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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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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

The role of mixed vibronic Q y -Q x states in green light absorption of light-harvesting complex II

The importance of green light for driving natural photosynthesis has long been underappreciated, however, under the presence of strong illumination, green light actually drives photosynthesis more efficiently than red light. This green light is absorbed by mixed vibronic Q y -Q x states, arising from chlorophyll (Chl)-Chl interactions, although almost nothing is known about these states. Here, we employ polarization-dependent two-dimensional electronic-vibrational spectroscopy to study the origin and dynamics of the mixed vibronic Q y -Q x states of light-harvesting complex II. We show the states in this region dominantly arise from Chl b and demonstrate how it is possible to distinguish between the degree of vibronic Q y versus Q x character. We find that the dynamics for states of predominately Chl b Q y versus Chl b Q x character are markedly different, as excitation persists for significantly longer in the Q x states and there is an oscillatory component to the Q x dynamics, which will be discussed. Our findings demonstrate the central role of electronic-nuclear mixing in efficient light-harvesting and the different functionalities of Chl a and Chl b .

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Continuous Light Absorption Photometer (CLAP) Instrument Handbook

Reliable measurements of aerosol light absorption are crucial for quantifying the radiative forcing of climate. As a consequence, light absorption measurements are recommended for all stations in the Global Atmosphere Watch network, which is coordinated by the World Meteorological Organization. Aerosol light absorption is often dominated by soot-like particles produced by the incomplete combustion of carbonaceous fuels, commonly termed "black carbon", and optical methods are the primary way that equivalent black carbon concentrations are derived. Two basic approaches are used for determining the aerosol light absorption coefficient: in situ methods where the absorption is measured while the particles are suspended in air, and filter-based methods where the particles are deposited on a filter for real-time optical analysis. In situ methods are inherently more accurate because the physical state of the particles can be changed by the act of filtration. Unfortunately, currently available instruments for in situ measurements are more expensive and difficult to operate than filter-based methods, making them better suited for use in intensive field campaigns or as laboratory reference instruments. Filter-based instruments, because of their lower cost and simpler operation, have been the preferred choice for long-term measurements of aerosol light absorption in monitoring networks.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1978

Plant canopy light absorption model with application to wheat

A light absorption model (LAM) for vegetative plant canopies has been derived from the Suits reflectance model. From the LAM the absorption of light in the photosynthetically active region of the spectrum (400-700 nm) has been calculated for a Penjamo wheat crop for several situations including (a) the percent absorption of the incident radiation by a canopy of LAI 3.1 having a four-layer structure, (b) the percent absorption of light by the individual layers within a four-layer canopy and by the underlying soil, (c) the percent absorption of light by each vegetative canopy layer for variable sun angle, and (d) the cumulative solar energy absorbed by the developing wheat canopy as it progresses from a single layer through its growth stages to a three-layer canopy. This calculation is also presented as a function of the leaf area index and is shown to be in agreement with experimental data reported by Kanemasu on Plainsman V wheat.

Chance, J. E.↗
NASA NTRS1977

A plant canopy light absorption model with application to wheat

From the light absorption model the absorption of light in the photosynthetically active region of the spectrum was calculated for a Penjamo wheat crop for several situations including: (1) the percent absorption of the incident radiation by a canopy having a four layer structure; (2) the percent absorption of light by the individual layers within a four layer canopy and by the underlying soil; (3) the percent absorption of light by each vegetative canopy layer for variable sun angle; and (4) the cumulative solar energy absorbed by the developing wheat canopy as it progresses from a single layer through its growth stages to a three layer canopy. This calculation was also presented as a function of the leaf area index.

Chance, J. E.↗
NASA NTRS1997

Light Absorption of Stratospheric Aerosols: Long-Term Trend and Contribution by Aircraft

Measurements of aerosol light-absorption coefficients are useful for studies of radiative transfer and heating rates. Ogren appears to have published the first light- absorption coefficients in the stratosphere in 1981, followed by Clarke in 1983 and Pueschel in 1992. Because most stratospheric soot appears to be due to aircraft operations, application of an aircraft soot aerosol emission index to projected fuel consumption suggests a threefold increase of soot loading and light absorption by 2025. Together, those four data sets indicate an increase in mid-visible light extinction at a rate of 6 % per year. This trend is similar to the increase per year of sulfuric acid aerosol and of commercial fleet size. The proportionality between stepped-up aircraft operations above the tropopause and increases in stratospheric soot and sulfuric acid aerosol implicate aircraft as a source of stratospheric pollution. Because the strongly light-absorbing soot and the predominantly light-scattering sulfuric acid aerosol increase at similar rates, however, the mid-visible stratospheric aerosol single scatter albedo is expected to remain constant and not approach a critical value of 0.98 at which stratospheric cooling could change to warming.

Pueschel , R. F.↗
DOE OSTI2022

Constraining the particle-scale diversity of black carbon light absorption using a unified framework

Abstract. Atmospheric black carbon (BC), the strongest absorber of visible solar radiation in the atmosphere, manifests across a wide spectrum of morphologies and compositional heterogeneity. Phenomenologically, the distribution of BC among diverse particles of varied composition gives rise to enhancement of its light absorption capabilities by over twofold in comparison to that of nascent or unmixed homogeneous BC. This situation has challenged the modeling community to consider the full complexity and diversity of BC on a per-particle basis for accurate estimation of its light absorption. The conventionally adopted core–shell approximation, although computationally inexpensive, is inadequate not only in estimating but also capturing absorption trends for ambient BC. Here we develop a unified framework that encompasses the complex diversity in BC morphology and composition using a single metric, the phase shift parameter (ρBC), which quantifies how much phase shift the incoming light waves encounter across a particle compared to that in its absence. We systematically investigate variations in ρBC across the multi-space distribution of BC morphology, mixing state, mass, and composition as reported by field and laboratory observations. We find that ρBC>1 leads to decreased absorption by BC, which explains the weaker absorption enhancements observed in certain regional BC compared to laboratory results of similar mixing state. We formulate universal scaling laws centered on ρBC and provide physics-based insights regarding core–shell approximation overestimating BC light absorption. We conclude by packaging our framework in an open-source Python application to facilitate community-level use in future BC-related research. The package has two main functionalities. The first functionality is for forward problems, wherein experimentally measured BC mixing state and assumed BC morphology are input, and the aerosol absorption properties are output. The second functionality is for inverse problems, wherein experimentally measured BC mixing state and absorption are input, and the morphology of BC is returned. Further, if absorption is measured at multiple wavelengths, the package facilitates the estimation of the imaginary refractive index of coating materials by combining the forward and inverse procedures. Our framework thus provides a computationally inexpensive source for calculation of absorption by BC and can be used to constrain light absorption throughout the atmospheric lifetime of BC.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Optimizing molecular light absorption in the strong coupling regime for solar energy harvesting

The strong coupling of optical absorbers (e.g., molecules or semiconductors) to confined photonic modes fundamentally alters the physical properties of the coupled system via the formation of hybrid light-matter states. One potential application of strong light-matter coupling relies on exploiting it to localize light-induced charge excitation processes to small volumes of material. Applications that would benefit from this localization include thin-film photovoltaics, photodetection, photocatalysis, and others, where the overall performance depends on the ability of a material to amplify light absorption (i.e., the formation of electron-hole pairs) within specific locations in space. This contribution investigates how strong light-matter coupling affects light absorption rates in molecular absorbers coupled to photonic nanostructures. Here, our results show that the molecular light absorption efficiencies are highest in configurations where the strongly coupled molecules interact directly with the incoming photon flux. We also identify a nonlinear dependence in the molecular absorption as a function of concentration, unique to the strongly coupled systems. Based on these results, we propose design principles for engineering nanostructured systems that allow for high efficiencies of charge carrier localization into strongly coupled absorbers.

14 SOLAR ENERGY↗
DOE OSTI2020

Vertical profiles of light absorption and scattering associated with black carbon particle fractions in the springtime Arctic above 79° N

Despite the potential importance of black carbon (BC) for radiative forcing of the Arctic atmosphere, vertically resolved measurements of the particle light scattering coefficient (σ sp ) and light absorption coefficient (σ ap ) in the springtime Arctic atmosphere are infrequent, especially measurements at latitudes at or above 80° N. Here, relationships among vertically distributed aerosol optical properties (σap, σsp and single scattering albedo or SSA), particle microphysics and particle chemistry are examined for a region of the Canadian archipelago between 79.9 and 83.4° N from near the surface to 50 hPa. Airborne data collected during April 2015 are combined with ground-based observations from the observatory at Alert, Nunavut and simulations from the Goddard Earth Observing System (GEOS) model, GEOS-Chem, coupled with the TwO-Moment Aerosol Sectional (TOMAS) model (collectively GEOS-Chem–TOMAS; Kodros et al., 2018) to further our knowledge of the effects of BC on light absorption in the Arctic troposphere. The results are constrained for σsp less than 15 Mm -1 , which represent 98% of the observed σsp, because the single scattering albedo (SSA) has a tendency to be lower at lower σsp, resulting in a larger relative contribution to Arctic warming. At 18.4 m 2 g -1 , the average BC mass absorption coefficient (MAC) from the combined airborne and Alert observations is substantially higher than the two averaged modelled MAC values (13.6 and 9.1 m2 g -1 ) for two different internal mixing assumptions, the latter of which is based on previous observations. The higher observed MAC value may be explained by an underestimation of BC, the presence of small amounts of dust and/or possible differences in BC microphysics and morphologies between the observations and model. In comparing the observations and simulations, we present σap and SSA, as measured, and σ ap 2 and the corresponding SSA to encompass the lower modelled MAC that is more consistent with accepted MAC values. Median values of the measured σap, rBC and the organic component of particles all increase by a factor of 1.8±0.1, going from near-surface to 750 hPa, and values higher than the surface persist to 600 hPa. Modelled BC, organics and σap agree with the near-surface measurements but do not reproduce the higher values observed between 900 and 600 hPa. The differences between modelled and observed optical properties follow the same trend as the differences between the modelled and observed concentrations of the carbonaceous components (black and organic). Model-observation discrepancies may be mostly due to the modelled ejection of biomass burning particles only into the boundary layer at the sources. For the assumption of the observed MAC value, the SSA range between 0.88 and 0.94, which is significantly lower than other recent estimates for the Arctic, in part reflecting the constraint of σsp<15 Mm -1 . The large uncertainties in measuring optical properties and BC, and the large differences between measured and modelled values here and in the literature, argue for improved measurements of BC and light absorption by BC and more vertical profiles of aerosol chemistry, microphysics and other optical properties in the Arctic.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Visible Light Absorption and Hot Carrier Trapping in Anatase TiO 2 : The Role of Surface Oxygen Vacancies

Anatase TiO 2 is an efficient water splitting photocatalyst using UV light, but solar energy harvesting requires the presence of midgap states to increase visible light absorption. Despite numerous studies, important questions remain regarding the photophysics in O vacancy doped TiO 2 . Here, by employing extreme ultraviolet reflection–absorption (XUV-RA) spectroscopy at the Ti M2,3-edge, spectral signatures of both large and small polaron states are identified, allowing ultrafast electron and hole dynamics in these states to be independently resolved. Results show that visible light absorption occurs via promotion of an electron from the small polaron state to the TiO 2 conduction band. In contrast, absorption of UV light results in direct band gap excitation followed by carrier relaxation during which hot holes trap as small polarons in 45 ± 42 fs, and hot electrons couple to polar optical phonons leading to vibrational coherence and large polaron formation in 945 ± 92 fs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Correcting for filter-based aerosol light absorption biases at the Atmospheric Radiation Measurement program's Southern Great Plains site using photoacoustic measurements and machine learning

Abstract. Measurement of light absorption of solar radiation by aerosols is vital for assessing direct aerosol radiative forcing, which affects local and global climate. Low-cost and easy-to-operate filter-based instruments, such as the Particle Soot Absorption Photometer (PSAP), that collect aerosols on a filter and measure light attenuation through the filter are widely used to infer aerosol light absorption. However, filter-based absorption measurements are subject to artifacts that are difficult to quantify. These artifacts are associated with the presence of the filter medium and the complex interactions between the filter fibers and accumulated aerosols. Various correction algorithms have been introduced to correct for the filter-based absorption coefficient measurements toward predicting the particle-phase absorption coefficient (Babs). However, the inability of these algorithms to incorporate into their formulations the complex matrix of influencing parameters such as particle asymmetry parameter, particle size, and particle penetration depth results in prediction of particle-phase absorption coefficients with relatively low accuracy. The analytical forms of corrections also suffer from a lack of universal applicability: different corrections are required for rural and urban sites across the world. In this study, we analyzed and compared 3 months of high-time-resolution ambient aerosol absorption data collected synchronously using a three-wavelength photoacoustic absorption spectrometer (PASS) and PSAP. Both instruments were operated on the same sampling inlet at the Department of Energy's Atmospheric Radiation Measurement program's Southern Great Plains (SGP) user facility in Oklahoma. We implemented the two most commonly used analytical correction algorithms, namely, Virkkula (2010) and the average of Virkkula (2010) and Ogren (2010)–Bond et al. (1999) as well as a random forest regression (RFR) machine learning algorithm to predict Babs values from the PSAP's filter-based measurements. The predicted Babs was compared against the reference Babs measured by the PASS. The RFR algorithm performed the best by yielding the lowest root mean square error of prediction. The algorithm was trained using input datasets from the PSAP (transmission and uncorrected absorption coefficient), a co-located nephelometer (scattering coefficients), and the Aerosol Chemical Speciation Monitor (mass concentration of non-refractory aerosol particles). A revised form of the Virkkula (2010) algorithm suitable for the SGP site has been proposed; however, its performance yields approximately 2-fold errors when compared to the RFR algorithm. To generalize the accuracy and applicability of our proposed RFR algorithm, we trained and tested it on a dataset of laboratory measurements of combustion aerosols. Input variables to the algorithm included the aerosol number size distribution from the Scanning Mobility Particle Sizer, absorption coefficients from the filter-based Tricolor Absorption Photometer, and scattering coefficients from a multiwavelength nephelometer. The RFR algorithm predicted Babs values within 5 % of the reference Babs measured by the multiwavelength PASS during the laboratory experiments. Thus, we show that machine learning approaches offer a promising path to correct for biases in long-term filter-based absorption datasets and accurately quantify their variability and trends needed for robust radiative forcing determination.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Photoluminescence probing of light absorption centers at silica laser damage

We use photoluminescence (PL) imaging to study damage growth precursors within laser damage sites on the surface of silica. Damage site evolution is induced by multiple shots of UV nanosecond pulsed laser at various energy densities and monitored throughout the early stages of growth. Wide-field PL imaging rapidly locates microscopic light absorption centers within the silica damage site. Our quantitative analysis shows that damage sites with strong local PL intensity show a higher probability of growth upon subsequent laser pulses. Scanning electron microscopy (SEM) paired with a study of PL spectrum shows that the strong PL intensity appears from the subsurface fractures with high defect density, which provides a local light absorption center leading to significant damage growth. We believe that this result offers an efficient optical damage mitigation strategy by providing a rapid and non-destructive optical inspection approach.

36 MATERIALS SCIENCE↗
NASA NTRS1997

Light Absorption in the Stratosphere: Trend, Soot Aerosol Concentration and Contribution by...

The light absorption coefficient, Beta(a) of the stratospheric aerosol is an important quantity that determines its radiative effects. When combined with the aerosol scattering coefficient, Beta(a) it becomes possible to evaluate the aerosol single scatter albedo, omega = Beta(s)/(Beta(s) + Beta(a)) which is essential for modeling the overall radiative effects of the stratospheric aerosol. Pollack1 determined that omega = 0.98 is a critical value that separates stratospheric cooling from warming.

Pueschel, R. F.↗
NASA NTRS2001

Dependence of Aerosol Light Absorption and Single-Scattering Albedo On Ambient Relative Humidity for Sulfate Aerosols with Black Carbon Cores

Atmospheric aerosols frequently contain hygroscopic sulfate species and black carbon (soot) inclusions. In this paper we report results of a modeling study to determine the change in aerosol absorption due to increases in ambient relative humidity (RH), for three common sulfate species, assuming that the soot mass fraction is present as a single concentric core within each particle. Because of the lack of detailed knowledge about various input parameters to models describing internally mixed aerosol particle optics, we focus on results that were aimed at determining the maximum effect that particle humidification may have on aerosol light absorption. In the wavelength range from 450 to 750 nm, maximum absorption humidification factors (ratio of wet to 'dry=30% RH' absorption) for single aerosol particles are found to be as large as 1.75 when the RH changes from 30 to 99.5%. Upon lesser humidification from 30 to 80% RH, absorption humidification for single particles is only as much as 1.2, even for the most favorable combination of initial ('dry') soot mass fraction and particle size. Integrated over monomodal lognormal particle size distributions, maximum absorption humidification factors range between 1.07 and 1.15 for humidification from 30 to 80% and between 1.1 and 1.35 for humidification from 30 to 95% RH for all species considered. The largest humidification factors at a wavelength of 450 nm are obtained for 'dry' particle size distributions that peak at a radius of 0.05 microns, while the absorption humidification factors at 700 nm are largest for 'dry' size distributions that are dominated by particles in the radius range of 0.06 to 0.08 microns. Single-scattering albedo estimates at ambient conditions are often based on absorption measurements at low RH (approx. 30%) and the assumption that aerosol absorption does not change upon humidification (i.e., absorption humidification equal to unity). Our modeling study suggests that this assumption alone can introduce absolute errors in estimates of the midvisible single-scattering albedo of up to 0.05 for realistic dry particle size distributions. Our study also indicates that this error increases with increasing wavelength. The potential errors in aerosol single-scattering albedo derived here are comparable in magnitude and in addition to uncertainties in single-scattering albedo estimates that are based on measurements of aerosol light absorption and scattering.

Redemann, Jens↗
NASA NTRS2014

A Synthesis of Light Absorption Properties of the Arctic Ocean: Application to Semi-analytical Estimates of Dissolved Organic Carbon Concentrations from Space

The light absorption coefficients of particulate and dissolved materials are the main factors determining the light propagation of the visible part of the spectrum and are, thus, important for developing ocean color algorithms. While these absorption properties have recently been documented by a few studies for the Arctic Ocean [e.g., Matsuoka et al., 2007, 2011; Ben Mustapha et al., 2012], the datasets used in the literature were sparse and individually insufficient to draw a general view of the basin-wide spatial and temporal variations in absorption. To achieve such a task, we built a large absorption database at the pan-Arctic scale by pooling the majority of published datasets and merging new datasets. Our results showed that the total non-water absorption coefficients measured in the Eastern Arctic Ocean (EAO; Siberian side) are significantly higher 74 than in the Western Arctic Ocean (WAO; North American side). This higher absorption is explained 75 by higher concentration of colored dissolved organic matter (CDOM) in watersheds on the Siberian 76 side, which contains a large amount of dissolved organic carbon (DOC) compared to waters off 77 North America. In contrast, the relationship between the phytoplankton absorption (a()) and chlorophyll a (chl a) concentration in the EAO was not significantly different from that in the WAO. Because our semi-analytical CDOM absorption algorithm is based on chl a-specific a() values [Matsuoka et al., 2013], this result indirectly suggests that CDOM absorption can be appropriately erived not only for the WAO but also for the EAO using ocean color data. Derived CDOM absorption values were reasonable compared to in situ measurements. By combining this algorithm with empirical DOC versus CDOM relationships, a semi-analytical algorithm for estimating DOC concentrations for coastal waters at the Pan-Arctic scale is presented and applied to satellite ocean color data.

Pan-Arctic↗
NASA NTRS1983

Stratospheric aerosol light absorption before and after El Chichon

Direct in-situ measurements of aerosol light absorption before, during, and after the eruption of Mt. St. Helens and El Chichon reveal the presence of light absorbing species at all times. Large enhancements which appear to drop rapidly with time are found at certain locations immediately following volcanic events. Although a general patchiness is present in the aerosol and its associated absorption coefficient, post eruption values appear to remain elevated in the mean when compared to early 1979 data prior to the El Chichon eruption. From the data collected for this period, lower bounds for the single scatter albedo are presented along with implications for associated radiative effects.

Clarke, A. D.↗
NASA NTRS2021

Performance of JAXA’s SGLI standard ocean color products for oceanic to coastal waters: chlorophyll a concentration and light absorption coefficients of colored dissolved organic matter

We present the performance of JAXA’s SGLI standard algorithms for estimating chlorophyll a (chl a) concentration and the light absorption coefcients of colored dissolved organic matter (CDOM) using recently compiled high-quality data obtained from oceanic to coastal waters. Prior to the evaluation of the algorithms, we frst compare two forward models (Gordon et al. in J Geophys Res 93(D9):10909-10924, 1988: G88 and Park and Ruddick in Appl Opt 44(7):1236–1249, 2005: PR05) using a wide range of inherent optical properties (IOPs) to (1) examine if the water refectance is appropriately reproduced and (2) correct measured refectance in terms of its bidirectionality. Based on a good reproducibility of water refectance using the PR05, the optimized IOPs are further used for explaining errors in estimates of chl a concentration and CDOM absorption when using the SGLI, the GSM (Maritorena et al. in Appl Opt 41:2705–2714, 2002), and the QAA (Lee et al. in Appl Opt 41:5755, 2002) inversion algorithms. Results show that the mean error for estimating chl a concentration using the SGLI algorithm is 110% for our dataset. Although this error is lower than that of the GSM and the QAA algorithms, a signifcant underestimate at chl a higher than 2.0 mg m−3 is observed, which is further shown by independent match-up analyses. Another SGLI CDOM product includes the mean error of 50% and shows deviation at high CDOM range (>1.0 per m). A similar trend is observed for the GSM but not for the QAA when a global relationship of CDOM to colored detrital matter is applied. The sources of errors are discussed for potentially improving the retrievals

Second-generation GLobal Imager (SGLI)↗
NASA NTRS2003

Vertical Profiles of Light Scattering, Light Absorption, and Single Scattering Albedo during the Dry, Biomass Burning Season in Southern Africa and Comparisons of In Situ and Remote Sensing Measurements of Aerosol Optical Depths

Airborne in situ measurements of vertical profiles of aerosol light scattering, light absorption, and single scattering albedo (omega (sub 0)) are presented for a number of locations in southern Africa during the dry, biomass burning season. Features of the profiles include haze layers, clean air slots, and marked decreases in light scattering in passing from the boundary layer into the free troposphere. Frequency distributions of omega (sub 0) reflect the strong influence of smoke from biomass burning. For example, during a period when heavy smoke was advected into the region from the north, the mean value of omega (sub 0) in the boundary layer was 0.81 +/- 0.02 compared to 0.89 +/- 0.03 prior to this intrusion. Comparisons of layer aerosol optical depths derived from the in situ measurements with those measured by a Sun photometer aboard the aircraft show excellent agreement.

Magi, Brian I.↗
DOE OSTI2024

Enhanced light absorption for solid-state brown carbon from wildfires due to organic and water coatings

Abstract Wildfires emit solid-state strongly absorptive brown carbon (solid S-BrC, commonly known as tar ball), critical to Earth’s radiation budget and climate, but their highly variable light absorption properties are typically not accounted for in climate models. Here, we show that from a Pacific Northwest wildfire, over 90% of particles are solid S-BrC with a mean refractive index of 1.49 + 0.056 i at 550 nm. Model sensitivity studies show refractive index variation can cause a ~200% difference in regional absorption aerosol optical depth. We show that ~50% of solid S-BrC particles from this sample uptake water above 97% relative humidity. We hypothesize these results from a hygroscopic organic coating, potentially facilitating solid S-BrC as nuclei for cloud droplets. This water uptake doubles absorption at 550 nm and the organic coating on solid S-BrC can lead to even higher absorption enhancements than water. Incorporating solid S-BrC and water interactions should improve Earth’s radiation budget predictions.

54 ENVIRONMENTAL SCIENCES↗