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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 469 records · Page 26
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Photochemical Diodes for Simultaneous Bias-Free Glycerol Valorization and Hydrogen Evolution

Artificial photosynthesis offers a route to producing clean fuel energy. However, the large thermodynamic requirement for water splitting along with the corresponding sluggish kinetics for the oxygen evolution reaction (OER) limits its current practical application. Here, we offer an alternative approach by replacing the OER with the glycerol oxidation reaction (GOR) for value-added chemicals. By using a Si photoanode, a low GOR onset potential of -0.05 V vs RHE and a photocurrent density of 10 mA/cm 2 at 0.5 V vs RHE can be reached. Coupled with a Si nanowire photocathode for the hydrogen evolution reaction (HER), the integrated system yields a high photocurrent density of 6 mA/cm 2 with no applied bias under 1 sun illumination and can run for over 4 days under diurnal illumination. In conclusion, the demonstration of the GOR-HER integrated system provides a framework for designing bias-free photoelectrochemical devices at appreciable currents and establishes a facile approach to artificial photosynthesis.

09 BIOMASS FUELS↗
DOE OSTI2023

Ferroelectric Polarization in BaTiO 3 Nanocrystals Controls Photoelectrochemical Water Oxidation and Photocatalytic Hydrogen Evolution

Ferroelectric (FE) semiconductors such as BaTiO 3 support a remnant polarization after the application of an electric field that can promote the separation of photogenerated charge carriers. Here, we demonstrate FE-enhanced photocatalytic hydrogen evolution and photoelectrochemical water oxidation with barium titanate nanocrystals for the first time. Nanocrystals of the ferroelectric tetragonal structure type were obtained by a hydrothermal synthesis from TiO 2 and barium hydroxide in 63% yield. BaTiO 3 nanocrystal films on tantalum substrates exhibit water oxidation photocurrents of 0.141 mA cm –2 at 1.23 V RHE under UV light (60 mW cm –2 ) illumination. Electric polarization at 52.8 kV cm –1 normal to the film plane increases the photocurrent by a factor of 2 or decreases it by a factor of 3.5, depending on the field polarity. It also shifts the onset potential by –0.15 or +0.09 V and it modifies the surface photovoltage signal. Lastly, exposure to an electric field increases the H 2 evolution rate of Pt/BaTiO 3 by a factor of ~1.5, and it raises the selectivity of photodeposition of silver onto the (001) facets of the nanocrystal. All FE enhancements can be removed by heating samples above the Curie temperature of BaTiO 3 . Furthermore, these findings can be explained by FE dipole-induced changes to the potential drop across the space charge layer of the material. The ability to use the ferroelectric effect to enhance hydrogen evolution and water oxidation is of potential interest for the development of improved solar energy for fuel conversion systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2011

Quantum Dot Size Dependent J - V Characteristics in Heterojunction ZnO/PbS Quantum Dot Solar Cells

The current-voltage (J-V) characteristics of ZnO/PbS quantum dot (QD) solar cells show a QD size-dependent behavior resulting from a Schottky junction that forms at the back metal electrode opposing the desirable diode formed between the ZnO and PbS QD layers. We study a QD size-dependent roll-over effect that refers to the saturation of photocurrent in forward bias and crossover effect which occurs when the light and dark J-V curves intersect. We model the J-V characteristics with a main diode formed between the n-type ZnO nanocrystal (NC) layer and p-type PbS QD layer in series with a leaky Schottky-diode formed between PbS QD layer and metal contact. We show how the characteristics of the two diodes depend on QD size, metal work function, and PbS QD layer thickness, and we discuss how the presence of the back diode complicates finding an optimal layer thickness. Finally, we present Kelvin probe measurements to determine the Fermi level of the QD layers and discuss band alignment, Fermi-level pinning, and the Voc within these devices.

36 MATERIALS SCIENCE↗
DOE OSTI2011

Hierarchical nanomorphologies promote exciton dissociation in polymer/fullerene bulk heterojunction solar cells.

PTB7 semiconducting copolymer comprising thieno[3,4-b]thiophene and benzodithiophene alternating repeat units set a historic record of solar energy conversion efficiency (7.4%) in polymer/fullerene bulk heterojunction solar cells. To further improve solar cell performance, a thorough understanding of structure-property relationships associated with PTB7/fullerene and related organic photovoltaic (OPV) devices is crucial. Traditionally, OPV active layers are viewed as an interpenetrating network of pure polymers and fullerenes with discrete interfaces. Here we show that the active layer of PTB7/fullerene OPV devices in fact involves hierarchical nanomorphologies ranging from several nanometers of crystallites to tens of nanometers of nanocrystallite aggregates in PTB7-rich and fullerene-rich domains, themselves hundreds of nanometers in size. These hierarchical nanomorphologies are coupled to significantly enhanced exciton dissociation, which consequently contribute to photocurrent, indicating that the nanostructural characteristics at multiple length scales is one of the key factors determining the performance of PTB7 copolymer, and likely most polymer/fullerene systems, in OPV devices.

14 SOLAR ENERGY↗
DOE OSTI2013

Highly Responsive Ultrathin GaS Nanosheet Photodetectors on Rigid and Flexible Substrates

The first GaS nanosheet-based photodetectors are demonstrated on both mechanically rigid and flexible substrates. Highly-crystalline, exfoliated GaS nanosheets are promising for optoelectronics due to strong absorption in the UV-visible wavelength region. Photocurrent measurements of GaS nanosheet photodetectors made on SiO2/Si substrates and flexible polyethylene terephthalate (PET) substrates exhibit a photo-responsivity at 254nm up to 4.2 AW-1 and 19.2 AW-1, respectively, which exceeds that of graphene, MoS2, or other 2D materials-based devices. Additionally, the linear dynamic range of the devices on SiO2/Si and PET substrates are 97.7dB and 78.73 dB, respectively. Both surpass that of currently-exploited InGaAs photodetectors (66 dB). Theoretical modeling of the electronic structures indicates that the reduction of the effective mass at the valence band maximum (VBM) with decreasing sheet thickness enhances the carrier mobility of the GaS nanosheets, contributing to the high photocurrents. Double-peak VBMs are theoretically predicted for ultrathin GaS nanosheets (thickness less than 5 monolayers), which is found to promote photon absorption. These theoretical and experimental results show that GaS nanosheets are promising materials for high performance photodetectors on both conventional silicon and flexible substrates.

Hu, Prof Pingan↗
DOE OSTI2011

Using Nanowires To Extract Excitons from a Nanocrystal Solid

Synthetic methods yielding highly uniform colloidal semiconductor nanocrystals with controlled shapes and sizes are now available for many materials. These methods have enabled geometrical control of optical properties, which are difficult or impossible to achieve in conventional bulk solids. However, incorporating nanocrystals efficiently into photodetectors remains challenging because of the low charge carrier mobilities typical of nanocrystal solids. Here we present an approach based on exciton energy transfer from CdSe/CdS core/shell nanocrystals to embedded CdSe nanowires. By combining the wide electronic tunability of nanocrystals with the excellent one-dimensional charge transport characteristics obtainable in nanowires, we are able to increase photocurrent extraction from a nanocrystal solid by 2–3 orders of magnitude. Furthermore, we correlate local device morphology with optoelectronic functionality by measuring the local photocurrent response in a scanning confocal microscope. We also discuss how nancocrystal/nanowire hybrid devices could be used in particle detector systems.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Enhanced photoelectrochemical efficiency and stability using a conformal TiO 2 film on a black silicon photoanode

Black silicon (b-Si) is a surface-nanostructured Si with extremely efficient light absorption capability and is therefore of interest for solar energy conversion. However, intense charge recombination and low electrochemical stability limit the use of b-Si in photoelectrochemical solar-fuel production. Here we report that a conformal, ultrathin, amorphous TiO 2 film deposited by low-temperature atomic layer deposition (ALD) on top of b-Si can simultaneously address both of these issues. Combined with a Co(OH) 2 thin film as the oxygen evolution catalyst, this b-Si/TiO 2 /Co(OH) 2 heterostructured photoanode was able to produce a saturated photocurrent density of 32.3 mA cm –2 at an external potential of 1.48 V versus reversible reference electrode (RHE) in 1 M NaOH electrolyte. The enhanced photocurrent relative to planar Si and unprotected b-Si photoelectrodes was attributed to the enhanced charge separation efficiency as a result of the effective passivation of defective sites on the b-Si surface. The 8-nm ALD TiO 2 layer extends the operational lifetime of b-Si from less than half an hour to four hours.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Giant switchable photovoltaic effect in organometal trihalide perovskite devices

Organolead trihalide perovskite (OTP) materials are emerging as naturally abundant materials for low-cost, solution-processed and highly efficient solar cells. Here, we show that, in OTP-based photovoltaic devices with vertical and lateral cell configurations, the photocurrent direction can be switched repeatedly by applying a small electric field of <1 V μm –1 . The switchable photocurrent, generally observed in devices based on ferroelectric materials, reached 20.1 mA cm –2 under one sun illumination in OTP devices with a vertical architecture, which is four orders of magnitude larger than that measured in other ferroelectric photovoltaic devices. This field-switchable photovoltaic effect can be explained by the formation of reversible p–i–n structures induced by ion drift in the perovskite layer. Furthermore, the demonstration of switchable OTP photovoltaics and electric-field-manipulated doping paves the way for innovative solar cell designs and for the exploitation of OTP materials in electrically and optically readable memristors and circuits.

14 SOLAR ENERGY↗
DOE OSTI2021

Determination of X-ray detection limit and applications in perovskite X-ray detectors

X-ray detection limit and sensitivity are important figure of merits for perovskite X-ray detectors, but literatures lack a valid mathematic expression for determining the lower limit of detection for a perovskite X-ray detector. In this work, we present a thorough analysis and new method for X-ray detection limit determination based on a statistical model that correlates the dark current and the X-ray induced photocurrent with the detection limit. The detection limit can be calculated through the measurement of dark current and sensitivity with an easy-to-follow practice. Alternatively, the detection limit may also be obtained by the measurement of dark current and photocurrent when repeatedly lowering the X-ray dose rate. While the material quality is critical, we show that the device architecture and working mode also have a significant influence on the sensitivity and the detection limit. Our work establishes a fair comparison metrics for material and detector development.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Microbial biofilms as living photoconductors due to ultrafast electron transfer in cytochrome OmcS nanowires

Light-induced microbial electron transfer has potential for efficient production of value-added chemicals, biofuels and biodegradable materials owing to diversified metabolic pathways. However, most microbes lack photoactive proteins and require synthetic photosensitizers that suffer from photocorrosion, photodegradation, cytotoxicity, and generation of photoexcited radicals that are harmful to cells, thus severely limiting the catalytic performance. Therefore, there is a pressing need for biocompatible photoconductive materials for efficient electronic interface between microbes and electrodes. Here we show that living biofilms of Geobacter sulfurreducens use nanowires of cytochrome OmcS as intrinsic photoconductors. Photoconductive atomic force microscopy shows up to 100-fold increase in photocurrent in purified individual nanowires. Photocurrents respond rapidly (<100 ms) to the excitation and persist reversibly for hours. Femtosecond transient absorption spectroscopy and quantum dynamics simulations reveal ultrafast (~200 fs) electron transfer between nanowire hemes upon photoexcitation, enhancing carrier density and mobility. Our work reveals a new class of natural photoconductors for whole-cell catalysis.

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

Broken symmetries associated with a Kagome chiral charge order

Chirality, or handedness, is ubiquitous in science, from cell biology to physics, and in condensed matter can underlie exotic phases such as chiral charge density waves and chiral superconductivity. However, detecting subtle broken symmetries that define such states is challenging, leading to debate and controversy. Here, using second-order optical response, we reveal the broken symmetries of a chiral charge density wave in the Kagome lattice KV 3 Sb 5 . Polarization-dependent mid-infrared photocurrent microscopy uncovers a longitudinal, helicity-dependent photocurrent associated with the charge order, indicating broken inversion and mirror symmetries. These findings, supported by theoretical analysis, directly establish the intrinsic chiral nature of the ordered state. Moreover, the absence of a circular photogalvanic effect perpendicular to the incident light imposes stringent constraints on the point-group symmetries. Our study not only visualizes the chiral nature of the Kagome charge order, but also highlights the nonlinear photogalvanic effect as a sensitive probe for detecting subtle symmetry breakings.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2019

Spatially dispersive circular photogalvanic effect in a Weyl semimetal

Weyl semimetals (WSMs) are gapless topological states of matter with broken inversion and/or time reversal symmetry. WSMs can support a circulating photocurrent when illuminated by circularly polarized light at normal incidence. Here, we report a spatially dispersive circular photogalvanic effect (s-CPGE) in a WSM that occurs with a spatially varying beam profile. Our analysis shows that the s-CPGE is controlled by a symmetry selection rule combined with asymmetric carrier excitation and relaxation dynamics. By evaluating the s-CPGE for a minimal model of a WSM, a frequency-dependent scaling behaviour of the photocurrent is obtained. Wavelength-dependent measurements from the visible to mid-infrared range show evidence of Berry curvature singularities and band inversion in the s-CPGE response. Here, we present the s-CPGE as a promising spectroscopic probe for topological band properties, with the potential for controlling photoresponse by patterning optical fields on topological materials to store, manipulate and transmit information.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Giant intrinsic photoresponse in pristine graphene

When the Fermi level is aligned with the Dirac point of gra-phene, reduced charge screening greatly enhances electron–electron scattering1–5. In an optically excited system, the kinematics of electron–electron scattering in Dirac fermions is predicted to give rise to novel optoelectronic phenomena6–11. In this paper, we report on the observation of an intrinsic pho-tocurrent in graphene, which occurs in a different parameter regime from all the previously observed photothermoelectric or photovoltaic photocurrents in graphene12–20: the photo-current emerges exclusively at the charge neutrality point, requiring no finite doping. Unlike other photocurrent types that are enhanced near p–n or contact junctions, the photo-current observed in our work arises near the edges/corners. By systematic data analyses, we show that the phenomenon stems from the unique electron–electron scattering kinemat-ics in charge-neutral graphene. Our results not only high-light the intriguing electron dynamics in the optoelectronic response of Dirac fermions, but also offer a new scheme for photodetection and energy harvesting applications based on intrinsic, charge-neutral Dirac fermions.

solar (photovoltaic), solid state lighting, photos↗
DOE OSTI2019

Electron–hole liquid in a van der Waals heterostructure photocell at room temperature

In semiconductors, photo-excited charge carriers exist as a gas of electrons and holes, bound electron–hole pairs (excitons), biexcitons and trions. At sufficiently high densities, the non-equilibrium system of electrons (e-) and holes (h + ) may merge into an electronic liquid droplet. Here, we report on the electron–hole liquid in ultrathin MoTe2 photocells revealed through multi-parameter dynamic photoresponse microscopy (MPDPM). By combining rich visualization with comprehensive analysis of very large data sets acquired through MPDPM, we find that ultrafast laser excitation at a graphene–MoTe 2 –graphene interface leads to the abrupt formation of ring-like spatial patterns in the photocurrent response as a function of increasing optical power at T = 297 K. The sudden onset to these patterns, together with extreme sublinear power dependence and picosecond-scale photocurrent dynamics, provide strong evidence for the formation of a two-dimensional electron–hole liquid droplet. The electron–hole liquid, which features a macroscopic population of correlated electrons and holes, may offer a path to room-temperature optoelectronic devices that harness collective electronic phenomena.

phonons, thermal conductivity, thermoelectric, spi↗
DOE OSTI2019

Lightwave-driven gapless superconductivity and forbidden quantum beats by terahertz symmetry breaking

Light-induced supercurrents chart a path forward for the electromagnetic design of emergent materials phases and collective modes for quantum engineering applications. However, controlled spatial–temporal modulation of the complex order parameter characterizing such non-equilibrium macroscopic quantum states remains elusive. Such ultrafast phase-amplitude modulation can manifest via high harmonic modes beyond those allowed by equilibrium symmetries. Here, we drive moving condensate states via subcycle dynamical symmetry breaking achieved with nonlinear oscillating terahertz photocurrents. These non-equilibrium macroscopic quantum states with broken inversion symmetry are controlled via Cooper pair acceleration by asymmetric and multi-cycle terahertz photoexcitations. Furthermore, the observed supercurrent-carrying states evolve during a lightwave cycle and exhibit three distinguishing features: Anderson pseudo-spin precessions forbidden by equilibrium symmetry, strong high harmonic coherent oscillations assisted by pairing and long-lived gapless superfluidity with minimal condensate quench. Lightwave tuning of persistent photocurrents can be extended for quantum control of unconventional superconductors and topological matter, with implications on quantum gate and sensing functionalities.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Ultra-high Photoresponsivity in Suspended Metal-Semiconductor-Metal Mesoscopic Multilayer MoS 2 Broadband Detector from UV-to-IR with Low Schottky Barrier Contacts

The design, fabrication, and characterization of ultra-high responsivity photodetectors based on mesoscopic multilayer MoS 2 is presented, which is a less explored system compared to direct band gap monolayer MoS 2 that has received increasing attention in recent years. The device architecture is comprised of a metal-semiconductor-metal (MSM) photodetector, where Mo was used as the contact metal to suspended MoS 2 membranes. The photoresponsivity R was measured to be ~1.4 × 10 4 A/W, which is > 10 4 times higher compared to prior reports, while the detectivity D* was computed to be ~2.3 × 10 11 Jones at 300 K at an optical power P of ~14.5 pW and wavelength λ of ~700 nm. In addition, the dominant photocurrent mechanism was determined to be the photoconductive effect (PCE), while a contribution from the photogating effect was also noted from trap-states that yielded a wide spectral photoresponse from UV-to-IR (400 nm to 1100 nm) with an external quantum efficiency (EQE) ~10 4 . From time-resolved photocurrent measurements, a decay time τ d ~ 2.5 ms at 300 K was measured from the falling edge of the photogenerated waveform after irradiating the device with a stream of incoming ON/OFF white light pulses.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Dynamic Wavelength-Tunable Photodetector Using Subwavelength Graphene Field-Effect Transistors

The holy grail of photodetector technology is dynamic wavelength tunability. Because of its atomic thickness and unique properties, graphene opens up new paradigms to realize this concept, but so far this has been elusive experimentally. We employ detailed quantum transport modeling of photocurrent in graphene field-effect transistors (including realistic electromagnetic fields) to show that wavelength tunability is possible by dynamically changing the gate voltage. We also reveal the phenomena that govern the behavior of this type of device and show significant departure from the simple expectations based on vertical transitions. We find strong focusing of the electromagnetic fields at the contact edges over the same length scale as the band-bending. Both of these spatially-varying potentials lead to an enhancement of non-vertical optical transitions, which dominate even in the absence of phonon or impurity scattering. Furthermore, we show that the vanishing density of states near the Dirac point leads to contact blocking and a gate-dependent modulation of the photocurrent. Several of the effects discussed here should be applicable to a broad range of one- and two-dimensional materials and devices.

36 MATERIALS SCIENCE↗