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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 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

Femtosecond laser diagnostics of the built-in electric field across the p{sup +}-Si/SiO{sub 2} interface and its ultrafast shielding

Ultrafast shielding of the built-in electric field E{sub 0} across the p{sup +}-Si/SiO{sub 2} interface of boron doped Si upon near infrared femtosecond (fs) laser pulse irradiation (73 {+-} 5 fs, 35 GW/cm{sup 2}{<=} I{sub peak}{sup ({omega})} {<=} 115 GW/cm{sup 2}) is shown to be dominated by electron-hole (e-h) pairs generated via two-photon absorption (TPA), whereas contributions from one-photon absorption (OPA) appear negligible. E{sub 0} shows up in the instantaneous signal I{sup (2{omega})}(t Almost-Equal-To 0) Almost-Equal-To I{sup (2{omega})}(E{sub 0}) of the Electric Field Induced Second Harmonic (EFISH). Its power law is derived from the linear log I{sup (2{omega})}(E{sub 0}) vs. log (I{sub peak}{sup ({omega})}){sup n} plots of six fs laser wavelengths 741.2 nm {<=} {lambda} {<=} 801.0 nm for the first time. These reveal 1.2 {<=} n({lambda}) {<=} 2.1 with the minimum at {lambda} = 752.4 nm (2h{nu} = 3.3 eV) related to resonantly enhanced TPA. Shielding of E{sub 0} by e-h pairs from OPA cannot be detected by EFISH in the same fs laser pulse as their generation requires relatively slow electron-phonon coupling.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Measurement of electron beam polarization from unstrained GaAs via two-photon photoemission

Two-photon absorption of 1560 nm light was used to generate polarized electron beams from unstrained GaAs photocathodes of varying thickness: 625 {mu}m, 0.32 {mu}m, and 0.18 {mu}m. For each photocathode, the degree of spin polarization of the photoemitted beam was less than 50%, contradicting earlier predictions based on simple quantum mechanical selection rules for spherically-symmetric systems but consistent with the more sophisticated model of Bhat et al. (Phys. Rev. B 71 (2005) 035209). Polarization via two-photon absorption was the highest from the thinnest photocathode sample and comparable to that obtained via one-photon absorption (using 778 nm light), with values 40.3 +- 1.0% and 42.6 +- 1.0%, respectively.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Can quantum coherent solar cells break detailed balance?

Carefully engineered coherent quantum states have been proposed as a design attribute that is hypothesized to enable solar photovoltaic cells to break the detailed balance (or radiative) limit of power conversion efficiency by possibly causing radiative recombination to be suppressed. However, in full compliance with the principles of statistical mechanics and the laws of thermodynamics, specially prepared coherent quantum states do not allow a solar photovoltaic cell—a quantum threshold energy conversion device—to exceed the detailed balance limit of power conversion efficiency. At the condition given by steady-state open circuit operation with zero nonradiative recombination, the photon absorption rate (or carrier photogeneration rate) must balance the photon emission rate (or carrier radiative recombination rate) thus ensuring that detailed balance prevails. Quantum state transitions, entropy-generating hot carrier relaxation, and photon absorption and emission rate balancing are employed holistically and self-consistently along with calculations of current density, voltage, and power conversion efficiency to explain why detailed balance may not be violated in solar photovoltaic cells.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Estimation of the extragalactic background light using TeV observations of BL Lac objects

The very high-energy (VHE) gamma-ray spectral index of high-energy peaked blazars correlates strongly with its corresponding redshift, whereas no such correlation is observed in the X-ray or GeV bands. We attribute this correlation to photon-photon absorption of TeV photons with the extragalactic background light (EBL), and utilizing this we compute the allowed flux range for the EBL, which is independent of previous estimates. The observed VHE spectrum of the sources in our sample can be well approximated by a power law, and if the de-absorbed spectrum is also assumed to be a power law, then we show that the spectral shape of EBL will be εn(ε) ∼ klog (ε/ε {sub p}). We estimate the range of values for the parameters defining the EBL spectrum, k and ε {sub p}, such that the correlation of the intrinsic VHE spectrum with redshift is nullified. The estimated EBL depends only on the observed correlation and the assumption of a power-law source spectrum. Specifically, it does not depend on the spectral modeling or radiative mechanism of the sources or on any theoretical shape of the EBL spectrum obtained through cosmological calculations. The estimated EBL spectrum is consistent with the upper and lower limits imposed by different observations. Moreover, it also agrees closely with the theoretical estimates obtained through cosmological evolution models.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS2004

Development of Thermally Stable and Highly Fluorescent IR Dyes

Fluorophores are the core component in various optical applications such as sensors and probes. Fluorphores with low-energy or long wavelength emission, in particular, in NIR region, possess advantages of low interference and high sensitivity. In this study, we has explored several classes of imidazole-based compounds for NIR fluorescent properties and concluded: (1) thiazole-based imidazole compounds are fluorescent; (2) emission energy is tunable by additional donor groups; (3) they also possess impressive two- photon absorption properties; and (4) fluorescence emission can be induced by two- photon input. This report summarizes (1) synthesis of new series of fluorophore; (2) impact of electron-withdrawing groups on fluorescent property; (3) unique property of two-photon absorption; and (4) on-going development.

Bu, Xiu R.↗
DOE OSTI2017

Charge Transfer from Carbon Nanotubes to Silicon in Flexible Carbon Nanotube/Silicon Solar Cells

Mechanical fragility and insufficient light absorption are two major challenges for thin flexible crystalline Si-based solar cells. Flexible hybrid single-walled carbon nanotube (SWNT)/Si solar cells are demonstrated by applying scalable room-temperature processes for the fabrication of solar-cell components (e.g., preparation of SWNT thin films and SWNT/Si p–n junctions). The flexible SWNT/Si solar cells present an intrinsic efficiency ≈7.5% without any additional light-trapping structures. By using these solar cells as model systems, the charge transport mechanisms at the SWNT/Si interface are investigated using femtosecond transient absorption. Although primary photon absorption occurs in Si, transient absorption measurements show that SWNTs also generate and inject excited charge carriers to Si. Such effects can be tuned by controlling the thickness of the SWNTs. Thus, findings from this study could open a new pathway for designing and improving the efficiency of photocarrier generation and absorption for high-performance ultrathin hybrid SWNT/Si solar cells.

14 SOLAR ENERGY↗
DOE OSTI2019

Emerging Design Principles for Enhanced Solar Energy Utilization with Singlet Fission

Singlet fission (SF), the generation of two triplet excitons per the absorption of one photon, is a promising strategy for increasing the efficiency of solar cells beyond the theoretical Shockley-Queisser limit of 34%. Upon photon absorption by a SF molecule, the initially created singlet excited state (S1) interacts with a neighboring chromophore and is first transformed into a triplet pair (TT), which can be subsequently separated into independent triplet excitons (2T1). These independent triplet excitons can be harvested through triplet charge extraction or triplet energy transfer to an acceptor. Research on SF systems has revealed rates and efficiencies of triplet formation and triplet pair decorrelation that are strongly dependent on interchromophore coupling, which is dictated by molecular structure and the resulting geometrical arrangement of chromophores adopted in covalent (e.g., dimers) and noncovalent (e.g., films and crystals) systems. Incorporation of SF materials into realistic device architectures introduces a host of new challenges to consider regarding the efficient extraction of triplets generated through SF. In this Feature Article, we review our work that has led to some degree of understanding and control of inter- and intramolecular SF rates placed in the context of solar energy harvesting architectures, including dye-sensitized solar cells, conjugated polymer films, and ligand-exchanged quantum dots. We emphasize the importance of understanding and manipulating interactions between SF molecules with each other and with the charge or energy collectors across an interface in order to strike a kinetic balance that leads to efficient utilization of triplet excitons.

14 SOLAR ENERGY↗
DOE OSTI2021

Mechanism and dynamics of fatty acid photodecarboxylase

Photoenzymes are rare biocatalysts driven by absorption of a photon at each catalytic cycle; they inspire development of artificial photoenzymes with valuable activities. Fatty acid photodecarboxylase (FAP) is a natural photoenzyme that has potential applications in the bio-based production of hydrocarbons, yet its mechanism is far from fully understood. RATIONALE To elucidate the mechanism of FAP, we studied the wild-type (WT) enzyme from Chlorella variabilis (CvFAP) and variants with altered active-site residues using a wealth of techniques, including static and time-resolved crystallography and spectroscopy, as well as biochemical and computational approaches. RESULTS A 1.8-Å-resolution CvFAP x-ray crystal structure revealed a dense hydrogen-bonding network positioning the fatty acid carboxyl group in the vicinity of the flavin adenine dinucleotide (FAD) cofactor. Structures solved from free electron laser and low-dose synchrotron x-ray crystal data further highlighted an unusual bent shape of the oxidized flavin chromophore, and showed that the bending angle (14°) did not change upon photon absorption (step 1) or throughout the photocycle. Calculations showed that bending substantially affected the energy levels of the flavin. Structural and spectroscopic analysis of WT and mutant proteins targeting two conserved active-site residues, R451 and C432, demonstrated that both residues were crucial for proper positioning of the substrate and water molecules and for oxidation of the fatty acid carboxylate by 1 FAD* (~300 ps in WT FAP) to form FAD ∙– (step 2). Time-resolved infrared spectroscopy demonstrated that decarboxylation occured quasi-instantaneously upon this forward electron transfer, consistent with barrierless bond cleavage predicted by quantum chemistry calculations and with snapshots obtained by time-resolved crystallography. Transient absorption spectroscopy in H 2 O and D 2 O buffers indicated that back electron transfer from FAD ∙– was coupled to and limited by transfer of an exchangeable proton or hydrogen atom (step 3). Unexpectedly, concomitant with FAD ∙– reoxidation (to a red-shifted form FAD RS ) in 100 ns, most of the CO 2 product was converted, most likely into bicarbonate (as inferred from FTIR spectra of the cryotrapped FAD RS intermediate). Calculations indicated that this catalytic transformation involved an active-site water molecule. Cryo-Fourier transform infrared spectroscopy studies suggested that bicarbonate formation (step 4) was preceded by deprotonation of an arginine residue (step 3). At room temperature, the remaining CO 2 left the protein in 1.5 μs (step 4'). The observation of residual electron density close to C432 in electron density maps derived from time-resolved and cryocrystallography data suggests that this residue may play a role in stabilizing CO 2 and/or bicarbonate. Three routes for alkane formation were identified by quantum chemistry calculations; the one shown in the figure is favored by the ensemble of experimental data. CONCLUSION Finally, we provide a detailed and comprehensive characterization of light-driven hydrocarbon formation by FAP, which uses a remarkably complex mechanism including unique catalytic steps. We anticipate that our results will help to expand the green chemistry toolkit.

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

Measurements of atoms and metastable species in N 2 and H 2 –N 2 nanosecond pulse plasmas

We report time-resolved, absolute number densities of metastable N 2 (A 3 Σ u + , v = 0, 1) molecules, ground state N 2 and H atoms, and rotational–translational temperature have been measured by tunable diode laser absorption spectroscopy and two-photon absorption laser-induced fluorescence in diffuse N 2 and N 2 –H 2 plasmas during and after a nanosecond pulse discharge burst. Comparison of the measurement results with the kinetic modeling predictions, specifically the significant reduction of the N 2 (A 3 Σ u + ) populations and the rate of N atom generation during the burst, suggests that these two trends are related. The slow N atom decay in the afterglow, on a time scale longer than the discharge burst, demonstrates that the latter trend is not affected by N atom recombination, diffusion to the walls, or convection with the flow. This leads to the conclusion that the energy pooling in collisions of N 2 (A 3 Σ u + ) molecules is a major channel of N 2 dissociation in electric discharges where a significant fraction of the input energy goes to electronic excitation of N 2 . Additional measurements in a 1% H 2 –N 2 mixture demonstrate a further significant reduction of N 2 (A 3 Σ u + , v = 0, 1) populations, due to the rapid quenching by H atoms accumulating in the plasma. Comparison with the modeling predictions suggests that the N 2 (A 3 Σ u + ) molecules may be initially formed in the highly vibrationally excited states. The reduction of the N 2 (A 3 Σ u + ) number density also diminishes the contribution of the energy pooling process into N2 dissociation, thus reducing the N atom number density. The rate of N atom generation during the burst also decreases, due to its strong coupling to N 2 (A 3 Σ u + , v) populations. On the other hand, the rate of H atom generation, produced predominantly by the dissociative quenching of the excited electronic states of N 2 by H 2 , remains about the same during the burst, resulting in a nearly linear rise in the H atom number density. Comparison of the kinetic model predictions with the experimental results suggests that the yield of H atoms during the quenching of the excited electronic state of N 2 by molecular H 2 is significantly less than 100%. The present results quantify the yield of N and H atoms in high-pressure H 2 –N 2 plasmas, which have significant potential for ammonia generation using plasma-assisted catalysis

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
NASA NTRS1977

Double resonance spectroscopy of multiple-photon excited molecules

Multiple infrared photon absorption is a quite general process which molecules can undergo when placed in a high flux of infrared energy, such as the focussed beam of a CO2 laser. In order to understand how this process works, one must be able to follow the evolution of the molecules through their internal states, populated by photon absorption. Double-resonance spectroscopy is the method of a choice for getting at this information. A system pumped by CO2 laser radiation can be examined with a tunable laser probe beam, such as that from a lead-salt diode laser. From such an experiment, one can directly observe Rabi modulation of the absorption lines, determine elementary state-to-state relaxation pathways, and locate higher excited vibrational states. Systems currently under investigation include SF6 and vinyl chloride. In suitable cases, the probe beam can be a tunable visible or UV source, such as a dye laser. Fluorescence spectroscopy can then be used to monitor the transient absorptions produced by multiple-photon excitation. Among the systems which can be examined are biacetyl and glyoxal.

Steinfeld, J. I.↗
DOE OSTI2015

Enhanced absorption in two-dimensional materials via Fano-resonant photonic crystals

The use of two-dimensional (2D) materials in optoelectronics has attracted much attention due to their fascinating optical and electrical properties. However, the low optical absorption of 2D materials arising from their atomic thickness limits the maximum attainable external quantum efficiency. For example, in the visible and near-infrared regimes monolayer MoS{sub 2} and graphene absorb only ∼10% and 2.3% of incoming light, respectively. Here, we experimentally demonstrate the use of Fano-resonant photonic crystals to significantly boost absorption in atomically thin materials. Using graphene as a test bed, we demonstrate that absorption in the monolayer thick material can be enhanced to 77% within the telecommunications band, the highest value reported to date. We also show that the absorption in the Fano-resonant structure is non-local, with light propagating up to 16 μm within the structure. This property is particularly beneficial in harvesting light from large areas in field-effect-transistor based graphene photodetectors in which separation of photo-generated carriers only occurs ∼0.2 μm adjacent to the graphene/electrode interface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Size dependent nonlinear optical properties of YCrO{sub 3} nanosystems

We report size-dependent optical limiting response of YCrO{sub 3} nanosystems upon illumination by nanosecond laser pulses at 532 nm. The limiting properties were investigated using the open aperture z-scan technique. Three-photon absorption coefficient is found to increase with particle size within the range of our investigations. We propose that the obtained nonlinearity is caused by two photon absorption, followed by excited state absorption.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

An analytical model for analyzing the current-voltage characteristics of bulk heterojunction organic solar cells

An analytical model for analyzing the current-voltage (J-V) characteristics of bulk heterojunction (BHJ) organic solar cells is developed by incorporating exponential photon absorption, dissociation efficiency of bound electron-hole pairs (EHPs), carrier trapping, and carrier drift and diffusion in the photon absorption layer. Modified Braun's model is used to compute the electric field-dependent dissociation efficiency of the bound EHPs. The charge carrier concentrations and hence the photocurrent are calculated by solving the carrier continuity equation for both holes and electrons in the organic layer. The overall load current is calculated considering the actual solar spectrum and voltage dependent forward dark current. The model is verified by published experimental results. The efficiency of the P3HT:PCBM based solar cells critically depends on the dissociation of bound EHPs. On the other hand, cells made of a blend of the conjugated polymer (PCDTBT) with the soluble fullerene derivative (PCBM) show nearly unity dissociation efficiency, and their cell efficiency strongly depends on the charge collection efficiency. The effects of carrier lifetimes on the performance of PCDTBT solar cells have also been studied. The model is also used to investigate the effect of titanium oxide (TiO{sub x}) layer (at the back contact) on the J-V characteristics of PCDTBT solar cells. The results of this paper indicate that improvement of charge carrier transport in PCDTBT:PCBM blend and dissociation of bound EHPs in P3HT:PCBM blend are extremely important to increase the power conversion efficiency of the respective BHJ solar cells.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Effect of electric field on carrier escape mechanisms in quantum dot intermediate band solar cells

Carrier escape and recombination from quantum dot (QD) states reduce the probability of two-step photon absorption (TSPA) by decreasing the available carrier population in the intermediate band (IB). In order to optimize the second photon absorption for future designs of quantum dot embedded intermediate band solar cells, this study combined the results of simulations and experiments to quantify the effect of electric field on the barrier height and the carrier escape from the QDs in InAs/GaAs quantum dot solar cells with five-layer QD superlattices. The electric field dependent effective barrier heights for ground state electrons were calculated using eight band k·p theory at short circuit conditions. With an increase in electric field surrounding the QDs from 5 kV/cm to 50 kV/cm, the effective barrier height of the ground state electrons was reduced from 147 meV to 136 meV, respectively. Thus, the increasing electric field not only exponentially enhances the ground state electron tunneling rate (effectively zero at 5 kV/cm and 7.9 × 10 6 s -1 at 50 kV/cm) but also doubles the thermal escape rate (2.2 × 10 11 s -1 at 5 kV/cm and 4.1 × 10 11 s -1 at 50 kV/cm). Temperature-dependent external quantum efficiency measurements were performed to verify that the increasing electric field decreases the effective barrier height. Additionally, the electric field dependent radiative lifetimes of the ground state were characterized with time-resolved photoluminescence experiments. This study showed that the increasing electric field extended the radiative recombination lifetime in the ground state of the QDs as a consequence of the reduced wave-function overlap between the electrons and holes. The balance of carrier escape and recombination determines the probability of TSPA.

14 SOLAR ENERGY↗
DOE OSTI2018

Propagation of a Self-Similar Pulse in a Medium with One-Photon Transient Absorption

The shape of an optical self-similar pulse that propagates in a medium of finite length with noninstantaneous nonlinear absorption is found analytically. The pulse has an asymmetric shape and, in addition, frequency modulation, which confirms that it belongs to a new type of self-similar propagation modes of laser radiation—chirped pulses with a self-similar shape. The existence of pulses of this kind is also confirmed by results of computer simulation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2017

Opacity from two-photon processes

Here, the recent iron opacity measurements performed at Sandia National Laboratory by Bailey and collaborators have raised questions about the completeness of the physical models normally used to understand partially ionized hot dense plasmas. We describe calculations of two-photon absorption, which is a candidate for the observed extra opacity. Our calculations do not yet match the experiments but show that the two-photon absorption process is strong enough to require careful consideration.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2019

Photoelectrochemical water splitting using strain-balanced multiple quantum well photovoltaic cells

Starting from the classical GaInP/GaAs tandem photoelectrochemical water splitting device, higher solar-to-hydrogen efficiencies can be pursued by extending photon absorption to longer wavelengths. We incorporate strain-balanced GaInAs/GaAsP quantum wells into the bottom GaAs junction, to increase the range of photon absorption. The inclusion of 1.34 eV quantum wells in the depletion region of the bottom cell extends the absorption edge to 930 nm. With a corresponding increase in the thickness of the top cell for current matching, the light-limiting photocurrent increases by >8%. The estimated solar-to-hydrogen efficiency is 13.6 ± 0.5%, and we show a pathway to further improvement. With the semiconductor device remaining on the growth substrate, this quantum well architecture may enable improved stability and durability of the photoelectrochemical electrodes.

14 SOLAR ENERGY↗
DOE OSTI2016

Internal transmission coefficient in charges carrier generation layer of graphene/Si based solar cell device

Internal transmission profile in charges carrier generation layer of graphene/Si based solar cell has been explored theoretically. Photovoltaic device was constructed from graphene/Si heterojunction forming a multilayer stuck with Si as generation layer. The graphene/Si sheet was layered on ITO/glass wafer then coated by Al forming Ohmic contact with Si. Photon incident propagate from glass substrate to metal electrode and assumed that there is no transmission in Al layer. The wavelength range spectra used in this calculation was 200 – 1000 nm. It found that transmission intensity in the generation layer show non-linear behavior and partitioned by few areas which related with excitation process. According to this information, it may to optimize the photons absorption to create more excitation process by inserting appropriate material to enhance optical properties in certain wavelength spectra because of the exciton generation is strongly influenced by photon absorption.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗