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Results for “doping mechanism”

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 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

A study on sub-bandgap photoexcitation in nitrogen- and boron-doped diamond with interdigitated device structure

Diamond is an ultrawide-bandgap semiconductor suitable for high power devices that require high current carrying capacity, high blocking voltages, and smaller form factors. We investigated various diamond structures for extrinsic photoconductive semiconductor switches, including an insulating high-pressure high-temperature type Ib (highly nitrogen-doped) substrate, a chemical vapor deposited (CVD) type IIa (unintentionally doped) substrate, a CVD grown semiconducting boron-doped epilayer on a type IIa substrate, and boron-implanted type Ib and IIa substrates. Using these samples, we fabricated and characterized planar interdigitated photoconductive switches with 30 μm, electrode gaps. 532 and 1064 nm Nd:YAG laser pulses with energies up to 3.5 mJ/pulse were used to trigger the switches. Photoresponses were measured at bias voltages ranging from 10 to 100 V, corresponding to electric fields of 3.3–33 kV/cm. In this field range, the type Ib device exhibited the highest average on/off-state current ratio, on the order of 10 11 , when triggered with 0.8 mJ/pulse, 532 nm laser pulses. However, only the CVD grown boron-doped epilayer and boron implanted IIa devices showed decent sensitivity to 1064 nm.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Superconductivity in magnetically doped SrTiO 3

Doped SrTiO 3 is a superconductor whose pairing mechanism is still not fully understood. The response of a superconductor to impurities has long been used to obtain insights into the nature of the superconducting state. In this work, we investigate the superconductivity of SrTiO 3 films that are doped or alloyed with different rare earth ions, which carry a magnetic moment.. It is shown that large concentrations (up to a few percent) of rare earth ions with unpaired f-electrons, such as Sm and Eu, do not reduce the superconducting critical temperature and critical fields. The finding is independent of whether the rare earth ion acts as a dopant or is an isovalent impurity. The interactions between the superconducting condensate and the magnetic dopants that could result in the observed insensitivity to magnetic impurities are discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Freestanding and Flexible Micrometer-Thick PEDOT:PSS Film with High Power Factor

High-efficiency thermoelectric materials are vital for sustainable energy. This work presents a reliable method to fabricate freestanding, flexible micrometer-thick films of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), achieving a power factor of 204 μW m –1 K –2 , 4 orders of magnitude higher than pristine films. Furthermore, this improvement stems from polymer chain realignment and enhanced charge transport via solvent doping, coupled with PSS reduction during post-treatment, which also strengthens film mechanics. Crucially, the freestanding nature ensures transferability, making them ideal for versatile applications. Besides thermoelectrics, these highly conductive, robust, and flexible PEDOT:PSS films provide attractive solutions for organic solar cells, battery electrodes, and flexible electronics.

Conjugated Polymers↗
DOE OSTI2021

Cr-Doped Ge-Core/Si-Shell Nanowire: An Antiferromagnetic Semiconductor

An antiferromagnet offers many important functionalities such as opportunities for electrical control of magnetic domains, immunity from magnetic perturbations, and fast spin dynamics. Introducing some of these intriguing features of an antiferromagnet into a low dimensional semiconductor core–shell nanowire offers an exciting pathway for its usage in antiferromagnetic semiconductor spintronics. Here, using a quantum mechanical approach, we predict that the Cr-doped Ge-core/Si-shell nanowire behaves as an antiferromagnetic semiconductor. In this work, the origin of antiferromagnetic spin alignments between Cr is attributed to the superexchange interaction mediated by the p z orbitals of the Ge atoms that are bonded to Cr. A weak spin–orbit interaction was found in this material, suggesting a longer spin coherence length. The spin-dependent quantum transport calculations in the Cr-doped nanowire junction reveals a switching feature with a high ON/OFF current ratio (~41 times higher for the ON state at a relatively small bias of 0.83 V).

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2025

Screening of Coulombic Interactions To Achieve a Higher Power Factor in Conjugated Polymers

Thermoelectric properties of conducting polymers typically suffer from molecular chain disordering, as charge transport is predominantly controlled by morphology. This is especially more problematic when counterions are introduced to tune the carrier concentration for optimal thermoelectric performance, which disturbs the morphology further. Here, in this work, we introduce a new avenue for enhancing thermoelectric properties without needing to regulate the morphology, namely, by controlling the coulombic interaction between polarons and counterions. We perform in situ de-doping thermoelectric experiments over 3 orders of magnitude change in electrical conductivity of three distinct thermoelectric polymers, namely, poly(3-hexylthiophene-2,5-diyl) (P3HT), poly[2,5-bis(3-dodecylthiophen-2-yl)thieno[3,2-b]thiophene] (PBTTT-C 12 ), and poly[2,5-(2-octyldodecyl)-3,6-diketopyrrolopyrrole-alt-5,5-(2,5-di(thien-2-yl)thieno[3,2-b]thiophene)] (OD-PDPP2T-TT) conjugated polymers, followed by grazing-incidence wide-angle X-ray scattering (GIWAXS) to study their respective morphologies. We demonstrate a 9-fold enhancement in the thermoelectric power factor in OD-PDPP2T-TT compared to PBTTT-C 12 and link it to the coulombic screening of charge carriers, including in the optimally doped regime. We support this hypothesis using Boltzmann transport equations and show that, in both P3HT and PBTTT-C 12 , as the polymer is doped, impurity scattering remains the dominant scattering mechanism, while in OD-PDPP2T-TT, the scattering mechanism changes from impurity to acoustic phonon limited, resulting in more effective screening of ionized counterions. Our results provide an additional knob to enhance the fundamental understanding of thermoelectric physics of conducting polymers and provide a pathway to achieve higher performance in the field of organic thermoelectrics.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Charge Carrier Lifetime Determination in Graded Absorber Solar Cells Using Time‐Resolved Photoluminescence Simulations and Measurements

Thin‐film photovoltaic device efficiencies are limited by carrier recombination, thus understanding recombination mechanisms is critical for performance improvements. Bulk minority carrier lifetime ( τ bulk ) is a critical parameter for solar cells but is difficult to determine in P–N junction devices, especially for high doping. As doping ≥10 16 cm −3 is required for efficient drift‐charge‐carrier‐collection devices, a method for τ bulk determination in doped P–N junction devices is necessary. This work utilizes time‐resolved photoluminescence (TRPL) simulations to quantify bulk and interface recombination properties in highly doped, graded absorber CdSeTe structures. The two methods developed here for τ bulk determination include utilization of an instantaneous lifetime representation to guide TRPL fitting and direct comparison between measured and simulated decays. Simulations verified that both methods are valid for state‐of‐the‐art device architectures which include graded bandgap absorbers, graded doping, and graded lifetimes. Shifts in the dominant recombination mechanism are identified for sufficiently long τ bulk , where front and back interface quality plays a more prominent role. Evaluation of surface recombination velocities and conduction band offset illustrate electro‐optical advantages of a positive conduction band offset and highlight the necessity of improved interfaces as bulk quality in photovoltaic devices improves.

14 SOLAR ENERGY↗
DOE OSTI2023

High-performance aqueous zinc-ion hybrid capacitors based on 3D printed metal-organic framework cathodes

The zinc-ion hybrid capacitor is a promising energy storage device, but current overall capacity is limited by the capacitance of the carbon cathode. We have produced a hierarchically porous, nitrogen-doped carbon cathode with good cycling and mechanical stability by 3D printing and pyrolysis of the zinc-based metal–organic framework ZIF-8. When incorporated into a zinc-ion hybrid capacitor, we achieved an areal capacitance of 16.9 F cm -2 and energy density of 7.23 mW h cm -2 , outperforming zinc-ion hybrid capacitors based on conventional cathodes.

25 ENERGY STORAGE↗
DOE OSTI2021

Ultrafast Charge Transfer Dynamics at the Origin of Photoconductivity in Doped Organic Solids

In spite of their growing importance for optoelectronic devices, the fundamental properties and photophysics of molecularly doped organic solids remain poorly understood. Such doping typically leads to a small fraction of free conductive charges, with most electronic carriers remaining Coulombically bound to the ionized dopant. Recently, we have reported photocurrent for devices containing vacuum-deposited TAPC (1,1-bis(4-bis(4- methylphenyl)aminophenyl)cyclohexane) doped with MoO 3 , showing that photoexcitation of charged TAPC molecules increases the concentration of free holes that contribute to conduction. Here, we elucidate the excited-state dynamics of such doped TAPC films to unravel the key mechanisms responsible for this effect. We demonstrate that excitation of different electronic transitions in charged and neutral TAPC molecules allows bound holes to overcome the Coulombic attraction to their MoO 3 counterions, resulting in an enhanced yield of long-lived free carriers. This is caused by ultrafast back-and-forth shuffling of charges and excitation energy between adjacent cations and neutral molecules, competing with relatively slow nonradiative decay from higher excited states of TAPC •+ . The light-induced generation of conductive carriers requires the coexistence of cationic and neutral TAPC, a favorable energy level alignment, and intermolecular interactions in the solid state.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Active doping controls the mode of failure in dense colloidal gels

Mechanical properties of disordered materials are governed by their underlying free energy landscape. In contrast to external fields, embedding a small fraction of active particles within a disordered material generates nonequilibrium internal fields, which can help to circumvent kinetic barriers and modulate the free energy landscape. In this work, we investigate through computer simulations how the activity of active particles alters the mechanical response of deeply annealed polydisperse colloidal gels. We show that the “swim force” generated by the embedded active particles is responsible for determining the mode of mechanical failure, i.e., brittle vs. ductile. We find, and theoretically justify, that at a critical swim force the mechanical properties of the gel decrease abruptly, signaling a change in the mode of mechanical failure. The weakening of the elastic modulus above the critical swim force results from the change in gel porosity and distribution of attractive forces among gel particles, while below the critical swim force, the ductility enhancement is caused by an increase of gel structural disorder. Above the critical swim force, the gel develops a pronounced heterogeneous structure characterized by multiple pore spaces, and the mechanical response is controlled by dynamical heterogeneities. We contrast these results with those of a simulated monodisperse gel that exhibits a nonmonotonic trend of ductility modulation with increasing swim force, revealing a complex interplay between the gel energy landscape and embedded activity.

Zhou, Tingtao (ORCID:000000021766719X)↗
DOE OSTI2022

Dual Protective Mechanism of AlPO 4 Coating on High-Nickel Cathode Material for High Energy Density and Long Cycle Life Lithium-Ion Batteries

Cathode material with high nickel content is a promising candidate for the future generation of Li-ion batteries (LIBs). However, severe structural degradation during cycling limits its practical use, especially for electric vehicles. Herein, AlPO 4 nanoparticles were synthesized and then coated onto the surface of a high-nickel layer-structured cathode via a dry coating method. The AlPO 4 nanoparticles coating significantly improved the cycling stability from 69.2% to over 80% capacity retention after 140 cycles. Furthermore, the structure and chemical composition of the AlPO 4 -coated cathode was investigated by XRD, SEM, XPS, and STEM. Compared with the non-coated cathode, we revealed a dual protective mechanism for enhanced cycling stability, where Al doping and Li 3 PO 4 coating play synergistic roles in protecting cathode material through long-term cycling. This work demonstrates a facile and environmentally friendly approach toward improving the performance of high-nickel LIB cathodes, which can be easily scaled up for industrial applications.

25 ENERGY STORAGE↗
DOE OSTI2022

High-Temperature Ceramic-Carbonate Dual-Phase Membrane Reactor for Pre-combustion Carbon Dioxide Capture (Final Scientific/Technical Report)

Arizona State University, in collaboration with University of South Carolina, worked on a project aimed at development of a new high temperature, high pressure CO 2 perm-selective membrane reactor for water-gas-shift reaction (WGS) with simulated gasifier syngas to produce a high concentration H 2 stream with CO 2 capture. The membrane reactor is made of a CO 2 semi-permeable ceramic-carbonate dual-phase (CCDP) membrane with high CO 2 perm-selectivity/permeance and thermal/mechanical stability for application in WGS reaction. The objectives of this project were to (1) synthesize the chemically/thermally stable tubular CCDP membranes with CO 2 permeance and selectivity (with respect to H 2 , CO or H 2 O) larger than 6.5×10-7 mol/m2·s·Pa and 500, respectively; (2) establish CCDP membrane reactor setup and study high pressure CO 2 permeation and WGS reaction with CO 2 capture using the setup; and (3) identify conditions for WGS in the CCDP membrane reactor that produce CO 2 and H 2 streams with purity of >99% and >90% respectively at CO conversion >95% and overall carbon capture >90%. The work in this project included both membrane development and membrane reactor process study. The membrane development efforts were focused on investigating a H 2 S resistant and highly oxygen-ionic conducting metal oxide material and membrane for CO 2 separation, fabrication of tubular samaria-doped-ceria/molten-carbonate CCDP membrane with high mechanical strength, and experimental and modeling study of high-pressure CO 2 permeation of the CCDP membranes. Mathematical models were developed to describe WGS in the CCDP membrane reactor without a catalyst or packed with a commercial high temperature WGS catalyst. Experiments on WGS in the CCDP membrane reactor with the commercial WGS catalyst, guided by the model analysis, were performed to identify optimum conditions for achieving the CO conversion, carbon capture, and the purity of the H 2 and CO 2 streams mentioned above. At 30 atm feed pressure, 750°C operation temperature, space velocity of 250 h-1, and with steam sweep, a single-stage CCDP membrane reactor with average CO 2 permeation flux of 0.5 cm3(STP)/min.cm2 can achieve CO 2 conversion of 95% and overall carbon capture of 94%, and produce CO 2 and H 2 streams with dry-based purity of >99% and 92% respectively. The project also included process design and techno-economic analysis (TEA) for a CCDP membrane reactor process for WGS reaction with CO 2 capture for a 550 MW coal-fired IGCC power plant, and its comparison with the conventional fixed-bed reactor system for WGS with follow-up CO 2 capture by an amine absorption process. The target performance for the reactor for WGS with CO 2 capture includes CO conversion >95%, hydrogen stream purity >90%, CO 2 stream purity >95%, and total carbon capture >90%. The CCDP membrane developed in this project can achieve the performance target, without subsequent CO 2 capture process at the optimum conditions identified in this project. The outcome of the process design and TEA analysis shows that the membrane reactor for WGS with in-situ CO 2 capture has an operating cost about 40% lower than that for the conventional fixed-bed reactor with a separate amine absorption process for CO 2 capture. However, the capital cost of the membrane reactor process is about twice that of the conventional process because of the higher cost of the CCDP membrane. Modeling analysis shows that a membrane reactor using a CCDP membrane with higher CO 2 permeance (about three times the current value) can deliver the targeted performance for WGS reaction with CO 2 capture at a much higher space velocity and lower membrane surface area to catalyst volume ratio, leading to a smaller catalyst amount and/or membrane area and hence significantly reduced membrane reactor capital costs.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2022

Boron Phosphide Films by Reactive Sputtering: Searching for a P‐Type Transparent Conductor

Abstract With an indirect band gap in the visible and a direct band gap at a much higher energy, boron phosphide (BP) holds promise as an unconventional p‐type transparent conductor. This work reports on reactive sputtering of amorphous BP films, their partial crystallization in a P‐containing annealing atmosphere, and extrinsic doping by C and Si. The highest hole concentration to date for p‐type BP (5 × 10 20 cm −3 ) is achieved using C doping under B‐rich conditions. Furthermore, bipolar doping is confirmed to be feasible in BP. An anneal temperature of at least 1000 °C is necessary for crystallization and dopant activation. Hole mobilities are low and indirect optical transitions are stronger than that predicted by theory. Low crystalline quality probably plays a role in both cases. High figures of merit for transparent conductors might be achievable in extrinsically doped BP films with improved crystalline quality.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Heteroatom-Doped Flash Graphene

Heteroatom doping can effectively tailor the local structures and electronic states of intrinsic two-dimensional materials, and endow them with modified optical, electrical, and mechanical properties. Recent studies have shown the feasibility of preparing doped graphene from graphene oxide and its derivatives via some post-treatments, including solid-state and solvothermal methods, but they require reactive and harsh reagents. However, direct synthesis of various heteroatom-doped graphene in larger quantities and high purity through bottom-up methods remains challenging. Here, we report catalyst-free and solvent-free direct synthesis of graphene doped with various heteroatoms in bulk via flash Joule heating (FJH). Seven types of heteroatom-doped flash graphene (FG) are synthesized through millisecond flashing, including single-element-doped FG (boron, nitrogen, oxygen, phosphorus, sulfur), two-element-co-doped FG (boron and nitrogen), as well as three-element-co-doped FG (boron, nitrogen, and sulfur). Here, a variety of low-cost dopants, such as elements, oxides, and organic compounds are used. The graphene quality of heteroatom-doped FG is high, and similar to intrinsic FG, the material exhibits turbostraticity, increased interlayer spacing, and superior dispersibility. Electrochemical oxygen reduction reaction of different heteroatom-doped FG is tested, and sulfur-doped FG shows the best performance. Lithium metal battery tests demonstrate that nitrogen-doped FG exhibits a smaller nucleation overpotential compared to Cu or undoped FG. The electrical energy cost for the synthesis of heteroatom-doped FG synthesis is only 1.2 to 10.7 kJ g –1 , which could render the FJH method suitable for low-cost mass production of heteroatom-doped graphene.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2020

Doping CdSexTe1-x/CdTe Graded Absorber Films with Arsenic for Thin-Film Photovoltaics

CdTe thin-film photovoltaics have demonstrated some of the lowest costs of electricity generation owing to its low material cost and ease of manufacturing. However, the full potential of polycrystalline CdTe photovoltaics can only be realized if the open-circuit voltage can be increased beyond 1 V Open-circuit voltage ~850-900 mV has been consistently observed for state-of-the-art polycrystalline CdTe solar cells. Open-circuit voltage of over 1V has been demonstrated for single crystal CdTe devices by doping with Group V elements. Therefore, this study is aimed at understanding behavior of polycrystalline CdTe devices with arsenic doping, its activation and process and performance optimization in order to overcome current voltage limitations in CdTe solar cells.

14 SOLAR ENERGY↗
DOE OSTI2024

Ion and Water Dynamics in the Transition from Dry to Wet Conditions in Salt-Doped PEG

The influence of the water content on ion and water transport mechanisms in polymer membranes under low to moderate hydration conditions remains poorly understood. In this study, we combine ion and water diffusivity (PFG-NMR) measurements with atomistic molecular dynamics simulations to better understand transport processes in hydrated salt-doped poly(ethylene glycol). Above the water percolation threshold, the experimental and simulated diffusivities are in good agreement with the free volume transport models. At low hydration levels, unlike dry systems, ion diffusion cannot be described by polymer segmental dynamics alone. We rationalize such observations by the interplay between ion–water and ion–polymer solvation of cations and between ion–water and cation–anion interactions for anions. Further, we demonstrate that a two-state model combining ion–water solvation and free volume transport can describe water dynamics across the entire hydration range of interest. Here, our findings provide a more encompassing analysis of ion and water transport in hydrated polyelectrolytes, specifically in the low hydration regime.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Synergistic Evolution of Segmental Motion and Cooperative Relaxation within the Amorphous Phase of Organic Mixed Ionic-Electronic Conductors

Organic mixed ionic-electronic conductors (OMIECs) facilitate a variety of electrochemical processes and feature a heterogeneous microstructure composed of both crystalline and amorphous phases. However, structural evolution in amorphous regions during electrochemical doping remains poorly understood, limiting our understanding of mixed conduction mechanisms. Here, in this work, we develop operando chip calorimetry to probe amorphous phase evolution in poly­(3,4-ethylenedioxythiophene):poly­(styrenesulfonate) (PEDOT:PSS) under swelling and electrochemical (de)­doping. Our results reveal that amorphous regions providing ionic transport pathways and those within electronic transport channels undergo heterogeneous, yet synergistic, evolution during electrochemical modulation. The cooperative interplay between segmental motion and relaxation maintains ionic conductivity and intergrain electronic transport upon electrowetting and doping, while facilitating efficient ion hopping and adaptable chain conformations during dedoping. Such synergies are more pronounced in loose structures featuring a fibrillar morphology, which exhibit lower glass transition temperatures (T g ) and higher fragility (m). High-throughput robotic screening further establishes a strong correlation between elevated m/T g ratios and enhanced mixed conduction. These findings elucidate the role of the amorphous phase in the synthesis of OMIECs and underscore the potential of operando chip calorimetry in uncovering structure–property relationships in electroactive polymers.

amorphous phase↗
DOE OSTI2020

Grand potential sintering simulations of doped UO 2 accident-tolerant fuel concepts

Chromium-doped UO is a widely-studied near-term deployable accident-tolerant fuel concept because it results in a dense, large-grain structure that increases the fuel resistance to densification, swelling, and fission gas release. A new charged-interstitial mechanism was recently proposed to describe the behavior of dopants like chromium in sintered UO 2 . Based on that mechanism, manganese was suggested as an even stronger dopant than chromium. In the current work we use mesoscale sintering simulations in an effort to validate the new mechanism. We compare the relative behavior of Cr-doped and undoped UO 2 against experimental data in the literature. We also make predictions of the relative behavior of Mn-doped UO 2 . Simulations are done using the phase field-based grand potential sintering model. Dopants have two effects on sintered UO 2 . They marginally increase the densification rate and greatly increase the average grain size. Both of these effects are individually tested in small-scale simulations. Then large 3D sintering simulations are used to test the combined behavior of both effects. The results for the densification rate simulations are consistent with experiments for Cr-doped fuels. However, we note the grain growth rates are lower than what is found in the literature for Cr-doped fuels.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗