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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Shedding Light on the Nature of Photoinduced States Formed in a Hydrogen-Generating Supramolecular RuPt Photocatalyst by Ultrafast Spectroscopy

Photoinduced electronic and structural changes of a hydrogen generating supramolecular RuPt photocatalyst are studied by a combination of time-resolved photoluminescence, optical transient absorption, and X-ray absorption spectroscopy. This work uses the element specificity of X-ray techniques to focus on the interplay between the photophysical and-chemical processes and the associated time scales at the catalytic Pt moiety. We observe very fast (<30 ps) photoreduction of the Pt catalytic site, followed by an similar to 600 ps step into a strongly oxidized Pt center. The latter process is likely induced by oxidative addition of reactive iodine species. The oxidized Pt species is long-lived and fully recovers to the original ground state complex on a >10 mu s time scale. However, the photosensitizing Ru moiety is fully restored on a much shorter similar to 300 ns time scale. In conclusion, this reaction scheme implies that we may withdraw two electrons from activated by a single photon.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1986

Solar particle history: 1983 version

It has long been known that the great majority of nuclear active solar particles are emitted in a few large storms in each 11 year cycle. A single storm in August 1972 dominated the fluence of particles of energy >10 MeV. Such storms can occur, it seems, at any time within the more active half ot the cycle. On a time scale long compared to 11 years, the knowledge comes from two sources. Terrestrial C-14 sets limits on the largest proton bursts that can have taken place in the 8000 years. Lunar surface samples have yielded data on mean fluxes on a time scale from the C-14 to the Mn-53 mean life. A mean flux was found of 70 protons >10 MeV and a rigidity constant R sub o = 100 MV to be robust on the 1,000,000 to 10,000,000 year time scale. Over the shorter periods represented by C-14 and Kr-81 the fluxes seem to have been higher by a factor of roughly three. Some examples of dating are discussed.

Arnold, J. R.↗
DOE OSTI2020

Gravitational Waves from Black Holes in Merging Ultra-Dwarf Galaxies

The origin of the black-hole:black-hole mergers discovered through gravitational waves with for example the LIGO/Virgo collaboration are a mystery. We investigate the idea that some of these black holes originate from the centers of extremely low-mass ultra-dwarf galaxies that have merged together in the distant past at $z>1$. Extrapolating the central black hole to stellar mass ratio suggests that the black holes in these mergers could arise from galaxies of masses $\sim 10^{5} - 10^{6}$ M$_{\odot}\,$. We investigate whether these galaxies merge enough, or too much, to be consistent with the observed GW rate of $\sim 9.7-101$ Gpc$^{-3}$ yr$^{-1}$ using the latest LIGO/Virgo results. We show that in the nearby universe the merger rate and number densities of ultra-dwarf galaxies are too low, by an order or magnitude, to produce these black hole mergers. However, by considering that the merger fraction, merger-time scales, and the number densities of low-mass galaxies all conspire at $z>1-1.5$ to increase the merger rate for these galaxies at higher redshifts we argue that it is possible that some of the observed GW events arise from BHs in the centers of low-mass galaxies. The major uncertainty in this calculation is the dynamical time-scales for black holes in low-mass galaxies. Our results however suggest a very long BH merger time-scale of 4-7 Gyr, consistent with an extended black hole merger history. Further simulations are needed to verify this possibility, however our theory can be tested by searching for host galaxies of gravitational wave events. Results from these searches would will put limits on dwarf galaxy mergers and/or the presence and formation mechanisms of black holes through PopIII stars in the lowest mass galaxies.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS2024

Rapid Variability of Mrk 421 During Extreme Flaring as Seen Through the Eyes of XMM-Newton

By studying the variability of blazars across the electromagnetic spectrum, it is possible to resolve the underlying processes responsible for rapid flux increases, so-called flares. We report on an extremely bright X-ray flare in the high-peaked BL Lacertae object Markarian 421 (Mrk 421) that occurred simultaneously with enhanced γ-ray activity detected at very high energies by First G-APD Cherenkov Telescope on 2019 June 9. We triggered an observation with XMM–Newton, which observed the source quasi-continuously for 25 h. We find that the source was in the brightest state ever observed using XMM–Newton, reaching a flux of 2.8 × 10 −9 erg cm -2 s -1 over an energy range of 0.3–10 keV. We perform a spectral and timing analysis to reveal the mechanisms of particle acceleration and to search for the shortest source-intrinsic time-scales. Mrk 421 exhibits the typical harder-when-brighter behaviour throughout the observation and shows a clock-wise hysteresis pattern, which indicates that the cooling dominates over the acceleration process. While the X-ray emission in different sub-bands is highly correlated, we can exclude large time lags as the computed z-transformed discrete correlation functions are consistent with a zero lag. We find rapid variability on time-scales of 1 ks for the 0.3–10 keV band and down to 300 s in the hard X-ray band (4–10 keV). Taking these time-scales into account, we discuss different models to explain the observed X-ray flare, and find that a plasmoid-dominated magnetic reconnection process is able to describe our observation best.

acceleration of particles↗
DOE OSTI2015

Methods of photoelectrode characterization with high spatial and temporal resolution

Here, materials and photoelectrode architectures that are highly efficient, extremely stable, and made from low cost materials are required for commercially viable photoelectrochemical (PEC) water-splitting technology. A key challenge is the heterogeneous nature of real-world materials, which often possess spatial variation in their crystal structure, morphology, and/or composition at the nano-, micro-, or macro-scale. Different structures and compositions can have vastly different properties and can therefore strongly influence the overall performance of the photoelectrode through complex structure–property relationships. A complete understanding of photoelectrode materials would also involve elucidation of processes such as carrier collection and electrochemical charge transfer that occur at very fast time scales. We present herein an overview of a broad suite of experimental and computational tools that can be used to define the structure–property relationships of photoelectrode materials at small dimensions and on fast time scales. A major focus is on in situ scanning-probe measurement (SPM) techniques that possess the ability to measure differences in optical, electronic, catalytic, and physical properties with nano- or micro-scale spatial resolution. In situ ultrafast spectroscopic techniques, used to probe carrier dynamics involved with processes such as carrier generation, recombination, and interfacial charge transport, are also discussed. Complementing all of these experimental techniques are computational atomistic modeling tools, which can be invaluable for interpreting experimental results, aiding in materials discovery, and interrogating PEC processes at length and time scales not currently accessible by experiment. In addition to reviewing the basic capabilities of these experimental and computational techniques, we highlight key opportunities and limitations of applying these tools for the development of PEC materials.

08 HYDROGEN↗
NASA NTRS2017

The Net Decay Time of Anomalies in Concentrations of Atmospheric Pollutants

This paper introduces a new parameter to characterize the random component in temporal variability of atmospheric pollutants and proposes a simple statistical technique for its evaluation. That parameter is the net decay time (or the time scale) of the local anomalies in concentrations of atmospheric pollutants, rather than the traditionally used chemical lifetimes of total amounts of the species. Using widely available data of hourly multi-year surface trace gas pollutant concentrations we demonstrate a simplified way to estimate the net decay time with an exponential approximation of lag-correlation functions. We assessed the decay times of fluctuations in observations of eight atmospheric pollutants (SO2, NO, NO2, NOy, O3, CO, NH3, and HNO3) at two urban sites and one cleaner rural site in the Eastern US. The time scales of temporal fluctuations (net decay times) vary from about one hour to slightly more than one day. These scales are generally much shorter in urban environments than in remote regions. We also compared day- and night-time observations in warm and cold seasons. At night in the cold season, time scales of fluctuations in atmospheric pollutants are usually the longest. Such estimates should be useful to air quality prediction, public health, and satellite remote sensing research communities.

air quality prediction↗
NASA NTRS1981

Rapid X-ray variability in the Seyfert galaxy NGC 6814

In contrast with the Tennant et al (1981) sample of over 30 active galactic nuclei, HEAO 1 A-2 high time resolution X-ray observations of the X-ray emitting Seyfert 1 galaxy NGC 6814 show strong X-ray variability on time scales of less than 3 hr. On a time scale of 90 min, the mean flux varied by a factor of about 2.5, and a characteristic time for variability of 100 + 60 or - 25 sec is obtained by autocorrelation analysis. There is no indication of spectral variability with an upper limit on a change in the power law spectral index of less than about 0.37, for a factor 2 change in intensity. The constraints of such rapid variability on a range of X-ray source mechanisms is discussed.

Tennant, A. F.↗
DOE OSTI2020

Blazar variability power spectra from radio up to TeV photon energies: Mrk 421 and PKS 2155−304

ABSTRACT We present the results of the power spectral density (PSD) analysis for the blazars Mrk 421 and PKS 2155−304, using good-quality, densely sampled light curves at multiple frequencies, covering 17 decades of the electromagnetic spectrum, and variability time-scales from weeks up to a decade. The data were collected from publicly available archives of observatories at radio from Owens Valley Radio Observatory, optical and infrared (B, V, R, I, J, H, and Kbands), X-rays from the Swift and the Rossi X-ray Timing Explorer, high and very high energy (VHE) γ-rays from the Fermi and Very Energetic Radiation Imaging Telescope Array System as well as the High Energy Stereoscopic System. Our results are: (1) the power-law form of the variability power spectra at radio, infrared, and optical frequencies have slopes ∼1.8, indicative of random-walk-type noise processes; (2) the power-law form of the variability power spectra at higher frequencies, from X-rays to VHE γ-rays, however, have slopes ∼1.2, suggesting a flicker noise-type process; and (3) there is significantly more variability power at X-rays, high and VHE γ-rays on time-scales ≲ 100 d, as compared to lower energies. Our results do not easily fit into a simple model, in which a single compact emission zone is dominating the radiative output of the blazars across all the time-scales probed in our analysis. Instead, we argue that the frequency-dependent shape of the variability power spectra points out a more complex picture, with highly inhomogeneous outflow producing non-thermal emission over an extended, stratified volume.

Goyal, Arti↗
DOE OSTI2022

A multi-scale time-series dataset of anthropogenic heat from buildings in Los Angeles County

The dataset contains hourly Anthropogenic heat (AH) from buildings in Los Angeles County, based on weather data from 2018. The hourly AH is aggregated at three spatial resolutions: 450m x 450m grid, 12km x 12km grid, and census tract. The AH is broken down into three components: building envelope surface convection, heating, ventilation, and air conditioning (HVAC) system heat release, and zone exfiltration and exhaust air heat loss. The dataset is created with the physics-based EnergyPlus building energy models to calculate individual buildings' AH considering WRF-UCM simulated microclimate conditions. Please refer to the paper "A multi-scale time-series dataset of anthropogenic heat from buildings in Los Angeles County" for more information about the data generation workflow and the data validation procedure. The data set contains two folders: the "output_data" folder holds the simulation results (EP_output and EP_output_csv), building metadata (building_metadata.geojson and building_metadata.csv), aggregated heat emission and energy consumption time-series data (hourly_heat_energy), and geographical data (geo_data) associated with the GEOID referenced in heat and energy consumption data. The "input_data" folder contains the raw data used to generate files in the "output_data" folder as well as data sets used in the validation. The code repository (https://github.com/IMMM-SFA/xu_etal_2022_sdata) holds the processing scripts for data curation, validation, and visualization.

Energy↗
NASA NTRS2007

Estimating Rain Rates from Tipping-Bucket Rain Gauge Measurements

This paper describes the cubic spline based operational system for the generation of the TRMM one-minute rain rate product 2A-56 from Tipping Bucket (TB) gauge measurements. Methodological issues associated with applying the cubic spline to the TB gauge rain rate estimation are closely examined. A simulated TB gauge from a Joss-Waldvogel (JW) disdrometer is employed to evaluate effects of time scales and rain event definitions on errors of the rain rate estimation. The comparison between rain rates measured from the JW disdrometer and those estimated from the simulated TB gauge shows good overall agreement; however, the TB gauge suffers sampling problems, resulting in errors in the rain rate estimation. These errors are very sensitive to the time scale of rain rates. One-minute rain rates suffer substantial errors, especially at low rain rates. When one minute rain rates are averaged to 4-7 minute or longer time scales, the errors dramatically reduce. The rain event duration is very sensitive to the event definition but the event rain total is rather insensitive, provided that the events with less than 1 millimeter rain totals are excluded. Estimated lower rain rates are sensitive to the event definition whereas the higher rates are not. The median relative absolute errors are about 22% and 32% for 1-minute TB rain rates higher and lower than 3 mm per hour, respectively. These errors decrease to 5% and 14% when TB rain rates are used at 7-minute scale. The radar reflectivity-rainrate (Ze-R) distributions drawn from large amount of 7-minute TB rain rates and radar reflectivity data are mostly insensitive to the event definition.

Wang, Jianxin↗
DOE OSTI2011

Effect of the plasma-generated magnetic field on relativistic electron transport

In the fast-ignition scheme, relativistic electrons transport energy from the laser deposition zone to the dense part of the target where the fusion reactions can be ignited. The magnetic fields and electron collisions play an important role in the collimation or defocusing of this electron beam. Detailed description of these effects requires large-scale kinetic calculations and is limited to short time intervals. In this paper, a reduced kinetic model of fast electron transport coupled to the radiation hydrodynamic code is presented. It opens the possibility to carry on hybrid simulations in a time scale of tens of picoseconds or more. It is shown with this code that plasma-generated magnetic fields induced by noncollinear temperature and density gradients may strongly modify electron transport in a time scale of a few picoseconds. These fields tend to defocus the electron beam, reducing the coupling efficiency to the target. This effect, that was not seen before in shorter time simulations, has to be accounted for in any ignition design using electrons as a driver.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2016

The propagation of particulate gravity currents in a V-shaped triangular cross section channel: Lock-release experiments and shallow-water numerical simulations

In this study, we investigate the motion of particulate gravity currents in a horizontal V-shaped channel. The particulate currents consisted of particles whose size varied between 0 and 100 μm but whose mean size increased. Particles were poorly sorted as the variance of the grain size distributions varied between 50 and 200. While the phases of propagation of homogeneous currents in such a geometry have been studied in the literature, this study considers the effects of the grain size on the propagation. The distance of propagation and front velocity of full-depth high-Reynolds-number lock-release experiments and shallow-water equation simulations were analyzed as the mean grain size of the initial particle distributions, defined by mass, was increased from 19 to 58 μm. Similar to the homogeneous currents, three consecutive phases of the front velocity could be identified but their characteristics and extent depend on the particle size. The initial phase, in particular, depends on a dimensionless settling number β that is defined as the ratio of two characteristic time scales, the propagation time x{sub 0}/U, where U is the scale for the front speed and x{sub 0} the lock length, and the settling time h{sub 0}/v{sub s}, where v{sub s} is the scale for the settling velocity and h{sub 0} the initial height of the current. For dimensionless settling numbers less than 0.001, the initial phase is characterized by a constant velocity for over about 6-7 lock lengths that is alike the initial slumping phase of perfectly constant velocity of the homogeneous currents. For dimensionless settling numbers greater than 0.001 and less than 0.015, the initial phase is no longer characterized by a constant velocity but an almost constant velocity for over about a similar 6-7 lock lengths. For dimensionless settling numbers greater than 0.015, however, as such, this phase is no longer seen. This initial phase is followed by a continuous decrease of the front advance, which results from the sedimentation of the particles. Unlike the homogeneous currents, this phase is a non-self-similar propagation. This phase is ended by a viscosity-dominated phase appearing to vary as ∼t{sup 1/7}. The good agreement between the front advance of the experiments and shallow-water equation simulations demonstrates that the mean size by mass is a fairly good proxy of poorly sorted particles.

42 ENGINEERING↗
NASA NTRS2010

Prediction Activities at NASA's Global Modeling and Assimilation Office

The Global Modeling and Assimilation Office (GMAO) is a core NASA resource for the development and use of satellite observations through the integrating tools of models and assimilation systems. Global ocean, atmosphere and land surface models are developed as components of assimilation and forecast systems that are used for addressing the weather and climate research questions identified in NASA's science mission. In fact, the GMAO is actively engaged in addressing one of NASA's science mission s key questions concerning how well transient climate variations can be understood and predicted. At weather time scales the GMAO is developing ultra-high resolution global climate models capable of resolving high impact weather systems such as hurricanes. The ability to resolve the detailed characteristics of weather systems within a global framework greatly facilitates addressing fundamental questions concerning the link between weather and climate variability. At sub-seasonal time scales, the GMAO is engaged in research and development to improve the use of land information (especially soil moisture), and in the improved representation and initialization of various sub-seasonal atmospheric variability (such as the MJO) that evolves on time scales longer than weather and involves exchanges with both the land and ocean The GMAO has a long history of development for advancing the seasonal-to-interannual (S-I) prediction problem using an older version of the coupled atmosphere-ocean general circulation model (AOGCM). This includes the development of an Ensemble Kalman Filter (EnKF) to facilitate the multivariate assimilation of ocean surface altimetry, and an EnKF developed for the highly inhomogeneous nature of the errors in land surface models, as well as the multivariate assimilation needed to take advantage of surface soil moisture and snow observations. The importance of decadal variability, especially that associated with long-term droughts is well recognized by the climate community. An improved understanding of the nature of decadal variability and its predictability has important implications for efforts to assess the impacts of global change in the coming decades. In fact, the GMAO has taken on the challenge of carrying out experimental decadal predictions in support of the IPCC AR5 effort.

Schubert, Siegfried↗
NASA NTRS1975

Time variations of UV emission features of Be stars

The UV spectra of three Be stars (gamma Cas, sigma Tau, eta Cen) were studied. Of the six Be stars observed in the first four lines of the Balmer series, three stars showed at least one of the Balmer lines to be variable in the equivalent width amounting to a few percent with time scales of 3 to 30 minutes. Photoelectric spectrum scans of five southern Wolf-Rayet stars showed night-to-night variations. A simple model is proposed to account for the behavior of these emission lines. Scans of gamma square Vel showed rapid variations of emission strengths of He II 4686 and C III - IV 4650. These variations have time scales of 1 minute and longer. Night-to-night variations were also found. Scans of four Be stars in H alpha showed a definite variation of 3 to 4 percent, with time scales of 1 minute and longer in sigma Tau. In 48 Per and kappa Dra the variations are not as well established. No variation of any significance was found for nu Gem.

Bahng, J. D. R.↗
DOE OSTI2019

Photoinduced non-adiabatic energy transfer pathways in dendrimer building blocks

The efficiency of the intramolecular energy transfer in light harvesting dendrimers is determined by their well-defined architecture with high degree of order. After photoexcitation, through-space and through-bond energy transfer mechanisms can take place, involving vectorial exciton migration among different chromophores within dendrimer highly branched structures. Their inherent intramolecular energy gradient depends on how the multiple chromophoric units have been assembled, subject to their inter-connects, spatial distances, and orientations. Herein, we compare the photoinduced nonadiabatic molecular dynamics simulations performed on a set of different combinations of a chain of linked dendrimer building blocks composed of two-, three-, and four-ring linear polyphenylene chromophoric units. The calculations are performed with the recently developed ab initio multiple cloning-time dependent diabatic basis implementation of the Multiconfigurational Ehrenfest (MCE) approach. Despite differences in short time relaxation pathways and different initial exciton localization, at longer time scales, electronic relaxation rates and exciton final redistributions are very similar for all combinations. Unlike the systems composed of two building blocks, considered previously, for the larger 3 block systems here we observe that bifurcation of the wave function accounted by cloning is important. In all the systems considered in this work, at the time scale of few hundreds of femtoseconds, cloning enhances the electronic energy relaxation by ~13% compared to that of the MCE method without cloning. Thus, accurate description of quantum effects is essential for understanding of the energy exchange in dendrimers both at short and long time scales.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

The simultaneous low state spectral energy distribution of 1ES 2344+514 from radio to very high energies

Here, BL Lacertae objects are variable at all energy bands on time scales down to minutes. To construct and interpret their spectral energy distribution (SED), simultaneous broad-band observations are mandatory. Up to now, the number of objects studied during such campaigns is very limited and biased towards high flux states. Furthermore, we present the results of a dedicated multi-wavelength study of the high-frequency peaked BL Lacertae (HBL) object and known TeV emitter 1ES 2344+514 by means of a pre-organised campaign. The observations were conducted during simultaneous visibility windows of MAGIC and AGILE in late 2008. The measurements were complemented by Metsähovi, RATAN-600, KVA+Tuorla, Swift and VLBA pointings. Additional coverage was provided by the ongoing long-term F-GAMMA and MOJAVE programs, the OVRO 40-m and CrAO telescopes as well as the Fermi satellite. The obtained SEDs are modelled using a one-zone as well as a self-consistent two-zone synchrotron self-Compton model. As a result, 1ES 2344+514 was found at very low flux states in both X-rays and very high energy gamma rays. Variability was detected in the low frequency radio and X-ray bands only, where for the latter a small flare was observed. The X-ray flare was possibly caused by shock acceleration characterised by similar cooling and acceleration time scales. MOJAVE VLBA monitoring reveals a static jet whose components are stable over time scales of eleven years, contrary to previous findings. There appears to be no significant correlation between the 15 GHz and R-band monitoring light curves. The observations presented here constitute the first multi-wavelength campaign on 1ES 2344+514 from radio to VHE energies and one of the few simultaneous SEDs during low activity states. The quasi-simultaneous Fermi -LAT data poses some challenges for SED modelling, but in general the SEDs are described well by both applied models. The resulting parameters are typical for TeV emitting HBLs. Consequently it remains unclear whether a so-called quiescent state was found in this campaign.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2024

Implementing Superresolution of Nonstationary Tides with Wavelets: An Introduction to CWT_Multi

Abstract Tides are often nonstationary due to nonastronomical influences. Investigating variable tidal properties implies a trade-off between separating adjacent frequencies (using long analysis windows) and resolving their time variations (short analysis windows). Previous continuous wavelet transform (CWT) tidal methods resolved tidal species. Here, we present CWT_Multi, a MATLAB code that 1) uses CWT linearity (via the “response coefficient method”) to implement superresolution, i.e., resolving tidal constituents beyond the Rayleigh criterion; 2) provides a Munk–Hasselmann constituent selection criterion appropriate for superresolution; and 3) introduces an objective, time-variable form of inference (“dynamic inference”) based on time-varying data properties. CWT_Multi resolves tidal species on time scales of days, and multiple constituents per species with fortnightly filters. It outputs astronomical phase lags and admittances, analyzes multiple records, and provides power spectra of the signal(s), residual(s), and reconstruction(s); confidence limits; and signal-to-noise ratios. Artificial data and water levels from the Lower Columbia River Estuary (LCRE) and San Francisco Bay Delta (SFBD) are used to test CWT_Multi and compare it to harmonic analysis programs NS_Tide and UTide. CWT_Multi provides superior reconstruction, detiding, dynamic analysis utility, and time resolution of constituents (but with broader confidence limits). Dynamic inference resolves closely spaced constituents (like K 1 , S 1 , and P 1 ) on fortnightly time scales, quantifying impacts of diel power peaking (with a 24-h period, like S 1 ) on water levels in the LCRE. CWT_Multi also helps quantify the impacts of high flows and a salt barrier closing on tidal properties in the SFBD. On the other hand, CWT_Multi does not excel at prediction, and results depend on analysis details, as for any method applied to nonstationary data. Significance Statement Ocean tides, especially in coastal and estuarine systems, are often nonstationary, in the sense that the mean and standard deviation of tidal properties vary over time, usually in response to some nontidal process. We introduce here a MATLAB code, CWT_Multi, that uses wavelet transforms to resolve both tidal species and constituents on time scales from a few days to months. Our code accommodates multiple scalar time series and has typical tidal analysis features like constituent selection and inference, plus two forms of uncertainty analyses. It is flexible, allowing the user to adapt analysis properties to diverse datasets. CWT_Multi is applicable to many problems involving time-variable tides, including sea level rise, compound flooding, sediment transport, and wetland habitat analyses. Application to vector data is a straightforward extension, but further development of our uncertainty analysis is merited. Because nonstationary tidal analysis is rapidly advancing, we also define the features of a “well-formed” analysis code.

Lobo, Matthew↗
DOE OSTI2016

Excited Electron Dynamics at Semiconductor–Molecule Type-II Heterojunction Interface: First-Principles Dynamics Simulation

Excited electron dynamics at semiconductor–molecule interfaces is ubiquitous in various energy conversion technologies. However, a quantitative understanding of how molecular details influence the quantum dynamics of excited electrons remains a great scientific challenge because of the complex interplay of different processes with various time scales. Here in this paper, we employ first-principles electron dynamics simulations to investigate how molecular features govern the dynamics in a representative interface between the hydrogen-terminated Si(111) surface and a cyanidin molecule. Hot electron transfer to the chemisorbed molecule was observed but was short-lived on the molecule. Interfacial electron transfer to the chemisorbed molecule was found to be largely decoupled from hot electron relaxation within the semiconductor surface. While the hot electron relaxation was found to take place on a time scale of several hundred femtoseconds, the subsequent interfacial electron transfer was slower by an order of magnitude. Finally, at the same time, this secondary process of picosecond electron transfer is comparable in time scale to typical electron trapping into defect states in the energy gap.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗