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DOE OSTI2026

GaN Core-shell Nanofin Vertical Transistor (CoNVerT): A New Direction for Power Electronics (Final Scientific/Technical Report)

A novel power transistor architecture, the GaN c ore-shell n anofin ver tical transistor (CoNVerT) to address fundamental challenges in realizing the ultimate limit of GaN power transistor performance was explored experimentally. This technology promises ultra-high-efficiency high voltage/high power applications (e.g. DC/DC converters, motor control, fast charging, actuation), as well as to operate in harsh environments. The device exploits a vertical superjunction structure based on an experimentally-validated core-shell nanofin growth process in which lateral p-n heterojunctions are formed in a single growth step, while still maintaining vertical current flow for compact die size and low cost. The concept leverages the best properties of GaN for mid-range voltage applications: high mobility, high breakdown voltage, and native heterojunction enhancement-mode operation. Due to the crystallographic nature of the nanofin growth by molecular beam epitaxy, the sidewall heterojunctions occur on non-polar planes, resulting in ultra-smooth interfaces for high mobility, no sidewall etch damage and related surface/interface states, and elimination of piezoelectric effects that can limit reliability in conventional structures. This also facilitates superjunction formation for maximum device performance, and the selective-area growth of the nanofin results in dislocation-free growth, even on low-cost Si (111) substrate. In this program, core-shell nanofins were grown by molecular beam epitaxy, test structures to evaluate the doping, resistivity, and other electrical properties were fabricated, and the material and test structures were characterized in detail. The work identified clear potential (e.g., the doping was well controlled as required for superjunction concepts), but also additional areas that require additional effort to resolve (some unexpected crystal defects were encountered that require additional engineering to overcome). Simulation studies of the proposed concept validate that the fundamental approach is very promising, but additional effort in experimental realization is needed.

42 ENGINEERING↗

DOE OSTI2015

Passivation dynamics in the anisotropic deposition and stripping of bulk magnesium electrodes during electrochemical cycling

Rechargeable magnesium (Mg) batteries show promise for use as a next generation technology for high-density energy storage, though little is known about the Mg anode solid electrolyte interphase and its implications for the performance and durability of a Mg-based battery. We explore in this report passivation effects engendered during the electrochemical cycling of a bulk Mg anode, characterizing their influences during metal deposition and dissolution in a simple, nonaqueous, Grignard electrolyte solution (ethylmagnesium bromide, EtMgBr, in tetrahydrofuran). Scanning electron microscopy images of Mg foil working electrodes after electrochemical polarization to dissolution potentials show the formation of corrosion pits. The pit densities so evidenced are markedly potential-dependent. When the Mg working electrode is cycled both potentiostatically and galvanostatically in EtMgBr these pits, formed due to passive layer breakdown, act as the foci for subsequent electrochemical activity. Detailed microscopy, diffraction, and spectroscopic data show that further passivation and corrosion results in the anisotropic stripping of the Mg {0001} plane, leaving thin oxide-comprising passivated side wall structures that demark the {0001} fiber texture of the etched Mg grains. Upon long-term cycling, oxide side walls formed due to the pronounced crystallographic anisotropy of the anodic stripping processes, leading to complex overlay anisotropic, columnar structures, exceeding 50 μm in height. Finally, the passive responses mediating the growth of these structures appear to be an intrinsic feature of the electrochemical growth and dissolution of Mg using this electrolyte.

36 MATERIALS SCIENCE↗

NASA NTRS2009

Evidence for Calcium Carbonate at the Phoenix Landing Site

The Phoenix mission has recently finished its study of the north polar environment of Mars with the aim to help understand both the current climate and to put constraints on past climate. An important part of understanding the past climate is the study of secondary minerals, those formed by reaction with volatile compounds such as H2O and CO2. This work describes observations made by the Thermal and Evolved-Gas Analyzer (TEGA) on the Phoenix Lander related to carbonate minerals. Carbonates are generally considered to be products of aqueous processes. A wet and warmer climate during the early history of Mars coupled with a much denser CO2 atmosphere are ideal conditions for the aqueous alteration of basaltic materials and the subsequent formation of carbonates. Carbonates (Mg- and Ca-rich) are predicted to be thermodynamically stable minerals in the present martian environment, however, there have been only a few indications of carbonates on the surface by a host of orbiting and landed missions to Mars. Carbonates (Mg-rich) have been suggested to be a component (2-5 wt %) of the martian global dust based upon orbital thermal emission spectroscopy. The identifications, based on the presence of a 1480 cm-1 absorption feature, are consistent with Mgcarbonates. A similar feature is observed in brighter, undisturbed soils by Mini-TES on the Gusev plains. Recently, Mg-rich carbonates have been identified in the Nili Fossae region by the CRISM instrument onboard the Mars Reconnaissance Orbiter. Carbonates have also been confirmed as aqueous alteration phases in martian meteorites so it is puzzling why there have not been more discoveries of carbonates by landers, rovers, and orbiters. Carbonates may hold important clues about the history of liquid water and aqueous processes on the surface of Mars.

Boynton, W. V.↗

NASA NTRS2010

Challenges in Transitioning Research Data to Operations: The SPoRT Paradigm

Established in 2002 to demonstrate the weather and forecasting application of real-time EOS measurements, the NASA Short-term Prediction Research and Transition (SPoRT) program has grown to be an end-to-end research to operations activity focused on the use of advanced NASA modeling and data assimilation approaches, nowcasting techniques, and unique high-resolution multispectral data from EOS satellites to improve short-term weather forecasts on a regional and local scale. With the ever-broadening application of real-time high resolution satellite data from current EOS and planned NPP, JPSS, and GOES-R sensors to weather forecast problems, significant challenges arise in the acquisition, delivery, and integration of the new capabilities into the decision making process of the operational weather community. For polar orbiting sensors such as MODIS, AIRS, VIIRS, and CRiS, the use of direct broadcast ground stations is key to the real-time delivery of the data and derived products in a timely fashion. With the ABI on the geostationary GOES-R satellite, the data volume will likely increase by a factor of 5- 10 from current data streams. However, the high data volume and limited bandwidth of end user facilities presents a formidable obstacle to timely access to the data. This challenge can be addressed through the use of subsetting techniques, innovative web services, and the judicious selection of data formats. Many of these approaches have been implemented by SPoRT for the delivery of real-time products to NWS forecast offices and other weather entities. Once available in decision support systems like AWIPS II, these new data and products must be integrated into existing and new displays that allow for the integration of the data with existing operational products in these systems. SPoRT is leading the way in demonstrating this enhanced capability. This paper will highlight the ways SPoRT is overcoming many of the challenges presented by the enormous data volumes of current and future satellite systems to get unique high quality research data into the operational weather environment.

Jedloved, Gary J.↗

NASA NTRS2013

SPoRT: Transitioning NASA and NOAA Experimental Data to the Operational Weather Community

Established in 2002 to demonstrate the weather and forecasting application of real-time EOS measurements, the NASA Short-term Prediction Research and Transition (SPoRT) program has grown to be an end-to-end research to operations activity focused on the use of advanced NASA modeling and data assimilation approaches, nowcasting techniques, and unique high-resolution multispectral data from EOS satellites to improve short-term weather forecasts on a regional and local scale. With the ever-broadening application of real-time high resolution satellite data from current EOS, Suomi NPP, and planned JPSS and GOES-R sensors to weather forecast problems, significant challenges arise in the acquisition, delivery, and integration of the new capabilities into the decision making process of the operational weather community. For polar orbiting sensors such as MODIS, AIRS, VIIRS, and CRiS, the use of direct broadcast ground stations is key to the real-time delivery of the data and derived products in a timely fashion. With the ABI on the geostationary GOES-R satellite, the data volumes will likely increase by a factor of 5-10 from current data streams. However, the high data volume and limited bandwidth of end user facilities presents a formidable obstacle to timely access to the data. This challenge can be addressed through the use of subsetting techniques, innovative web services, and the judicious selection of data formats. Many of these approaches have been implemented by SPoRT for the delivery of real-time products to NWS forecast offices and other weather entities. Once available in decision support systems like AWIPS II, these new data and products must be integrated into existing and new displays that allow for the integration of the data with existing operational products in these systems. SPoRT is leading the way in demonstrating this enhanced capability. This paper will highlight the ways SPoRT is overcoming many of the challenges presented by the enormous data volumes of current and future satellite systems to get unique high quality research data into the operational weather environment.

Jedlovec, Gary J.↗

DOE OSTI2016

RuO 2 nanoparticles supported on MnO 2 nanorods as high efficient bifunctional electrocatalyst of lithium-oxygen battery

RuO2 nanoparticles supported on MnO2 nanorods (denoted as np-RuO2/nr-MnO2) were synthesized via a two-step hydrothermal reaction. SEM and TEM images both illustrated that RuO2 nanoparticles are well dispersed on the surface of MnO2 nanorods in the as-prepared np-RuO2/nr-MnO2 material. Electrochemical results demonstrated that the np-RuO2/nr-MnO2 as oxygen cathode of Li-O-2 batteries could maintain a reversible capacity of 500 mA h g(-1) within 75 cycles at a rate of 50 mA g(-1), and a higher capacity of 4000 mA h g(-1) within 20 cycles at a rate as high as 200 mA g(-1). Moreover, the cell with the np-RuO2/nr-MnO2 catalyst presented much lower voltage polarization (about 0.58 V at a rate of 50 mA g(-1)) than that measured with only MnO2 nanorods during charge/discharge processes. The catalytic property of the np-RuO2/nr-MnO2 and MnO2 nanorods were further compared by conducting studies of using rotating disk electrode (RDE), chronoamperommetry and linear sweep voltammetry. The results illustrated that the np-RuO2/nr-MnO2 exhibited excellent bifunctional electrocatalytic activities towards both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Furthermore, in-situ high-energy X-ray diffraction was employed to trace evolution of species on the np-RuO2/nr-MnO2 cathode during the discharge processes. In-situ XRD patterns demonstrated the formation process of the discharge products that consisted of mainly Li2O2. Ex-situ SEM images were recorded to investigate the morphology and decomposition of the sphere-like Li2O2, which could be observed clearly after discharge process, while are decomposed almost after charge process. The excellent electrochemical performances of the np-RuO2/nr-MnO2 as cathode of Li-O-2 battery could be contributed to the excellent bifunctional electrocatalytic activities for both the ORR and OER, and to the one-dimensional structure which would benefit the diffusion of oxygen and the storage of Li2O2 in the discharge process of Li-O-2 battery.

Xu, Yue-Feng↗

DOE OSTI2018

X-Ray Line Polarization of Ne-Like Mo Spectra from X-pinch Plasmas

In this study, linearly polarized spectral emission is induced by non-Maxwellian electrons with anisotropic velocity distributions through collisional processes with ions in plasmas. X-ray line polarization is a viable diagnostic tool for the study of these electrons, which has been tested in controlled settings, e.g., the electron beam ion trap, but due to strong depolarization effects, has been relatively unexplored in laboratory-produced high-energy-density plasmas. This paper explores the X-ray line polarization for the study of Ne-like molybdenum X-pinch plasmas. Previous polarization studies have focused mostly on K-shell spectral lines, whereas the current paper expands on these studies by investigating L-shell line polarization. The X-pinch is favorable due to its high-density plasma formation, high radiation yield, fixed hotspot location, and reliable electron beam production. L-shell X-ray line polarization and spectral emission of Mo X-pinches were investigated through dual α-quartz (2d=6.687 Å) crystal spectropolarimetry with axial and radial spatial resolution. In particular, line polarization is evaluated through a comparative analysis of relative line intensities observed over a range of Ne-like Mo transitions simultaneously recorded with two spectrometers with different sensitivity to polarization. An appreciable degree of X-ray line polarization (up to 15%) is observed in the Ne-like Mo plasmas and analyzed using depolarization effects. Lastly, these results are the first polarization measurements in high-Z pulsed power plasmas.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

NASA NTRS1986

Circumstellar dust

The presence of dust in the general interstellar medium is inferred from the extinction, polarization, and scattering of starlight; the presence of dark nebulae; interstellar depletions; the observed infrared emission around certain stars and various types of interstellar clouds. Interstellar grains are subject to various destruction mechanisms that reduce their size or even completely destroy them. A continuous source of newly formed dust must therefore be present for dust to exist in the various phases of the interstellar medium (ISM). The working group has the following goals: (1) review the evidences for the formation of dust in the various sources; (2) examine the clues to the nature and composition of the dust; (3) review the status of grain formation theories; (4) examine any evidence for the processing of the dust prior to its injection into the interstellar medium; and (5) estimate the relative contribution of the various sources to the interstellar dust population.

Dwek, E.↗

DOE OSTI2014

Plant Root Characteristics and Dynamics in Arctic Tundra Ecosystems, 1960-2012

Plant roots play a critical role in ecosystem function in arctic tundra, but root dynamics in these ecosystems are poorly understood. To address this knowledge gap, we synthesized available literature on tundra roots, including their distribution, dynamics, and contribution to ecosystem carbon and nutrient fluxes, and we highlighted key aspects of their representation in terrestrial biosphere models. Across all tundra ecosystems, belowground plant biomass exceeded aboveground biomass, with the exception of polar desert tundra. Roots were shallowly-distributed in the thin layer of soil that thaws annually, and were often found in surface organic soil horizons. Root traits including distribution, chemistry, anatomy, and resource partitioning play an important role in controlling plant species competition, and therefore ecosystem carbon and nutrient fluxes, under changing climatic conditions, but have only been quantified for a small fraction of tundra plants. Further, the annual production and mortality of fine roots are key components of ecosystem processes in tundra, but extant data are sparse. Tundra root traits and dynamics should be the focus of future research efforts. Better representation of the dynamics and characteristics of tundra roots will improve the utility of models for evaluating the responses of tundra ecosystems to changing environmental conditions. Includes a data file in *.csv, and *.xlsx format and a *.pdf. The Next-Generation Ecosystem Experiments: Arctic (NGEE Arctic), was a research effort to reduce uncertainty in Earth System Models by developing a predictive understanding of carbon-rich Arctic ecosystems and feedbacks to climate. NGEE Arctic was supported by the Department of Energy's Office of Biological and Environmental Research. The NGEE Arctic project had two field research sites: 1) located within the Arctic polygonal tundra coastal region on the Barrow Environmental Observatory (BEO) and the North Slope near Utqiagvik (Barrow), Alaska and 2) multiple areas on the discontinuous permafrost region of the Seward Peninsula north of Nome, Alaska. Through observations, experiments, and synthesis with existing datasets, NGEE Arctic provided an enhanced knowledge base for multi-scale modeling and contributed to improved process representation at global pan-Arctic scales within the Department of Energy's Earth system Model (the Energy Exascale Earth System Model, or E3SM), and specifically within the E3SM Land Model component (ELM).

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2017

Polar Fluctuations in Metal Halide Perovskites Uncovered by Acoustic Phonon Anomalies

Solution-processable metal-halide perovskites (MHPs) offer great promise for efficient light harvesting and emitting devices due to their long carrier lifetime and superior carrier transport characteristics. Ferroelectric effects, a hallmark of traditional oxide perovskites, was proposed to be a mechanism to suppress carrier recombination and enhance charge transport in MHPs, but the existence and influence of such polar order is still of considerable debate. Here we performed transient reflection measurements on single crystals of both inorganic and organic-inorganic (hybrid) MHPs over a range of temperatures, and demonstrate significant phonon softening in the cubic phases close to the cubic-to-tetragonal phase transition temperatures. Such phonon softening indicates the formation of polar domains, which grow in size upon cooling and can persist in the low-temperature tetragonal and orthorhombic phases. Our results link the extraordinary electronic properties of MHPs to the spontaneous polarizations which can contribute to more efficient charge separation and characteristics of an indirect bandgap.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Optimizing minimum free-energy crossing points in solution: Linear-response free energy/spin-flip density functional theory approach

Examining photochemical processes in solution requires understanding the solvent effects on the potential energy profiles near conical intersections (CIs). For that purpose, the CI point in solution is determined as the crossing between nonequilibrium free energy surfaces. In this work, the nonequilibrium free energy is described using the combined method of linear-response free energy and collinear spin-flip time-dependent density functional theory. The proposed approach reveals the solvent effects on the CI geometries of stilbene in an acetonitrile solution and those of thymine in water. Polar acetonitrile decreases the energy difference between the twisted minimum and twisted-pyramidalized CI of stilbene. For thymine in water, the hydrogen bond formation stabilizes significantly the CI puckered at the carbonyl carbon atom. The result is consistent with the recent simulation showing that the reaction path via this geometry is open in water. Therefore, the present method is a promising way of identifying the free-energy crossing points that play an essential role in photochemistry of solvated molecules.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

Magnetic field control of microstructural development in melt-spun Pr 2 Co 14 B

In the processing of commercial rare earth permanent magnets, use of external magnetic fields is limited mainly to the alignment of anisotropic particles and the polarization of the finished magnets. Here we explore the effects of high magnetic fields on earlier stages of magnet synthesis, including the crystallization and chemical phase transformations that produce the 2:14:1 phase in the Pr-Co-B system. Pr 2 Co 14 B alloys produced by melt-spinning were annealed in the presence of strong applied magnetic fields (H=90 kOe). The resulting materials were characterized by x-ray diffraction, electron microscopy, and magnetization measurements. We find that magnetic fields suppress the nucleation and growth of crystalline phases, resulting in significantly smaller particle sizes. In addition, magnetic fields applied during processing strongly affects chemical phase selection, suppressing the formation of Pr 2 Co 14 B and α-Co in favor of Pr 2 Co 17 . Here, the results demonstrate that increased control over key microstructural properties is achievable by including a strong magnetic field as a processing parameter for rare-earth magnet materials.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Complete polarization of electronic spins in OLEDs

At low temperatures and high magnetic fields, electron and hole spins in an organic light-emitting diode become polarized so that recombination preferentially forms molecular triplet excited-state species. For low device currents, magnetoelectroluminescence perfectly follows Boltzmann activation, implying a virtually complete polarization outcome. As the current increases, the magnetoelectroluminescence effect is reduced because spin polarization is suppressed by the reduction in carrier residence time within the device. Under these conditions, an additional field-dependent process affecting the spin-dependent recombination emerges, possibly related to the build-up of triplet excitons and their interaction with free charge carriers. Suppression of the EL alone does not prove electronic spin polarization. We therefore probe changes in the spin statistics of recombination directly in a dual singlet-triplet emitting material, which shows a concomitant rise in phosphorescence intensity as fluorescence is suppressed. Finite spin-orbit coupling in these materials gives rise to a microscopic distribution in effective g-factors of electrons and holes, Δg, i.e., a distribution in Larmor frequencies. This Δg effect in the pair, which mixes singlet and triplet, further suppresses singlet-exciton formation at high fields in addition to thermal spin polarization of the individual carriers.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2016

MAGNETIC FLUX SUPPLEMENT TO CORONAL BRIGHT POINTS

Coronal bright points (BPs) are associated with magnetic bipolar features (MBFs) and magnetic cancellation. Here we investigate how BP-associated MBFs form and how the consequent magnetic cancellation occurs. We analyze longitudinal magnetograms from the Helioseismic and Magnetic Imager to investigate the photospheric magnetic flux evolution of 70 BPs. From images taken in the 193 Å passband of the Atmospheric Imaging Assembly (AIA) we dermine that the BPs’ lifetimes vary from 2.7 to 58.8 hr. The formation of the BP MBFs is found to involve three processes, namely, emergence, convergence, and local coalescence of the magnetic fluxes. The formation of an MBF can involve more than one of these processes. Out of the 70 cases, flux emergence is the main process of an MBF buildup of 52 BPs, mainly convergence is seen in 28, and 14 cases are associated with local coalescence. For MBFs formed by bipolar emergence, the time difference between the flux emergence and the BP appearance in the AIA 193 Å passband varies from 0.1 to 3.2 hr with an average of 1.3 hr. While magnetic cancellation is found in all 70 BPs, it can occur in three different ways: (I) between an MBF and small weak magnetic features (in 33 BPs); (II) within an MBF with the two polarities moving toward each other from a large distance (34 BPs); (III) within an MBF whose two main polarities emerge in the same place simultaneously (3 BPs). While an MBF builds up the skeleton of a BP, we find that the magnetic activities responsible for the BP heating may involve small weak fields.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS2019

Evaluation of Global Simulations of Aerosol Particle and Cloud Condensation Nuclei Number, with Implications for Cloud Droplet Formation

cloud droplets↗

DOE OSTI2020

Polaron and Spin Dynamics in Organic–Inorganic Lead Halide Perovskite Nanocrystals

Long-lived carrier population and spin-based behavior in lead halide perovskite nanocrystals (NCs) are very interesting for implementing photovoltaic devices with efficiencies exceeding the Shockley–Queisser limit and quantum information processing, respectively. However, a comprehensive understanding of polaron-mediated charge carrier interactions and an accurate description of the spin-polarized states for spintronics are still lacking. Herein, the carrier and spin interactions are studied under controlled conditions in FAPbI 3 and Cs 0.01 FA 0.99 Pb(Br 0.11 I 0.89 ) 3 NCs through ultrafast transient absorption (TA) spectroscopy. At early timescales, TA spectrum shows an asymmetric derivative feature originating from the hot carrier-induced spectral redshift in FAPbI 3 NCs (55 ± 3 meV) and Cs0.01FA0.99Pb(Br0.11I0.89)3 NCs (54 ± 2 meV) at the bandedges that stabilizes to 9 ± 1 and 11 ± 2 meV, respectively, at 1 ps due to the polaron formation. The kinetic analysis indicates that the polaron populations in FAPbI3 and Cs 0.01 FA 0.99 Pb(Br 0.11 I 0.89 ) 3 NCs decay with an average lifetime of 657 ± 34 and 532 ± 28 ps, respectively. The circular polarization-resolved TA reveals that polaron formation can control spin relaxation in NCs, thus providing a powerful tool to explore the development of their prospective applications in spintronics.

36 MATERIALS SCIENCE↗

DOE OSTI2019

Evaluation of global simulations of aerosol particle and cloud condensation nuclei number, with implications for cloud droplet formation

A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 model shave been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011–2015 are compared with aerosol measurements(aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan.The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal andshort-term variability in the aerosol properties. There is no single model that systematically performs best across all environments represented by the observations. Models tend to underestimate the observed aerosol particle and CCN number concentrations, with average normalized mean bias (NMB) of all models and for all stations, where dataare available, of –24% and –35% for particles with dry diameters <50 and <120 nm, as well as –36% and –34% for CCNat supersaturations of 0.2% and 1.0%, respectively. Yet, they seem to behave differently for particles activating at very low supersaturations (<0.1%) than at higher ones. A total of 15 models have been used to produce ensemble annual median distributions of relevant parameters. The model diversity (defined as the ratio of standard deviation to mean) is up to about 3 for simulated N 3 (number concentration of particles with dry diameters larger than 3 nm) and up to about 1 for simulated CCN in the extra-polar regions. A global mean reduction of a factor of about 2 is found in the model diversity for CCN at a supersaturation of 0.2% (CCN 0.2 ) compared to that for N 3 , maximizing over regions where new particle formation is important. An additional model has been used to investigate potential causes of model diversity in CCN and bias compared to the observations by performing a perturbed parameter ensemble (PPE) accounting for uncertainties in 26 aerosol-related model input parameters. This PPE suggests that biogenic secondary organic aerosol formation and the hygroscopic properties of the organic material are likely to be the major sources of CCN uncertainty in summer, with dry deposition and cloud processing being dominant in winter. Models capture the relative amplitude of the seasonal variability of the aerosol particle number concentration for all studied particle sizes with available observations (dry diameters larger than 50, 80 and 120 nm). The short-term persistence time (on the order of a few days) of CCN concentrations, which is a measure of aerosol dynamic behavior in the models, is underestimated o naverage by the models by 40% during winter and 20% in summer. In contrast to the large spread in simulated aerosol particle and CCN number concentrations, the CDNC derived from simulated CCN spectra is less diverse and in better agreement with CDNC estimates consistently derived from the observations (average NMB –13% and –22% for updraft velocities 0.3 and 0.6m s –1 , respectively). In addition, simulated CDNC is in slightly better agreement with observationally derived values at lower than at higher updraft velocities (index of agreement 0.64 vs. 0.65). The reduced spread of CDNC compared to that of CCN is attributed to the sublinear response of CDNC to aerosol particle number variations and the negative correlation between the sensitivities of CDNC to aerosol particle number concentration( ∂ N d / ∂ N a ) and to updraft velocity ( ∂ N d / ∂ w ). Overall, we find that while CCN is controlled by both aerosol particle number and composition, CDNC is sensitive to CCN at low and moderate CCN concentrations and to the updraft velocity when CCN levels are high. Discrepancies are found in sensitivities ∂ N d / ∂ N a and ∂ N d / ∂ w ; models may be predisposed to be too“aerosol sensitive” or “aerosol insensitive” in aerosol–cloud–climate interaction studies, even if they may capture average droplet numbers well.This is a subtle but profound finding that only the sensitivities can clearly reveal and may explain inter-model biases on the aerosol indirect effect.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2015

Ultrafast Multiphoton Pump-probe Photoemission Excitation Pathways in Rutile TiO2(110)

We investigate the spectroscopy and photoinduced electron dynamics within the conduction band of reduced rutile TiO2(110) surface by multiphoton photoemission (mPP) spectroscopy with wavelength tunable ultrafast (!20 fs) laser pulse excitation. Tuning the mPP photon excitation energy between 2.9 and 4.6 eV reveals a nearly degenerate pair of new unoccupied states located at 2.73 ± 0.05 and 2.85 ± 0.05 eV above the Fermi level, which can be analyzed through the polarization and sample azimuthal orientation dependence of the mPP spectra. Based on the calculated electronic structure and optical transition moments, as well as related spectroscopic evidence, we assign these resonances to transitions between Ti 3d bands of nominally t2g and eg symmetry, which are split by crystal field. The initial states for the optical transition are the reduced Ti3+ states of t2g symmetry populated by formation oxygen vacancy defects, which exist within the band gap of TiO2. Furthermore,we studied the electron dynamics within the conduction band of TiO2 by three-dimensional time-resolved pump-probe interferometric mPP measurements. The spectroscopic and time-resolved studies reveal competition between 2PP and 3PP processes where the t2g-eg transitions in the 2PP process saturate, and are overtaken by the 3PP process initiated by the band-gap excitation from the valence band of TiO2.

Environmental Molecular Sciences Laboratory↗