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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 OSTI2023

Signatures of hot carriers and hot phonons in the re-entrant metallic and semiconducting states of Moiré-gapped graphene

Abstract Stacking of graphene with hexagonal boron nitride (h-BN) can dramatically modify its bands from their usual linear form, opening a series of narrow minigaps that are separated by wider minibands. While the resulting spectrum offers strong potential for use in functional (opto)electronic devices, a proper understanding of the dynamics of hot carriers in these bands is a prerequisite for such applications. In this work, we therefore apply a strategy of rapid electrical pulsing to drive carriers in graphene/h-BN heterostructures deep into the dissipative limit of strong electron-phonon coupling. By using electrical gating to move the chemical potential through the “Moiré bands”, we demonstrate a cyclical evolution between metallic and semiconducting states. This behavior is captured in a self-consistent model of non-equilibrium transport that considers the competition of electrically driven inter-band tunneling and hot-carrier scattering by strongly non-equilibrium phonons. Overall, our results demonstrate how a treatment of the dynamics of both hot carriers and hot phonons is essential to understanding the properties of functional graphene superlattices.

42 ENGINEERING↗
DOE OSTI2022

Toward Hot Carrier Extraction in Intervalley Photovoltaic Devices

InGaAs heterostructures have demonstrated the means to maintain hot carrier behavior under practical operating conditions via valley photovoltaics. However, enhancing the extraction to create a fully operational hot carrier solar cell requires an enhanced understanding of the barriers inside such devices. A set of four InGaAs heterostructures altering the n + top layer of the structure has been produced to enable comparative analysis of the current density-voltage characterization and the relationship to the band and valley alignments.

14 SOLAR ENERGY↗
DOE OSTI2020

Determining plasmonic hot-carrier energy distributions via single-molecule transport measurements

Hot carriers in plasmonic nanostructures, generated via plasmon decay, play key roles in applications such as photocatalysis and in photodetectors that circumvent bandgap limitations. However, direct experimental quantification of steady-state energy distributions of hot carriers in nanostructures has so far been lacking. We present transport measurements from single-molecule junctions, created by trapping suitably chosen single molecules between an ultrathin gold film supporting surface plasmon polaritons and a scanning probe tip, that can provide quantification of plasmonic hot-carrier distributions. Our results show that Landau damping is the dominant physical mechanism of hot-carrier generation in nanoscale systems with strong confinement. The technique developed in this work will enable quantification of plasmonic hot-carrier distributions in nanophotonic and plasmonic devices.

Science & Technology - Other Topics↗
DOE OSTI2020

Phonon linewidths in InAs/AlSb superlattices derived from first-principles—application towards quantum well hot carrier solar cells

Hot electrons generated by the absorption of high-energy photons typically thermalize by dissipating energy through phonon mediated relaxation pathways. Existence of non-equilibrium optical phonon populations (hot phonons) can suppress thermalization of electrons by facilitating a stable hot carrier population. In this work, we derive optical phonon scattering rates in InAs/AlSb superlattices using first-principles calculations and compare them with bulk InAs. Computations are performed for the two shortest period superlattices with equal widths of InAs and AlSb. While in pure InAs, the highest optical phonon scattering rates reach 5 cm -1 ; in the superlattice, the peak scattering rates of optical phonons with frequencies above the energy gap, are much smaller, reaching ~1 cm -1 . Finally, these lower scattering rates in the superlattice have important implications for design of high efficiency hot carrier solar cells and explain some of the robust hot carriers observed recently in InAs/AlAsSb quantum wells.

14 SOLAR ENERGY↗
DOE OSTI2024

Evidence of hot carrier extraction in metal halide perovskite solar cells

The presence of hot carriers is presented in the operational properties of an (FA,Cs)Pb(I, Br, Cl) 3 solar cell at ambient temperatures and under practical solar concentration. Albeit, in a device architecture that is not suitably designed as a functional hot carrier solar cell. At 100 K, clear evidence of hot carriers is observed in both the high energy tail of the photoluminescence spectra and from the appearance of a nonequilibrium photocurrent at higher fluence in light J–V measurements. At room temperature, however, the presence of hot carriers in the emission at elevated laser fluence is shown to compete with a gradual red shift in the PL peak energy as photoinduced halide segregation begins to occur at higher lattice temperature. The effects of thermionic emission of hot carriers and the presence of a nonequilibrium carrier distribution are also shown to be distinct from simple lattice heating. In conclusion, this results in large unsaturated photocurrents at high powers as the Fermi distribution exceeds that of the heterointerface controlling carrier transport and rectification.

14 SOLAR ENERGY↗
DOE OSTI2020

A Noble-Transition Alloy Excels at Hot-Carrier Generation in the Near Infrared

Above-equilibrium “hot”-carrier generation in metals is a promising route to convert photons into electrical charge for efficient near-infrared optoelectronics. However, metals that offer both hot-carrier generation in the near-infrared and sufficient carrier lifetimes remain elusive. Alloys can offer emergent properties and new design strategies compared to pure metals. In this work, it is shown that a noble-transition alloy, Au x Pd 1-x , outperforms its constituent metals concerning generation and lifetime of hot carriers when excited in the near-infrared. At optical fiber wavelengths (e.g., 1550 nm), Au 50 Pd 50 provides a 20-fold increase in the number of ≈0.8 eV hot holes, compared to Au, and a threefold increase in the carrier lifetime, compared to Pd. The discovery that noble-transition alloys can excel at hot-carrier generation reveals a new material platform for near-infrared optoelectronic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2021

The critical role of hot carrier cooling in optically excited structural transitions

The hot carrier cooling occurs in most photoexcitation-induced phase transitions (PIPTs), but its role has often been neglected in many theoretical simulations as well as in proposed mechanisms. Here, by including the previously ignored hot carrier cooling in real-time time-dependent density functional theory (rt-TDDFT) simulations, we investigated the role of hot carrier cooling in PIPTs. Taking IrTe2 as an example, we reveal that the cooling of hot electrons from the higher energy levels of spatially extended states to the lower energy levels of the localized Ir–Ir dimer antibonding states strengthens remarkably the atomic driving forces and enhances atomic kinetic energy. These two factors combine to dissolute the Ir–Ir dimers on a timescale near the limit of atomic motions, thus initiating a deterministic kinetic phase transition. We further demonstrate that the subsequent cooling induces nonradiative recombination of photoexcited electrons and holes, leading to the ultrafast recovery of the Ir–Ir dimers observed experimentally. These findings provide a complete picture of the atomic dynamics in optically excited structural phase transitions.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Probing and Understanding the Spatial and Energy Distributions of Plasmonic Hot Carriers via Single-Molecule Quantum Transport

The generation of hot carriers in plasmonic nanostructures offers new transformative opportunities for a range of applications, including solar energy harvesting, photochemistry, and photodetection. To better understand such phenomena, this project aims to develop an experimental approach to study and understand hot carrier distributions in photoexcited plasmonic nanostructures. The developed experimental approach, combining scanning probe-based single-molecule quantum transport measurements with plasmonic excitation methods, leverages nanoscopic single molecules as quantum energy filters to selectively access hot carriers in a variety of plasmonic nanostructures. This report summarizes the key outcomes, impacts, and lessons learned in the first two years of the project. Over the past two years, important progress was made in achieving the project's goals, including the development of the scanning probe-based experimental platform, fabrication of plasmonic nanostructures, and design and synthesis of the desired molecular candidates. Insights from this research will pave the path toward the development of technologies that will improve the way we harvest solar energy and drive chemical reactions and ultimately help transition the U.S. to a clean and sustainable society.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2020

Hot-Carrier Transfer at Photocatalytic Silicon/Platinum Interfaces

Interfacial charge transfer from silicon to heterogeneous catalysts plays a key role in silicon-based photoelectrochemical systems. In general, prior to interfacial charge transfer, carriers that are generated by photons with energies above the bandgap dissipate the excess kinetic energy via hot-carrier cooling, and such energy loss limits the maximum power conversion efficiency. The excess energy of hot-carriers, however, could be utilized through hot-carrier transfer from silicon to the catalysts, but such hot-carrier extraction has not yet been demonstrated. In this work, we exploit transient reflection spectroscopy to interrogate charge transfer at the interface between silicon and platinum. Additionally, quantitative modeling of the surface carrier kinetics indicates that the velocity of charge transfer from silicon to platinum exceeds 2.6 x 10 7 cm s -1 , corresponding to an average carrier temperature of extracted carriers of ~600 K, two times higher than the lattice temperature. The charge transfer velocity can be controllably reduced by inserting silica spacing layers between silicon and platinum.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Plasmon-Induced Hot-Carrier Excited-State Dynamics in Plasmonic Semiconductor Nanocrystals

The variance of carrier relaxation pathways for WO 3–x plasmonic semiconductor nanocrystals (PSNCs) is monitored by transient absorption spectroscopy following excitation of the localized surface plasmon resonance (LSPR) versus the optical band gap (E g,opt ). Excitation of the LSPR leads to efficient hot carrier population above the Fermi level in WO 3–x via Landau damping, in analogy to noble metal LSPR relaxation mechanisms. Hot carrier depopulation occurs on the femtosecond timescale, observed as the concomitant recovery of an LSPR bleach with the appearance of discrete interband and intraband photoinduced absorption features. Further, by comparison, the direct excitation of E g,opt results in trion recombination at donor–acceptor sites within the WO 3–x NC, consistent with exciton decay dynamics observed for typical wide-band-gap semiconductor NCs. From the analysis of pump power dependency data, a hot-carrier electron–phonon coupling constant of 1.47 × 10 11 J K –1 s –1 cm –3 is extracted. The direct comparison of the decay dynamics following E g,opt versus LSPR excitation confirms that the observed plasmon in trioctylphosphine oxide passivated, spherical WO 3–x is a resonance state in which hot carriers are generated only from excitation on resonance with the LSPR frequency. This study on WO 3–x PSNCs provides a toolset that can be used to evaluate the role of hot carriers following LSPR excitation of n-type, plasmonic transparent conducting oxide NCs, where enhancement of photocatalysis, photovoltaic performance, and optical enhancement has been reported.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Theory of Plasmonic Hot-Carrier Generation and Relaxation

Hot-carrier (HC) generation from (localized) surface plasmon decay has recently attracted much attention due to its promising applications in physical, chemical, materials, and energy science. However, the detailed mechanisms of plasmonic HC generation, relaxation, and trapping are less studied. In this work, we developed and applied a quantum-mechanical model and coupled master equation method to study the generation of HCs from plasmon decay and their following relaxation processes with different mechanisms treated on equal footing. First, a quantum-mechanical model for HC generation is developed. Its connection to existing semiclassical models and time-dependent density functional theory (TDDFT) is discussed. Second, the relaxation and lifetimes of HCs are investigated in the presence of electron–electron and electron–phonon interactions. A GW-like approximation is introduced to account for the electron–electron scattering. The numerical simulations on the Jellium nanoparticles with a size up to 1.6 nm demonstrate the electron–electron scattering and electron–phonon scattering dominate different time scale in the relaxation dynamics. We also generalize the model to study the extraction of HCs to attached molecules. The quantum yield of extracting HCs for other applications is found to be size-dependent. In general, the smaller size of NP improves the quantum yield, which is in agreement with recent experimental measurements. Even though we demonstrate this newly developed theoretical formalism with Jellium model, the theory applies to any other atomistic models.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Hot-Carrier Extraction in Nanowire-Nanoantenna Photovoltaic Devices

Nanowires bring new possibilities to the field of hot-carrier photovoltaics by providing flexibility in combining materials for band engineering and using nanophotonic effects to control light absorption. Previously, an open-circuit voltage beyond the Shockley–Queisser limit was demonstrated in hot-carrier devices based on InAs–InP–InAs nanowire heterostructures. However, in these first experiments, the location of light absorption, and therefore the precise mechanism of hot-carrier extraction, was uncontrolled. In this study, we combine plasmonic nanoantennas with InAs–InP–InAs nanowire devices to enhance light absorption within a subwavelength region near an InP energy barrier that serves as an energy filter. From photon-energy- and irradiance-dependent photocurrent and photovoltage measurements, we find that photocurrent generation is dominated by internal photoemission of nonthermalized hot electrons when the photoexcited electron energy is above the barrier and by photothermionic emission when the energy is below the barrier. We estimate that an internal quantum efficiency up to 0.5–1.2% is achieved. Insights from this study provide guidelines to improve internal quantum efficiencies based on nanowire heterostructures.

14 SOLAR ENERGY↗
DOE OSTI2021

Hot carrier relaxation and inhibited thermalization in superlattice heterostructures: The potential for phonon management

One of the main loss mechanisms in photovoltaic solar cells is the thermalization of photogenerated hot carriers via phonon-mediated relaxation. By inhibiting these relaxation mechanisms and reducing thermalization losses, it may be possible to improve the power conversion efficiency of solar cells beyond the single gap limit. Here, type-II InAs/AlAsSb multi-quantum well (MQW) structures are investigated to study the impact of the phononic properties of the AlAsSb barrier material in hot carrier thermalization. Experimental and theoretical results show that by increasing the barrier thickness (increasing the relative contribution of AlAsSb content in the superlattices), the relaxation of hot carriers is reduced as observed in power-dependent photoluminescence and thermalization analysis. Furthermore, this is attributed to an increase in the phononic bandgap of the MQW with increasing AlAsSb composition reducing the efficiency of the dominant Klemens mechanism as the phononic properties shift toward a more AlSb-like behavior.

14 SOLAR ENERGY↗
DOE OSTI2021

Switching of the electron-phonon interaction in 1 T –VSe 2 assisted by hot carriers

We apply an intense infrared laser pulse in order to perturb the electronic and vibrational states in the three-dimensional charge density wave material 1T-VSe 2 . Ultrafast snapshots of the light-induced hot carrier dynamics and nonequilibrium quasiparticle spectral function are collected using time- and angle-resolved photoemission spectroscopy. Furthermore, the hot carrier temperature and time-dependent electronic self-energy are extracted from the time-dependent spectral function, revealing that incoherent electron-phonon interactions heat the lattice above the charge density wave critical temperature on a timescale of (200 ± 40) fs. Density functional perturbation theory calculations establish that the presence of hot carriers alters the overall phonon dispersion and quenches efficient low-energy acoustic phonon scattering channels, which results in a new quasiequilibrium state that is experimentally observed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Hot-carrier dynamics in InAs/AlAsSb multiple-quantum wells

A type-II InAs/AlAs 0.16 Sb 0.84 multiple-quantum well sample is investigated for the photoexcited carrier dynamics as a function of excitation photon energy and lattice temperature. Time-resolved measurements are performed using a near-infrared pump pulse, with photon energies near to and above the band gap, probed with a terahertz probe pulse. The transient terahertz absorption is characterized by a multi-rise, multi-decay function that captures long-lived decay times and a metastable state for an excess-photon energy of >100 meV. For sufficient excess-photon energy, excitation of the metastable state is followed by a transition to the long-lived states. Excitation dependence of the long-lived states map onto a nearly-direct band gap (E g ) density of states with an Urbach tail below E g . As temperature increases, the long-lived decay times increase < E g , due to the increased phonon interaction of the unintentional defect states, and by phonon stabilization of the hot carriers > E g . Additionally, Auger (and/or trap-assisted Auger) scattering above the onset of the plateau may also contribute to longer hot-carrier lifetimes. Meanwhile, the initial decay component shows strong dependence on excitation energy and temperature, reflecting the complicated initial transfer of energy between valence-band and defect states, indicating methods to further prolong hot carriers for technological applications.

14 SOLAR ENERGY↗
NASA NTRS1991

The influences of fluorine and process variations on polysilicon film stress and MOSFET hot carrier effects

The use of fluorinated gate oxides may provide an improvement in nMOSFET reliability by enhancing hot carrier resistance. In order to clarify the mechanisms by which polysilicon processing and fluorination influence the oxide behavior, a matrix of nMOSFET structures was prepared using various processing, doping, and implantation strategies. These structures were evaluated for crystalline morphology and chemical element distribution. Mechanical stress measurements were taken on the polysilicon films from room temperature to cryogenic temperature. These examinations showed that fluorination of a structure with randomly oriented polysilicon can reduce residual mechanical stress and improve hot carrier resistance at room temperature.

Lowry, Lynn E.↗
NASA NTRS1993

Evaluation of radiation effects in re-oxidized nitrided oxide devices by hot carrier stressing at 77 K

An attempt has been made to understand the mechanisms of radiation induced degradation by using different types of hot carrier (HC) stressing experiments. The degradation of re-oxidized nitrided oxide gate dielectric due to irradiation and hot carriers are reported. The effect of electron and hole traps of the virgin device on radiation induced threshold voltage shift is discussed.

Das, N. C.↗