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NASA NTRS2005

Development of mid-IR lasers for Laser Remote Sensing

There is an existing need in JPL and in NASA for development of mid-IR lasers, such as Quantum Cascade (QC) lasers, for in-situ and remote laser spectrometers. Mid-IR, compact, low power consumption laser spectrometers have a great potential for detection and measurements of planetary gases and biological important biomarker molecules such as H20, H202, CH4, and many additional chemical species on Mars and other Solar system planets. Another potential application of QC lasers for future NASA mission is in high power remote Laser Reflectance Spectrometers (LRS). In LSR instrument, mid-infrared lasers will act as the illumination source for conducting active mid-IR reflectance spectroscopy of solid-surfaced objects in the outer Solar System. These spectrometers have the potential to provide an incredible amount of information about the compositions of surfaces in the outer Solar System. In this work, we will discuss our current effort at JPL to advance QC lasers to a level that the laser performance, operational requirements and reliability be compatible with the instruments demands for space exploration applications.

Mid - IR lasers↗

NASA NTRS2005

Mapping Weathering and Alteration Minerals in the Comstock and Geiger Grade Areas using Visible to Thermal Infrared Airborne Remote Sensing Data

To support research into both precious metal exploration and environmental site characterization a combination of high spatial/spectral resolution airborne visible, near infrared, short wave infrared (VNIR/SWIR) and thermal infrared (TIR) image data were acquired to remotely map hydrothermal alteration minerals around the Geiger Grade and Comstock alteration regions, and map the mineral by-products of weathered mine dumps in Virginia City. Remote sensing data from the Airborne Visible Infrared Imaging Spectrometer (AVIRIS), SpecTIR Corporation's airborne hyperspectral imager (HyperSpecTIR), the MODIS-ASTER airborne simulator (MASTER), and the Spatially Enhanced Broadband Array Spectrograph System (SEBASS) were acquired and processed into mineral maps based on the unique spectral signatures of image pixels. VNIR/SWIR and TIR field spectrometer data were collected for both calibration and validation of the remote data sets, and field sampling, laboratory spectral analyses and XRD analyses were made to corroborate the surface mineralogy identified by spectroscopy. The resulting mineral maps show the spatial distribution of several important alteration minerals around each study area including alunite, quartz, pyrophyllite, kaolinite, montmorillonite/muscovite, and chlorite. In the Comstock region the mineral maps show acid-sulfate alteration, widespread propylitic alteration and extensive faulting that offsets the acid-sulfate areas, in contrast to the larger, dominantly acid-sulfate alteration exposed along Geiger Grade. Also, different mineral zones within the intense acid-sulfate areas were mapped. In the Virginia City historic mining district the important weathering minerals mapped include hematite, goethite, jarosite and hydrous sulfate minerals (hexahydrite, alunogen and gypsum) located on mine dumps. Sulfate minerals indicate acidic water forming in the mine dump environment. While there is not an immediate threat to the community, there are clearly sources of acidic drainage that were identified remotely.

imaging spectroscopy↗

NASA NTRS2007

Identification of Iron-Bearing Phases on the Martian Surface and in Martian Meteorites and Analogue Samples by Moessbauer Spectroscopy

The Moessbauer spectrometers on the Mars Exploration Rovers (MER) Spirit (Gusev Crater) and Opportunity (Meridiani Planum) have each analyzed more than 100 targets during their ongoing missions (>1050 sols). Here we summarize the Fe-bearing phases identified to date and compare the results to Moessbauer analyses of martian meteorites and lunar samples. We use lunar samples as martian analogues because some, particularly the low-Ti Apollo 15 mare basalts, have bulk chemical compositions that are comparable to basaltic martian meteorites [1,2]. The lunar samples also provide a way to study pigeonite-rich samples. Pigeonite is a pyroxene that is not common in terrestrial basalts, but does often occur on the Moon and is present in basaltic martian meteorites

Klingelhoefer, G.↗

NASA NTRS2012

NASA Tech Briefs, March 2012

The topics include: 1) Spectral Profiler Probe for In Situ Snow Grain Size and Composition Stratigraphy; 2) Portable Fourier Transform Spectroscopy for Analysis of Surface Contamination and Quality Control; 3) In Situ Geochemical Analysis and Age Dating of Rocks Using Laser Ablation-Miniature Mass Spectrometer; 4) Physics Mining of Multi-Source Data Sets; 5) Photogrammetry Tool for Forensic Analysis; 6) Connect Global Positioning System RF Module; 7) Simple Cell Balance Circuit; 8) Miniature EVA Software Defined Radio; 9) Remotely Accessible Testbed for Software Defined Radio Development; 10) System-of-Systems Technology-Portfolio-Analysis Tool; 11) VESGEN Software for Mapping and Quantification of Vascular Regulators; 12) Constructing a Database From Multiple 2D Images for Camera Pose Estimation and Robot Localization; 13) Adaption of G-TAG Software for Validating Touch and Go Asteroid Sample Return Design Methodology; 14) 3D Visualization for Phoenix Mars Lander Science Operations; 15) RxGen General Optical Model Prescription Generator; 16) Carbon Nanotube Bonding Strength Enhancement Using Metal Wicking Process; 17) Multi-Layer Far-Infrared Component Technology; 18) Germanium Lift-Off Masks for Thin Metal Film Patterning; 19) Sealing Materials for Use in Vacuum at High Temperatures; 20) Radiation Shielding System Using a Composite of Carbon Nanotubes Loaded With Electropolymers; 21) Nano Sponges for Drug Delivery and Medicinal Applications; 22) Molecular Technique to Understand Deep Microbial Diversity; 23) Methods and Compositions Based on Culturing Microorganisms in Low Sedimental Fluid Shear Conditions; 24) Secure Peer-to-Peer Networks for Scientific Information Sharing; 25) Multiplexer/Demultiplexer Loading Tool (MDMLT); 26) High-Rate Data-Capture for an Airborne Lidar System; 27) Wavefront Sensing Analysis of Grazing Incidence Optical Systems; 28) Foam-on-Tile Damage Model; 29) Instrument Package Manipulation Through the Generation and Use of an Attenuated-Fluent Gas Fold; 30) Multicolor Detectors for Ultrasensitive Long-Wave Imaging Cameras; 31) Lunar Reconnaissance Orbiter (LRO) Command and Data Handling Flight Electronics Subsystem; and 32) Electro-Optic Segment-Segment Sensors for Radio and Optical Telescopes.

Source record↗

NASA NTRS2013

Experimental Evidence for Weathering and Martian Sulfate Formation Under Extremely Cold Weather-Limited Environments

Niles, Paul B.↗

NASA NTRS2013

Olivine Weathering aud Sulfate Formation Under Cryogenic Conditions

High resolution photography and spectroscopy of the martian surface (MOC, HiRISE) from orbit has revolutionized our view of Mars with one of the most important discoveries being wide‐spread layered sedimentary deposits associated with sulfate minerals across the low to mid latitude regions of Mars. The mechanism for sulfate formation on Mars has been frequently attributed to playa‐like evaporative environments under prolonged warm conditions. An alternate view of the ancient martian climate contends that prolonged warm temperatures were never present and that the atmosphere and climate has been similar to modern conditions throughout most of its history. This view has had a difficult time explaining the sedimentary history of Mars and in particular the presence of sulfate minerals which seemingly need more water. We suggest here that mixtures of atmospheric aerosols, ice, and dust have the potential for creating small films of cryo‐concentrated acidic solutions that may represent an important unexamined environment for understanding weathering processes on Mars. This study seeks to test whether sulfate formation may be possible at temperatures well below 0degC in water limited environments removing the need for prolonged warm periods to form sulfates on early Mars. To test this idea we performed laboratory experiments to simulate weathering of mafic minerals under Mars‐like conditions. The weathering rates measured in this study suggest that fine grained olivine on Mars would weather into sulfate minerals in short time periods if they are exposed to H2SO4 aerosols at temperatures at or above ‐40degC. In this system, the strength of the acidic solution is maximized through eutectic freezing in an environment where the silicate minerals are extremely fine grained and have high surface areas. This provides an ideal environment despite the very low temperatures. On Mars the presence of large deposits of mixed ice and dust is undisputed. The presence of substantial sulfur‐rich volcanism, and sulfur‐rich surface deposits also makes it very likely that sulfate aerosols have also been an important component of the martian atmosphere. Thus mixtures of ice, dust, and sulfate aerosols are likely to have been common on the martian surface. Given the fact that it is not difficult to achieve surface temperatures above ‐40degC on Mars throughout its history, it seems likely that sulfate formation on Mars is controlled by the availability of sulfate aerosols and not by the martian climate. The current polar regions of Mars and Earth provide interesting analogs. Large regions of sulfaterich material have been detected on and around the modern north polar region of Mars. The prevalence of ice‐dust mixtures in this region and the existence of sulfates within the ice cap itself are strong evidence for the origin of the sulfates from inside the ice deposits. In addition sulfates have been found in ice deposits in Greenland and Mount Fuji on Earth that have been attributed to forming within the ice deposit. These sulfates can form either through interaction with dust particles in the atmosphere or through weathering inside the ice itself.

Niles, Paul B.↗

NASA NTRS2014

Sedimentary Mounds on Mars: Tracing Present-day Formation Processes into the Past

High resolution photography and spectroscopy of the martian surface (MOC, HiRISE) from orbit has revolutionized our view of Mars with one and revealed spectacular views of finely layered sedimentary materials throughout the globe [1]. Some of these sedimentary deposits are 'mound' shaped and lie inside of craters (Fig 1). Crater mound deposits are found throughout the equatorial region, as well as ice-rich deposits found in craters in the north and south polar region [2-4]. Despite their wide geographical extent and varying volatile content, the 'mound' deposits have a large number of geomorphic and structural similarities that suggest they formed via equivalent processes. Thus, modern depositional processes of ice and dust can serve as an invaluable analog for interpreting the genesis of ancient sedimentary mound deposits.

Niles, P. B.↗

NASA NTRS1993

Below Band-Gap Laser Ablation of Diamond for Transmission Electron Microscopy

A 248-nm excimer laser was used to thin naturally occurring type 1a diamond substrates at normal and glancing (22 deg) incidence. Perforation of a 250 micron thick substrate was achieved in about 15 minutes at normal incidence. Whilst the substrate thinned at glancing incidence was found to have large electron-transparent areas, that thinned at normal incidence required additional argon milling to achieve electron transparency. X-ray photoelectron spectroscopy of the back surface of the diamond failed to detect any graphite or glassy carbon, confirming that damage due to laser ablation occurs only at the incident surface. Samples prepared using this technique imaged in the transmission electron microscope were observed to have retained the nitrogen platelets

Posthill, J. B.↗

NASA NTRS2019

Enhancing Global Change Experiments Through Integration of Remote‐Sensing Techniques

Global change experiments are often spatially and temporally limited because they are time‐ and labor‐intensive, and expensive to carry out. We describe how the incorporation of remote‐sensing techniques into global change experiments can complement traditional methods and provide additional information about system processes. We describe five emerging near‐surface remote‐sensing techniques: spectroscopy, thermal and fluorescence imaging, terrestrial laser scanning, digital repeat photography, and unmanned aerial systems. The addition of such techniques can reduce cost and effort, provide novel information, and expand existing observations by improving their context, accuracy, and completeness. In addition, we contend that use of airborne and satellite remote‐sensing data during site selection can improve the ecological representativeness of future experiments. We conclude by recommending a high level of communication and collaboration between remote‐sensing scientists and ecologists at all stages of global change experimentation.

Alexey N Shiklomanov↗

NASA NTRS2022

Sodium Distribution on the Moon

The Moon is significantly depleted in volatile elements when compared to Earth, an observation that has resulted in various formation scenarios leading to the loss of volatiles. Sodium is a moderately volatile element that is a lithophile, which can be utilized as a tracer of the volatile history in planetary bodies. It is also well observed in the exosphere of several bodies in our solar system and exoplanetary systems. But lunar surface sodium abundances have so far been measured only in samples brought back to Earth. We report on results from the first effort to provide a global-scale measurement of sodium on the lunar surface using X-ray fluorescent spectra from Chandrayaan-2. A global average of 1.33 ± 0.03 wt% derived here is higher than previously known. Trends in the sodium abundance indicate a long-lived adsorbate component that could explain the higher abundances reported here, which would act as a reservoir that sustains the lunar sodium exosphere.

Surface composition↗

NASA NTRS2024

Detectability Simulations of a Near-infrared Surface Biosignature on Proxima Centauri b with Future Space Observatories

Telescope missions are currently being designed that will make direct imaging of habitable exoplanets possible in the near future, and studies are needed to quantify the detectability of biosignature features in the planet's reflectance spectrum. We simulated the detectability of a near-infrared-absorbing surface biosignature feature with simulated observations of the nearby exoplanet Proxima Centauri b. We modeled a biosignature spectral feature with a reflectance spectrum based on an anoxygenic photosynthetic bacterial species that has strong absorption at 1 μm, which could make it well suited for life on an M-dwarf-hosted planet. We modeled the distribution of this organism across the planet's surface based on climate states from a 3D general circulation model (GCM) that were Archean- and Proterozoic-like exo-Earth analogs. We included the GCM states' prognostically simulated water clouds and added organic haze into the Archean-like atmospheres. We simulated observations of these Proxima Centauri b scenarios with the LUVOIR-A and B telescope concepts, with LUVOIR-B serving as a proxy to the planned Habitable Worlds Observatory. We calculated the integration times necessary to detect the biosignature and found that it would be detectable on Proxima Centauri b if the organism is moderately abundant (greater than a 1%–4% global surface area coverage), as long as the atmosphere is transmitting in the wavelength range under consideration. Small amounts of methane, clouds, and haze do not greatly impede detectability. We found preliminary evidence that such a biosignature would be detectable on exoplanets within 15 pc, but further investigations are needed to corroborate this.

Exoplanet astronomy↗

DOE OSTI2021

Efficient passivation of n-type and p-type silicon surface defects by hydrogen sulfide gas reaction

An efficient surface defect passivation is observed by reacting clean Si in a dilute hydrogen sulfide-argon gas mixture (< 5% H2S in Ar) for both n-type and p-type Si wafers with planar and textured surfaces. Surface recombination velocities of 1.5 and 8 cm/s are achieved on n-type and p-type Si wafers, respectively, at an optimum reaction temperature of 550oC that are comparable to the best surface passivation quality used in high efficiency Si solar cells. Surface chemical analysis using x-ray photoelectron spectroscopy shows that sulfur is primarily bonded in a sulfide environment, and synchrotron-based soft x-ray emission spectroscopy of the adsorbed sulfur atoms suggests the formation of S-Si bonds. Furthermore, the sulfur surface passivation layer is unstable in air, attributed to surface oxide formation and a simultaneous decrease of sulfide bonds. However, the passivation can be stabilized by a low-temperature (300oC) deposited amorphous silicon nitride (a-Si:NX:H) capping layer.

14 SOLAR ENERGY↗

DOE OSTI2021

Suppressing Auger Recombination in Multiply Excited Colloidal Silicon Nanocrystals with Ligand-Induced Hole Traps

Nonradiative Auger recombination in multiply excited nanocrystals is a dominant efficiency loss pathway for nanocrystal-containing optoelectronic devices that rely on high-rate emission and absorption operating conditions. Overcoming Auger recombination in these quantum-confined systems is therefore a longstanding challenge to the synthetic nanocrystal as well as device manufacturing communities. Several successful strategies have been realized to reduce Auger recombination, but they rely on complex and time-consuming nanocrystal core/shell synthesis. Alternatively, controlling Auger rates by varying the nanocrystal–ligand-binding chemistry is a promising route to obtain functional tunability, which reduces the barrier to large-scale manufacturing. The covalent surface chemistry and the extremely long-lived photoexcited lifetimes of silicon nanocrystals (Si NCs) make them a unique system among colloidal semiconductor NCs to study the intersection between surface chemistry and photoexcited carrier dynamics. Here, we show that changing the functional group that binds a saturated dodecyl ligand to the surface of nonthermal plasma-synthesized Si NCs from alkyl to thiolate slows Auger recombination rates within multiply excited Si NCs. This reduction in Auger rate persists across Si NC sizes ranging from 3.5 to 8 nm in diameter, but the expected linear dependence of Auger rates on the NC volume is retained for both alkyl and alkylthiolate surface terminations. To understand the origin behind this elongation, we carry out steady-state and time-resolved photoluminescence measurements as well as time-resolved terahertz spectroscopy measurements. These measurements reveal that thiolate groups introduce mid-gap surface states, which, we argue, reduces the photoexcited electron–hole overlap and elongates Auger recombination times. These results highlight how a typically detrimental chemical species—mid-band gap NC surface states—can be beneficial under high-rate absorption/emission conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Investigation of N2 adsorption on Fe3O4(001) using ambient pressure X-ray photoelectron spectroscopy and density functional theory

Reactions on iron oxide surfaces are prevalent in various chemical processes from heterogeneous catalysts to minerals. Nitrogen (N2) is known to dissociate on iron surfaces, a precursor for ammonia production in the Haber–Bosch process, where the dissociation of N2 is the limiting step in the reaction under equilibrium conditions. However, little is known about N2 adsorption on other iron-based materials, such as iron oxide surfaces that are ubiquitous in soils, steel pipelines, and other industrial materials. An atomistic description is reported for the binding of N2 on the Fe3O4(001) surface using first principles calculations with ambient pressure X-ray photoelectron spectroscopy. Two primary adsorption sites are experimentally identified from N2 dissociation on Fe3O4(001). The electronic signatures associated with the valence band region unambiguously show how the electronic structure of magnetite transforms near ambient pressures due to the binding of atomic nitrogen to different surface sites. Overall, the experimental and theoretical results of our study bridge the gap between ultra-high vacuum studies and reaction conditions to provide insight into other nitrogen-based chemistry on iron oxide surfaces that impact the agriculture and energy industries.

Degaga, Gemechis D. (ORCID:0000000205097118)↗

DOE OSTI2024

Facet-Dependent Ni Segregation in a Micron-Sized Single-Crystal Li 1.2 Ni 0.2 Mn 0.6 O 2 Cathode

Elemental surface segregation in cathode materials is critical for determining the phase and interfacial reaction between electrode and electrolyte, which consequently affects the electrochemical properties. Single-crystal cathode of Li 1.2 Ni 0.2 Mn 0.6 O 2 and Li 1.2 Ni 0.2 Mn 0.6 O 1.95 F 0.05 with an octahedral morphology of (102) and (003) dominated facets have been manifested to show enhanced electrochemical properties. However, the surface structural features of such single crystals have not been investigated. Herein, using scanning transmission electron microscopy, energy dispersive X-ray spectroscopy, and electron energy loss spectroscopy, we probe the elemental surface segregation characteristics in these single-crystal cathode. We reveal that Ni surface segregation shows dependence on the crystal facet such that it occurs on crystal facets with a mix of cations and anions, but not on the facets with only cations or anions. Furthermore, facet-dependent surface reconstructions are observed, featuring a spinel-like structure at the Ni-rich facet but rock-salt structure at the facet without Ni segregation. The commonly known Mn reduction appears at the single crystal surfaces, more pronounced at the facet without Ni segregation. We further reveal that fluorination leads to the stabilization of surface oxygens. In conclusion, this study provides detailed structural and chemical information about the facet-dependent Ni surface segregation and the resulted phase formation in the rather less explored micron-sized octahedral Li 1.2 Ni 0.2 Mn 0.6 O 2 and Li 1.2 Ni 0.2 Mn 0.6 O 1.95 F 0.05 single crystals, which is key to further exploration of electrochemical properties of cathode in the form of micro-sized single crystal.

25 ENERGY STORAGE↗

DOE OSTI2026

Photovoltage behaviour of p-Sb 2 S 3 photocathodes for hydrogen evolution: effect of n-In 2 S 3 passivation layers

The 1.76 eV band gap of antimony(iii) sulphide (Sb 2 S 3 ) makes this semiconductor material a promising light absorber for photoelectrochemical water splitting, but scalable fabrication approaches to efficient devices are still lacking. Here we show that compact Sb 2 S 3 films on FTO can be obtained by electrochemical growth from aqueous colloidal sulphur and antimony trichloride solutions, followed by mild annealing. These films can be converted into hydrogen evolution photocathodes after coating with In 2 S 3 passivation layers and the addition of Pt proton reduction co-catalysts. For the first time, vibrating Kelvin probe surface photovoltage (VKP-SPV) spectroscopy is used to observe the carrier dynamics in such photoelectrodes. While the bare Sb 2 S 3 films suffer from high surface recombination rates and poor electron extraction, the In 2 S 3 overlayer is found to raise the photovoltage and cathodic photocurrent density, due to passivation of surface defects and formation of a p–n heterojunction. In thick In 2 S 3 films, these benefits are offset by shading and slow electron transfer. Also, we find that O 2 strongly affects the band bending in the Sb 2 S 3 –air and In 2 S 3 –air junctions and their photovoltage. The optimised devices evolve H 2 at 77.5% Faradaic efficiency and with 0.084% applied bias photon-to-current efficiency (ABPE) at 0.12 V vs. RHE. The low ABPE value is attributed to Sb 2 S 3 sub-bandgap defects visible in SPV spectra, the random orientation of Sb 2 S 3 crystallites in the films, which inhibits charge transport, the absence of crystal facets of Sb 2 S 3 , and a detrimental Schottky junction at the FTO|Sb 2 S 3 interface.

de Araújo, Moisés A. [University of California, Da↗

DOE OSTI2025

Probing Plasmonic Near-Fields in Oxide-Modified Aluminum Nanocubes Using Photon-Induced Near-Field Electron Microscopy

Plasmonic nanoparticles generate strong electric fields near their surface upon photoexcitation, enabling applications in sensing, spectroscopy, and photocatalysis. Electron microscopy techniques – such as cathodoluminescence and electron energy loss spectroscopy – have been leveraged to produce nanoscale maps of localized surface plasmon (LSP) modes. More recently, photon-induced near-field electron microscopy (PINEM) has emerged as a powerful technique for imaging evanescent near-fields generated by ultrafast laser excitation. In this work, we employ PINEM within an ultrafast electron microscope, complemented by numerical calculations to investigate how optical polarization, surface modification, and light intensity affect the evanescent fields associated with LSPs on oxide-modified aluminum nanocubes. Polarization control of the incident light field enables spatial mapping of the nanocube’s LSPs at the single particle level. Systematic variation of the oxide layer thickness reveals that increased coating thickness correlates with a stronger PINEM signal and a greater energy gain of probing electrons. Additionally, higher light intensities at fixed polarization and oxide coating further amplify the PINEM signal. These findings demonstrate the utility of PINEM as a high-resolution technique for optical near-field imaging and spectroscopy of single plasmonic nanoparticles. The ability to probe single particle behavior offers new opportunities for advancing the design and characterization of nanophotonic and plasmonic materials.

PINEM↗

DOE OSTI2023

Measuring Photoexcited Electron and Hole Dynamics in ZnTe and Modeling Excited State Core-Valence Effects in Transient Extreme Ultraviolet Reflection Spectroscopy

Transient extreme ultraviolet (XUV) spectroscopy is becoming a valuable tool for characterizing solar energy materials because it can separate photoexcited electron and hole dynamics with element specificity. We use surface-sensitive femtosecond XUV reflection spectroscopy to separately measure photoexcited electron, hole, and band gap dynamics of ZnTe, a promising photocathode for CO 2 reduction. We develop an ab initio theoretical framework based on density functional theory and the Bethe-Salpeter equation to robustly assign the complex transient XUV spectra to the material's electronic states. Applying this framework, we identify the relaxation pathways and quantify their time scales in photoexcited ZnTe, including subpicosecond hot electron and hole thermalization, surface carrier diffusion, ultrafast band gap renormalization, and evidence of acoustic phonon oscillations.

14 SOLAR ENERGY↗