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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 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

Photoswitchable Molecular Rings for Solar-Thermal Energy Storage

Solar-thermal fuels reversibly store solar energy in the chemical bonds of molecules by photoconversion, and can release this stored energy in the form of heat upon activation. Many conventional photoswichable molecules could be considered as solar thermal fuels, although they suffer from low energy density or short lifetime in the photoinduced high-energy metastable state, rendering their practical use unfeasible. We present a new approach to the design of chemistries for solar thermal fuel applications, wherein well-known photoswitchable molecules are connected by different linker agents to form molecular rings. This approach allows for a significant increase in both the amount of stored energy per molecule and the stability of the fuels. Our results suggest a range of possibilities for tuning the energy density and thermal stability as a function of the type of the photoswitchable molecule, the ring size, or the type of linkers.

Durgun, E↗
DOE OSTI2016

Tuning the driving force for exciton dissociation in single-walled carbon nanotube heterojunctions

Understanding the kinetics and energetics of interfacial electron transfer in molecular systems is crucial for the development of a broad array of technologies, including photovoltaics, solar fuel systems and energy storage. The Marcus formulation for electron transfer relates the thermodynamic driving force and reorganization energy for charge transfer between a given donor/acceptor pair to the kinetics and yield of electron transfer. Here we investigated the influence of the thermodynamic driving force for photoinduced electron transfer (PET) between single-walled carbon nanotubes (SWCNTs) and fullerene derivatives by employing time-resolved microwave conductivity as a sensitive probe of interfacial exciton dissociation. For the first time, we observed the Marcus inverted region (in which driving force exceeds reorganization energy) and quantified the reorganization energy for PET for a model SWCNT/acceptor system. The small reorganization energies (about 130 meV, most of which probably arises from the fullerene acceptors) are beneficial in minimizing energy loss in photoconversion schemes.

14 SOLAR ENERGY↗
DOE OSTI2015

Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses

Ultrafast photoinduced electron transfer preceding energy equilibration still poses many experimental and conceptual challenges to the optimization of photoconversion since an atomic-scale description has so far been beyond reach. Here we combine femtosecond transient optical absorption spectroscopy with ultrafast X-ray emission spectroscopy and diffuse X-ray scattering at the SACLA facility to track the non-equilibrated electronic and structural dynamics within a bimetallic donor–acceptor complex that contains an optically dark centre. Exploiting the 100-fold increase in temporal resolution as compared with storage ring facilities, these measurements constitute the first X-ray-based visualization of a non-equilibrated intramolecular electron transfer process over large interatomic distances. Thus experimental and theoretical results establish that mediation through electronically excited molecular states is a key mechanistic feature. The present study demonstrates the extensive potential of femtosecond X-ray techniques as diagnostics of non-adiabatic electron transfer processes in synthetic and biological systems, and some directions for future studies, are outlined.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Ternary molecular switching in a single-crystal optical actuator with correlated crystal strain

A growing portfolio of single-crystal optical actuators is forging a new class of photonic materials that hold prospects for quantum technologies. Ruthenium-based complexes that exhibit this phenomenon via SO 2 -linkage photoisomerisation are of particular interest since they display multiple metastable states, once induced by green light; yet, complete photoconversion into each SO 2 -isomeric state is rarely achieved. We discover a new complex, trans-[Ru(SO 2 )(NH 3 ) 4 (4-bromopyridine)]tosylate 2 , that produces 100% photoconverted η 1 -OSO isomeric crystal structures at 90 K, which fully transition into η 2 -(OS)O photoisomers upon warming to 100 K, while the dark-state η 1 -SO 2 structure is wholly recovered by heating the crystal to room temperature. Crystal structures and optical-absorption profiles of each state are captured via in-situ light-induced single-crystal X-ray diffraction and optical-absorption spectroscopy. Results show that both photoisomeric species behave as optical switches, but with distinct optical properties. The photoisomerisation process causes thermally-reversible micro- and nanoscopic crystal strain, as characterised by optical microscopy and in-situ light-induced atomic-force microscopy.

actuators↗
DOE OSTI2020

Singlet fission for quantum information and quantum computing: the parallel JDE model

Abstract Singlet fission is a photoconversion process that generates a doubly excited, maximally spin entangled pair state. This state has applications to quantum information and computing that are only beginning to be realized. In this article, we construct and analyze a spin-exciton hamiltonian to describe the dynamics of the two-triplet state. We find the selection rules that connect the doubly excited, spin-singlet state to the manifold of quintet states and comment on the mechanism and conditions for the transition into formally independent triplets. For adjacent dimers that are oriented and immobilized in an inert host, singlet fission can be strongly state-selective. We make predictions for electron paramagnetic resonance experiments and analyze experimental data from recent literature. Our results give conditions for which magnetic resonance pulses can drive transitions between optically polarized magnetic sublevels of the two-exciton states, making it possible to realize quantum gates at room temperature in these systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Probing excitonic states in suspended two-dimensional semiconductors by photocurrent spectroscopy

The optical response of semiconducting monolayer transition-metal dichalcogenides (TMDCs) is dominated by strongly bound excitons that are stable even at room temperature. However, substrate-related effects such as screening and disorder in currently available specimens mask many anticipated physical phenomena and limit device applications of TMDCs. Here, we demonstrate that that these undesirable effects are strongly suppressed in suspended devices. Extremely robust (photogain > 1,000) and fast (response time < 1 ms) photoresponse allow us to study, for the first time, the formation, binding energies, and dissociation mechanisms of excitons in TMDCs through photocurrent spectroscopy. By analyzing the spectral positions of peaks in the photocurrent and by comparing them with first-principles calculations, we obtain binding energies, band gaps and spin-orbit splitting in monolayer TMDCs. For monolayer MoS2, in particular, we obtain an extremely large binding energy for band-edge excitons, Ebind ≥ 570 meV. Along with band-edge excitons, we observe excitons associated with a van Hove singularity of rather unique nature. In conclusion, the analysis of the source-drain voltage dependence of photocurrent spectra reveals exciton dissociation and photoconversion mechanisms in TMDCs.

36 MATERIALS SCIENCE↗
DOE OSTI2015

A scanning probe investigation of the role of surface motifs in the behavior of p-WSe 2 photocathodes

The spatial variation in the photoelectrochemical performance for the reduction of an aqueous one-electron redox couple, Ru(NH 3 ) 6 3+/2+ , and for the evolution of H 2 (g) from 0.5 M H 2 SO 4 (aq) at the surface of bare or Pt-decorated p-type WSe 2 photocathodes has been investigated in situ using scanning photocurrent microscopy (SPCM). The measurements revealed significant differences in the charge-collection performance (quantified by the values of external quantum yields, Φ ext ) on various macroscopic terraces. Local spectral response measurements indicated a variation in the local electronic structure among the terraces, which was consistent with a non-uniform spatial distribution of sub-band-gap states within the crystals. The photoconversion efficiencies of Pt-decorated p-WSe2 photocathodes were greater for the evolution of H 2 (g) from 0.5 M H 2 SO 4 than for the reduction of Ru(NH 3 ) 6 3+/2+ , and terraces that exhibited relatively low values of Φext for the reduction of Ru(NH 3 ) 6 3+/2+ could in some cases yield values of Φ ext for the evolution of H 2 (g) comparable to the values of Φ ext yielded by the highest-performing terraces. In conclusion, although the spatial resolution of the techniques used in this work frequently did not result in observation of the effect of edge sites on photocurrent efficiency, some edge effects were observed in the measurements; however the observed edge effects differed among edges, and did not appear to determine the performance of the electrodes.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Stacked Cu 1.8 S nanoplatelets as Counter Electrode for Quantum Dot-Sensitized Solar Cell

It is found that electrocatalytic activity of Cu 2-x S thin films used in quantum dots sensitized solar cells (QDSSC) as countner electrode (CE) for the reduction of polysulfide electrolyte depends on the the surface active sulfur species and defficiency of Cu. The preferential bonding between Cu 2+ and S 2- leading to the selective formation of Cu 1.8 S stacked platelets like morphology is determined by Cetyl Trimethyl Ammonium Bromide surfactant with temperature and crab like Cu-S coordination bond formed dictates the surface area to volume ratio of the Cu 1.8 S thin films and the electrocatalytic activity. The Cu deficiency enhances the conductivity of the Cu 1.8 S thin films and exhibits near- infrared localized surface plasmon resonanc due to free carrier intraband absorption and UV-VIS absorption spectra shows excitonic effect due to quantum size effect. When these Cu 1.8 S thin films were employed as CE in QDSSC, robust photoconversion efficiency of 5.2 % is yielded by the film deposited at 60°C by a sinlge step chemical bath deposition method.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2018

A new family of fullerene derivatives: fullerene-curcumin conjugates for biological and photovoltaic applications

The synthesis and characterization of a family of [60]fullerocurcuminoids obtained via Bingel reactions is reported. The new C 60 derivatives include curcumin and curcuminoids with a variety of end groups. Preliminary biological experiments show the potential activity of the compound containing a curcumin addend, which exhibits moderate anti-HIV-1 and radical scavenger properties, but no anti-cancer activity. In addition, the new fullerocurcuminoids exhibit HOMO/LUMO energy levels that are reasonably matched with those of perovskites and when they were tested in perovskite solar cells (PSCs) as the electron transporting material (ETM), photoconversion efficiencies ranging from 14.04–14.95% were obtained, whereas a value of 16.23% was obtained for [6,6]-phenyl-C61-butyric acid methyl ester (PC 61 BM) based devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Effect of nanotube coupling on exciton transport in polymer-free monochiral semiconducting carbon nanotube networks

Semiconducting single-walled carbon nanotubes (s-SWCNTs) are attractive light-harvesting components for solar photoconversion schemes and architectures, and selective polymer extraction has emerged as a powerful route to obtain highly pure s-SWCNT samples for electronic applications. Here we demonstrate a novel method for producing electronically coupled thin films of near-monochiral s-SWCNTs without wrapping polymer. Detailed steady-state and transient optical studies on such samples provide new insights into the role of the wrapping polymer on controlling intra-bundle nanotube–nanotube interactions and exciton energy transfer within and between bundles. Complete removal of polymer from the networks results in rapid exciton trapping within nanotube bundles, limiting long-range exciton transport. The results suggest that intertube electronic coupling and associated exciton delocalization across multiple tubes can limit diffusive exciton transport. Here, the complex relationship observed here between exciton delocalization, trapping, and long-range transport, helps to inform the design, preparation, and implementation of carbon nanotube networks as active elements for optical and electronic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Irradiance and temperature considerations in the design and deployment of high annual energy yield perovskite/CIGS tandems

The annual energy yields for metal halide perovskite/copper indium gallium diselenide (CIGS) tandem photovoltaics have been calculated for 16 different bandgap combinations, using both 2 terminal and 4 terminal device designs, with fixed-tilt mounting as well as 1- and 2-axis tracking. Measured complex index of refraction data were used for the materials comprising the devices, and hourly irradiance data were extracted from Version 3 of the National Solar Radiation Database. Simulations were performed for Toledo OH, Golden CO, Phoenix AZ, and New Orleans LA, and the effect of local temperature variation was also considered. The combination of irradiance and temperature variations throughout the year cause different devices to be optimal at different times of the year. Interestingly, devices constructed to maximize AM1.5 photoconversion efficiency do not necessarily maximize the annual energy yield. A detailed analysis of the monthly energy yields at the different locations reveals the interplay between the changing light and temperature conditions. Over the course of the year these effects average to some degree so that annual energy yields that are close to the maximum possible value can be achieved by several different tandem device designs. The conclusions are valid for devices made with relatively thin perovskite layers, such as those used in champion efficiency devices. When the perovskite layers are thicker, however, the device is less tolerant to variation. Our results show that close matching of bandgap pairs is not essential for the fabrication of high-performance tandems. These findings should allow manufacturing efforts to proceed without the need for precise compositional control during formation of the absorber layers.

14 SOLAR ENERGY↗
DOE OSTI2026

Aliovalent gallium dopants remove Ti 3+ defects and improve photocatalytic and photoelectrochemical water oxidation properties of LaTiO 2 N

LaTiO 2 N is a promising semiconductor for the water splitting reaction due to its 2.1 eV band gap and stability against corrosion. However, its solar energy conversion is limited by Ti 3+ recombination defects introduced during ammonolysis. Here we show for the first time that Ti 3+ defects in LaTiO 2 N can be suppressed with incorporation of 2, 5, and 10% aliovalent gallium (Ga 3+ ) dopants during synthesis via the layered La 2 Ti 2 O 7 intermediate. Electron paramagnetic resonance (EPR) spectroscopy on the solid powders confirms a reduction in the Ti 3+ donor density from 2.97 × 10 17 cm −3 for the non-doped material to ∼6.24 × 10 16 cm −3 for 5% Ga-doped LaTiO 2 N. The remaining Ti 3+ defects are concentrated near the LaTiO 2 N surface, according to X-ray photoelectron spectroscopy. The defect reduction shifts the optical absorption edge from 2.02 to 2.09 eV and eliminates a broad absorption band at 1050 nm from the optical absorption spectra. It also removes a 1.0–1.7 eV sub-band gap photovoltage signal from surface photovoltage spectra. This suggests that empty Ti 3+ d-orbitals are located 1.0–1.7 eV above the LaTiO 2 N valence band edge. Removing these recombination states with increasing Ga 3+ content enhances the photoconversion efficiency of LaTiO 2 N during water oxidation. The optimized 2 wt% CoO x -loaded 5% Ga-doped LaTi O2 N material has a 16% AQE (400 nm) for O 2 production from aqueous silver nitrate solution and a ∼2.1 mA cm −2 water oxidation photocurrent at 1.23 V under 100 mW cm −2 Xe arc lamp illumination. The water oxidation photocurrent is stable during a 50 min test, and the Faraday efficiency for O 2 generation is 97%, confirming short-term corrosion stability of LaTiO 2 N. Altogether, these results provide a better understanding of the distribution, concentration, and impact of Ti 3+ defects on the optical, photovoltage, and photoelectrochemical properties of LaTiO 2 N. In combination with other defect control strategies, aliovalent Ga 3+ doping can help bring the solar energy conversion efficiency of LaTiO 2 N closer to the theoretical limit.

Wang, Li [University of California, Davis, CA (Uni↗
DOE OSTI2013

Layered insulator hexagonal boron nitride for surface passivation in quantum dot solar cell

Single crystalline, two dimensional (2D) layered insulator hexagonal boron nitride (h-BN), is demonstrated as an emerging material candidate for surface passivation on mesoporous TiO{sub 2}. Cadmium selenide (CdSe) quantum dot based bulk heterojunction (BHJ) solar cell employed h-BN passivated TiO{sub 2} as an electron acceptor exhibits photoconversion efficiency ∼46% more than BHJ employed unpassivated TiO{sub 2}. Dominant interfacial recombination pathways such as electron capture by TiO{sub 2} surface states and recombination with hole at valence band of CdSe are efficiently controlled by h-BN enabled surface passivation, leading to improved photovoltaic performance. Highly crystalline, confirmed by transmission electron microscopy, dangling bond-free 2D layered h-BN with self-terminated atomic planes, achieved by chemical exfoliation, enables efficient passivation on TiO{sub 2}, allowing electronic transport at TiO{sub 2}/h-BN/CdSe interface with much lower recombination rate compared to an unpassivated TiO{sub 2}/CdSe interface.

14 SOLAR ENERGY↗
DOE OSTI2015

Limiting efficiency calculation of silicon single-nanowire solar cells with considering Auger recombination

Single-nanowire solar cells (SNSCs) have attracted considerable attention due to their unique light-harvesting capability mediated by the optical antenna effect and the high photoconversion efficiency due to the orthogonalization of the carrier collection to the photon incidence. We present a detailed prediction of the light-conversion efficiency of Si SNSCs based on finite-element simulation and thermodynamic balance analysis, with especially focusing on the comparison between SNSCs and film systems. Carrier losses due to radiative and Auger recombinations are introduced in the analysis of the limiting efficiency, which show that the Auger recombination plays a key role in accurately predicting the efficiency of Si SNSCs, otherwise, the device performance would be strongly overestimated. The study paves a more realistic way to evaluate the nanostructured solar cells based on indirect-band photoactive materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Carbon quantum dots coated BiVO{sub 4} inverse opals for enhanced photoelectrochemical hydrogen generation

Carbon quantum dots (CQDs) coated BiVO{sub 4} inverse opal (io-BiVO{sub 4}) structure that shows dramatic improvement of photoelectrochemical hydrogen generation has been fabricated using electrodeposition with a template. The io-BiVO{sub 4} maximizes photon trapping through slow light effect, while maintaining adequate surface area for effective redox reactions. CQDs are then incorporated to the io-BiVO{sub 4} to further improve the photoconversion efficiency. Due to the strong visible light absorption property of CQDs and enhanced separation of the photoexcited electrons, the CQDs coated io-BiVO{sub 4} exhibit a maximum photo-to-hydrogen conversion efficiency of 0.35%, which is 6 times higher than that of the pure BiVO{sub 4} thin films. This work is a good example of designing composite photoelectrode by combining quantum dots and photonic crystal.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2015

Microscopy of hierarchically organized TiO{sub 2} photoelectrode for dye solar cells

Research on improving the performance of dye solar cells has various aspects of the device being investigated. This paper analyzes the deliberately hierarchized photoelectrode configuration for DSC applications to improve the performance of DSCs. Multiple layers of differently composed TiO{sub 2} particle types namely aggregates and nanoparticles were deposited to form a photoelectrode with thickness of about 12 µm. The photoelectrodes were assembled into working DSCs with an active area of 1 cm{sup 2}. Measurement for solar power conversion performance was measured under 1 sun at AM1.5 spectrum simulated sunlight. Electron microscopy for photoelectrode analysis was conducted using Field Emission Scattering Electron Microscopy with enhanced resolution. External Quantum Efficiency was measured using a purpose built instrument. Kinetics were investigated using the Electrochemical Impedance Spectroscopy (EIS) measurement with a potentiostat. The best performing DSC is of the hierarchically organized photoelectrode with a photoconversion efficiency of 4.58%, an increase of 14% in comparison to the reference samples with fully aggregates configuration. Short circuit current density, Jsc increases by about 2.223 mA cm{sup −2} relative to the blanks. The electron microscopy confirmed expected thickness at around 10 µm and layers forming the photoelectrode being hierarchically deposited with ∼20 nm TiO{sub 2} nanoparticles and 450 nm TiO{sub 2} aggregates mixture composition. EQE improved especially for visible region of 500-550 nm light wavelengths with 12 % increase in the response of in that region. Improvement to the diffusion coefficient as measured by the EIS contributed to the performance increase of the photoelectrode configuration under investigation.

14 SOLAR ENERGY↗
DOE OSTI2015

Surface-plasmon enhanced photodetection at communication band based on hot electrons

Surface plasmons can squeeze light into a deep-subwavelength space and generate abundant hot electrons in the nearby metallic regions, enabling a new paradigm of photoconversion by the way of hot electron collection. Unlike the visible spectral range concerned in previous literatures, we focus on the communication band and design the infrared hot-electron photodetectors with plasmonic metal-insulator-metal configuration by using full-wave finite-element method. Titanium dioxide-silver Schottky interface is employed to boost the low-energy infrared photodetection. The photodetection sensitivity is strongly improved by enhancing the plasmonic excitation from a rationally engineered metallic grating, which enables a strong unidirectional photocurrent. With a five-step electrical simulation, the optimized device exhibits an unbiased responsivity of ∼0.1 mA/W and an ultra-narrow response band (FWHM = 4.66 meV), which promises to be a candidate as the compact photodetector operating in communication band.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗