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DOE OSTI2021

VFA Biorefinery Design for Informed Production of Ground and Aviation Fuels

The rising demand for low-carbon intensity fuel options requires evaluation of a system which can support their production economically and sustainably. Volatile fatty acids (VFAs) ranging from C2 to C8 can be derived in high yield from arrested anaerobic digestion of biomass. This talk provides an overview of our work in which we upgrade wet waste-derived VFAs using ketonization to elongate their carbon backbone to reach a range relevant to jet or diesel fuels. Kinetic models were used to predict ketone profiles from varying VFA profiles, thereby informing potential carbon flow to either (a) mixed paraffins for use in diesel or aviation fuel, or (b) ethers for use in diesel fuel. To do this, the anticipated products were screened for critical fuel characteristics using predictive tools. The criteria for neat and blended bioblendstocks were chosen based on conventional petrofuel requirements, and they were applied to inform fuel targets, identify limiting characteristics, and guide conversion development. While paraffins can serve as either diesel or aviation fuels, the latter has stringent criteria which include a precise distillation curve range tied to carbon distribution. Fuels which fall outside this range typically fail to meet other property metrics, and as such flashpoint and viscosity were identified as potentially limiting properties of this VFA aviation fuel. However, paraffin fractions which fall outside aviation criteria may meet diesel fuel requirements, which are looser except for the flashpoint minimum. Flashpoint was also a concern for smaller VFA diesel ethers, which posed an additional oxygenate risk of high water solubility. This fuel-informed conversion design process was demonstrated through production of paraffins with reduced sooting as compared to petrodiesel (~34%), and increased renewable aviation fuel blend levels (>70%). VFA-derived ethers improved petrodiesel by increasing fuel autoignition quality by 56% and reducing sooting by 86%. These VFA aviation and diesel fuels could enable greenhouse gas (GHG) reductions of over 165% and 50%, respectively, relative to their purely fossil-derived counterparts. Collectively, this work provides (i) an overview of how we leveraged the flexibility of VFAs for fuel production; and (ii) insight into the potential of a VFA biorefinery to accommodate varied feed and fuel applications, while also considering the merit of tailored fuel production pathways and GHG reduction potential.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2024

Quantifying carrier density in monolayer MoS 2 by optical spectroscopy

The successful design and device integration of nanoscale heterointerfaces hinges upon precise manipulation of both ground- and excited-state charge carrier (electron and hole) densities. However, it is particularly challenging to quantify these charge carrier densities in nanoscale materials, leading to uncertainties in the mechanisms of many carrier density-dependent properties and processes. Here, we demonstrate a method that utilizes steady-state and transient absorption spectroscopies to correlate monolayer MoS 2 electron density with the easily measured metric of excitonic optical absorption quenching in a variety of mixed-dimensionality s-SWCNT/MoS 2 heterostructures. By employing a 2D phase-space filling model, the resulting correlation elucidates the relationship between charge density, local dielectric environment, and concomitant excitonic properties. The phase-space filling model is also able to describe existing trends from the literature on transistor-based measurements on MoS 2 , WS 2 , and MoSe 2 monolayers that were not previously compared to a physical model, providing additional support for our method and results. The findings provide a pathway to the community for estimating both ground- and excited-state carrier densities in a wide range of TMDC-based systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1989

Halogen Occultation Experiment (HALOE) optical filter characterization

The Halogen Occultation Experiment (HALOE) is a solar occultation experiment that will fly on the Upper Atmosphere Research Satellite to measure mixing ratio profiles of O3, H2O, NO2, NO, CH4, HCl, and HF. The inversion of the HALOE data will be critically dependent on a detailed knowledge of eight optical filters. A filter characterization program was undertaken to measure in-band transmissions, out-of-band transmissions, in-band transmission shifts with temperature, reflectivities, and age stability. Fourier Transform Infrared Spectrometers were used to perform measurements over the spectral interval 400/cm to 6300/cm (25 micrometers to 1.6 micrometers). Very high precision (0.1 percent T) in-band measurements and very high resolution (0.0001 percent T) out-of-band measurements have been made. The measurements revealed several conventional leaks at 0.01 percent transmission and greatly enhanced (1,000) leaks to the 2-element filters when placed in a Fabry-Perot cavity. Filter throughput changes by 5 percent for a 25 C change in filter temperature.

Harvey, Gale A.↗

DOE OSTI2023

One-Component, Vinyl-Functional Fluorosilicone Pastes for Direct Ink Write Additive Manufacturing

In this study, one-component (“all-in-one”) fluorosilicone pastes specifically designed for application in direct ink write (DIW) additive manufacturing (AM) have been developed. They consist of vinyl-functional, methyltrifluoropropyl-containing (MeTfpS) terpolysiloxane base polymer(s), hydrosilyl-functional cross-linker(s), UV-sensitive hydrosilylation catalyst, thixotropic additive, and trimethylsilylated fumed silica filler, with other additives that are optional. Their base polymers were completely amorphous and linear, with molecular weights (M n ) ranging from approximately 7000 to 50,000 and specifically targeted for the viscosity range ideal for DIW. These polymers were prepared by anionic ring-opening polymerizations (A-ROP) of appropriate mixtures of cyclic siloxanes initiated by oligomeric, difunctional tetramethylammonium silanolate in the presence of a difunctional tetramethyldivinyldisiloxane end-blocker and molecular weight regulator. Two series of these terpolymers were prepared: one containing 5 mol % MeTfpS repeat units but varying degrees of polymerization (DP) from 80 to 600 and the other containing 5, 10, and 15 mol % MeTfpS at a constant DP of 600. All polymers contained mostly random distributions of MeTfpS repeat units. The pastes were prepared by speed-mixing, ready for use in DIW, they exhibited ideal thixotropy, long-term (over a year) rheological stability, and can be quickly (within seconds) and permanently cured by room-temperature, UV-activated hydrosilylation in air. The resulting elastomers showed base polymer molecular weight- and composition-dependent stress-induced crystallization (SIC) at higher molecular weights and lower trifluoropropyl contents and tunable Shore A hardness (30A–40A) typical for soft polysiloxane rubbers. Preliminary DIW tests indicated excellent printability with high precision of printed shapes and clearly present these one-component pastes as prime candidates for simple and practical printing of silicone elastomer objects.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Multi-cation perovskites prevent carrier reflection from grain surfaces

The composition of perovskite has been optimized combinatorially such that it often contains six components (A x B y C 1-x-y PbX z Y 3-z ) in state-of-art perovskite solar cells. Questions remain regarding the precise role of each component, and the lack of a mechanistic explanation limits the practical exploration of the large and growing chemical space. Here, aided by transient photoluminescence microscopy, we find that, in perovskite single crystals, carrier diffusivity is in fact independent of composition. In polycrystalline thin films, the different compositions play a crucial role in carrier diffusion. In this work, we report that methylammonium (MA)-based films show a high carrier diffusivity of 0.047 cm 2 s -1 , while MA-free mixed caesium-formamidinium (CsFA) films exhibit an order of magnitude lower diffusivity. Elemental composition studies show that CsFA grains display a graded composition. This curtails electron diffusion in these films, as seen in both vertical carrier transport and surface potential studies. Incorporation of MA leads to a uniform grain core-to-edge composition, giving rise to a diffusivity of 0.034 cm 2 s -1 in CsMAFA films. A model that invokes competing crystallization processes allows us to account for this finding, and suggests further strategies to achieve homogeneous crystallization for the benefit of perovskite optoelectronics.

36 MATERIALS SCIENCE↗

NASA NTRS2012

Conformal Ablative Thermal Protection System for Planetary and Human Exploration Missions

The Office of Chief Technologist (OCT), NASA has identified the need for research and technology development in part from NASAs Strategic Goal 3.3 of the NASA Strategic Plan to develop and demonstrate the critical technologies that will make NASAs exploration, science, and discovery missions more affordable and more capable. Furthermore, the Game Changing Development Program (GCDP) is a primary avenue to achieve the Agencys 2011 strategic goal to Create the innovative new space technologies for our exploration, science, and economic future. In addition, recently released NASA Space Technology Roadmaps and Priorities, by the National Research Council (NRC) of the National Academy of Sciences stresses the need for NASA to invest in the very near term in specific EDL technologies. The report points out the following challenges (Page 2-38 of the pre-publication copy released on February 1, 2012): Mass to Surface: Develop the ability to deliver more payload to the destination. NASA's future missions will require ever-greater mass delivery capability in order to place scientifically significant instrument packages on distant bodies of interest, to facilitate sample returns from bodies of interest, and to enable human exploration of planets such as Mars. As the maximum mass that can be delivered to an entry interface is fixed for a given launch system and trajectory design, the mass delivered to the surface will require reductions in spacecraft structural mass more efficient, lighter thermal protection systems more efficient lighter propulsion systems and lighter, more efficient deceleration systems. Surface Access: Increase the ability to land at a variety of planetary locales and at a variety of times. Access to specific sites can be achieved via landing at a specific location(s) or transit from a single designated landing location, but it is currently infeasible to transit long distances and through extremely rugged terrain, requiring landing close to the site of interest. The entry environment is not always guaranteed with a direct entry, and improving the entry systems robustness to a variety of environmental conditions could aid in reaching more varied landing sites. The National Research Council (NRC) Space Technology Roadmaps and Priorities report highlights six challenges and they are: 1) Mass to Surface, 2) Surface Access, 3) Precision Landing, 4) Surface Hazard Detection and Avoidance, 5) Safety and Mission Assurance, and 6) Affordability. In order for NASA to meet these challenges, the report recommends immediate focus on Rigid and Flexible Thermal Protection Systems. Rigid TPS systems such as Avcoat or SLA are honeycomb based and PICA is in the form of tiles. The honeycomb systems is manufactured using techniques that require filling of each (3/8 cell) by hand and within a limited amount of time once the ablative compound is mixed, all of the cells have to be filled and the entire heat-shield has to be cured. The tile systems such as PICA pose a different challenge as the mechanical strength characteristic and the manufacturing limitations require large number of small tiles with gap-fillers between the tiles. Recent investments in flexible ablative systems have given rise to the potential for conformal ablative TPS> A conformal TPS over a rigid aeroshell has the potential to solve a number of challenges faced by traditional rigid TPS materials.

Beck, R.↗

DOE OSTI2024

Hydrogen underground storage for grid electricity storage: An optimization study on techno-economic analysis

Here, this study performs a techno-economic analysis of hydrogen underground storage systems for grid electricity storage, evaluating their economic viability at the plant scale using dynamic optimization. It explores the feasibility of various system configurations and revenue models in the context of volatile electricity prices and the necessity for multiple revenue streams. The hypothesis tested is that large-scale hydrogen storage, despite its low round-trip efficiency, can be economically viable with the right mix of revenue streams. This study uses scenario-based analysis to assess the impacts of different system configurations, including engaging in time-shifting arbitrage, ancillary service markets and blending hydrogen with natural gas. Results indicate potential annual net cash flows of up to $\$$1.5 million from ancillary services integration and $\$$5.2 million from natural gas blending, contingent on specific system sizes. The study concludes that hydrogen underground storage for grid electricity storage can be profitable, and emphasizes that proper system design and precise electricity price forecasting are crucial for optimizing system performance and economic returns. This research sets the stage for further investigations into the scalability of hydrogen storage systems and their broader implications for grid electricity storage and energy market dynamics.

25 ENERGY STORAGE↗

DOE OSTI2020

Ultracompact 3D microfluidics for time-resolved structural biology

To advance microfluidic integration, we present the use of two-photon additive manufacturing to fold 2D channel layouts into compact free-form 3D fluidic circuits with nanometer precision. We demonstrate this technique by tailoring microfluidic nozzles and mixers for time-resolved structural biology at X-ray free-electron lasers (XFELs). We achieve submicron jets with speeds exceeding 160 ms -1 , which allows for the use of megahertz XFEL repetition rates. By integrating an additional orifice, we implement a low consumption flow-focusing nozzle, which is validated by solving a hemoglobin structure. Also, aberration-free in operando X-ray microtomography is introduced to study efficient equivolumetric millisecond mixing in channels with 3D features integrated into the nozzle. Such devices can be printed in minutes by locally adjusting print resolution during fabrication. This technology has the potential to permit ultracompact devices and performance improvements through 3D flow optimization in all fields of microfluidic engineering.

3-D reconstruction↗

NASA NTRS2001

An Assessment of the Ability of Potential Space-Borne Instruments to Resolve Spatial and Temporal Variability of Atmospheric Carbon Dioxide

Mounting concern regarding the possibility that increasing carbon dioxide concentrations will initiate climate change has stimulated interest in the feasibility of measuring CO2 mixing ratios from satellites. Currently, the most comprehensive set of atmospheric CO2 data is from the NOAA CMDL cooperative air sampling network, consisting of more than 40 sites where flasks of air are collected approximately weekly. Sporadic observations in the troposphere and stratosphere from airborne in situ and flask samplers are also available. Although the surface network is extensive, there is a dearth of data in the Southern Hemisphere and most of the stations were intentionally placed in remote areas, far from major sources. Sufficiently precise satellite observations with adequate spatial and temporal resolution would substantially increase our knowledge of the atmospheric CO2 distribution and would undoubtedly lead to improved understanding of the global carbon budget. We use a 3-D chemical transport model to investigate the ability of potential satellite instruments with a variety of orbits, horizontal resolution and vertical weighting functions to capture the variation in the modeled CO2 fields. The model is driven by analyzed winds from the Goddard Data Assimilation Office. Simulated CO2 fields are compared with existing surface and aircraft data, and the effects of the model convection scheme and representation of the planetary boundary layer are considered.

Andrews, Arlyn E.↗

NASA NTRS2002

An Assessment of the Ability of Potential Satellite Instruments to Resolve Spatial and Temporal Variability of Atmospheric CO2

Sufficiently precise satellite observations with adequate spatial and temporal resolution would substantially increase our knowledge of the atmospheric CO2 distribution and would undoubtedly lead to reduced uncertainty in estimates of the global carbon budget. An overview of possible strategies for measuring CO2 from space will be presented, including IR and nearby measurements, active sensors and broad band and narrow band passive sensors. The ability of potential satellite instruments with a variety of orbits, horizontal resolution and vertical weighting functions to capture the variation in atmospheric CO2 mixing ratios will be illustrated using a combination of surface data, aircraft data and model results.

Andrews, A.↗

NASA NTRS2001

An Assessment of the Ability of Potential Spaceborne Instruments to Resolve Spatial and Temporal Variability of Atmospheric Carbon Dioxide

Andrews, Arlyn E.↗

NASA NTRS2005

A Climatology of Midlatitude Continental Clouds from the ARM SGP Site: Low-Level Cloud Macrophysical, Microphysical, and Radiative Properties - Part I

A record of single-layer and overcast low cloud (stratus) properties has been generated using approximately 4000 hours of data collected from January 1997 to December 2002 at the Atmospheric Radiation Measurement (ARM) Southern Great Plains Central Facility (SCF). The cloud properties include liquid-phase and liquid-dominant, mixed-phase, low cloud macrophysical, microphysical, and radiative properties including cloud-base and -top heights and temperatures, and cloud physical thickness derived from a ground-based radar and lidar pair, and rawinsonde sounding; cloud liquid water path (LWP) and content (LWC), and cloud-droplet effective radius (r(sub e)) and number concentration (N) derived from the macrophysical properties and radiometer data; and cloud optical depth (tau), effective solar transmission (gamma), and cloud/top-of-atmosphere albedos (R(sub cldy)/R(sub TOA)) derived from Eppley precision spectral pyranometer measurements. The cloud properties were analyzed in terms of their seasonal, monthly, and hourly variations. In general, more stratus clouds occur during winter and spring than in summer. Cloud-layer altitudes and physical thicknesses were higher and greater in summer than in winter with averaged physical thicknesses of 0.85 km and 0.73 km for day and night, respectively. The seasonal variations of LWP, LWC, N. tau, R(sub cldy), and R(sub TOA) basically follow the same pattern with maxima and minima during winter and summer, respectively. There is no significant variation in mean r(sub e), however, despite a summertime peak in aerosol loading, Although a considerable degree of variability exists, the 6-yr average values of LWP, LWC, r(sub e), N, tau, gamma, R(sub cldy) and R(sub TOA) are 150 gm(exp -2) (138), 0.245 gm(exp -3) (0.268), 8.7 micrometers (8.5), 213 cm(exp -3) (238), 26.8 (24.8), 0.331, 0.672, 0.563 for daytime (nighttime). A new conceptual model of midlatitude continental low clouds at the ARM SGP site has been developed from this study. The low stratus cloud amount monotonically increases from midnight to early morning (0930 LT), and remains large until around local noon, then declines until 1930 LT when it levels off for the remainder of the night. In the morning, the stratus cloud layer is low, warm, and thick with less LWC, while in the afternoon it is high, cold, and thin with more LWC. Future parts of this series will consider other cloud types and cloud radiative forcing at the ARM SCF.

Dong, Xiquan↗

DOE OSTI2024

The Cauchy Problem for Boltzmann Bi-linear Systems: The Mixing of Monatomic and Polyatomic Gases

Abstract From a unified vision of vector valued solutions in weighted Banach spaces, this paper establishes the existence and uniqueness for space homogeneous Boltzmann bi-linear systems with conservative collisional forms arising in complex gas dynamical structures. This broader vision is directly applied to dilute multi-component gas mixtures composed of both monatomic and polyatomic gases. Such models can be viewed as extensions of scalar Boltzmann binary elastic flows, as much as monatomic gas mixtures with disparate masses and single polyatomic gases, providing a unified approach for vector valued solutions in weighted Banach spaces. Novel aspects of this work include developing the extension of a general ODE theory in vector valued weighted Banach spaces, precise lower bounds for the collision frequency in terms of the weighted Banach norm, energy identities, angular or compact manifold averaging lemmas which provide coerciveness resulting into global in time stability, a new combinatorics estimate for p -binomial forms producing sharper estimates for the k -moments of bi-linear collisional forms. These techniques enable the Cauchy problem improvement that resolves the model with initial data corresponding to strictly positive and bounded initial vector valued mass and total energy, in addition to only a $$2^+$$ 2 + moment determined by the hard potential rates discrepancy, a result comparable in generality to the classical Cauchy theory of the scalar homogeneous Boltzmann equation.

Physics↗

DOE OSTI2025

Highly excited electron cyclotron for QCD axion and dark-photon detection

We propose using highly excited cyclotron states of a trapped electron to detect meV axion and dark-photon dark matter, marking a significant improvement over our previous proposal and demonstration [One-electron quantum cyclotron as a milli-ev dark-photon detector, .]. When the axion mass matches the cyclotron frequency ω c , the cyclotron state is resonantly excited, with a transition probability proportional to its initial quantum number, n c . The sensitivity is enhanced by taking n c ∼ 10 6 ( 0.1 meV ω c ) 2 . By optimizing key experimental parameters, we minimize the required averaging time for cyclotron detection to t ave ∼ 10 − 6 s, permitting detection of such a highly excited state before its decay. An open–end-cap trap design enables the external photon signal to be directed into the trap, rendering our background-free detector compatible with large focusing cavities, such as the BREAD proposal, while capitalizing on their strong magnetic fields. Furthermore, the axion conversion rate can be coherently enhanced by incorporating layers of dielectrics with alternating refractive indices within the cavity. Collectively, these optimizations enable us to probe the QCD axion parameter space from 0.1 to 2.3 meV (25–560 GHz), covering a substantial portion of the predicted postinflationary QCD axion mass range. This sensitivity corresponds to probing the kinetic mixing parameter of the dark photon down to ε ≈ 2 × 10 − 16 . Published by the American Physical Society 2025

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2025

Mapping in situ the assembly and dynamics in aqueous supramolecular polymers

Supramolecular polymers, bonded through directional non-covalent interactions, closely mimic dynamic behaviors of biological nanofibers. However, the complexity of assembly pathways makes it highly challenging to unravel the nature of supramolecular dynamics in aqueous environments. Here we introduce a precise combinatorial titration methodology to probe in situ the assembly of peptide amphiphiles (PAs). This approach reveals a binary assembly mechanism governed by equilibrium between spheroidal micelles and β-sheet polymers. Weakening hydrogen bonding shifts the equilibrium towards micelles and decreases the internal structural order of filamentous polymers, promoting supramolecular dynamics. Extending this methodology to two-component copolymerization systems, we find a surprising tendency to form blocky nanostructures with reduced internal phase separation as the mismatch in peptide sequence decreases. Interestingly, while well-mixed copolymers acquire different dynamics, mismatched ones retain the characteristic supramolecular motion of their homopolymer counterparts. These critical insights into supramolecular dynamics offer strategies to tailor the dynamic functions of supramolecular nanomaterials.

Molecular self-assembly↗

DOE OSTI2023

Enhanced dilepton emission from a phase transition in dense matter

It is demonstrated that the presence of a phase transition in heavy-ion collisions, at beam energies that probe dense quantum chromodynamics (QCD) matter, leads to a significant enhancement of the dilepton yield at low invariant mass and requires the embedding of low beam energies per produced pion due to the extended emission time. In addition, the temperature of low-mass dileptons shows a modest decrease due to the mixed phase. The emission of dileptons in the SIS18–SIS100 beam energy range is studied by augmenting the ultra-relativistic quantum molecular dynamics (UrQMD) transport model with a realistic density-dependent equation of state, as well as two different phase transitions. This is achieved by extending the molecular dynamics interaction part of the UrQMD model to a density-dependent interaction potential with a high-density minimum, leading to a phase transition and metastable coexisting high-density states. Together with a high-precision measurement, these simulations will be able to constrain the existence of a phase transition in QCD up to densities of several times nuclear saturation density.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2025

Autonomous Synthesis of Metastable Materials Using a Modular Mixed-Flow Reactor

Understanding and controlling atomic-level processes at solid-liquid interfaces is key to advancing technologies in energy storage, carbon capture, critical element recovery, and materials synthesis. Many of these processes are dominated by the formation of short-lived intermediate precipitates that determine the final properties of synthesized materials. However, studying these intermediates is challenging due to their sensitivity and the reliance on trial-and-error methods. To address this, we developed an automated variable-volume mixed-flow reactor (MFR) to optimize metastable material synthesis and investigate rapid kinetic processes. This state-of-the-art MFR system, paired with an automated modeling framework, enables efficient synthesis and real-time analysis of transient phases. Benchmarking with advanced capabilities, such as wide-/small-angle X-ray scattering, allows us to resolve fast nucleation and growth dynamics that were previously inaccessible. By combining automation, ML-guided optimization, and tailored kinetic modeling, this approach provides a robust platform for improving material design and achieving precise control over solid-liquid reactions.

36 MATERIALS SCIENCE↗

NASA NTRS2010

Global Precipitation at Your Fingertips, Part I: Data

The most accurate satellite estimates come from the first precipitation radar (PR) to fly in space, aboard the Tropical Rainfall Measuring Mission (TRMM) satellite. Although important for research, the PR's coverage is too limited to give routine monitoring of global precipitation. Rather, we depend on observations of the Earth system's natural emission of microwave energy. Even these data are not available at all times since the satellites on which the microwave sensors fly are in "low Earth orbit", or LEO, some 400-800 km above the surface. Such LEO satellites pass over any given spot on Earth twice a day. In contrast, "geosynchronous Earth orbit", or GEO, satellites at an altitude of about 35,000 km orbit at the same speed that the Earth revolves and therefore always view the same part of the surface. The trade-off is that GEO sensors provide less-precise estimates computed from the Earth system's natural emissions of infrared (IR) energy. Other satellite datasets are used to provide estimates in regions where both microwave and IR have difficulty, such as polar regions or times before mid-1987 when microwave data became available. Finally, rain gauge data where available, have proved to be valuable for helping to reduce biases in the satellite data, which are persistent differences between the satellite estimate and the precipitation that actually occurred. The datasets discussed below take slightly different approaches to mixing and matching the various kinds of input data to create global estimates of precipitation that answer different needs and/or take advantage of different input data. Each is produced at the NASA Goddard Space Flight Center, in Greenbelt, Maryland, USA. [Other combination datasets are produced at other data centers.]

Huffman, George J.↗