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DOE OSTI2019

In Situ TEM Study of the Amorphous-to-Crystalline Transition during Dielectric Breakdown in TiO 2 Film

Dielectric breakdown of oxides is a main limiting factor for improvement of the performance of electronic devices. Present understanding suggests that defects produced by intense voltage accumulate in the oxide to form a percolation path connecting the two electrodes and trigger the dielectric breakdown. However, reports on directly visualizing the process at nanoscale are very limited. Here, we apply in situ transmission electron microscopy to characterize the structural and compositional changes of amorphous TiO 2 under extreme electric field (~100 kV/mm) in a Si/TiO 2 /W system. Upon applying voltage pulses, the amorphous TiO 2 gradually transformed to crystalline sub-stoichiometric rutile TiO 2-x and the Magnéli phase Ti 3 O 5 . The transitions started fromat the anode/oxide interface under both field polarities. Preferred growth orientation Epitaxial growth of rutile TiO 2-x with respect toon the Si substrate was observed when Si was the anode, while oxidation and melting of the W probe occurred when W was the anode. We associate the TiO 2 crystallization process with the electrochemical reduction of TiO 2 , polarity-dependent oxygen migration, and Joule heating. The experimental results are supported by our phase-field modeling. These findings provide direct details of the defect formation process during dielectric breakdown in amorphous oxides and will help the design of electronic devices with higher efficiency and reliability.

36 MATERIALS SCIENCE↗

NASA NTRS2008

An Overview of the Impact of Energetic Particle Precipitation on the Mesosphere and Stratosphere

Energetic precipitating particles (EPPs) can cause significant constituent changes in the polar mesosphere and stratosphere (middle atmosphere) during certain periods. Both protons and electrons can influence the polar middle atmosphere through ionization and dissociation processes. EPPs can enhance HOx (H, OH, HO2) through the formation of positive ions followed by complex ion chemistry and NOx (N, NO, NO2) through the dissociation of molecular nitrogen. The HO, increases can lead to ozone destruction in the mesosphere and upper stratosphere via several catalytic loss cycles. Such middle atmospheric HOx,-caused ozone loss is rather short-lived due to the relatively short lifetime (hours) of the HOx constituents. The HOx,-caused ozone depletion has been observed during several solar proton events (SPEs) in the past 40 years. HOx enhancements due to SPEs were confirmed by observations in the past solar cycle. A number of modeling studies have been undertaken over this time period that show predictions of enhanced HO, accompanied by decreased ozone due to energetic particles. The NO, family has a longer lifetime than the HOx family and can also lead to catalytic ozone destruction. EPP-caused enhancements of the NOx family can affect ozone promptly, if produced in the stratosphere, or subsequently, if produced in the 1ow.er thermosphere or mesosphere and transported to the stratosphere. NOx enhancements due to auroral electrons, medium and high energy electrons, relativistic electron precipitation (REP) events, and SPEs have been measured and/or modeled for decades Only a small number of SPEs (less than 10) in each solar cycle have sufficient flux of high energy protons (greater than 30 MeV) to produce a significant amount of NOx directly in the stratosphere to cause a measurable ozone destruction. Very high energy electrons (greater than 1500 keV) during REP events can also produce NOx directly in the stratosphere, however, the frequency and intensity of these electrons is uncertain. Indirect stratospheric EPP effects result when NO, is produced in the mesosphere and lower thermosphere and transported to the stratosphere during the late fall or winter. Such EPP-produced NOx may last up to months beyond its initial production. This EPP-produced mesospheric and lower thermospheric NOx primarily results from auroral electrons (approx. 1- 30 keV), medium- and high-energy electrons (approx. 30-1500 keV), and medium energy protons (approx. 1-30 MeV). The EPP-caused direct and indirect effects on the stratosphere are important in the polar regions during particular years, especially near solar maximum. This talk will attempt to provide an overview of several of the EPP-related important processes and their impact on the mesosphere and stratosphere. Much progress has been made in this field in the past several years and it is anticipated that other workshop participants will address aspects of this topic in their presentations.

Jackman, Charles H.↗

NASA NTRSDate not supplied

New insights into PSCs from the nearly 17-year CALIPSO data record

Polar stratospheric clouds (PSCs) play important roles in stratospheric ozone depletion during winter and spring at high latitudes (e.g., the Antarctic ozone hole). PSC particles provide sites for heterogeneous reactions that convert stable chlorine reservoir species to radicals that destroy ozone catalytically. PSCs also prolong ozone depletion by delaying chlorine deactivation through the removal of gas-phase HNO3 and H2O by sedimentation of large nitric acid trihydrate (NAT) and ice particles. A more complete picture of PSC processes on vortex-wide scales has emerged from the CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) instrument on the CALIPSO satellite that has been observing PSCs at latitudes up to 82 degrees in both hemispheres since June 2006. This nearly 17-year data record has fundamentally improved our knowledge of PSC spatial and temporal distributions, composition, and formation processes. In this presentation, we provide a brief overview of the CALIOP PSC data record and highlight some of the recent advances in our understanding of PSC processes.

polar stratospheric clouds↗

DOE OSTI2018

Modulation of the Photophysical Properties of β-substituted BODIPY Dyes

Photophysical properties of BODIPY dyes containing acetyl acetone and benzoyl acetone BF2 unit as an electron accepting substituent at beta position linked via double bond have been investigated using a wide range of solvents of different polarities. The substitution effect at beta position of the BODIPY dyes on their absorption, emission and quantum yield of fluorescence have been the aim of present study. For the synthesized BODIPY dyes fluorescence quantum yields and lifetimes show very sharp decrease with an increase in the solvent polarity, suggesting the involvement of highly polar ICT state de-excitation mechanism along with the local excitation process. The polarity dependent changes in average fluorescence life time and quantum yield values rationalize the formation of ICT states.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2022

Failure analysis of solid oxide fuel cells nickel-yttria stabilized zirconia anode under siloxane contamination

In this study, the failure process of the solid oxide fuel cell (SOFC) Ni-yttria-stabilized zirconia (YSZ) anode is investigated with D4 siloxane (octamethylcyclotetrasiloxane) contamination. In order to evaluate the influence of the electrochemical reaction on the siloxane deposition process, the SOFC experiments were operated at open circuit voltage (OCV) and 50 mA cm -2 conditions at 800°C. During the failure process, electrochemical, morphology and exhaust gas component analysis testing are conducted at the critical points. An equivalent circuit model and corresponding microstructure parameter calculations for separated physicochemical processes were utilized for the quantitative analysis of the failure process. Further, the results confirm the siloxane chemical adsorption deposition mechanism proposed in previous work. As a result, the failure of the anode was attributed to the gas diffusion blockage by dense silicon dioxide layer formation. The anode failure process with siloxane contamination is faster when the anode is operated under polarization.

25 ENERGY STORAGE↗

DOE OSTI2022

Ozone depletion in the Arctic and Antarctic stratosphere induced by wildfire smoke

Abstract. A record-breaking stratospheric ozone loss was observed over the Arctic and Antarctica in 2020. Strong ozone depletion occurred over Antarctica in 2021 as well. The ozone holes developed in smoke-polluted air. In this article, the impact of Siberian and Australian wildfire smoke (dominated by organic aerosol) on the extraordinarily strong ozone reduction is discussed. The study is based on aerosol lidar observations in the North Pole region (October 2019–May 2020) and over Punta Arenas in southern Chile at 53.2∘ S (January 2020–November 2021) as well as on respective NDACC (Network for the Detection of Atmospheric Composition Change) ozone profile observations in the Arctic (Ny-Ålesund) and Antarctica (Neumayer and South Pole stations) in 2020 and 2021. We present a conceptual approach on how the smoke may have influenced the formation of polar stratospheric clouds (PSCs), which are of key importance in the ozone-depleting processes. The main results are as follows: (a) the direct impact of wildfire smoke below the PSC height range (at 10–12 km) on ozone reduction seems to be similar to well-known volcanic sulfate aerosol effects. At heights of 10–12 km, smoke particle surface area (SA) concentrations of 5–7 µm2 cm−3 (Antarctica, spring 2021) and 6–10 µm2 cm−3 (Arctic, spring 2020) were correlated with an ozone reduction in terms of ozone partial pressure of 0.4–1.2 mPa (about 30 % further ozone reduction over Antarctica) and of 2–3.5 mPa (Arctic, 20 %–30 % reduction with respect to the long-term springtime mean). (b) Within the PSC height range, we found indications that smoke was able to slightly increase the PSC particle number and surface area concentration. In particular, a smoke-related additional ozone loss of 1–2 mPa (10 %–20 % contribution to the total ozone loss over Antarctica) was observed in the 14–23 km PSC height range in September–October 2020 and 2021. Smoke particle number concentrations ranged from 10 to 100 cm−3 and were about a factor of 10 (in 2020) and 5 (in 2021) above the stratospheric aerosol background level. Satellite observations indicated an additional mean column ozone loss (deviation from the long-term mean) of 26–30 Dobson units (9 %–10 %, September 2020, 2021) and 52–57 Dobson units (17 %–20 %, October 2020, 2021) in the smoke-polluted latitudinal Antarctic belt from 70–80∘ S.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2012

An Overview of Energetic Particle Precipitation Effects on the Earth's Atmosphere and (Potentially) Climate

Energetic precipitating particles (EPPs) can cause significant constituent changes in the polar mesosphere and stratosphere (middle atmosphere) during certain periods. Both protons and electrons can influence the polar middle atmosphere through ionization and dissociation processes. EPPs can enhance HOx (H, OH, HO2) through the formation of positive ions followed by complex ion chemistry and NOx (N, NO, NO2) through the dissociation of molecular nitrogen. The solar EPP-created HOx increases can lead to ozone destruction in the mesosphere and upper stratosphere via several catalytic loss cycles. Such middle atmospheric HOx-caused ozone loss is rather short-lived due to the relatively short lifetime (hours) of the HOx constituents. The HOx-caused ozone depletion of greater than 30% has been observed during several large solar proton events (SPEs) in the past 50 years. HOx enhancements due to SPEs were confirmed by observations in solar cycle 23. A number of modeling studies have been undertaken over this time period that show predictions of enhanced HOx accompanied by decreased ozone due to energetic particles. The solar EPP-created NOx family has a longer lifetime than the HOx family and can also lead to catalytic ozone destruction. EPP-caused enhancements of the NOx family can affect ozone promptly, if produced in the stratosphere, or subsequently, if produced in the lower thermosphere or mesosphere and transported to the stratosphere. NOx enhancements due to auroral electrons, medium and high energy electrons, relativistic electron precipitation (REP) events, and SPEs have been measured and/or modeled for decades. Model predictions and measurements show that certain years have significant winter-time meteorological events, which result in the transport of EPP-caused NOx enhancements in the upper mesosphere and lower thermosphere to lower altitudes. The NOx-caused ozone depletion has also been observed during several solar proton events (SPEs) in the past 50 years. Model predictions indicate that the longer-lived SPE-caused polar stratospheric and mesospheric ozone decrease can be >10% for up to five months past the largest events and is statistically significant; however, total ozone measurements do not indicate any long-term SPE impact.

Jackman, Charles H.↗

DOE OSTI2019

A new method to trace three-dimensional magnetic field structure within molecular clouds using dust polarization

The complete three-dimensional structure of the magnetic field within molecular clouds has eluded determination despite its high value in determining controlling factors in the star formation process, as it cannot be directly probed observationally. Considering that inclination of the magnetic field relative to the plane of sky is one of the major sources of depolarization of thermal emission from dust in molecular clouds, we propose a new method to estimate the inclination angle of the cloud-scale magnetic field based on the statistical properties of the observed polarization fraction. We test this method using a series of Monte Carlo experiments and find that the method works well, provided that deviations of magnetic field direction from the averaged values are small. When applied to synthetic observations of numerical simulations of star-forming clouds, our method gives fairly accurate measurements of the mean magnetic field inclination angle (within 10°–25°), which can further be improved if we restrict our technique to regions of low dispersion in polarization angles S. We tested our method on the BLASTPol polarimetric observations of the Vela C molecular cloud complex, which suggests that the magnetic field of Vela C has a high inclination angle (~60°), consistent with previous analyses.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS2015

9+ Years of CALIOP PSC Data: An Evolving Climatology

Polar stratospheric clouds (PSCs) play key roles in the springtime chemical depletion of ozone at high latitudes. PSC particles provide sites for heterogeneous chemical reactions that transform stable chlorine and bromine reservoir species into highly reactive ozone-destructive forms. Furthermore, large nitric acid trihydrate (NAT) PSC particles can irreversibly redistribute odd nitrogen through gravitational sedimentation, which prolongs the ozone depletion process by slowing the reformation of the stable chlorine reservoirs. However, there are still significant gaps in our understanding of PSC processes, particularly concerning the details of NAT particle formation. Spaceborne observations from the CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) lidar on the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) satellite are providing a rich new dataset for studying PSCs on unprecedented vortex-wide scales. In this paper, we examine the vertical and spatial distribution of PSCs in the Antarctic and Arctic on vortex-wide scales for entire PSC seasons over the more than nine-year data record.

Pitts, Michael C.↗

NASA NTRS1992

The polar layered deposits on Mars: Inference from thermal inertia modeling and geologic studies

It is widely believed that the Martian polar layered deposits record climate variations over at least the last 10 to 100 m.y., but the details of the processes involved and their relative roles in layer formation and evolution remain obscure. Weathering of the Martian layered deposits by sublimation of water ice can account for the thermal inertias, water vapor abundances, and geologic relationships observed in the Martian polar regions. The nonvolatile components of the layered deposits appears to consist mainly of bright red dust, with small amounts of dark dust. Dark dust, perhaps similar to the magnetic material found at the Viking Lander sites, may preferentially form filamentary residue particles upon weathering of the deposits. Once eroded, these particles may saltate to form the dark dunes found in both polar regions. This scenario for the origin and evolution of the dark material within the polar layered deposits is consistent with the available imaging and thermal data. Further experimental measurements of the thermophysical properties of magnetite and maghemite under Martian conditions are needed to better test this hypothesis.

Herkenhoff, K. E.↗

DOE OSTI2025

Ultrafast Electron–Dipole Interactions in TeO- Photodetachment

We present direct experimental evidence of ultrafast coupling between ejected electrons and dynamically forming dipole moments in TeO, captured during the photodetachment of TeO?. By combining high-resolution cryogenic photoelectron spectroscopy with velocity-map imaging, we assess previously inaccessible excited states and resolve rich photoelectron angular distributions (PADs) that encode electron–dipole interactions. Systematic comparison of PADs from femtosecond and picosecond lasers reveals striking deviations from free-electron behavior, representing direct evidence of a transient dipole moment evolving on femtosecond timescales. Quantitative analysis pinpoints the dipole buildup time to be within ~60 fs, providing real-time access to the birth of a molecular dipole field. This work establishes a general approach to probing electron-dipole interactions in their formation stages, offering fundamental insights into the ultrafast interplay between departing electrons and transient polar systems — a process that lies at the core of atomic, molecular, and ultrafast physics.

Yang, Fan↗

NASA NTRS2011

Direct EPP Affects on the Middle Atmosphere

Energetic precipitating particles (EPPs) can cause significant direct constituent changes in the mesosphere and stratosphere (middle atmosphere) during certain periods. Both protons and electrons can influence the polar middle atmosphere through ionization and dissociation processes. EPPs can enhance HOx (H, OH, HO2) through the formation of positive ions followed by complex ion chemistry and NOx (N, NO, NO2) through the dissociation of molecular nitrogen. The HOx increases result in direct ozone destruction in the mesosphere and upper stratosphere via several catalytic loss cycles. Such middle atmospheric HOx-caused ozone loss is rather short-lived due to the relatively short lifetime (hours) of the HOx constituents. The NOx family has a considerably longer lifetime than the HOx family and can also lead to catalytic ozone destruction. EPP-caused enhancements of the NOx family can affect ozone directly, if produced in the stratosphere. Ozone decreases from the EPPs lead to a reduction in atmospheric heating and, subsequent atmospheric cooling. Conversely, EPPs can cause direct atmospheric heating through Joule heating. Measured HOx constituents OH and HO2 showed increases due to solar protons. Observed NOx constituents NO and NO2 were enhanced due to both solar protons and precipitating electrons. Other hydrogen- and nitrogen-ocntaining constituents were also measured to be directly influenced by EPPs, including N2O, HNO3, HO2NO2, N2OS, H2O2, ClONO2, HCl, and HOCl. Observed constituents ClO and CO were directly affected by EPPs as well. Many measurements indicated significant direct ozone decreases. A significant number of satellites housed instruments, which observed direct EPP-caused atmospheric effects, including Nimbus 4 (BUV), Nimbus 7 (SBUV), several NOAA platforms (SBUV/2), SME, UARS (HALOE, CLAES), SCISAT-1 (ACE-FTS), Odin (OSIRIS), Envisat-l (GOMOS, MIPAS, SCIAMACHY), and Aura (MLS). Measurements by rockets and ground-based radar also indicated EPP direct impacts. Atmospheric models have been used with some success in predicting the direct EPP impacts on the mesosphere and stratosphere. A review of the observed direct effects of EPP on the middle atmosphere will be given in this presentation.

Jackman, Charles H.↗

NASA NTRS2012

The Icebreaker Life Mission to Mars: A Search for Biomolecular Evidence for Life

The search for evidence of life on Mars is the primary motivation for the exploration of that planet. The results from previous missions, and the Phoenix mission in particular, indicate that the ice-cemented ground in the north polar plains is likely to be the most recently habitable place that is currently known on Mars. The near-surface ice likely provided adequate water activity during periods of high obliquity, ~ 5 Myr ago. Carbon dioxide and nitrogen is present in the atmosphere, and nitrates may be present in the soil. Perchlorate in the soil together with iron in basaltic rock provides a possible energy source for life. Furthermore, the presence of organics must once again be considered, as the results of the Viking GCMS are now suspect given the discovery of the thermally reactive perchlorate. Ground-ice may provide a way to preserve organic molecules for extended periods of time, especially organic biomarkers. The Mars Icebreaker Life mission focuses on the following science goals: 1. Search for specific biomolecules that would be conclusive evidence of life. 2. A general search for organic molecules in the ground ice. 3. Determine the processes of ground ice formation and the role of liquid water. 4. Understand the mechanical properties of the Mars polar ice-cemented soil. 5. Assess the recent habitability of the environment with respect to required elements to support life, energy sources, and possible toxic elements. And 6. Compare the elemental composition of the northern plains with mid-latitude sites. The Icebreaker Life payload has been designed around the Phoenix spacecraft and is targeted to a site near the Phoenix landing site. However, the Icebreaker payload could be supported on other Mars landing systems. Preliminary studies of the SpaceX Dragon lander show that it could support the Icebreaker payload for a landing either at the Phoenix site or at mid-latitudes. Duplicate samples could be cached as a target for possible return by a Mars Sample Return mission. If the samples were shown to contain organic biomarkers interest in returning them to Earth would be high.

Life detection↗

DOE OSTI2015

Solution Phase Exciton Diffusion Dynamics of a Charge-Transfer Copolymer PTB7 and a Homopolymer P3HT

Using ultrafast polarization-controlled transient absorption (TA) measurements, dynamics of the initial exciton states were investigated on the time scale of tens of femtoseconds to about 80 ps in two different types of conjugated polymers extensively used in active layers of organic photovoltaic devices. These polymers are poly(3-fluorothienothiophenebenzodithiophene) (PTB7) and poly-3-hexylthiophene (P3HT), which are charge-transfer polymers and homopolymers, respectively. In PTB7, the initial excitons with excess vibrational energy display two observable ultrafast time constants, corresponding to coherent exciton diffusion before the vibrational relaxation, and followed by incoherent exciton diffusion processes to a neighboring local state after the vibrational relaxation. In contrast, P3HT shows only one exciton diffusion or conformational motion time constant of 34 ps, even though its exciton decay kinetics are multiexponential. Based on the experimental results, an exciton dynamics mechanism is conceived taking into account the excitation energy and structural dependence in coherent and incoherent exciton diffusion processes, as well as other possible deactivation processes including the formation of the pseudo-charge-transfer and charge separate states, as well as interchain exciton hopping or coherent diffusion.

36 MATERIALS SCIENCE↗

NASA NTRS1981

Studies of high latitude current systems using MAGSAT vector data

The magnetic disturbance fields caused by global external current systems are considered with particular emphasis on improving the understanding of the physical processes which control high latitude current systems. Following processing the MAGSAT data were routinely plotted in the Universal Time (UT) format as well as in a polar plot format. The H'D'U' coordinate system, was adopted as the standard for representing the MAGSAT residual magnetic field vectors. A data file was generated and the TPOLAR computer code was developed to determine from the orbital elements, the time, latitude, and MLT of the extremum latitude of each transpolar segment of orbit. The precision of the vector data set from MAGSAT prompted an extended exploratory phase for data analysis procedures, modeling techniques and phenomenology.

Burrows, J. R.↗

NASA NTRS1989

Sand dune materials and polar layered deposits on Mars

The possible place of sand in the Martian polar layered deposits is examined. The erosional features in layered deposits and the morphologic relationship of dunes and the layered deposits are discussed. The colors of the polar dunes are shown to be similar to the colors of dunes at other latitudes, suggesting that the polar dunes can be explained without any special or exotic mechanism. Consideration is given to mixing and segregation of materials by eolian processes observed on Mars, showing that sand was probably carried to the polar regions during part of the formation of the layered deposits.

Thomas, Peter↗

NASA NTRS1994

Contributions of a Tunable Diode Laser Instrument (ATLAS) to the Stratospheric Ozone Depletion Question

The Airborne Tunable Laser Absorption Spectrometer - ATLAS - was designed and built at the NASA Ames Research Center and operates on the NASA ER-2 high altitude research aircraft. ATLAS has taken part in a number of important polar and mid-latitude research campaigns, since 1987, focused on various aspects of stratospheric ozone chemistry and dynamics. The chief measurement carried out by the ATLAS second harmonic diode laser spectrometer is of the important atmospheric tracer N2O. Using N2O as an inert tracer we have been able to gain significant new information on polar vortex dynamics and on the correlations of several important long-lived tracers in the stratosphere. The correlation of N2O with NOy (total reactive nitrogen) has been shown to be linear for a great variety of unperturbed stratospheric conditions, and the breakdown of this correlation has been used to detect denitrification by PSCs in the polar vortex, especially in the Antarctic spring. Denitrification is an important step in the process of ozone hole formation in the austral spring. Correlations of N2O with CFCs and CH4 have led to improved estimates of atmospheric lifetimes of these important molecules. Finally the correlation of N2O with CO2, the latter now being measured with great precision by a new instrument on the ER-2, has led to a significant new tool for studying horizontal and vertical mixing in the lower stratosphere, a tool which is very useful in assessing the potential effects of high speed civil transport aircraft in the lower stratosphere. A new, light-weight version of ATLAS is currently being built for unmanned high altitude aircraft, specifically the new Perseus vehicle. We will give a brief description of this effort.

Loewenstein, Max↗

NASA NTRS1982

Integrated optics technology study

The materials and processes available for the fabrication of single mode integrated electrooptical components are described. Issues included in the study are: (1) host material and orientation, (2) waveguide formation, (3) optical loss mechanisms, (4) wavelength selection, (5) polarization effects and control, (6) laser to integrated optics coupling,(7) fiber optic waveguides to integrated optics coupling, (8) souces, (9) detectors. The best materials, technology and processes for fabrication of integrated optical components for communications and fiber gyro applications are recommended.

Chen, B.↗