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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 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Charge carrier dynamics in two-dimensional hybrid perovskites: Dion–Jacobson vs. Ruddlesden–Popper phases

Two-dimensional (2D) halide perovskites are promising materials for environmentally stable next-generation optoelectronic device applications. Besides the widely investigated Ruddlesden–Popper (RP) phases, Dion–Jacobson (DJ) phases are attracting considerable attention due to their rapid emergence as efficient solar cell materials. However, there is very little atomistic understanding of the charge carrier dynamics under ambient conditions for these DJ-phases, limiting the possibilities to tune their optoelectronic performances through compositional engineering routes. In this study, by combining nonadiabatic molecular dynamics with time-domain density functional theory methods at room temperature, we compare the dominant non-radiative carrier recombination and dephasing processes in RP and DJ monolayered lead halide perovskites. Our systematic study demonstrates that performance-limiting nonradiative carrier recombination processes greatly depends on the electron–phonon interactions induced by structural fluctuations and instantaneous charge localization in these materials. The stiffer interlayer packing due to the presence of single spacer dications, which separates the lead iodide slabs, reduces the thermal fluctuations in the DJ-phase to a greater extent than that in the RP-phase 2D-perovskites. Specific electronic coupling between the closely spaced lead iodide layers enhances the delocalization of band-edge charge densities in DJ-phase systems. Compared to the RP-phase, reduced inelastic electron–phonon scattering in DJ-phase perovskites significantly limits intrinsic non-radiative recombination processes. The consequent enhancement in the photogenerated charge carrier lifetime makes DJ-phase perovskites potentially suitable for various optoelectronic devices. The computational insights gained from this study allow us to outline a set of robust design principles for DJ-phase perovskites to strategically tune their optoelectronic properties.

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

Unraveling the Origin of Photocatalytic Deactivation in CeO 2 /Nb 2 O 5 Heterostructure Systems during Methanol Oxidation: Insight into the Role of Cerium Species

The study provides deep insight into the origin of photocatalytic deactivation of Nb 2 O 5 after modification with ceria. Of particular interest was to fully understand the role of ceria species in diminishing the photocatalytic performance of CeO 2 /Nb 2 O 5 heterostructures. For this purpose, ceria was loaded on niobia surfaces by wet impregnation. The as-prepared materials were characterized by powder X-ray diffraction, nitrogen physisorption, UV-visible spectroscopy, X-ray photoelectron spectroscopy, high-resolution transmission electron microscopy, and photoluminescence measurements. Photocatalytic activity of parent metal oxides (i.e., Nb 2 O 5 and CeO 2 ) and as-prepared CeO 2 / Nb 2 O 5 heterostructures with different ceria loadings were tested in methanol photooxidation, a model gas-phase reaction. Deep insight into the photocatalytic process provided by operando-IR techniques combined with results of photoluminescence studies revealed that deactivation of CeO 2 /Nb 2 O 5 heterostructures resulted from increased recombination of photo-excited electrons and holes. The main factor contributing to more efficient recombination of the charge carriers in the heterostructures was the ultrafine size of the ceria species. The presence of such highly dispersed ceria species on the niobia surface provided a strong interface between these two semiconductors, enabling efficient charge transfer from Nb 2 O 5 to CeO 2 . However, the ceria species supported on niobia exhibited a high defect site concentration, which acted as highly active recombination centers for the photo-induced charge carriers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Field-Effect Passivation by Desired Charge Injection into SiNx Passivation in Crystalline-Silicon Solar Cells

Effective surface passivation is a necessity for high efficiency crystalline silicon solar cells. The field effect passivation of p-type surfaces is typically accomplished using aluminum oxide (Al 2 O 3 ) which contains a high density of negative fixed charges. The accumulation layer formed by the negative charges prevents surface recombination loss of photo-generated carriers by repelling minority carriers (electrons) from the surface with interface state recombination centers. However, the Al 2 O 3 surface passivation technology has two key concerns of cost and safety associated with the precursor material tri-methyl-aluminum (TMA).

14 SOLAR ENERGY↗
DOE OSTI2022

Renormalization of excitonic properties by polar phonons

Here we employ quasiparticle path integral molecular dynamics to study how the excitonic properties of model semiconductors are altered by electron–phonon coupling. We describe ways within a path integral representation of the system to evaluate the renormalized mass, binding energy, and radiative recombination rate of excitons in the presence of a fluctuating lattice. To illustrate this approach, we consider Fröhlich-type electron–phonon interactions and employ an imaginary time influence functional to incorporate phonon-induced effects nonperturbatively. The effective mass and binding energies are compared with perturbative and variational approaches, which provide qualitatively consistent trends. We evaluate electron-hole recombination rates as mediated through both trap-assisted and bimolecular processes, developing a consistent statistical mechanical approach valid in the reaction limited regime. These calculations demonstrate how phonons screen electron–hole interactions, generically reducing exciton binding energies and increasing their radiative lifetimes.

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

Quantum Mechanical Evaluation of CZTS Properties for Photovoltaic Applications

As a quaternary semiconductor, CZTS (Cu 2 ZnSnS 4 ) shows promise as a thin-film solar cell material. The constituent elements in CZTS are abundant and non-toxic, and CZTS has an ideal band gap (~1.5 eV) for solar cell applications, which produces a large absorption coefficient. Unfortunately, the low efficiencies and difficulties in synthesizing the desired crystallographic phase (kesterite) and the associated formation of antisite defects limit its deployment. Using theoretical and computational tools, we investigated these current limitations, explored strategies to resolve these issues, and developed design guidelines to improve the efficiency of CZTS-based sunlight absorbers. We first sought to understand the challenges associated with synthesizing the kesterite phase and proposed ways to favor kesterite growth, thus adding to the understanding of CZTS photovoltaics. We also analyzed the major limitations at the atomic scale lowering the efficiency of CZTS: the low open-circuit voltage (V oc ) and the short carrier lifetime, thus addressing the technical effectiveness of CZTS photovoltaics. We believe the latter is due to Shockley-Read-Hall (SRH) recombination centers associated with point defects. We also studied the electronic structure of interfaces and defects introducing such recombination centers, and explored doping strategies to reduce SRH recombination. Ultimately, these efforts will benefit the public by contributing to the development of cheap and efficient solar energy conversion technologies made from abundant, non-toxic materials.

14 SOLAR ENERGY↗
DOE OSTI2026

Degradation Mode Identification by Photocarrier Lifetime Spectroscopy on Devices and Test Structures

In this presentation, I examine the basic concepts of the device physics that can be used to distinguish various degradation and recovery modes on a cell level. The known degradation modes (bulk LeTID and LID, UVID, etc.) are due to defects and impurities that cause the photocarrier recombination according to Shockley-Reed-Hall (SRH) statistics. The SRH recombination rate strongly depends on the balance of electron and hole capture rates into the defects, which in turn, are governed by their local concentrations. The strongest recombination takes place at approximately equal concentrations of electrons and holes, while at low injection conditions (when one type of carrier dominates) the SRH recombination is suppressed. For cell degradation modes that affect the passivated interface (UVID, H-induced TOPCon contact degradation) the defects are at the interface under low-injection conditions due to either high local doping or the adjacent built-in charge in the dielectric. This mode is characterized by changes in the "diode prefactor" J01 slope in the inverse lifetime-injection level curve. In contrast, bulk degradation (LeTID, LID) affects bulk lifetime, with J01 slope unchanged. Carrier lifetime - injection level plots therefore serve as clear indicators of different degradation modes and are shown by experimental examples.

14 SOLAR ENERGY↗
DOE OSTI2025

Trap-assisted Auger-Meitner recombination in GaN p-i-n diodes

Most properties of semiconductor devices are dominated by shallow impurities. However, deep defects often play an important role, for instance, in recombination processes or high field transport. While a variety of techniques are available to assess the density and energy levels of impurities, other properties, such as the recombination mechanisms of the defects, escape observation. We report on the direct measurement of hot electrons generated by trap-assisted Auger-Meitner recombination (TAAR) in GaN p-i-n diodes. By performing electron emission spectroscopy (EES) on diodes with surfaces activated to negative electron affinity by cesium, we observe the expected overflow electrons of p-i-n diodes under low current injection. However, when operating the devices at higher current densities, as low as ∼25 A/c⁢m 2 , we measure the emission of high-energy electrons. At variance with the observed hot electrons in light-emitting diodes (LEDs) using EES, the hot electrons generated in p-i-n diodes at our tested currents cannot be from eeh Auger-Meitner recombination due to the diodes' significantly lower carrier densities compared to those in LEDs. During our measurements, we observe the emission of accumulated electrons with energies ∼0.42 eV, ∼0.99 eV, ∼1.43 eV, and ∼2.32 eV above the conduction-band minimum (CBM) at various bias conditions, suggesting the existence of conduction-band features in GaN at these energies where electrons can be long-lived, such as satellite-valley minima and inflection points. We also measure incompletely relaxed hot electrons approaching energies 1.97 ± 0.13 eV and 2.94 ± 0.13 eV above the CBM, as the diodes are biased to high currents, suggesting at least some of the TAAR partaking defects have an energy level ≳1.97 eV and ≳2.94 eV away from either the conduction or valence band edges. Additionally, at our highest operating currents, we measure hot electrons with energies 3.28 ± 0.13 eV above the CBM, providing direct evidence of TAAR processes involving shallow impurities. This unexpected observation of TAAR in GaN p-i-n diodes spotlights the importance of further studies of defects in GaN and the necessity to incorporate the multi-phonon emission, radiative, and TAAR capture steps of defect-assisted recombination cycles into device modeling. Furthermore, this experiment demonstrates the applicability of the simplest semiconductor structures, p-i-n diodes, as a test bed to study the rich recombination physics of semiconductor materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Synthetic Ligand Selection Affects Stoichiometry, Carrier Dynamics, and Trapping in CuInSe 2 Nanocrystals

CuInSe 2 nanocrystals exhibit tunable near-infrared bandgaps that bolster utility in photovoltaic applications as well as offer potential as substitutes for more-toxic Cd- and Pb-based semiconductor compositions. However, they can present a variety of defect states as well as unusual photophysics. In this work, we examine the effects of ligand composition (oleylamine, diphenylphosphine, and tributylphosphine) on carrier dynamics in these materials. Via spectroscopic measurements such as photoluminescence and transient absorption, we find that ligands present during the synthesis of CuInSe 2 nanocrystals impart non-radiative electronic states which compete with radiative recombination and give rise to low photoluminescence quantum yields. We characterize the nature of these defect states (hole vs. electron traps) and investigate whether they exist at the surface or interior of the nanocrystals. Carrier lifetimes are highly dependent on ligand identity where oleylamine-capped nanocrystals exhibit rapid trapping (< 20 ps) followed by diphenylphosphine (< 500 ps) and finally tributylphosphine (> 2 ns). A majority of carrier population localizes at indium copper antisites (electrons), copper vacancies (holes), or surface traps (electrons and/or holes), all of which are non-emissive.

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

Distinctive features of structural evolution and thermodynamic response in wide-bandgap semiconductors driven by intense electronic excitation

Radiation-tolerant material selection requires balancing lattice rigidity, defect dynamics, and electronic stability, as shown by covalent SiC outperforming ionic Ga 2 O 3 and GaN under extreme environments. Responding to intense electronic excitation, irradiation-driven phase segregation (β → δ/κ in Ga 2 O 3 ) and core–shell track (disordered structure in GaN), accompanied by elemental redistribution, contrastingly, exceptional radiation tolerance manifested by comparatively minimal lattice distortion (0.17 % strain variation) was demonstrated in SiC. These differential responses are primarily attributed to two fundamental mechanisms: (i) thermodynamic driving forces governing defect migration and phase separation, and (ii) the synergistic effects of robust covalent bonding composition coupled with efficient defect recombination processes. Here, the stronger electron–phonon (e-ph) coupling in Ga 2 O 3 (4.34 × 1018 W m −3 K −1 ) and GaN (3.55 × 10 18 W m −3 K −1 ) enhances lattice energy deposition, triggering thermal spikes (ΔT ≫ T m ) and structural transition behaviors, whereas weaker e-ph coupling in SiC (3.69 × 10 18 W m −3 K −1 ), relatively high thermodynamic parameters and efficient energy dissipation suppress thermal spikes to maintaining lattice integrity. The photoresponse degradation driven by enhanced radiative recombination is dominant in N-doped SiC, while V-doped systems achieve defect-mediated photoconduction optimization characterized by abrupt current transitions, matching fluorescence yield evolutions, and directly connecting defect engineering to optoelectronic performance.

Intense electronic excitation↗
DOE OSTI2024

Simulation of DIII-D disruption with argon pellet injection and runaway electron beam

Abstract The next generation of large tokamaks, including ITER, will be equipped with a disruption mitigation system (DMS) that can be activated if a disruption is deemed to be imminent. Introducing impurities by pellet (large or shattered) or massive gas injection has been shown to be an effective mitigation mechanism on many tokamaks. The goal of the mitigation is to lessen the thermal and electromagnetic loads from the disruption without generating enough high-energy (runaway) electrons to damage the device. Variations of this mitigation process with impurity injection are presently being tested on many experiments. We have modeled one such impurity injection experiment on DIII-D using the M3D-C1 nonlinear 3D extended MHD code (Jardin et al 2012 Comput. Sci. Discovery 6 014002), The model includes an argon large pellet injection and ablation model, impurity ionization, recombination, and radiation, and runaway electron formation and subsequent evolution, including both Dreicer and avalanche sources. We obtain reasonable agreement with the experimental results for the timescale of the thermal and current quench and for the magnitude of the runaway electron plateau formed during the mitigation. This is the first 3D full MHD simulation with pellets and REs to simulate the disruption process and it also provides a partial validation of the M3D-C1 DMS model.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Long interior carrier lifetime in selective-area InAs nanowires on silicon

Catalyst-free, position-controlled indium arsenide (InAs) nanowires (NWs) of variable diameters were grown on Si (111) by selective-area epitaxy (SAE). Ultrafast pump-probe spectroscopy was conducted, from which carrier recombination mechanisms on the NW surface and interior were resolved and characterized. NWs grown using SAE demonstrated high optical quality, showing minority carrier lifetimes more than two-fold longer than that of the randomly-positioned (RP) NWs. The extracted SAE-InAs NW interior recombination lifetime was found to be as long as 7.2 ns , 13X longer than previous measurements on RP-NWs; and the surface recombination velocity 4154 cm · s - 1 . Transmission electron microscopy revealed a high density of stacking defects within the NWs, suggesting that interior recombination lifetime can be further increased by improving NW interior crystalline quality.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Spin selective charge recombination in chiral donor-bridge-acceptor triads

In this paper, we outline a physically motivated framework for describing spin-selective recombination processes in chiral systems, from which we derive spin-selective reaction operators for recombination reactions of donor–bridge–acceptor molecules, where the electron transfer is mediated by chirality and spin–orbit coupling. In general, the recombination process is selective only for spin-coherence between singlet and triplet states, and it is not, in general, selective for spin polarization. We find that spin polarization selectivity only arises in hopping-mediated electron transfer. We describe how this effective spin-polarization selectivity is a consequence of spin-polarization generated transiently in the intermediate state. Furthermore, the recombination process also augments the coherent spin dynamics of the charge separated state, which is found to have a significant effect on the recombination dynamics and to destroy any long-lived spin polarization. Although we only consider a simple donor–bridge–acceptor system, the framework we present here can be straightforwardly extended to describe spin-selective recombination processes in more complex systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Structural Gating Enhances Long-Distance Light-Driven Interfacial Electron Transfer

Structural gating provides a molecular means to transfer electrons preferentially in one desired vectorial direction, a behavior needed for applications in artificial photosynthesis. At the interfaces utilized herein, visible-light absorption by a transition metal complex opens a “structural gate” by planarization of otherwise rotating phenyl rings in p-phenylene ethynylene (PE) bridge units. Planarization provides a conjugated pathway for electron flow toward a conductive oxide surface. Interfacial electron transfer to the oxide restores rotation and closes the gate to the unwanted recombination reaction. This structural gating results in nearly quantitative long-distance (>20 Å) interfacial electron transfer that occurs ~1000 times faster than transfer in the opposite direction. A comparative kinetic study of these complexes with those that contain ionic bridge units, without gating function, as a function of the applied potential and hence –ΔG° provided a physical basis for the structural gating. A small distance-dependent reorganization energy with weak electronic coupling underlies the success of this gate that enables efficient long-distance electron transfer and slow recombination.

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

Atomic Gradient Structure Alters Electronic Structure in 3D across the Bulk and Enhances Photoactivity

Abstract Understanding structure–function relationships enables the design of materials with tailored functionalities. The long‐standing challenge is to design materials with high active volume to improve efficiency. Tailored grain boundaries and lattice defects are traditionally used to tune the electronic structure near interfaces or defects to promote electron and hole separation. However, the active volume of point defect sites or interfaces in these traditional photocatalysts is extremely low. This study reports a structure with continuous atomic positional deformation across the bulk, altering the electronic structure in 3D and creating a significantly higher active volume. Such a structure in anatase is obtained and tuned by phase transformation during the heating process. Transmission electron microscopy and density functional theory results reveal that atomic deformations result in continuous band bending across the particles, facilitating electron–hole separation, inhibiting their recombination, and inducing dramatically enhanced photoactivity. These findings enable a different materials design paradigm that can potentially be harnessed for a broad range of applications.

Ren, Peng↗
DOE OSTI2021

Atomic Gradient Structures: Atomic Gradient Structure Alters Electronic Structure in 3D across the Bulk and Enhances Photoactivity

Understanding structure–function relationships enables the design of materials with tailored functionalities. The long-standing challenge is to design materials with high active volume to improve the efficiency. Tailored grain boundaries and lattice defects are traditionally used to tune the electronic structure near interfaces or defects to promote electron and hole separation. However, the active volume of point defect sites or interfaces in these traditional photocatalysts is extremely low. In this work, we report a structure with continuous atomic positional deformation across the bulk, altering the electronic structure in three-dimension and creating a significantly high active volume. Such a structure in anatase is obtained and tuned by phase transformation during heating process. Transmission electron microscopy and density functional theory results reveal that atomic deformations result in continuous band bending across the particles, facilitating electron–hole separation, inhibiting their recombination, and inducing dramatically enhanced photoactivity. These findings enable a different materials design paradigm that can potentially be harnessed for a broad range of applications.

TiO2↗
DOE OSTI2020

Crown Ether Modulation Enables over 23% Efficient Formamidinium-Based Perovskite Solar Cells

The use of molecular modulators to reduce the defect density at the surface and grain boundaries of perovskite materials has been demonstrated to be an effective approach to enhance the photovoltaic performance and device stability of perovskite solar cells. Herein, we employ crown ethers to modulate perovskite films, affording passivation of undercoordinated surface defects. This interaction has been elucidated by solid-state nuclear magnetic resonance and density functional theory calculations. The crown ether hosts induce the formation of host-guest complexes on the surface of the perovskite films, which reduces the concentration of surface electronic defects and suppresses nonradiative recombination by 40%, while minimizing moisture permeation. As a result, we achieved substantially improved photovoltaic performance with power conversion efficiencies exceeding 23%, accompanied by enhanced stability under ambient and operational conditions. This work opens a new avenue to improve the performance and stability of perovskite-based optoelectronic devices through supramolecular chemistry.

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

Dielectric screening in perovskite photovoltaics

Abstract The performance of perovskite photovoltaics is fundamentally impeded by the presence of undesirable defects that contribute to non-radiative losses within the devices. Although mitigating these losses has been extensively reported by numerous passivation strategies, a detailed understanding of loss origins within the devices remains elusive. Here, we demonstrate that the defect capturing probability estimated by the capture cross-section is decreased by varying the dielectric response, producing the dielectric screening effect in the perovskite. The resulting perovskites also show reduced surface recombination and a weaker electron-phonon coupling. All of these boost the power conversion efficiency to 22.3% for an inverted perovskite photovoltaic device with a high open-circuit voltage of 1.25 V and a low voltage deficit of 0.37 V (a bandgap ~1.62 eV). Our results provide not only an in-depth understanding of the carrier capture processes in perovskites, but also a promising pathway for realizing highly efficient devices via dielectric regulation.

14 SOLAR ENERGY↗
DOE OSTI2025

Arsenic activation and compensation in single crystal CdTe bilayers

In state-of-the art polycrystalline CdTe photovoltaics, group-V dopant activation is about 2%. Low activation can create electronic defects and lead to recombination and band tail losses. To develop methods to overcome this limitation, dopant activation was systematically investigated using molecular beam epitaxy (MBE) grown single crystal bilayers of As-doped CdTe on undoped CdTe. Results suggest multiple paths for improved As-activation in polycrystalline CdTe-based devices. It was found that the carrier concentration in this MBE material saturated at ∼3 × 1016 cm−3, with high levels (>50%) of As-activation possible. High activation could be achieved with a post-growth activation temperature of ∼450 °C, when the initial doping level was below the saturation level. However, at typical polycrystalline As incorporation levels (>5 × 1016 cm−3), the excess As is inactive or compensating, requiring elevated temperatures (500–600 °C) to achieve high activation. Oxygen in the annealing ambient was detrimental, while the effect of CdCl2 in the ambient is more case-dependent. A 575 °C activation anneal was combined with a 450 °C CdCl2 treatment to better understand the implications for polycrystalline CdTe. Interestingly, on highly doped samples, processes ending with a high temperature step displayed high activation, while those ending at 450 °C significantly reduced the carrier concentration (with or without CdCl2 in the ambient). Low activation can be restored with another high temperature anneal, allowing reproducible toggling between high and low activation based on the final temperature. Photoluminescence revealed the presence of donor–acceptor pairs in the low activation state that appear to be associated with a compensating defect.

14 SOLAR ENERGY↗