Progress Report on Charged Particle Transport in MCNP6
Explore the source record for details and available documents.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
SEARCH · Search NASA
Results for “Charge transport”
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.
Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.
Development of Structure–Property Relationships for Ammonium Transport through Charged Organogels
Ammonia is a promising carbon-free fuel, but current methods to produce ammonia are energy intensive. New methods are thereby needed, with one promising method being electrochemical nitrogen reduction cells. Efficient cell operation requires robust catalysts but also efficient membrane separators that permit the selective transport of ions while minimizing the transport of the products across the cell. Commercial membranes have an unknown morphology which makes designing improved cells challenging. To address this problem, we synthesized a series of membranes with controlled crosslinking density and chemical composition to understand their impact on ammonium transport. Higher crosslinking density led to lower ammonium permeability. At the highest crosslinking density, similar ammonium permeability was observed independent of the water volume fraction and hydrophobicity of the monomers. These results suggest new directions to develop membranes with reduced ammonium crossover to improve the efficiency of these electrochemical cells.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Charged Hole‐Transporting Materials Based on Imidazolium for Defect Passivation in Inverted Perovskite Solar Cells
The hole‐transporting material (HTM) in perovskite solar cells (PSCs) provides an ideal interface with the perovskite layer for hole collection while influencing the perovskite crystalline structure and morphology. This article presents SIM and DIM, two new dopant‐free imidazolium‐based HTMs with charged units accompanied by counter ions that show the potential to function as ionic HTMs and ionic liquid additives and help improve the efficiency and stability of inverted PSCs. DIM‐based PSCs demonstrates exceptional performance with a high‐power conversion efficiency of 19.15%, attributed to improved passivation of perovskite interface defects. Furthermore, these new imidazolium salt‐based HTMs can be manufactured economically, making them a viable option for mass production and PSC commercialization.
Tingare, Yogesh S.↗
Chain rigidity controlled aggregation ability and solid-state microstructures for efficient stretchable conjugated polymer films
Stretchable conjugated polymer films with good electrical performance under mechanical deformation are highly desirable for soft electronics. However, the mechanical and electrical properties of these films, particularly in conjugated polymer:elastomer blends, are not fully understood at molecular level. Here, this study explores the relationships among molecular structure, aggregation ability, film microstructure, and the electrical/mechanical properties of three diketopyrrolopyrrole-based conjugated polymers (P1, P2, P3) with decreasing backbone rigidity and their corresponding polymer:elastomer blends. The most flexible polymer P3 shows strong aggregation, which forms highly crystalline fibers to produce fragile neat film and produces large isolated crystallites restricting charge transport in blend film. As chain rigidity increases, the P1 and P2 polymers show weaker aggregation, and produce smaller crystallites in neat films with enhanced ductility. P1 and P2 based blend films display nanocrystallites polymer networks with dispersed elastomer domains. As a result, we achieved near-constant charge mobility before and after stretching under 50 % strain for P2-based blend films with well-controlled pathways for both charge transport and energy dissipation. This study demonstrates the critical role of backbone rigidity in regulating the properties of stretchable conjugated polymer films, paving the way for more reliable and deformable materials in soft electronics.
36 MATERIALS SCIENCE↗
Dielectric constant engineering of nonfullerene acceptors enables a record fill factor of 83.58% and a high efficiency of 20.80% in organic solar cells
Organic solar cells (OSCs) have achieved power conversion efficiencies (PCEs) surpassing 20%, but their development remains hindered by the inherently low dielectric constant (εr) of organic semiconductors, which limits charge transport and contributes to serious recombination losses. Herein, we present a comprehensive strategy to overcome the challenge by engineering the dielectric properties of nonfullerene acceptors (NFAs). Two Y-series NFAs of BTP-N3F and BTP-C3F have been synthesized featuring trifluoromethyl (CF 3 ) end-capped alkyl side chains. This molecular design significantly enhances the dipole moment and ε r (up to ∼5.9) when compared to the reference acceptor Y6 (∼3), reducing the exciton binding energy (E b ) and improving charge transport. Furthermore, the incorporation of a high-εr polymer additive, poly(pentafluorostyrene) (PPFS), synergistically improves the active layer morphology and dielectric properties, enabling efficient charge extraction and reduced recombination losses. Devices based on the optimized D18-Cl/BTP-C3F system have achieved a record-high fill factor (FF) of 83.58% and an impressive PCE of 20.80%, setting a new benchmark for OSCs. Finally, our results underscore the pivotal role of ε r in enhancing device performance and establish a versatile pathway for advancing OSC efficiency and stability through molecular and morphological optimization.
36 MATERIALS SCIENCE↗
Semiconductor Thermal and Electrical Properties Decoupled by Localized Phonon Resonances
Abstract Thermoelectric materials convert heat into electricity through thermally driven charge transport in solids or vice versa for cooling. To compete with conventional energy‐conversion technologies, a thermoelectric material must possess the properties of both an electrical conductor and a thermal insulator. However, these properties are normally mutually exclusive because of the interconnection between scattering mechanisms for charge carriers and phonons. Recent theoretical investigations on sub‐device scales have revealed that nanopillars attached to a membrane exhibit a multitude of local phonon resonances, spanning the full spectrum, that couple with the heat‐carrying phonons in the membrane and cause a reduction in the in‐plane thermal conductivity, with no expected change in the electrical properties because the nanopillars are outside the pathway of voltage generation and charge transport. Here this effect is demonstrated experimentally for the first time by investigating device‐scale suspended silicon membranes with GaN nanopillars grown on the surface. The nanopillars cause up to 21% reduction in the thermal conductivity while the power factor remains unaffected, thus demonstrating an unprecedented decoupling in the semiconductor's thermoelectric properties. The measured thermal conductivity behavior for coalesced nanopillars and corresponding lattice‐dynamics calculations provide evidence that the reductions are mechanistically tied to the phonon resonances. This finding paves the way for high‐efficiency solid‐state energy recovery and cooling.
Spann, Bryan T.↗
Electron transfer calculations between edge sharing octahedra in hematite, goethite, and annite
A key reaction underlying the charge transport in iron containing oxides, clays, micas is the Fe$^{2+}$-Fe$^{3+}$ exchange reaction between edge-sharing iron octahedra. These reactions facilitate conduction in these minerals by the thermally-activated hopping of small polarons across the lattice. Depending on the mineral and local charge state the small polaron can either encase an electron or hole. The probability for conduction of small polarons depends strongly on the height and adiabicity of the reaction barrier, with larger and more diabatic barriers yielding slow conduction associated with either weak coupling or a large prerequisite rearrangement of the lattice during charge transport. To model these reactions, a first principle electron transfer (ET) method was developed to model the small polaron hopping between the edge-sharing octahedra sites in hematite ($e^{-}$ polaron), goethite ($e^{-}$ polaron), and annite ($h^{+}$ polaron) bulk structures. The ET method is based on electronic structure methods (i.e., plane-wave Density Functional Theory) capable of performing calculations with periodic cells and large size systems efficiently while at the same time being accurate enough to be used in the estimation of the electron-transfer coupling matrix element, $V_{AB}$, and the electron transfer transmission factor, $\kappa_{el}$. Additionally, the calculations confirmed the existence of small polarons in all three minerals, and the reactions were predicted to be strongly adiabatic. It was found that transfer of a hole in the octahedral layer of annite had an adiabatic barrier of $0.311$ eV, and the transfer of an extra electron in hematite and goethite had adiabatic barriers of $0.242$ eV and $0.232$ eV respectively. The electronic coupling parameters,$V_{AB}$, were found to be $0.188$ eV, $0.196$ eV, and $0.102$ eV respectively for hematite, goethite, and annite. While similar bonding topologies pertain, the underlying basis for the differences is the subtle differences in local structures.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
The Role of Tie Chains on the Mechano-Electrical Properties of Semiconducting Polymer Films
Not provided.
Materials Science↗
Enhancing ion transport in charged block copolymers by stabilizing low symmetry morphology: Electrostatic control of interfaces
Recently, the interest in charged polymers has been rapidly growing due to their uses in energy storage and transfer devices. Yet, polymer electrolyte-based devices are not on the immediate horizon because of the low ionic conductivity. In the present study, we developed a methodology to enhance the ionic conductivity of charged block copolymers comprising ionic liquids through the electrostatic control of the interfacial layers. Unprecedented reentrant phase transitions between lamellar and A15 structures were seen, which cannot be explained by well-established thermodynamic factors. X-ray scattering experiments and molecular dynamics simulations revealed the formation of fascinating, thin ionic shell layers composed of ionic complexes. The ionic liquid cations of these complexes predominantly presented near the micellar interfaces if they had strong binding affinity with the charged polymer chains. Therefore, the interfacial properties and concentration fluctuations of the A15 structures were crucially dependent on the type of tethered acid groups in the polymers. Overall, the stabilization energies of the A15 structures were greater when enriched, attractive electrostatic interactions were present at the micellar interfaces. Contrary to the conventional wisdom that block copolymer interfaces act as “dead zone” to significantly deteriorate ion transport, this study establishes a prospective avenue for advanced polymer electrolyte having tailor-made interfaces.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
High Performing Inverted Flexible Perovskite Solar Cells via Solution Phase Deposition of Yttrium-Doped SnO 2 Directly on Perovskite
Solution processing of flexible perovskite solar cells (f-PSCs) provides an avenue for scalable, high-throughput printing of lightweight, scalable, and cost-effective flexible solar cells. However, the deposition of fully solution-processed metal oxide charge transport layers on perovskites has been limited by solvent incompatibilities and high processing temperatures for metal oxide nanoparticles. In this study, we present high-performance, inverted f-PSCs from the direct deposition of yttrium doped SnO 2 nanoparticles functionalized with acetate on top of perovskite as an ink in anhydrous ethanol via blade coating. Yttrium doping improved device performance by improving the charge extraction leading with a decreased series resistance leading to improvements in the open-circuit voltage and fill factor. Furthermore, the champion power conversion efficiency for 0.1 cm 2 devices increased from 14.3% for undoped SnO 2 to 18.2% with 2% Y:SnO 2 doping, which is unprecedented for f-PSCs on ITO-PET substrate employing SnO 2 as an ETL.
14 SOLAR ENERGY↗
Electronic coarse-graining of long conjugated molecules: Case study of non-fullerene acceptors
By considering only one electronic state per molecule, charge transport models of molecular solids neglect intramolecular charge transfer. This approximation excludes materials with quasi-degenerate spatially separated frontier orbitals, such as non-fullerene acceptors (NFAs) and symmetric thermally activated delayed fluorescence emitters. By analyzing the electronic structure of room-temperature molecular conformers of a prototypical NFA, ITIC-4F, we conclude that the electron is localized on one of the two acceptor blocks with the mean intramolecular transfer integral of 120 meV, which is comparable with intermolecular couplings. Therefore, the minimal basis for acceptor–donor–acceptor (A–D–A) molecules consists of two molecular orbitals localized on the acceptor blocks. This basis is robust even with respect to geometry distortions in an amorphous solid, in contrast to the basis of two lowest unoccupied canonical molecular orbitals withstanding only thermal fluctuations in a crystal. The charge carrier mobility can be underestimated by a factor of two when using single site approximation for A–D–A molecules in their typical crystalline packings.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
In Situ Electrochemistry of Buried Interfaces in Metal Halide Perovskites: Probing Energy Bands, Halide Redox Activity, and Kinetics
Control over charge injection and extraction processes across buried interfaces is fundamental for all (opto)electronic multilayer device platforms, necessitating detailed understanding of local structural and chemical differences that promote defect formation, distort energetic band-edge alignments, and alter charge transport processes. Herein, the implementation of a low-cost electroanalytical methodologies’ tool suite is described to quantitatively characterize buried interfaces and redox reactions in printable, mixed electrical–ionic, and redox-active metal halide perovskites and a prototypical hole-transporting nickel oxide (NiO x ) thin film. The objective is to demonstrate the power of electrochemical methodologies to improve the nanoscale understanding of complex interfaces within optoelectronic devices by providing case studies on how to: i) differentiate between electronic and chemical properties in NiO x contacts; ii) measure changes in reversibility of halide redox reactions via NiO x surface states; iii) assess energy alignment and charge transport across (modified) buried interfaces; and iv) quantify defects at buried interfaces that change with modifiers and differences in perovskite processing, including increasing defect concentrations when films are slot-die-coated versus spin-cast. The collective approach addresses major challenges in understanding the precise energy landscape and interface reactivity under relevant electric fields that mimic operando conditions (away from equilibrium) and across length scales in thin film device formats.
(spectro)electrochemistry↗
Regiospecific N -alkyl substitution tunes the molecular packing of high-performance non-fullerene acceptors
The rapid development of non-fullerene acceptors (NFAs) with strong near-infrared absorption has led to remarkably enhanced short-circuit current density (J sc ) values in organic solar cells (OSCs). NFAs based on the benzotriazole (Bz) fused-ring π-core have great potential in delivering both high J sc and decent open-circuit voltage values due to their strong intramolecular charge transfer with reasonably low energy loss. Here in this work, we have designed and synthesized a series of Bz-based NFAs, PN6SBO-4F, AN6SBO-4F and EHN6SEH-4F, via regiospecific N-alkyl engineering based on the high-performance NFA mBzS-4F that was reported previously. The molecular packing of mBzS-4F, AN6SBO-4F, and EHN6SEH-4F single crystals was analyzed using X-ray crystallography in order to provide a comprehensive understanding of the correlation between the molecular structure, the charge-transporting properties, and the solar cell performance. Compared with the typical honeycomb single-crystal structure of Y6 derivatives, these NFAs exhibit distinctly different molecular packing patterns. The strong interactions of terminal indanone groups in mBzS-4F and the J-aggregate-like packing in EHN6SEH-4F lead to the formation of ordered 3D networks in single-crystals with channels for efficient charge transport. Consequently, OSCs based on mBzS-4F and EHN6SEH-4F show efficient photon-to-current conversions, achieving the highest power conversion efficiency of 17.48% with a Jsc of 28.83 mA cm -2 .
36 MATERIALS SCIENCE↗
Achieving 20.1% Efficiency in Organic Solar Cells Through Interconnected Fibrillar Networks via Local Molecular Stacking
ABSTRACT The performance of organic solar cells (OSCs) is governed by how molecular packing evolves into interconnected networks that facilitate exciton dissociation and charge transport. Using an all‐small‐molecule blend DR3TSBDT:Y6 as a model system, we study how local molecular stacking evolves into performance‐relevant morphology during solvent vapor annealing (SVA) and subsequent thermal annealing (TA). SVA promotes end‐to‐end stacking of amorphous acceptors to form interconnected fibrils, while TA compacts inter‐fibril spacing without disrupting favorable local order. Such molecular‐to‐morphological refinements broaden light absorption, enhance charge transport, and markedly improve device efficiency. Extending this approach to additional blend systems (D18:Y6, D18:L8‐BO, and DR3TSBDT:L8‐BO) yields similar structural evolution and performance gains, with the D18:L8‐BO system achieving up to 20.10% PCE. Our study establishes control over local stacking in amorphous acceptors into fibrillar networks as a general and effective route to realize high‐performance OSCs.
Wu, Junying↗
LLNL-LDRD-Final report
The main focus of this study is the X-ray spectroscopy and complementary modeling characterization of the range of perovskite materials. Specific areas covered in this study include: • Quantitative characterization of individual (both CB and VB) band edge movement as a function of Sn concentration; • The effects of creating an interface with the charge transport layer and back contact on both the interfacial bonding and unoccupied band structure – i.e., how does the interfacial eDOS evolve when the interface is assembled; • How does this interface change (local bonding, CB edge) evolve with degradation – this includes depth profiling; • Additional insights from the spectroscopy – e.g., the pathway of degradation (Sn(II) oxide formation to a significant depth before Sn(IV) oxide formation, etc.), do different charge transport layers have distinct properties in slowing degradation, etc.
14 SOLAR ENERGY↗
Mild-Annealed Molecular Layer Deposition (MLD) Tincone Thin Film as Photoelectrochemically Stable and Efficient Electron Transport Layer for Si Photocathodes
Metalcone thin films, composed of inorganic–organic hybrids, are synthesized using molecular layer deposition (MLD) through reactions between organometallic precursors (e.g., Sn, Al, and Ti) and organic reactants (e.g., ethylene glycol and glycerol). Despite their unique properties, metalcones exhibit significant vulnerability to water due to their organic components, limiting their potential in electrochemical applications. This study focuses on enhancing the photoelectrochemical stability of tincone thin films in aqueous electrolyte while preserving their hybrid characteristics through mild annealing in air at 250 °C. As-deposited and vacuum-annealed tincone thin films exhibited significant degradation under these conditions, while high-temperature-annealed (500 °C) tincone thin films offered improved stability with a significant decline in charge transfer efficiency. In contrast, mild annealing in air maintained the C–O bond at half level and improved the stability and charge transport without compromising the unique characteristics of tincone. This was confirmed by ellipsometry, X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectroscopy (FTIR). Mild-annealed tincone deposited on a lightly doped p-type silicon (p-Si) photocathode produced a 20-fold increase in CO volume compared to high-temperature annealed tincone in a CO 2 -saturated potassium bicarbonate (KHCO 3 ) electrolyte with dispersed graphene oxide–cobalt phthalocyanine (GO-CoPc) under 1 sun illumination at 0.9 V vs reversible hydrogen electrode (RHE), while maintaining the faradaic efficiency for CO and H 2 . These results suggest that mild-annealed tincone thin films hold significant potential as protective charge transport layers on silicon photocathodes for the aqueous CO 2 reduction reaction (CO 2 RR).
Annealing (metallurgy)↗
Enhanced charge carrier lifetime and mobility as a result of Rb and Cs incorporation in hybrid perovskite
Alkali addition in organic–inorganic perovskite has become the standard recipe for achieving solar cells with efficiencies exceeding 20%, but the mechanism is not well understood. We use non-contact carrier lifetime measurements, mobility measurements, and synchrotron-based x-ray characterization techniques to show that there is a unique benefit to adding hybrid perovskite samples with Rb and Cs simultaneously. When either Rb or Cs is added, charge carrier mobility increases with alkali concentration. Charge carrier lifetime benefits from alkali incorporation as well, but is optimized with only moderate concentration at 1%. When both Rb and Cs are introduced, however, the high mobility is maintained and the charge carrier lifetime increases considerably. Our results show that when incorporated alone, Rb and Cs have very similar roles in a perovskite crystal, but when co-added, halide distribution becomes homogenized correlating with improved charge transport properties.
Erodici, Matthew P.↗
Unraveling the influence of non-fullerene acceptor molecular packing on photovoltaic performance of organic solar cells
In non-fullerene organic solar cells, the long-range structure ordering induced by end-group π–π stacking of fused-ring non-fullerene acceptors is considered as the critical factor in realizing efficient charge transport and high power conversion efficiency. Here, we demonstrate that side-chain engineering of non-fullerene acceptors could drive the fused-ring backbone assembly from a π–π stacking mode to an intermixed packing mode, and to a non-stacking mode to refine its solid-state properties. Different from the above-mentioned understanding, we find that close atom contacts in a non-stacking mode can form efficient charge transport pathway through close side atom interactions. The intermixed solid-state packing motif in active layers could enable organic solar cells with superior efficiency and reduced non-radiative recombination loss compared with devices based on molecules with the classic end-group π–π stacking mode. Our observations open a new avenue in material design that endows better photovoltaic performance.
59 BASIC BIOLOGICAL SCIENCES↗