Results for “Condensed phase systems” — Page 17

DOE OSTI2024

Prediction of s ± -Wave Superconductivity Enhanced by Electronic Doping in Trilayer Nickelates La 4 Ni 3 O 10 under Pressure

Motivated by the recently reported signatures of superconductivity in trilayer La 4 ⁢Ni 3 ⁢O 10 under pressure, here we comprehensively study this system using ab initio and random-phase approximation techniques. Without electronic interactions, the Ni d 3z 2 –r 2 orbitals show a bonding-antibonding and nonbonding splitting behavior via the O p z orbitals inducing a “trimer” lattice in La 4⁢ Ni 3 ⁢O 10 , analogous to the dimers of La 3 ⁢Ni 2 ⁢O 7 . The Fermi surface consists of three electron sheets with mixed e g orbitals, and a hole and an electron pocket made up of the d 3⁢z 2 –r 2 orbital, suggesting a Ni two-orbital minimum model. In addition, we find that superconducting pairing is induced in the s ± -wave channel due to partial nesting between the M = (π,π) centered pockets and portions of the Fermi surface centered at the Γ = (0,0) point. With changing electronic density n, the s ± instability remains leading and its pairing strength shows a domelike behavior with a maximum around n = 4.2 ( ~6.7% electron doping). The superconducting instability disappears at the same electronic density as that in the new 1313 stacking La 3 ⁢Ni 2 ⁢O 7 , correlated with the vanishing of the hole pocket that arises from the trilayer sublattice, suggesting that the high-T c superconductivity of La 3⁢ Ni 2 ⁢O 7 does not originate from a trilayer and monolayer structure. Furthermore, we confirm the experimentally proposed spin state in La 4 ⁢Ni 3 ⁢O 10 with an in-plane (π, π) order and antiferromagnetic coupling between the top and bottom Ni layers, and spin zero in the middle layer.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Embracing disorder in quantum materials design

Many of the most exciting materials discoveries in fundamental condensed matter physics are made in systems hosting some degree of intrinsic disorder. While disorder has historically been regarded as something to be avoided in materials design, it is often of central importance to correlated and quantum materials. This is largely driven by the conceptual and theoretical ease to handle, predict, and understand highly uniform systems that exhibit complex interactions, symmetries, and band structures. In this Perspective, we highlight how flipping this paradigm has enabled exciting possibilities in the emerging field of high entropy materials, focusing primarily on high entropy oxide and chalcogenide quantum materials. These materials host high levels of cation or anion compositional disorder while maintaining unexpectedly uniform single crystal lattices. The diversity of atomic scale interactions of spin, charge, orbital, and lattice degrees of freedom are found to emerge into coherent properties on much larger length scales. Thus, altering the variance and magnitudes of the atomic scale properties through elemental selection can open new routes to tune global correlated phases, such as magnetism, metal–insulator transitions, ferroelectricity, and even emergent topological responses. The strategy of embracing disorder in this way provides a much broader pallet from which functional states can be designed for next-generation microelectronic and quantum information systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Embracing Disorder in Quantum Materials Design

Many of the most exciting materials discoveries in fundamental condensed matter physics are made in systems hosting some degree of intrinsic disorder. While disorder has historically been regarded as something to be avoided in materials design, it is often of central importance to correlated and quantum materials. This is largely driven by the conceptual and theoretical ease to handle, predict, and understand highly uniform systems that exhibit complex interactions, symmetries, and band structures. In this Perspective, we highlight how flipping this paradigm has enabled exciting possibilities in the emerging field of high entropy materials, focusing primarily on high entropy oxide and chalcogenide quantum materials. These materials host high levels of cation or anion compositional disorder while maintaining unexpectedly uniform single crystal lattices. The diversity of atomic scale interactions of spin, charge, orbital, and lattice degrees of freedom are found to emerge into coherent properties on much larger length scales. Thus, altering the variance and magnitudes of the atomic scale properties through elemental selection can open new routes to tune global correlated phases, such as magnetism, metal–insulator transitions, ferroelectricity, and even emergent topological responses. The strategy of embracing disorder in this way provides a much broader pallet from which functional states can be designed for next-generation microelectronic and quantum information systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS1984

The turbulent twisted magnetic flux tube gas

The kinematic behavior of a dilute, two-dimensional 'gas' of parallel twisted magnetic flux tubes in a highly conducting fluid is considered. Collisions between flux tubes with the same sense of twist are inelastic due to the reconnection of their oppositely directed azimuthal magnetic field components at impact. In some collisions, the tension in the reconnected magnetic flux is sufficient to bind the two flux tubes together. Collisions between flux tubes with the opposite sense of twist are elastic. It is shown that a tenuous gas of individual twisted flux tubes condenses into two large-scale regions of magnetic field with opposite twists. This calculation illustrates the results of Montgomery and co-workers on the migration of magnetic energy towards small wavenumbers in two-dimensional magnetohydrodynamic (MHD) turbulence. In particular, this problem illustrates the dynamical nonequilibrium of the relaxation phase in turbulent MHD systems.

Bogdan, T. J.↗

NASA NTRS1993

Grain surface features of Apollo 17 orange and black glass

Lunar soil sample 74220 and core samples 74001/2 consist mainly of orange glass droplets, droplet fragments, and their crystallized equivalents. These samples are now generally accepted to be pyroclastic ejecta from early lunar volcanic eruptions. It has been known that they contain surface coatings and material rich in volatile condensable phases including S, Zn, F, Cl, and many volatile metals. Meyer summarizes the voluminous published chemical data and calculates the volatile enrichment ratios for most of the surface condensates. In an attempt to more completely understand this enrichment of surface volatiles, we have searched for carbon and carbon-bearing phases on droplet surfaces. We have reviewed many of our existing photomicrographs and energy dispersive analysis (EDX) of grain surfaces and have reexamined some of our older SEM mounts using an improved EDXA system capable of light element detection and analysis (oxygen, nitrogen, and carbon). In addition, we have made fresh mounts using procedures which should minimize carbon contamination or extraneous carbon x-rays and have analyzed for carbon.

Mckay, David S.↗

NASA NTRSDate not supplied

Observing Ice Phase Clouds and Precipitation with Millimeter- and Submillimeter-wave Radiometry during the IMPACTS field campaign: Algorithm Development for the Emerging Class of Microwave Radiometers

Millimeter- and submillimeter-wave (mmWave, submm) radiometers provide significant information content on atmospheric water in liquid, ice, and vapor phases. Recent sensors, such as the Global Precipitation Measurement (GPM) or the Temporal Experiment for Storms and Tropical Systems Technology – Demonstration (TEMPEST-D), use mmWave bands to improve estimation of ice-phase precipitation, and future missions, such as the Atmosphere Observing System (AOS), will extend to submm to provide additional information on thinner ice clouds, linking clouds and precipitation and therefore elucidating the links between weather, climate, and the water cycle. To support the expanded use of mmWave/submm radiometry and exploit the available information content on condensed water mass, we demonstrate ice and liquid water path retrievals for NASA Goddard Space Flight Center's airborne radiometers the Conical Scanning Millimeter-wave Imaging Radiometer (CoSMIR) and the Configurable Scanning Submillimeter-wave Instrument/Radiometer (CoSSIR, formerly the Compact Scanning Submillimeter Imaging Radiometer). The analysis is based on data collected during the Investigation of Microphysics and Precipitation for Atlantic Coast-Threatening Storms (IMPACTS) field campaign. A simulation study compares and contrasts retrievals for CoSMIR and CoSSIR, with CoSSIR demonstrating higher skill in ice retrievals, particularly for thin clouds, and the CoSMIR frequencies performing better for liquid. Additionally, we look at dual-polarized radiances observed by CoSMIR during the first two IMPACTS deployments to understand the polarization signatures induced by oriented hydrometeors. Results will be presented in the context of upcoming missions and sensors including AOS and the Ice Cloud Imager (ICI). We will describe the objectives for the expected first flight of the newly upgraded CoSSIR during the final IMPACTS deployment, and we will share novel science investigations we plan to undertake with CoSSIR's new capabilities. Popular Summary: Ice in clouds and falling snow is an important component of weather, climate, and water resources. To better use a new class of sensors that provide information on atmospheric ice, we developed an approach to measure ice clouds and falling snow using airborne data taken during the Investigation of Microphysics and Precipitation for Atlantic Coast-Threatening Storms (IMPACTS), a field campaign to study winter storms. We look at the results for two similar instruments to understand how those differences affect these measurements of clouds and snow, and we further investigate the information the sensors can provide on properties of the clouds and snow.

Ian S Adams↗

NASA NTRSDate not supplied

Observing Ice Phase Clouds and Precipitation with Millimeter- and Submillimeter-wave Radiometry during the IMPACTS field campaign: Algorithm Development for the Emerging Class of Microwave Radiometers

Millimeter- and submillimeter-wave (mmWave, submm) radiometers provide significant information content on atmospheric water in liquid, ice, and vapor phases. Recent sensors, such as the Global Precipitation Measurement (GPM) or the Temporal Experiment for Storms and Tropical Systems Technology – Demonstration (TEMPEST-D), use mmWave bands to improve estimation of ice-phase precipitation, and future missions, such as the Atmosphere Observing System (AOS), will extend to submm to provide additional information on thinner ice clouds, linking clouds and precipitation and therefore elucidating the links between weather, climate, and the water cycle. To support the expanded use of mmWave/submm radiometry and exploit the available information content on condensed water mass, we demonstrate ice and liquid water path retrievals for NASA Goddard Space Flight Center's airborne radiometers the Conical Scanning Millimeter-wave Imaging Radiometer (CoSMIR) and the Configurable Scanning Submillimeter-wave Instrument/Radiometer (CoSSIR, formerly the Compact Scanning Submillimeter Imaging Radiometer). The analysis is based on data collected during the Investigation of Microphysics and Precipitation for Atlantic Coast-Threatening Storms (IMPACTS) field campaign. A simulation study compares and contrasts retrievals for CoSMIR and CoSSIR, with CoSSIR demonstrating higher skill in ice retrievals, particularly for thin clouds, and the CoSMIR frequencies performing better for liquid. Additionally, we look at dual-polarized radiances observed by CoSMIR during the first two IMPACTS deployments to understand the polarization signatures induced by oriented hydrometeors. Results will be presented in the context of upcoming missions and sensors including AOS and the Ice Cloud Imager (ICI). We will describe the objectives for the expected first flight of the newly upgraded CoSSIR during the final IMPACTS deployment, and we will share novel science investigations we plan to undertake with CoSSIR's new capabilities. Popular Summary: Ice in clouds and falling snow is an important component of weather, climate, and water resources. To better use a new class of sensors that provide information on atmospheric ice, we developed an approach to measure ice clouds and falling snow using airborne data taken during the Investigation of Microphysics and Precipitation for Atlantic Coast-Threatening Storms (IMPACTS), a field campaign to study winter storms. We look at the results for two similar instruments to understand how those differences affect these measurements of clouds and snow, and we further investigate the information the sensors can provide on properties of the clouds and snow.

Ian S Adams↗

NASA NTRS1992

Potential pressurized payloads: Fluid and thermal experiments

Space Station Freedom (SSF) presents the opportunity to perform long term fluid and thermal experiments in a microgravity environment. This presentation provides perspective on the need for fluids/thermal experimentation in a microgravity environment, addresses previous efforts, identifies possible experiments, and discusses the capabilities of a proposed fluid physics/dynamics test facility. Numerous spacecraft systems use fluids for their operation. Thermal control, propulsion, waste management, and various operational processes are examples of such systems. However, effective ground testing is very difficult. This is because the effect of gravity induced phenomena, such as hydrostatic pressure, buoyant convection, and stratification, overcome such forces as surface tension, diffusion, electric potential, etc., which normally dominate in a microgravity environment. Hence, space experimentation is necessary to develop and validate a new fluid based technology. Two broad types of experiments may be performed on SSF: basic research and applied research. Basic research might include experiments focusing on capillary phenomena (with or without thermal and/or solutal gradients), thermal/solutal convection, phase transitions, and multiphase flow. Representative examples of applied research might include two-phase pressure drop, two-phase flow instabilities, heat transfer coefficients, fluid tank fill/drain, tank slosh dynamics, condensate removal enhancement, and void formation within thermal energy storage materials. In order to better support such fluid/thermal experiments on board SSF, OSSA has developed a conceptual design for a proposed Fluid Physics/Dynamics Facility (FP/DF). The proposed facility consists of one facility rack permanently located on SSF and one experimenter rack which is changed out as needed to support specific experiments. This approach will minimize the on-board integration/deintegration required for specific experiments. The FP/DF will have acceleration/vibration compensation, power and thermal interfaces, computer command/data collection, a video imaging system, and a portable glove box for operations. This facility will allow real-time astronaut interaction with the testing.

Swanson, Theodore D.↗

NASA NTRS1976

The formation of Saturn's satellites and rings, as influenced by Saturn's contraction history

The paper investigates constraints imposed on the ice content of Saturn's satellites and rings by the planet's high luminosity during the early part of its quasi-equilibrium contraction phase. It is assumed that the addition of ices to the satellites was not completed until after the start of the quasi-equilibrium contraction and that the condensation of ices ceased at the same time within the primordial nebulae of Jupiter and Saturn. Using previously derived limits on the time of condensation cessation for Jupiter's system, the following tentative conclusions are made: (1) Titan is the innermost satellite at whose position a methane-containing ice could condense; (2) water ice could have condensed at the positions of all the satellites; (3) the systematic decrease in the mass of the regular satellites with decreasing distance from the planet may have been caused, in part, by the larger time intervals, for the closer satellites, between the start of contraction and the first condensation of ices at their positions; and (4) ammonia ices, primarily NH4SH, were able to condense at the positions of all but the innermost satellites. It is also shown that water ice could have condensed in the region of the rings near the end of the condensation period.

Pollack, J. B.↗

NASA NTRS1985

Volatiles on satellites of the outer solar system

Molecules of cosmochemically abundant elements can act as volatiles and hence play a dominant role in the climatic and surficial evolution of solid bodies. Examples on terrestrial planets are H2O on Earth and H2O and CO2 on Mars. Analogous processes in the outer solar system focussing on CH4, its associated hydrocarbons, and N2 on Titan and Triton, the large moons of Saturn and Neptune were explored. A kilometer-deep C2H6-CH4 ocean was proposed for the surface of Titan to reconcile data on the lower atmosphere with understanding of the photochemical conversion of methane to heavier hydrocarbons. If such ocean exists, then it has dissolved in it an amount of N2 equal to the present atmospheric abundance. Since N2 contributes with CH4 a substantial greenhouse effect, the atmospheric physical and chemical characteristics are strongly coupled to those of the ocean, which change with time as methane is photolyzed in the stratosphere. Some relationship exists to the runaway greenhouse model for primordial Venus and the possible climatic implications of the buffering of Earth's atmospheric CO2 by the oceans. Two important diagnostics, measurable in Titan's atmosphere, of the conditions under which icy satellites formed are the abundances of noble gases and the CHd/CH4 radio. Both of these indicators have been altered during the evolution of Titan's surface-atmosphere system, the former by interaction with the ocean and the latter by progressive photolysis of methane into heavier hydrocarbons. The physical state and composition of volatiles on the surface of Triton is controversial, but plausibly could include CH4 N2 and perhaps CO. If condensed CH4 and N2 are widespread, their transformation to and from the vapor phase dominates the surface energy balance with sunlight. The extreme seasonal modulation of subsolar latitude on Triton is thus primarily expressed by volatile transport rather than large teperature changes, with possibly drastic observational consequences. The presence of two volatile species differing greatly in their vapor pressures make Triton a crude analog of Mars. Triton might be more appropriately regarded as a deep-freeze version of Titan.

Lunine, J. I.↗

NASA NTRS1999

Ignition and Combustion of Bulk Metals in a Microgravity Environment

Results of a study of heterogeneous and homogeneous combustion of metals in reduced gravity are presented. Cylindrical titanium and magnesium samples are radiatively ignited in pure-oxygen at 1 atm. Qualitative observations, propagation rates, and burning times are extracted from high-speed cinematography. Time-resolved emission spectra of gas-phase reactions are acquired with an imaging spectrograph. Lower propagation rates of the reacting mass on titanium and of ignition waves on magnesium are obtained at reduced gravity. These rates are compared to theoretical results from fire-spread analyses with a diffusion/convection controlled reaction. The close agreement found between experimental and theoretical propagation rates indicates the strong influence of natural-convection-enhanced oxygen transp6rt on burning rates. Lower oxygen flux and lack of condensed product removal appear to be responsible for longer burning times of magnesium gas-phase diffusion flames in reduced gravity. Spherically symmetric explosions in magnesium flames at reduced gravity (termed radiation-induced metal explosions, or RIME) may be driven by increased radiation heat transfer from accumulated condensed products to an evaporating metal core covered by a porous, flexible oxide coating. In titanium specimens, predominantly heterogeneous burning characterizes the initial steady propagation of the molten mass, while homogeneous gas-phase reactions are detected around particles ejected from the molten mixture. In magnesium specimens, band and line reversal of all the UV spectral systems of Mg and MgO are attributed to the interaction between small oxide particles and the principal gaseous emitters.

Branch, Melvyn C.↗

NASA NTRS2003

The I-Xe Age of Orgueil Magnetite: New Results

I-Xe ages of Murchison and Orgueil magnetites were reported to be the oldest [1] and interpreted as the condensation time of the solar nebula. More recent measurements, conducted on a highly magnetic separate from Orgueil (but not pure magnetite), gave much younger I-Xe ages [2]. We have since performed new studies on two pure separates of Orgueil magnetite, confirming the later closing time of the I-Xe system in this mineral phase. In the previous work of Lewis and Anders [1] special attention was paid to the purity of the analyzed material. It was shown, that the trapped Xe resided mostly in hydrated silicates and the radiogenic 129Xe in magnetite [3]. Therefore, Orgueil was finely ground and stirred with a saturated LiCl solution for 8 days at 60 C to remove the silicate-magnetite intergrowth. Although this procedure yields magnetic fractions that are at least 90% pure [1], it could potentially contaminate the magnetite with iodine and produce noncorrelated 128Xe and spurious I-Xe ages. To avoid this possibility, in our first work with Orgueil we deliberately omitted separation in LiCl solution. Instead, the meteorite was ground into a fine powder and the highly magnetic fraction was separated with a hand magnet and was confirmed to be largely magnetite [2]. The new work, reported here, was done in order to confirm our previous results and investigate the effects of the LiCl treatment on the I-Xe system in magnetite.

Pravdivtseva, O. V.↗

NASA NTRS2003

Proposed Space Flight Experiment Hardware

The primary thrust for this plan is to develop design tools and fundamental understanding that are timely and consistent with the goal of the various exploration initiatives. The plan will utilize ISS facilities, such as the Fluids Integrated Rack (FIR) and the Microgravity Science Glovebox (MSG). A preliminary flow schematic of Two-Phase Flow Facility (T(phi)FFy) which would utilize FIR is shown in Figure 3. MSG can be utilized to use the Boiling eXperiment Facility (BXF) and Contact Line Dynamics Experiment (CLiDE) Facility. The T(phi)FFy system would have multiple test sections whereby different configurations of heat exchangers could be used to study boiling and condensation phenomena. The test sections would be instrumented for pressure drop, void fraction, heat fluxes, temperatures, high-speed imaging and other diagnostics. Besides a high-speed data acquisition system with a large data storage capability, telemetry could be used to update control and test parameters and download limited amounts of data. In addition, there would be multiple accumulators that could be used to investigate system stability and fluid management issues. The system could accommodate adiabatic tests through either the space station nitrogen supply or have an experiment-specific compressor to pressurize a sufficient amount of air or other non-condensable gas for reuse as the supply bottle is depleted.

Source record↗

NASA NTRS2013

Silicon Heat Pipe Array

Improved methods of heat dissipation are required for modern, high-power density electronic systems. As increased functionality is progressively compacted into decreasing volumes, this need will be exacerbated. High-performance chip power is predicted to increase monotonically and rapidly with time. Systems utilizing these chips are currently reliant upon decades of old cooling technology. Heat pipes offer a solution to this problem. Heat pipes are passive, self-contained, two-phase heat dissipation devices. Heat conducted into the device through a wick structure converts the working fluid into a vapor, which then releases the heat via condensation after being transported away from the heat source. Heat pipes have high thermal conductivities, are inexpensive, and have been utilized in previous space missions. However, the cylindrical geometry of commercial heat pipes is a poor fit to the planar geometries of microelectronic assemblies, the copper that commercial heat pipes are typically constructed of is a poor CTE (coefficient of thermal expansion) match to the semiconductor die utilized in these assemblies, and the functionality and reliability of heat pipes in general is strongly dependent on the orientation of the assembly with respect to the gravity vector. What is needed is a planar, semiconductor-based heat pipe array that can be used for cooling of generic MCM (multichip module) assemblies that can also function in all orientations. Such a structure would not only have applications in the cooling of space electronics, but would have commercial applications as well (e.g. cooling of microprocessors and high-power laser diodes). This technology is an improvement over existing heat pipe designs due to the finer porosity of the wick, which enhances capillary pumping pressure, resulting in greater effective thermal conductivity and performance in any orientation with respect to the gravity vector. In addition, it is constructed of silicon, and thus is better suited for the cooling of semiconductor devices.

Yee, Karl Y.↗

NASA NTRS1999

Adsorption processes in spacecraft environmental control and life support systems

The environmental control and life support system on a spacecraft maintains a safe and comfortable environment in which the crew can live and work by supplying oxygen and water and by removing carbon dioxide, water vapor, and trace contaminants from cabin air. Although open-loop systems have been used successfully in the past for short-duration missions, the economics of current and future long-duration missions in space will make nearly complete recycling of air and water imperative. A variety of operations will be necessary to achieve the goal of nearly complete recycling. These include separation and reduction of carbon dioxide, removal of trace gas-phase contaminants, recovery and purification of humidity condensate, purification and polishing of wastewater streams, and others. Several of these can be performed totally or in part by adsorption processes. These processes are good candidates to perform separations and purifications in space due to their gravity independence, high reliability, relative high energy efficiency, design flexibility, technological maturity, and regenerative nature. For these reasons, adsorption has historically played a key role in life support on U.S. and Russian piloted spacecraft. Among the life support applications that can be achieved through use of adsorption technology are removal of trace contaminants and carbon dioxide from cabin air and recovery of potable water from waste streams. In each of these cases adsorption technology has been selected for use onboard the International Space Station. The requirements, science, and hardware for these applications are discussed. Human space exploration may eventually lead to construction of planetary habitats. These habitats may provide additional opportunities for use of adsorption processes, such as control of greenhouse gas composition, and may have different resources available to them, such as gases present in the planetary atmosphere. Separation and purification processes based on adsorption can be expected to continue to fulfill environmental control and life support needs on future missions.

Review, Tutorial↗

DOE OSTI2025

Phase Diagram of the Easy-Axis Triangular-Lattice 𝐽 1 −𝐽 2 Model

Our work studies the largely unexplored phase diagram of the S = 1/2 easy-axis triangular-lattice J 1 -J 2 model, motivated by recent interest in rare-earth and transition-metal compounds that exhibit strong quantum fluctuations and broad spin excitation continua—hallmarks of spin-liquid behavior. Combining density-matrix renormalization group simulations with analytical insights, we present a comprehensive study of the model that describes these materials. Our results provide compelling evidence for a robust spin-liquid phase stabilized between the exotic supersolid Y phase and the collinear stripe phase, remarkably persistent even in the presence of symmetry-breaking anisotropy. Additionally, we analyze the supersolid Y phase, offering a quantitative characterization of its order parameters and clarifying the surprising absence of a ferromagnetic moment; both features relevant to recent experiments on Ising-like triangular-lattice magnets. Altogether, our work provides the necessary framework and important theoretical guidance to the ongoing searches of the spin liquid and other exotic states in the rare-earth and transition-metal triangular-lattice compounds, as well as for advancing the understanding of anisotropic-exchange magnets.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2026

Disentangling High Harmonic Generation from Surface and Bulk States of a Topological Insulator

The discovery of topological phases has introduced a new dimension to materials science. Three-dimensional (3D) topological insulators (TIs) are a remarkable class of matter that is insulating in the bulk while hosting conductive topological surface states (TSSs) with unique charge and spin properties. High-order harmonic generation (HHG) has emerged as a powerful tool to probe condensed matter systems by providing insights into their electronic structure and dynamic behavior. Here, we investigate HHG in the prototype 3D-TI Bi$_2$Se$_3$. We demonstrate that the contributions of bulk and surface states to the harmonic emission can be controlled by tuning the thickness of thin film samples. An ultrathin (6 nm) film substantially enhances HHG from the surface states, while the bulk states dominate HHG in a thicker (50 nm) film. By applying a quasi-static terahertz perturbing field, we disentangle the bulk and surface responses and reveal the significant impact of the surface states' shift vector and Berry curvature on HHG. Our study provides effective methods for isolating the optical responses of TSSs from those of the bulk, which opens the door to resolving an ongoing debate regarding whether it is possible to reliably extract topological signatures in HHG.

Atomic Physics (physics.atom-ph)↗

DOE OSTI2024

Observation-constrained kinetic modeling of isoprene SOA formation in the atmosphere

Isoprene has the largest global non-methane hydrocarbon emission, and the oxidation of isoprene plays a crucial role in the formation of secondary organic aerosol (SOA). Two primary processes are known to contribute to SOA formation from isoprene oxidation: (1) the reactive uptake of isoprene-derived epoxides on acidic or aqueous particle surfaces and (2) the absorptive gas–particle partitioning of low-volatility oxidation products. In this study, we developed a new multiphase condensed isoprene oxidation mechanism that includes these processes with key molecular intermediates and products. The new mechanism was applied to simulate isoprene gas-phase oxidation products and SOA formation from previously published chamber experiments under a variety of conditions and atmospheric observations during the Southern Oxidant and Aerosol Studies (SOAS) field campaign. Our results show that SOA formation from most of the chamber experiments is reasonably reproduced using our mechanism, except when the concentration ratios of initial nitric oxide to isoprene exceed ~ 2, the formed SOA is significantly underpredicted. The SOAS simulations also reasonably agree with the measurements regarding the diurnal pattern and concentrations of different product categories, while the total isoprene SOA remains underestimated. The molecular compositions of the modeled SOA indicate that multifunctional low-volatility products contribute to isoprene SOA more significantly than previously thought, with a median mass contribution of ~ 57 % to the total modeled isoprene SOA. However, this contribution is intricately intertwined with IEPOX-derived SOA (IEPOX: isoprene-derived epoxydiols), posing challenges for their differentiation using bulk aerosol composition analysis (e.g., the aerosol mass spectrometer with positive matrix factorization). Furthermore, the SOA from these pathways may vary greatly, mainly dependent on the volatility estimation and treatment of particle-phase processes (i.e., photolysis and hydrolysis). Our findings emphasize that the various pathways to produce these low-volatility species should be considered in models to more accurately predict isoprene SOA formation. The new condensed isoprene chemical mechanism can be further incorporated into regional-scale air quality models, such as the Community Multiscale Air Quality Modelling System (CMAQ), to assess isoprene SOA formation on a larger scale.

54 ENVIRONMENTAL SCIENCES↗