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411 records · Page 23
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Electronic excitations of α - Fe 2 O 3 heteroepitaxial films measured by resonant inelastic x-ray scattering at the Fe L edge

Resonant inelastic x-ray scattering (RIXS) spectra of hematite (α-Fe 2 O 3 ) were measured at the Fe L 3 edge for heteroepitaxial thin films which were undoped and doped with 1% Ti, Sn, or Zn, in the energy-loss range in excess of 1 eV to study electronic transitions. The spectra were measured for several momentum transfers q, conducted at both low temperature (T=14 K) and room temperature. While we cannot rule out dispersive features possibly owing to propagating excitations, the coarse envelopes of the general spectra did not appreciably change shape with q, implying that the bulk of the observed L-edge RIXS intensity originates from (mostly) nondispersive ligand field excitations. Summing the RIXS spectra over q and comparing the results at T=14 K to those at T=300 K revealed pronounced temperature effects, including an intensity change and energy shift of the ≈1.4 eV peak, a broadband intensity increase of the 3-4 eV range, and higher energy features. The q-summed spectra and their temperature dependencies are virtually identical for nearly all of the samples with different dopants, save for the temperature dependence of the Ti-doped sample's spectrum, which we attribute to being affected by a large number of free charge carriers. Comparing with magnetization measurements for different temperatures and dopings likewise did not show a clear correlation between the RIXS spectra and the magnetic ordering states. To clarify the excited states, we performed spin multiplet calculations which were in excellent agreement with the RIXS spectra over a wide energy range and provide detailed electronic descriptions of the excited states. Furthermore, the implications of these findings to the photoconversion efficiency of hematite photoanodes is discussed.

36 MATERIALS SCIENCE↗
NASA NTRS2006

White-Light Whispering-Gallery-Mode Optical Resonators

Whispering-gallery-mode (WGM) optical resonators can be designed to exhibit continuous spectra over wide wavelength bands (in effect, white-light spectra), with ultrahigh values of the resonance quality factor (Q) that are nearly independent of frequency. White-light WGM resonators have potential as superior alternatives to (1) larger, conventional optical resonators in ring-down spectroscopy, and (2) optical-resonator/electro-optical-modulator structures used in coupling of microwave and optical signals in atomic clocks. In these and other potential applications, the use of white-light WGM resonators makes it possible to relax the requirement of high-frequency stability of lasers, thereby enabling the use of cheaper lasers. In designing a white-light WGM resonator, one exploits the fact that the density of the mode spectrum increases predictably with the thickness of the resonator disk. By making the resonator disk sufficiently thick, one can make the frequency differences between adjacent modes significantly less than the spectral width of a single mode, so that the spectral peaks of adjacent modes overlap, making the resonator spectrum essentially continuous. Moreover, inasmuch as the Q values of the various modes are determined primarily by surface Rayleigh scattering that does not depend on mode numbers, all the modes have nearly equal Q. By use of a proper coupling technique, one can ensure excitation of a majority of the modes. For an experimental demonstration of a white-light WGM resonator, a resonator disk 0.5-mm thick and 5 mm in diameter was made from CaF2. The shape of the resonator and the fiberoptic coupling arrangement were as shown in Figure 1. The resonator was excited with laser light having a wavelength of 1,320 nm and a spectral width of 4 kHz. The coupling efficiency exceeded 80 percent at any frequency to which the laser could be set in its tuning range, which was >100-GHz wide. The resonator response was characterized by means of ring-down tests in which the excitation was interrupted by a shutter having a rise and a fall time of 5 ns. The ring-down time of photodiodes and associated circuitry used to measure the interrupted excitation and the resonator output was <1 ns. Figure 2 shows the shapes of representative input and output light pulses. The average ring-down time was found to be 120 ns, corresponding to Q=2x10(exp 8). The variations of Q with the laser carrier frequency were found to be <5 percent. Hence, the resonator was shown to have the desired white light properties.

Matsko, Andrey↗
DOE OSTI2020

Ultrafast dynamics in the high-symmetry and in the charge density wave phase of 2 H –NbSe 2

Here we investigate carrier and collective mode dynamics in 2H-NbSe 2 using time-resolved optical pump-probe spectroscopy and compare the results with first-principles calculations. Broadband ultrafast reflectivity studies of 2H-NbSe 2 in a wide temperature interval covering the normal, charge density wave (CDW) and superconducting phase were performed. Spectral features observed in the transient reflectivity experiment were associated with specific optical transitions obtained from band structure calculations. Displacive excitation of coherent phonons showed CDW-associated coherent oscillations of the soft phonon mode across the whole spectral range. Temperature evolution of this coherent phonon mode in the low-excitation linear regime shows softening of the mode down to the CDW transition temperature T CDW with subsequent hardening below T CDW . The global fit of the broadband probe data reveals four different relaxation times associated with characteristic electron-electron, electron-phonon, and phonon-phonon relaxation processes. From first-principles calculations of electron-phonon coupling we associate the few picosecond electron-phonon relaxation time $\tau_2$ with a specific group of phonons with frequencies around 20 meV. On the other hand, the anomalously long relaxation time of $\tau_3 \sim$ to 100 ps is associated with anharmonicity-driven phonon-phonon scattering. All relaxation processes result from anomalies near the second order CDW phase transition that are reflected in the temperature dependencies of the characteristic relaxation times and amplitudes of coherent oscillations. At the highest fluences we observe electronic melting of the CDW and disappearance of the mode hardening below T CDW .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Tuning Organic Semiconductor Packing and Morphology through Non-equilibrium Solution Processing (Final Report)

Organic semiconductors (OSCs) are a promising candidate to produce low-cost, large area, and flexible electronics. There has previously been successful development of organic field effect transistors (OFETs), photovoltaics (OPV), and bioelectronics using OSCs. Solution processing of these materials allows for the fabrication of large-area devices in the kinetic crystallization regime. The charge transport capabilities have been shown to depend on the morphology and molecular packing of the OSC within thin films. Our hypothesis is that solution processing conditions may significantly impact OSC morphology and as a result the charge transport. Therefore, this work has focused on obtaining a fundamental understanding of the morphology and molecular packing of OSCs for optimal device performance. Through our work, we have gained a better understanding of how these structural conditions were influenced by the solution processing conditions. Our studies have led to a more systematic understanding of the various parameters that impact OSC morphology. Solution processing leads to non-equilibrium films, thus allowing for the formation of diverse morphologies that are inaccessible by other fabrication methods. Previously, our group has focused on tuning the morphology of small-molecular OSCs [53, 55-57]. However, little work had been devoted to polymer OSCs. There was a lack of detailed studies characterizing the solution-state of polymer OSCs in terms of their conformation, degree of entanglement, polymer aggregation, and chain relaxation dynamics. The solution state properties are also likely to be influenced by the rigidity and molecular weight of the polymer OSCs investigated. Thus, we have focused our attention on gaining a better insight of polymer OSC films and solution processing methods. Through this proposal, our approach is to investigate the correlation between solution-state properties and the morphology of the resulting polymer OSC films. We worked three specific aims: investigate the effects of 1) polymer OSC solution-state properties on final film morphology; 2) molecular additives on the solution-state and final film properties; 3) controlled pre-aggregation in the solution-state in the final film morphology. More rigid and planar polymer backbones should promote interchain charge transport and more efficient interchain hopping between polymer chains. Through tailoring the polymer backbone, polymer sidechains, and molecular weight, we expected the altered solution-state properties to affect the final film morphology. In addition, reducing the entanglements and promoting chain alignment will likely prevent charge carrier trapping through conformation disorders. We thus studied different mechanisms, such as molecular additives, to reduce entanglements in solution. Devices fabricated from these solutions were expected to have improved charge transport abilities. In addition to tailoring the solution-state characteristics of the polymer OSCs, we investigated the effect of solution processing methods on the molecular packing and morphology of polymer OSC films. Two main solution processing techniques, e.g., spin-coating and solution shearing, were employed to fabricate OFETs. Spin coating was employed to prepare OSC films, which produce isotropic films. This technique creates several parameters to tune such as spin coating speed, acceleration, and time. Additionally, our research group developed the solution shearing method, which consists of the solution initially sandwiched between two plates. By sliding the top plate, the solution front is exposed and drying begins. This technique allows for the creation of aligned large crystalline domains. Solution shearing consists of different processing parameters which can affect the final morphology, such as shearing speed, substrate temperature and temperature gradient, distance between both plates, and the tilt angle of the top plate. Due to the complexity of the polymer systems investigated, numerous techniques were employed to characterize the polymer OSC solution state and films. All the materials were characterized using the DOE supported synchrotron X-ray scattering facilities at the Stanford Synchrotron Radiation Lightsource (SSRL). Using grazing incidence X-ray scattering (GIXS) and Near Edge X-ray Absorption Fine Structure (NEXAFS) techniques, the crystalline structure and molecular orientations of the thin films were measured. Optical absorption (UV-Vis) spectroscopy was employed to determine the aggregation state in solution and films of the polymer systems. Polarized UV-Vis also allowed for the determination of the relative degree of polymer chain alignment for solution sheared films. Additionally, various other techniques were used to investigate other properties within the film, such as atomic force microscopy (AFM) and solution rheology. Finally, the device performance is quantified through the fabrication and characterization of OFETs, which will highlight the effects of morphology on charge transport.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Thermal conductivity of rutile germanium dioxide

Power electronics seek to improve power conversion of devices by utilizing materials with a wide bandgap, high carrier mobility, and high thermal conductivity. Due to its wide bandgap of 4.5 eV, b-Ga 2 O 3 has received much attention for high-voltage electronic device research. However, it suffers from inefficient thermal conduction that originates from its low-symmetry crystal structure. Rutile germanium oxide (r-GeO 2 ) has been identified as an alternative ultra-wide-bandgap (4.68 eV) semiconductor with predicted high electron mobility and ambipolar dopability; however, its thermal conductivity is unknown. Here, we characterize the thermal conductivity of r-GeO 2 as a function of temperature by first-principles calculations, experimental synthesis, and thermal characterization. The calculations predict an anisotropic phonon-limited thermal conductivity for r-GeO 2 of 37W m –1 K –1 along the a direction and 58W m –1 K –1 along the c direction at 300K where the phonon-limited thermal conductivity predominantly occurs via the acoustic modes. Experimentally, we measured the value of 51W m –1 K –1 at 300K for hot-pressed, polycrystalline r-GeO2 pellets. The measured value is close to our directionally averaged theoretical value, and the temperature dependence of ~1/T is also consistent with our theory prediction, indicating that thermal transport in our r-GeO 2 samples at room temperature and above is governed by phonon scattering. Furthermore, our results reveal that high-symmetry UWBG materials, such as r-GeO 2 , may be the key to efficient power electronics.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Photonic circuits for laser stabilization with integrated ultra-high Q and Brillouin laser resonators

The integration of stabilized lasers, sources that generate spectrally pure light, will provide compact, low-cost solutions for applications including quantum information sciences, precision navigation and timing, metrology, and high-capacity fiber communications. We report a significant advancement in this field, demonstrating stabilization of an integrated waveguide Brillouin laser to an integrated waveguide reference cavity, where both resonators are fabricated using the same CMOS-compatible integration platform. We demonstrate reduction of the free running Brillouin laser linewidth to a 292 Hz integral linewidth and carrier stabilization to a 4.9 × 10 –13 fractional frequency at 8 ms reaching the cavity-intrinsic thermorefractive noise limit for frequencies down to 80 Hz. We achieve this level of performance using a pair of 56.4 x 10 6 quality factor Si 3 N 4 waveguide ring-resonators that reduce the high-frequency noise by the nonlinear Brillouin process and the low-frequency noise by Pound–Drever–Hall locking to the ultra-low loss resonator. These results represent an important step toward integrated stabilized lasers with reduced sensitivity to environmental disturbances for atomic, molecular, and optical physics (AMO), quantum information processing and sensing, and other precision scientific, sensing, and communications applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRSDate not supplied

An Overview of SHERLOC Raman and Fluorescence Spectroscopy Results Obtained During Perseverance’s Green Zone Campaign at Jezero Crater, Mars

The Perseverance rover landed in Jezero crater, Mars, in February 2021. The field site was chosen because orbiter data provided evidence that the crater hosted an ancient (>2.7 Ga) fluvio-lacustrine environment. The Octavia E. Butler landing site is located ~1.9 km east of the erosional remnant of the Jezero river delta. Scanning Habitable Environments with Raman and Luminescence for Organics and Chemicals (SHERLOC) is an arm-mounted instrument that combines fluorescence and Raman spectroscopy with microscopic imaging to analyze geological materials in order to better understand the history of the environments recorded in the rocks within Jezero crater and to search for potential biosignatures. SHERLOC has two microscopic cameras, the Autofocus and Context Imager (ACI) and the Wide-Angle Topographic Sensor for Operations and eNgineering, (WATSON). These subsystems obtain high spatial resolution (10.1–100 µm/pixel) images to identify grain-scale structure and texture. SHERLOC spectroscopy enables high-sensitivity detection, characterization, and spatially-resolved correlation of trace organic materials. SHERLOC’s 248.6 nm deep UV laser generates a 100 µm-diameter spot. Photons generated by Raman scattering and fluorescence emission are collected and the spectra are downlinked to Earth for analysis. Knowledge of where the laser is pointed allows for mineral and compositional maps to be generated and overlain in ACI and WATSON images. Early spectroscopy observations focused on natural rock surfaces at targets named Nataani (sol 83), Bi_la_sana (sol 98) and Foux (sol 141). These surfaces included patches of aeolian dust that had settled upon the rocks. Perseverance’s abrasion tool is expected to become available in August 2021; it will grind to depths of 14 mm to remove dust and penetrate coatings and weathering rinds. This presentation will summarize major results from analysis of the rocks examined by SHERLOC during Perseverance’s first science and sample coring campaign (Green Zone Campaign).

Luther W Beegle↗
DOE OSTI2021

Effect of interfacial structures on phonon transport across atomically precise Si/Al heterojunctions

Phonons are important carriers of energy and information in many cryogenic devices used for quantum information science and in fundamental physics experiments such as dark matter detectors. In these systems phonon behavior can be dominated by interfaces, hence there is increasing demand for a more detailed understanding of interfacial phonon transport in relevant material systems. Previous studies have focused on understanding thermal transport over the entire phonon spectrum at and above room temperature. At ultra-low temperatures, however, knowledge is missing regarding athermal phonon behavior due to the challenge in modeling the extreme conditions in micro-scale, heterogeneous cryogenic systems, as well as extracting single-phonon information from a large ensemble. In this work, we delineate interfacial phonon transport using a combination of classical molecular dynamics (MD) and phonon wave packet simulations, to illustrate the consistency and differences between the ensemble- and single-phonon dynamics. We consider three single-crystal Si surface reconstructions --- (1×1), (v3×v3) and (7×7) --- and model both experimentally observed Si(1×1)/Al interfaces and hypothesized Si(v3×v3)/Al and Si(7×7)/Al interfaces. The overall interfacial thermal conductance calculated from non-equilibrium MD shows that for the Si(1×1)/Al system, the presence of Al twin grain boundaries can hinder phonon transport and reduce thermal conductance by 2--12% relative to single-crystal Al; whereas the Si (v3×v3) and (7×7) reconstructions can enhance it by 6--19%. Normal mode decomposition reveals that both the increase and decrease in conductance are related to inelastic phonon scattering. Single-phonon wave packet simulations show results consistent with NEMD, while further suggesting that phonon polarization conversion is significant even when elastic transmission dominates, and that the interfacial structures have anisotropic impacts on atomic vibrations along different lattice directions. Our findings suggest alternative perspectives in achieving selective phonon transport through controlling interfacial structures of materials with atomically-precise fabrication techniques, and that the phonon wave packet formalism is a potentially powerful method for developing a detailed understanding of non-equilibrium phenomena in the low-temperature limit.

Lu, Zexi↗
DOE OSTI2025

Evolution of charge correlations in the hole-doped kagome superconductor CsV 3−𝑥⁢ Ti 𝑥 ⁢Sb 5

The interplay between superconductivity and charge correlations in the kagome metal CsV 3⁢ Sb 5 can be tuned by external perturbations such as doping or pressure. Here we present a study of charge correlations and superconductivity upon hole doping via Ti substitution on the V kagome sites in CsV 3−𝑥 ⁢Ti 𝑥 ⁢Sb 5 via synchrotron x-ray diffraction and scanning superconducting quantum interference device measurements. While the superconducting phase, as viewed via the vortex structure, remains conventional and unchanged across the phase diagram, the nature of charge correlations evolves as a function of hole doping from the first superconducting dome into the second superconducting dome. For Ti doping in the first superconducting dome, competing 2×2×2 and 2×2×4 supercells form within the charge density wave state and are suppressed rapidly with carrier substitution. In the second superconducting dome, no charge correlations are detected. Here, comparing these results to those observed for CsV 3 ⁢Sb 5−𝑥 ⁢Sn 𝑥 suggests important differences between hole doping via chemical substitution on the V and Sb sites, particularly in the disorder potential associated with each dopant.

Charge density waves↗
DOE OSTI2023

Exciton Lifetime and Optical Line Width Profile via Exciton–Phonon Interactions: Theory and First-Principles Calculations for Monolayer MoS 2

Exciton dynamics dictates the evolution of photoexcited carriers in photovoltaic and optoelectronic devices. However, interpreting their experimental signatures is a challenging theoretical problem due to the presence of both electron–phonon and many-electron interactions. Here, we develop and apply here a first-principles approach to exciton dynamics resulting from exciton–phonon coupling in monolayer MoS 2 and reveal the highly selective nature of exciton–phonon coupling due to the internal spin structure of excitons, which leads to a surprisingly long lifetime of the lowest-energy bright A exciton. Moreover, we show that optical absorption processes rigorously require a second-order perturbation theory approach, with photon and phonon treated on an equal footing, as proposed by Toyozawa and Hopfield. Such a treatment, thus far neglected in first-principles studies, gives rise to off-diagonal exciton–phonon self-energy, which is critical for the description of dephasing mechanisms and yields exciton line widths in excellent agreement with experiment.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2020

Direct Observation of Bandgap Oscillations Induced by Optical Phonons in Hybrid Lead Iodi.de Perovskites

Hybrid organic-inorganic perovskites such as methylammonium lead iodide have emerged as promising semiconductors for energy-relevant applications. The interactions between charge carriers and lattice vibrations, giving rise to polarons, have been invoked to explain some of their extraordinary optoelectronic properties. Here, time-resolved optical spectroscopy is performed, with off-resonant pumping and electronic probing, to examine several representative lead iodide perovskites. The temporal oscillations of electronic bandgaps induced by coherent lattice vibrations are reported, which is attributed to antiphase octahedral rotations that dominate in the examined 3D and 2D hybrid perovskites. The off-resonant pumping scheme permits a simplified observation of changes in the bandgap owing to the A(g) vibrational mode, which is qualitatively different from vibrational modes of other symmetries and without increased complexity of photogenerated electronic charges. The work demonstrates a strong correlation between the lead-iodide octahedral framework and electronic transitions, and provides further insights into the manipulation of coherent optical phonons and related properties in hybrid perovskites on ultrafast timescales.

coherent optical phonons↗
NASA NTRS1999

Waves in Radial Gravity Using Magnetic Fluid

Terrestrial laboratory experiments studying various fluid dynamical processes are constrained, by being in an Earth laboratory, to have a gravitational body force which is uniform and unidirectional. Therefore fluid free-surfaces are horizontal and flat. Such free surfaces must have a vertical solid boundary to keep the fluid from spreading horizontally along a gravitational potential surface. In atmospheric, oceanic, or stellar fluid flows that have a horizontal scale of about one-tenth the body radius or larger, sphericity is important in the dynamics. Further, fluids in spherical geometry can cover an entire domain without any sidewall effects, i.e. have truly periodic boundary conditions. We describe spherical body-force laboratory experiments using ferrofluid. Ferrofluids are dilute suspensions of magnetic dipoles, for example magnetite particles of order 10 nm diameter, suspended in a carrier fluid. Ferrofluids are subject to an additional body force in the presence of an applied magnetic field gradient. We use this body force to conduct laboratory experiments in spherical geometry. The present study is a laboratory technique improvement. The apparatus is cylindrically axisymmetric. A cylindrical ceramic magnet is embedded in a smooth, solid, spherical PVC ball. The geopotential field and its gradient, the body force, were made nearly spherical by careful choice of magnet height-to-diameter ratio and magnet size relative to the PVC ball size. Terrestrial gravity is eliminated from the dynamics by immersing the "planet" and its ferrofluid "ocean" in an immiscible silicone oil/freon mixture of the same density. Thus the earth gravity is removed from the dynamics of the ferrofluid/oil interface and the only dynamically active force there is the radial magnetic gravity. The entire apparatus can rotate, and waves are forced on the ferrofluid surface by exterior magnets. The biggest improvement in technique is in the wave visualization. Fluorescing dye is added to the oil/freon mixture and an argon ion laser generates a horizontal light that can be scanned vertically. Viewed from above, the experiment is a black circle with wave deformations surrounded by a light background. A contour of the image intensity at any light sheet position gives the surface of the ferrofluid "ocean" at that "latitude". Radial displacements of the waves as a function of longitude are obtained by subtracting the contour line positions from a no-motion contour at that laser sheet latitude. The experiments are run by traversing the forcing magnet with the laser sheet height fixed and images are frame grabbed to obtain a time-series at one latitude. The experiment is then re-run with another laser-sheet height to generate a full picture of the three-dimensional wave structure in the upper hemisphere of the ball as a function of time. We concentrate here on results of laboratory studies of waves that are important in Earth's atmosphere and especially the ocean. To get oceanic scaling in the laboratory, the experiment must rotate rapidly (4-second rotation period) so that the wave speed is slow compared to the planetary rotation speed as in the ocean. In the Pacific Ocean, eastward propagating Kelvin waves eventually run into the South American coast. Theory predicts that some of the wave energy should scatter into coastal-trapped Kelvin waves that propagate north and south along the coast. Some of this coastal wave energy might then scatter into mid-latitude Rossby waves that propagate back westward. Satellite observations of the Pacific Ocean sea-surface temperature and height seem to show signatures of westward propagating mid-latitude Rossby waves, 5 to 10 years after the 1982-83 El Nino. The observational data is difficult to interpret unambiguously owing to the large range of motions that fill the ocean at shorter timescales. This series of reflections giving eastward, north- ward, and then westward traveling waves is observed cleanly in the laboratory experiments, confirming the theoretical expectations.

Ohlsen, D. R.↗
DOE OSTI2021

Perseverance’s Scanning Habitable Environments with Raman and Luminescence for Organics and Chemicals (SHERLOC) Investigation

The Scanning Habitable Environments with Raman and Luminescence for Organics and Chemicals (SHERLOC) is a robotic arm-mounted instrument on NASA’s Perseverance rover. SHERLOC has two primary boresights. The Spectroscopy boresight generates spatially resolved chemical maps using fluorescence and Raman spectroscopy coupled to microscopic images (10.1 μm/pixel). The second boresight is a Wide Angle Topographic Sensor for Operations and eNgineering (WATSON); a copy of the Mars Science Laboratory (MSL) Mars Hand Lens Imager (MAHLI) that obtains color images from microscopic scales (~13 μm/pixel) to infinity. SHERLOC Spectroscopy focuses a 40 μs pulsed deep UV neon-copper laser (248.6 nm), to a ~100 μm spot on a target at a working distance of ~48 mm. Fluorescence emissions from organics, and Raman scattered photons from organics and minerals, are spectrally resolved with a single diffractive grating spectrograph with a spectral range of 250 to ~370 nm. Because the fluorescence and Raman regions are naturally separated with deep UV excitation (<250 nm), the Raman region ~ 800 – 4000 cm -1 (250 to 273 nm) and the fluorescence region (274 to ~370 nm) are acquired simultaneously without time gating or additional mechanisms. SHERLOC science begins by using an Autofocus Context Imager (ACI) to obtain target focus and acquire 10.1 μm/pixel greyscale images. Chemical maps of organic and mineral signatures are acquired by the orchestration of an internal scanning mirror that moves the focused laser spot across discrete points on the target surface where spectra are captured on the spectrometer detector. ACI images and chemical maps (< 100 μm/mapping pixel) will enable the first Mars in situ view of the spatial distribution and interaction between organics, minerals, and chemicals important to the assessment of potential biogenicity (containing CHNOPS). Single robotic arm placement chemical maps can cover areas up to 7x7 mm in area and, with the < 10 min acquisition time per map, larger mosaics are possible with arm movements. This microscopic view of the organic geochemistry of a target at the Perseverance field site, when combined with the other instruments, such as Mastcam-Z, PIXL, and SuperCam, will enable unprecedented analysis of geological materials for both scientific research and determination of which samples to collect and cache for Mars sample return.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
NASA NTRS2021

Perseverance’s Scanning Habitable Environments with Raman and Luminescence for Organics and Chemicals (SHERLOC) Investigation

The Scanning Habitable Environments with Raman and Luminescence for Organics and Chemicals (SHERLOC) is a robotic arm-mounted instrument on NASA’s Perseverance rover. SHERLOC has two primary boresights. The Spectroscopy boresight generates spatially resolved chemical maps using fluorescence and Raman spectroscopy coupled to microscopic images (10.1 μm/pixel). The second boresight is a Wide Angle Topographic Sensor for Operations and eNgineering (WATSON); a copy of the Mars Science Laboratory (MSL) Mars Hand Lens Imager (MAHLI) that obtains color images from microscopic scales (∼13 μm/pixel) to infinity. SHERLOC Spectroscopy focuses a 40 μs pulsed deep UV neon-copper laser (248.6 nm), to a ∼100 μm spot on a target at a working distance of ∼48 mm. Fluorescence emissions from organics, and Raman scattered photons from organics and minerals, are spectrally resolved with a single diffractive grating spectrograph with a spectral range of 250 to ∼370 nm. Because the fluorescence and Raman regions are naturally separated with deep UV excitation (<250 nm), the Raman region ∼ 800 – 4000 cm−1 (250 to 273 nm) and the fluorescence region (274 to ∼370 nm) are acquired simultaneously without time gating or additional mechanisms. SHERLOC science begins by using an Autofocus Context Imager (ACI) to obtain target focus and acquire 10.1 μm/pixel greyscale images. Chemical maps of organic and mineral signatures are acquired by the orchestration of an internal scanning mirror that moves the focused laser spot across discrete points on the target surface where spectra are captured on the spectrometer detector. ACI images and chemical maps (< 100 μm/mapping pixel) will enable the first Mars in situ view of the spatial distribution and interaction between organics, minerals, and chemicals important to the assessment of potential biogenicity (containing CHNOPS). Single robotic arm placement chemical maps can cover areas up to 7x7 mm in area and, with the < 10 min acquisition time per map, larger mosaics are possible with arm movements. This microscopic view of the organic geochemistry of a target at the Perseverance field site, when combined with the other instruments, such as Mastcam-Z, PIXL, and SuperCam, will enable unprecedented analysis of geological materials for both scientific research and determination of which samples to collect and cache for Mars sample return.

Rohit Bhartia↗
DOE OSTI2026

Task Sharing of Proton Incorporation in Vertically Aligned Nanocomposite Triple Conductors: Growth, Structure, and Surface Exchange Kinetics

As protonic ceramic electrolysis cells emerge for efficient H 2 production, there is a need to develop air electrode materials enabling fast, durable steam splitting and proton incorporation. Single-phase triple conductors may fail to satisfy the myriad performance/stability requirements, and their critical charge-carriers (holes, oxygen vacancies, and protons) are in competition, limiting their concentrations. Instead, we propose task-sharing, vertically aligned nanocomposites (VANs), comprising a proton conductor (BaZr 0.9 Y 0.1 O 3-δ ) and a redox-active mixed ionic electronic conductor (Ce 0.9 Pr 0.1 O 2-δ ), that may enable rapid proton surface exchange at the solid–gas interface and transport along the solid–solid heterointerfaces. We grew VANs by pulsed laser deposition and investigated the interplay between their processing conditions, structure, and proton and oxygen surface exchange kinetics. We varied the substrate temperature, laser repetition rate, laser fluence, and processing oxygen pressure. The crystallinity and phases were characterized by grazing-incidence X-ray diffraction, and the strain and structural order as a function of depth were evaluated by angle-dependent synchrotron X-ray pair distribution function analysis. To evaluate the potential for interdiffusion, the formation energies of substitutional defects were simulated with density functional theory. Corresponding structural analysis and elemental mapping were performed by scanning/transmission electron microscopy, energy-dispersive X-ray spectroscopy, and electron energy-loss spectroscopy, indicating distinct nanoscale compositional regions with a hierarchical structure embedded in individual VANs columns and minimal interdiffusion across a bilayer film. Proton and oxygen surface exchange coefficients (k H , k O ) and polarization resistances were evaluated by electrical and optical relaxations and impedance spectroscopy of VAN-incorporated protonic ceramic electrochemical cells, respectively, at 400–500 °C, demonstrating values comparable to some of the best-known triple and mixed conductors.

36 MATERIALS SCIENCE↗