SEARCH · Engineering Papers
Results for “Absorption”
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.
Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.
Light Absorption Properties and Radiative Effects of Primary Organic Aerosol Emissions
Organic aerosols (OAs) in the atmosphere affect Earth's energy budget by not only scattering but also absorbing solar radiation due to the presence of the so-called "brown carbon" (BrC) component. However, the absorptivities of OAs are not represented or are poorly represented in current climate and chemical transport models. In this study, we provide a method to constrain the BrC absorptivity at the emission inventory level using recent laboratory and field observations. We review available measurements of the light-absorbing primary OA (POA), and quantify the wavelength-dependent imaginary refractive indices (k(OA), the fundamental optical parameter determining the particle's absorptivity) and their uncertainties for the bulk POA emitted from biomass/biofuel, lignite, propane, and oil combustion sources. In particular, we parametrize the k(OA) of biomass/biofuel combustion sources as a function of the black carbon (BC)-to-OA ratio, indicating that the absorptive properties of POA depend strongly on burning conditions. The derived fuel-type-based k(OA) profiles are incorporated into a global carbonaceous aerosol emission inventory, and the integrated k(OA) values of sectoral and total POA emissions are presented. Results of a simple radiative transfer model show that the POA absorptivity warms the atmosphere significantly and leads to similar to 27% reduction in the amount of the net global average POA. cooling compared to results from the nonabsorbing assumption.
Hierarchical calibration and validation framework of bench-scale computational fluid dynamics simulations for solvent-based carbon capture. Part 2: Chemical absorption across a wetted wall column: Original Research Article: Hierarchical calibration and validation framework of bench-scale computational fluid dynamics simulations
Part 1 of this paper presents a numerical model for non-reactive physical mass transfer across a wetted wall column (WWC). In Part 2, we improved the existing computational fluid dynamics (CFD) model to simulate chemical absorption occurring in a WWC as a bench-scale study of solvent-based carbon dioxide (CO 2 ) capture. In this study, to generate data for WWC model validation, CO 2 mass transfer across a monoethanolamine (MEA) solvent was first measured on a WWC experimental apparatus. The numerical model developed in this work can account for both chemical absorption and desorption of CO 2 in MEA. In addition, the overall mass transfer coefficient predicted using traditional/empirical correlations is conducted and compared with CFD prediction results for both steady and wavy falling films. A Bayesian statistical calibration algorithm is adopted to calibrate the reaction rate constants in chemical absorption/desorption of CO 2 across a falling film of MEA. The posterior distributions of the two transport properties, i.e., Henry's constant and gas diffusivity in the non-reacting nitrous oxide (N 2 O)/MEA system obtained from Part 1 of this study, serves as priors for the calibration of CO 2 reaction rate constants after using the N 2 O/CO 2 analogy method. Finally, the calibrated model can be used to predict the CO 2 mass transfer in a WWC for a wider range of operating conditions.
Combining X-ray Absorption and X-ray Diffraction Techniques for in Situ Studies of Chemical Transformations in Heterogeneous Catalysis:Advantages and Limitations
Recent advances in catalysis instrumentations include synchrotron-based facilities where time-resolved X-ray scattering and absorption techniques are combined in the same in situ or operando experiment to study catalysts at work. To evaluate the advances and limitations of this method, we performed a series of experiments at the new XAFS/XRD instrument in the National Synchrotron Light Source. Nearly simultaneous X-ray diffraction (XRD) and X-ray absorption fine-structure (XAFS) measurements of structure and kinetics of several catalysts under reducing or oxidizing conditions have been performed and carefully analyzed. For CuFe{sub 2}O{sub 4} under reducing conditions, the combined use of the two techniques allowed us to obtain accurate data on kinetics of nucleation and growth of metallic Cu. For the inverse catalyst CuO/CeO{sub 2} that underwent isothermal reduction (with CO) and oxidation (with O{sub 2}), the XAFS data measured in the same experiment with XRD revealed strongly disordered Cu species that went undetected by diffraction. These and other examples emphasize the unique sensitivity of these two complementary methods to follow catalytic processes in the broad ranges of length and time scales.
Comparison of x-ray absorption spectra between water and ice: New ice data with low pre-edge absorption cross-section
The effect of crystal growth conditions on the O K-edge x-ray absorption spectra of ice is investigated through detailed analysis of the spectral features. The amount of ice defects is found to be minimized on hydrophobic surfaces, such as BaF{sub 2}(111), with low concentration of nucleation centers. This is manifested through a reduction of the absorption cross-section at 535 eV, which is associated with distorted hydrogen bonds. Furthermore, a connection is made between the observed increase in spectral intensity between 544 and 548 eV and high-symmetry points in the electronic band structure, suggesting a more extended hydrogen-bond network as compared to ices prepared differently. The spectral differences for various ice preparations are compared to the temperature dependence of spectra of liquid water upon supercooling. A double-peak feature in the absorption cross-section between 540 and 543 eV is identified as a characteristic of the crystalline phase. The connection to the interpretation of the liquid phase O K-edge x-ray absorption spectrum is extensively discussed.
Total Absorption Study of Beta Decays Relevant for Nuclear Applications and Nuclear Structure
An overview is given of our activities related to the study of the beta decay of neutron rich nuclei relevant for nuclear applications. Recent results of the study of the beta decay of {sup 87,88}Br using a new segmented total absorption spectrometer are presented. The measurements were performed at the IGISOL facility using trap-assisted total absorption spectroscopy.
Modular Total Absorption Spectrometer at the HRIBF (ORNL, Oak Ridge)
The Modular Total Absorption Spectrometer (MTAS) array has been designed, constructed, characterized, and applied to the decay studies of {sup 238}U fission products at the Holifield Radioactive Ion Beam Facility (HRIBF) at Oak Ridge National Laboratory. A MTAS commissioning run was performed in January 2012 at the mass separator on-line to the HRIBF Tandem accelerator. Preliminary results of MTAS data confirm known decay patterns of {sup 142}Ba and {sup 142}La deduced from an earlier study using a total absorption spectrometer technique.
Efficient Algorithms for Estimating the Absorption Spectrum within Linear Response TDDFT
We present a special symmetric Lanczos algorithm and a kernel polynomial method (KPM) for approximating the absorption spectrum of molecules within the linear response time-dependent density functional theory (TDDFT) framework in the product form. In contrast to existing algorithms, the new algorithms are based on reformulating the original non-Hermitian eigenvalue problem as a product eigenvalue problem and the observation that the product eigenvalue problem is self-adjoint with respect to an appropriately chosen inner product. This allows a simple symmetric Lanczos algorithm to be used to compute the desired absorption spectrum. The use of a symmetric Lanczos algorithm only requires half of the memory compared with the nonsymmetric variant of the Lanczos algorithm. The symmetric Lanczos algorithm is also numerically more stable than the nonsymmetric version. The KPM algorithm is also presented as a low-memory alternative to the Lanczos approach, but the algorithm may require more matrix-vector multiplications in practice. We discuss the pros and cons of these methods in terms of their accuracy as well as their computational and storage cost. Applications to a set of small and medium-sized molecules are also presented.
Broadband antireflection and absorption enhancement of ultrathin silicon solar microcells enabled with density-graded surface nanostructures
Density-graded surface nanostructures are implemented on ultrathin silicon solar microcells by silver-nanoparticle-catalyzed wet chemical etching to enable near-zero surface reflection over a broad wavelength range of incident solar spectrum as well as non-zeroth order diffraction and light trapping for longer wavelength photons, thereby achieving augmented photon absorption for ultrathin silicon microcells in a simple, cost-effective manner. The increase of absorbed photon flux through the “black silicon (b-Si)” surface translates directly into the corresponding enhancement of photovoltaic performance, where 5.7-μm b-Si microcells with the rational design of device configuration exhibit improved energy conversion efficiency by 148% and 50% with and without a diffuse backside reflector, respectively, compared to devices from the bare silicon without b-Si implementation. Systematic studies on nanostructured morphology, optical and electrical properties of b-Si microcells, together with semi-empirical numerical modeling of photon absorption, provide key aspects of underlying materials science and physics.
Förster resonance energy transfer, absorption and emission spectra in multichromophoric systems. III. Exact stochastic path integral evaluation
A numerically exact path integral treatment of the absorption and emission spectra of open quantum systems is presented that requires only the straightforward solution of a stochastic differential equation. The approach converges rapidly enabling the calculation of spectra of large excitonic systems across the complete range of system parameters and for arbitrary bath spectral densities. With the numerically exact absorption and emission operators, one can also immediately compute energy transfer rates using the multi-chromophoric Förster resonant energy transfer formalism. Benchmark calculations on the emission spectra of two level systems are presented demonstrating the efficacy of the stochastic approach. This is followed by calculations of the energy transfer rates between two weakly coupled dimer systems as a function of temperature and system-bath coupling strength. It is shown that the recently developed hybrid cumulant expansion (see Paper II) is the only perturbative method capable of generating uniformly reliable energy transfer rates and emission spectra across a broad range of system parameters.
Integrated three-dimensional photonic nanostructures for achieving near-unity solar absorption and superhydrophobicity
In this paper, we proposed and realized 3D photonic nanostructures consisting of ultra-thin graded index antireflective coatings (ARCs) and woodpile photonic crystals. The use of the integrated ARC and photonic crystal structure can achieve broadband, broad-angle near unity solar absorption. The amorphous silicon based photonic nanostructure experimentally shows an average absorption of ∼95% for λ = 400–620 nm over a wide angular acceptance of θ = 0°–60°. Theoretical studies show that a Gallium Arsenide (GaAs) based structure can achieve an average absorption of >95% for λ = 400–870 nm. Furthermore, the use of the slanted SiO{sub 2} nanorod ARC surface layer by glancing angle deposition exhibits Cassie-Baxter state wetting, and superhydrophobic surface is obtained with highest water contact angle θ{sub CB} ∼ 153°. These properties are fundamentally important for achieving maximum solar absorption and surface self-cleaning in thin film solar cell applications.
Dramatic enhancement of near-infrared intersubband absorption in c-plane AlInN/GaN superlattices
We report substantial improvement of near-infrared (2–2.6 μm) intersubband absorption in c-plane AlInN/GaN superlattices grown by molecular beam epitaxy. Progress was obtained through optimization of AlInN growth conditions using an AlInN growth rate of 0.9-nm/min at substrate temperature of 550 °C, as well as by judiciously placing the charge into two delta-doping sheets. Structural characterization suggests that AlInN crystal quality is enhanced and interface roughness is reduced. Importantly, near-infrared absorption data indicate that the optical quality of the AlInN/GaN superlattices is now comparable with that of AlN/GaN superlattices designed to exploit near-infrared intersubband transitions.
Ab Initio Methods for L-edge X-ray Absorption Spectroscopy
The theoretical prediction of X-ray absorption spectra (XAS) has become common- place in electronic structure theory. The ability to better model and understand L-edge spectra is of great interest in the study of transition metal complexes and a wide variety of solid state materials. However, until recently few rst-principles works have mod- eled L-edge XAS due to the presence of strong spin-orbit coupling in the 2p orbitals which splits the observed peaks into multiple groups of features. Therefore, a proper description of spin-orbit coupling is vital for the successful prediction of L-edge spectra. A number of new approaches that incorporate spin-orbit coupling have recently made advances in the computation of L-edge spectra. In this review, we describe recent work in computational L-edge XAS and how these methods may continue to improve in the future. Comparison of the advantages and disadvantages of the various approaches are considered, with special attention to not only the computational cost of the level of theory, but also the various approaches that can be used to compute the absorption spectra with a large number of high energy excited states.
A comprehensive study of broad absorption line quasars. i. Prevalence of He i* absorption line multiplets in low-ionization objects
Neutral helium multiplets, He i* λλ3189,3889,10830, are very useful diagnostics for the geometry and physical conditions of the absorbing gas in quasars. So far only a handful of He i* detections have been reported. Using a newly developed method, we detected the He i*λ3889 absorption line in 101 sources of a well-defined sample of 285 Mg ii broad absorption line (BAL) quasars selected from SDSS DR5. This has increased the number of He i* BAL quasars by more than one order of magnitude. We further detected He i*λ3189 in 50% (52/101) of the quasars in the sample. The detection fraction of He i* BALs in Mg ii BAL quasars is ∼35% as a whole, and it increases dramatically with increasing spectral signal-to-noise ratio (S/N), from ∼18% at S/N ⩽ 10 to ∼93% at S/N ⩾ 35. This suggests that He i* BALs could be detected in most Mg ii LoBAL quasars, provided the spectra S/N is high enough. Such a surprisingly high He i* BAL fraction is actually predicted from photoionization calculations based on a simple BAL model. The result indicates that He i* absorption lines can be used to search for BAL quasars at low z, which cannot be identified by ground-based optical spectroscopic surveys with commonly seen UV absorption lines. Using He i* λ3889, we discovered 19 BAL quasars at z<0.3 from the available SDSS spectral database. The fraction of He i* BAL quasars is similar to that of LoBAL objects.
Enabling liquid solvent structure analysis using hard x-ray absorption spectroscopy with a transferrable microfluidic reactor
In this study, a vacuum compatible microfluidic device, system for analysis at the liquid vacuum interface, is integrated to hard x-ray absorption spectroscopy to obtain the local structure of K 3 [Fe(CN) 6 ] in aqueous solutions with three concentrations of 0.5 M, 0.05 M, and 0.005 M. The solutions were sealed in a microchannel 500 µm wide and 300 µm deep in a portable microfluidic device. The Fe K-edge x-ray absorption spectra indicate a presence of Fe(III) in the complex in water, with an octahedral geometry coordinated with 6 C atoms in the first shell with a distance of ~1.92 Å and 6 N atoms in the second shell with a distance of ~3.10 Å. Varying the concentration has no observable influence on the structure of K 3 [Fe(CN) 6 ]. Our results demonstrate the feasibility of using microfluidic based liquid cells in large synchrotron facilities. Using portable microfludic reactors provides a viable approach to enable multifaceted measurements of liquids in the future.
Atomic Layer Deposition of Vanadium Oxide to Reduce Parasitic Absorption and Improve Stability in n-i-p Perovskite Solar Cells for Tandems
Two critical issues associated with semi-transparent, n-i-p perovskite solar cells for 2-terminal tandem devices are parasitic absorption and long-term instability associated with the widely used spiro-OMeTAD and MoOx hole transport and buffer layers, respectively. In this work, we present an alternative hole contact bilayer that consists of a 30 nm undoped layer of spiro-TTB in conjunction with 9 nm of air-stable vanadium oxide (VOx) deposited via atomic layer deposition. The low absorption of UV and visible light in this bilayer results in the fabrication of a semi-transparent perovskite cell with 18.9 mA cm-2 of photocurrent, a 14% increase compared to the 16.6 mA cm-2 generated in a control device with 150 nm of doped spiro-OMeTAD. The ALD VOx buffer layer shows promise as a stable alternative to MoOx; an unencapsulated Cs0.17FA0.83Pb(Br0.17I0.83)3 device with ALD VOx and ITO as the top contact maintains its efficiency following 1000 hours at 85 degrees C in a N2 environment. Lastly, we use transfer matrix modeling of the optimized perovskite stack to predict its optical performance in a monolithic tandem cell with heterojunction silicon.
Toward inverse backscatter absorption gas imaging: imaging a dry gas plume with ambient H 2 O absorption
This paper introduces inverse backscatter absorption gas imaging (iBAGI), a transparent gas imaging technique based on absorption spectroscopy of gases naturally present in ambient air being displaced by transparent gases. We demonstrate reconstruction of a 2-D image of a dry gas plume by measuring light of a raster-scanned diode laser tuned to an absorption line of atmospheric H 2 O. We quantify the performance depending on the distance to the backdrop and show that the key transmission metric is independent of absorption path length. We conclude with an outlook toward calibration-free, single-ended iBAGI using scattering from low-reflectivity backdrops.