Dielectric Function through Atomic-Scale Heterostructures

Surface phonon polaritons (SPhPs) - the surface-bound electromagnetic modes of a polar material resulting from the coupling of light with optic phonons - offer immense technological opportunities for nanophotonics in the infrared (IR) spectral region. Here, we present a novel approach to overcome the major limitation of SPhPs, namely the narrow, material-specific spectral range where SPhPs can be supported, called the Reststrahlen band. We use an atomic-scale superlattice (SL) of two polar semiconductors, GaN and AlN, to create a hybrid material featuring layer thickness-tunable optic phonon modes. As the IR dielectric function is governed by the optic phonon behavior, such control provides a means to create a new dielectric function distinct from either constituent material and to tune the range over which SPhPs can be supported. This work offers the first glimpse of the guiding principles governing the degree to which the dielectric function can be designed using this approach.

cond-mat.mtrl-sci↗

arXiv2018

High pressure, high temperature molecular doping of nanodiamond

The development of color centers in diamond as the basis for emerging quantum technologies has been limited by the need for ion implantation to create the appropriate defects. We present a versatile method to dope diamond without ion implantation, by synthesis of a doped amorphous carbon precursor and transformation at high temperatures and high pressures. To explore this bottom-up method for color center generation, we rationally create silicon-vacancy defects in nanodiamond and investigate them for optical pressure metrology. In addition, we show that this process can generate noble gas defects within diamond from the typically-inactive argon pressure medium, which may explain the hysteresis effects observed in other high pressure experiments and the presence of noble gases in some meteoritic nanodiamonds. Our results illustrate a general method to produce color centers in diamond, and may enable the controlled generation of designer defects.

cond-mat.mtrl-sci↗

arXiv2018

High Abundances of Presolar Grains and $^{15}$N-rich Organic Matter in CO3.0 Chondrite Dominion Range 08006

NanoSIMS C-, N-, and O-isotopic mapping of matrix in CO3.0 chondrite Dominion Range (DOM) 08006 revealed it to have in its matrix the highest abundance of presolar O-rich grains (257 +76 / -96 ppm, 2$σ$) of any meteorite. It also has a matrix abundance of presolar SiC of 35 (+25 / -17, 2$σ$) ppm, similar to that seen across primitive chondrite classes. This provides additional support to bulk isotopic and petrologic evidence that DOM 08006 is the most primitive known CO meteorite. Transmission electron microscopy of five presolar silicate grains revealed one to have a composite mineralogy similar to larger amoeboid olivine aggregates and consistent with equilibrium condensation, two non-stoichiometric amorphous grains and two olivine grains, though one is identified as such solely based on its composition. We also found insoluble organic matter (IOM) to be present primarily as sub-micron inclusions with ranges of C- and N-isotopic anomalies similar to those seen in primitive CR chondrites and interplanetary dust particles. In contrast to other primitive extraterrestrial materials, H isotopic imaging showed normal and homogeneous D/H. Most likely, DOM 08006 and other CO chondrites accreted a similar complement of primitive and isotopically anomalous organic matter to that found in other chondrite classes and IDPs, but the very limited amount of thermal metamorphism experienced by DOM 08006 has caused loss of D-rich organic moieties, while not substantially affecting either the molecular carriers of C and N anomalies or most inorganic phases in the meteorite. One C-rich grain that was highly depleted in $^{13}$C and $^{15}$N was identified; we propose it originated in the Sun's parental molecular cloud.

astro-ph.EP↗

arXiv2017

Photothermal effects during nanodiamond synthesis from a carbon aerogel in a laser-heated diamond anvil cell

Nanodiamonds have emerged as promising materials for quantum computing, biolabeling, and sensing due to their ability to host color centers with remarkable photostability and long spin-coherence times at room temperature. Recently, a bottom-up, high-pressure, high-temperature (HPHT) approach was demonstrated for growing nanodiamonds with color centers from amorphous carbon precursors in a laser-heated diamond anvil cell (LH-DAC) that was supported by a near-hydrostatic noble gas pressure medium. However, a detailed understanding of the photothermal heating and its effect on diamond growth, including the phase conversion conditions and the temperature-dependence of color center formation, has not been reported. In this work, we measure blackbody radiation during LH-DAC synthesis of nanodiamond from carbon aerogel to examine these temperature-dependent effects. Blackbody temperature measurements suggest that nanodiamond growth can occur at 16.3 GPa and 1800 K. We use Mie theory and analytical heat transport to develop a predictive photothermal heating model. This model demonstrates that melting the noble gas pressure medium during laser heating decreases the local thermal conductivity to drive a high spatial resolution of phase conversion to diamond. Finally, we observe a temperature-dependent formation of nitrogen vacancy centers and interpret this phenomenon in the context of HPHT carbon vacancy diffusion using CBΩ theory.

cond-mat.mtrl-sci↗

arXiv2016

The Effect of Preparation Conditions on Raman and Photoluminescence of Monolayer WS2

We report on preparation dependent properties observed in monolayer WS2 samples synthesized via chemical vapor deposition (CVD) on a variety of common substrates (Si/SiO2, sapphire, fused silica) as well as samples that were transferred from the growth substrate onto a new substrate. The as-grown CVD materials (as-WS2) exhibit distinctly different optical properties than transferred WS2 (x-WS2). In the case of CVD growth on Si/SiO2, following transfer to fresh Si/SiO2 there is a ~50 meV shift of the ground state exciton to higher emission energy in both photoluminescence emission and optical reflection. This shift is indicative of a reduction in tensile strain by ~0.25%. Additionally, the excitonic state in x-WS2 is easily modulated between neutral and charged exciton by exposure to moderate laser power, while such optical control is absent in as-WS2 for all growth substrates investigated. Finally, we observe dramatically different laser power-dependent behavior for as-grown and transferred WS2. These results demonstrate a strong sensitivity to sample preparation that is important for both a fundamental understanding of these novel materials as well as reliable reproduction of device properties.

cond-mat.mtrl-sci↗