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At least 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Microscopic Origin of Polarization Charges at Ga N / ( Al , Ga ) N Interfaces

Ga⁢N/(Al,Ga)⁢N heterojunctions are at the heart of high-electron-mobility transistors that are being adopted for high-power and high-frequency applications. The strong polarization fields present at this interface significantly enhance the density of the two-dimensional electron gas (2DEG) that is confined on the Ga⁢ N side of the junction. The microscopic origin of these electrons has been debated over the years: after excluding that they would be contributed by bulk donors, a model that identifies surface states on the (Al, Ga)⁢N surface as the source of electrons has become widely adopted. Recently, it has become clear, however, that the measured density of surface states is insufficient to account for the high electron density in the 2DEG. Here we demonstrate, based on state-of-the-art first-principles calculations, that the source of electrons is intrinsic to the overall structure and that the negative charge in the 2DEG is balanced by fixed charge on the surface. We perform a rigorous study of polarization, using our recently developed methodology for quantifying polarization fields within the finite-sized systems that can be addressed with density-functional calculations. The results show that the electrons that appear in the 2DEG originate locally at the interface, and that the net charge at the interface is predominantly compensated by fixed charge on the surface, rather than surface states. We elucidate the source of this fixed charge and associate it with surface reconstructions or the presence of heterovalent impurities (such as oxygen). Our results force a reassessment of the impact of surface states on the density of the 2DEG: rather than serving as a supply of electrons, the surface states mainly act to pin the Fermi level. Our conclusions allow a fresh interpretation of experimental observations and allow devising guidelines for optimizing carrier densities in the 2DEG.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS2000

Charge Generation and Propagation in Igneous Rocks

Resistivity changes, ground potentials, electromagnetic (EM) and luminous signals prior to or during earthquakes have been reported, in addition to ground uplift and tilt, and to changes in the seismic wave propagation parameters. However, no physical model exists that ties these diverse phenomena together. Through time-resolved impacts experiments it has been observed that, when igneous rocks (gabbro, diorite, granite) are impacted at low velocities (approx. 100 m/sec), highly mobile electronic charge carriers are generated, spreading from a small volume near the impact point, causing electric potentials, EM and light emission. The rock becomes momentarily conductive. When impacted at higher velocities (approx. 1.5 km/sec), the propagation of the P and S waves is registered through the transient piezoelectric response of quartz. At the same time, the rock volume is filled with mobile charge carriers, and a positive surface potential is registered. During the next 1-2 msec the surface potential oscillates, due to electron injection from ground. These observations are consistent with positive holes, e.g. defect electrons in the O(2-) sublattice, that can travel via the O 2p-dominated valence band of the silicate minerals at the speed of a phonon-mediated charge transfer. Before activation, the positive hole charge carriers lay dormant in form of positive hole pairs, PHP, electrically inactive, chemically equivalent to peroxy links in the structures of constituent minerals. PHPs are introduced by way of hydroxyl (O3Si-OH) incorporated into nominally anhydrous minerals when they crystallize in water-laden environments. Given that sound waves of even relatively low intensity appear to cause PHPs dissociation, thus generating mobile positive holes, it is proposed that microfracturing during rock deformation cause PHP dissociation. Depending on where and how much the rock volume is stressed, the positive holes are expected to form fluctuating charge clouds in the earthquake source region that may account for earthquake-related electrical phenomena and the reported low frequency EM signals.

Freund, Friedemann↗
DOE OSTI2023

Fine‐Tuning Alkyl Chains on Quinoxaline Nonfullerene Acceptors Enables High‐Efficiency Ternary Organic Solar Cells with Optimizing Molecular Stacking and Reducing Energy Loss

Abstract Material design of guest acceptor is always a big challenge for improving the efficiency of ternary organic solar cells (OSCs). Here, a pair of isomeric nonfullerene acceptors based on quinoxaline core, Qx–p‐C 7 H 8 O and Qx–m‐C 7 H 8 O, is designed and synthesized. By moving the alkoxy chain attached on side phenyl frommeta‐position topara‐position, both π–π stacking distance and crystallinity are enhanced simultaneously. They obtain the uplifted lowest unoccupied molecular orbital level. Compared to Qx–m‐C 7 H 8 O, Qx–p‐C 7 H 8 O exhibits wider absorption spectrum and higher extinction coefficient. Using D18‐Cl:N3 as host materials, the addition of guest acceptor Qx–p‐C 7 H 8 O significantly improves the power conversion efficiency (PCE) from 17.61% to 18.49% because of higher open‐circuit voltage (0.875 V) and short‐circuit current density (27.85 mA cm −2 ). This can be attributed to the faster exciton dissociation, more balanced carrier mobility, fine fiber morphology, and lower energy loss in the ternary devices. However, Qx–m‐C 7 H 8 O‐based ternary device achieves relatively low PCE of 17.17% because this device shows extremely low electron mobility. The results indicate that molecular stacking, film morphology, etc., can be effectively modulated by fine‐tuning the side chains of guest materials, which may be an effective design rule for further improving the PCE of OSCs.

Chemistry↗
DOE OSTI2024

Structural anisotropy in Sb thin films

Sb thin films have attracted wide interest due to their tunable band structure, topological phases, high electron mobility, and thermoelectric properties. We successfully grow epitaxial Sb thin films on a closely lattice-matched GaSb(001) surface by molecular beam epitaxy. We find a novel anisotropic directional dependence on their structural, morphological, and electronic properties. The origin of the anisotropic features is elucidated using first-principles density functional theory (DFT) calculations. The growth regime of crystalline and amorphous Sb thin films was determined by mapping the surface reconstruction phase diagram of the GaSb(001) surface under Sb 2 flux, with confirmation of structural characterizations. Crystalline Sb thin films show a rhombohedral crystal structure along the rhombohedral (211) surface orientation parallel to the cubic (001) surface orientation of the GaSb substrate. At this coherent interface, Sb atoms are aligned with the GaSb lattice along the [1̄10] crystallographic direction but are not aligned well along the [110] crystallographic direction, which results in anisotropic features in reflection of high-energy electron diffraction patterns, misfit dislocation formation, surface morphology, and transport properties. Our DFT calculations show that the preferential orientation of the rhombohedral Sb (211) plane may originate from the GaSb surface, where Sb atoms align with the Ga and Sb atoms on the reconstructed surface. The formation energy calculations confirm the stability of the experimentally observed structures. Our results provide optimal film growth conditions for further studies of novel properties of Bi 1-x Sb x thin films with similar lattice parameters and an identical crystal structure, as well as functional heterostructures of them with III–V semiconductor layers along the (001) surface orientation, supported by a theoretical understanding of the anisotropic film orientation.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Melting, reentrant ordering and peak effect for Wigner crystals with quenched and thermal disorder

Abstract We consider simulations of Wigner crystals in solid state systems interacting with random quenched disorder in the presence of thermal fluctuations. When quenched disorder is absent, there is a well defined melting temperature determined by the proliferation of topological defects, while for zero temperature, there is a critical quenched disorder strength above which topological defects proliferate. When both thermal and quenched disorder are present, these effects compete, and the thermal fluctuations can reduce the effectiveness of the quenched disorder, leading to a reentrant ordered phase in agreement with the predictions of Nelson (1983 Phys. Rev. B 27 2902–14). There are two competing theories for the low temperature behavior, and our simulations show that both capture aspects of the actual response. The critical disorder strength separating ordered from disordered states remains finite as the temperature goes to zero, as predicted by Cha and Fertig (1995 Phys. Rev. Lett. 74 4867–70), instead of dropping to zero as predicted by Nelson. At the same time, the critical disorder strength decreases with decreasing temperature, as predicted by Nelson, instead of remaining constant, as predicted by Cha and Fertig. The onset of the reentrant phase can be deduced based on changes in the transport response, where the reentrant ordering appears as an increase in the mobility or the occurrence of a depinning transition. We also find that when the system is in the ordered state and thermally melts, there is an increase in the effective damping or pinning. This produces a drop in the electron mobility that is similar to the peak effect phenomenon found in superconducting vortices, where thermal effects soften the lattice or break down its elasticity, allowing the particles to better adjust their positions to take full advantage of the quenched disorder.

36 MATERIALS SCIENCE↗
NASA NTRS2003

A 94 GHz RF Electronics Subsystem for the CloudSat Cloud Profiling Radar

The CloudSat spacecraft, scheduled for launch in 2004, will carry the 94 GHz Cloud Profiling Radar (CPR) instrument. The design, assembly and test of the flight Radio Frequency Electronics Subsystem (RFES) for this instrument has been completed and is presented here. The RFES consists of an Upconverter (which includes an Exciter and two Drive Amplifiers (DA's)), a Receiver, and a Transmitter Calibrator assembly. Some key performance parameters of the RFES are as follows: dual 100 mW pulse-modulated drive outputs at 94 GHz, overall Receiver noise figure < 5.0 dB, a highly stable W-band noise source to provide knowledge accuracy of Receiver gain of < 0.4 dB over the 2 year mission life, and a W-band peak power detector to monitor the transmitter output power to within 0.5 dB over life. Some recent monolithic microwave integrated circuit (MMIC) designs were utilized which implement the DA's in 0.1 micron GaAs high electron-mobility transistor (HEMT) technology and the Receiver low-noise amplifier (LNA) in 0.1 micron InP HEMT technology.

radio frequency electronics subsystem (RFES)↗
DOE OSTI2022

Origin of the 2D Electron Gas at the SrTiO 3 Surface

Bulk SrTiO 3 is a well-known band insulator and the most common substrate used in the field of complex oxide heterostructures. Its surface and interface with other oxides, however, have demonstrated a variety of remarkable behaviors distinct from those expected. In this work, using a suite of in situ techniques to monitor both the atomic and electronic structures of the SrTiO 3 (001) surface prior to and during growth, the disappearance and re-appearance of a 2D electron gas (2DEG) is observed after the completion of each SrO and TiO 2 monolayer, respectively. The 2DEG is identified with the TiO 2 double layer present at the initial SrTiO 3 surface, which gives rise to a surface potential and mobile electrons due to vacancies within the TiO 2-x adlayer. Much like the electronic reconstruction discovered in other systems, two atomic planes are required, here supplied by the double layer. The combined in situ scattering/spectroscopy findings resolve a number of longstanding issues associated with complex oxide interfaces, facilitating the employment of atomic-scale defect engineering in oxide electronics.

2D electron gas↗
DOE OSTI2020

Naphthalene‐Diimide‐Based Ionenes as Universal Interlayers for Efficient Organic Solar Cells

Abstract Self‐doping ionene polymers were efficiently synthesized by reacting functional naphthalene diimide (NDI) with 1,3‐dibromopropane ( NDI‐NI ) or trans ‐1,4‐dibromo‐2‐butene ( NDI‐CI ) via quaternization polymerization. These NDI‐based ionene polymers are universal interlayers with random molecular orientation, boosting the efficiencies of fullerene‐based, non‐fullerene‐based, and ternary organic solar cells (OSCs) over a wide range of interlayer thicknesses, with a maximum efficiency of 16.9 %. NDI‐NI showed a higher interfacial dipole (Δ), conductivity, and electron mobility than NDI‐CI , affording solar cells with higher efficiencies. These polymers proved to efficiently lower the work function ( WF ) of air‐stable metals and optimize the contact between metal electrode and organic semiconductor, highlighting their power to overcome energy barriers of electron injection and extraction processes for efficient organic electronics.

Liu, Ming↗
DOE OSTI2020

Naphthalene‐Diimide‐Based Ionenes as Universal Interlayers for Efficient Organic Solar Cells

Abstract Self‐doping ionene polymers were efficiently synthesized by reacting functional naphthalene diimide (NDI) with 1,3‐dibromopropane ( NDI‐NI ) or trans ‐1,4‐dibromo‐2‐butene ( NDI‐CI ) via quaternization polymerization. These NDI‐based ionene polymers are universal interlayers with random molecular orientation, boosting the efficiencies of fullerene‐based, non‐fullerene‐based, and ternary organic solar cells (OSCs) over a wide range of interlayer thicknesses, with a maximum efficiency of 16.9 %. NDI‐NI showed a higher interfacial dipole (Δ), conductivity, and electron mobility than NDI‐CI , affording solar cells with higher efficiencies. These polymers proved to efficiently lower the work function ( WF ) of air‐stable metals and optimize the contact between metal electrode and organic semiconductor, highlighting their power to overcome energy barriers of electron injection and extraction processes for efficient organic electronics.

Liu, Ming↗
DOE OSTI2025

Spectroscopic Investigation into P(NDI2OD-T2) Charge Localization

P(NDI2OD-T2), commonly referred to as N2200, stands out as a promising electron-transporting (n-type) polymer for low-cost, flexible (photo)electrochemical applications due to its reversible two-electron reduction and high electron mobility. UV–vis spectroelectrochemistry in the tetrabutyl ammonium hexafluorophosphate/acetonitrile electrolyte shows two sets of chemically reversible redox signals in the cyclic voltammetry corresponding to the reduction of the neutral polymer film to polaronic and bipolaronic species. These electrochemical signatures suggest a distinct electronic reorganization upon reduction (polaron/bipolaron formation), highlighting the need for molecular-level insights into how charges are accommodated within the polymer backbone. While it has been previously hypothesized that charge predominantly localizes on the naphthalene diimide (NDI) unit during reductive charging, specific changes in atomic environments that confirm this localization have not been characterized in n-type polymers. Herein, we use near-edge X-ray absorption fine structure (NEXAFS) spectroscopy to probe electronic transitions in an electrochemically charged polymer to deduce charge localization. The O K-edge (1s) spectra exhibit two distinct π* peaks; the intensity of the lower-energy π* a peak that corresponds to an excitation to a largely localized carbonyl state decreases with reductive potentials relative to the higher-energy π* b peak. We corroborate this with Raman spectroscopy at different potentials, which shows a decrease in intensity on the C–C/C═C and C═O stretching bands of NDI as well as a red shift of the carbonyl band due to the formation of a polaron on the NDI. Additionally, new Raman active NDI signals associated with elongated C═O and C═C bonds are observed at lower energy during the formation of charged states. Together with theoretical calculations, these findings show that the injected charge spatially localizes on the NDI units and is dominantly distributed on the carbonyl groups. In conclusion, the combination of NEXAFS, optical and vibrational spectroscopies, and theoretical calculations is generalizable to other pi-conjugated polymers and can identify charge localization for the further development of organic semiconductors.

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

Assessing Carrier Mobility, Dopability, and Defect Tolerance in the Chalcogenide Perovskite Ba Zr S 3

The chalcogenide perovskite Ba Zr S 3 has attracted much attention as a promising solar absorber for thin-film photovoltaics. Here we use first-principles calculations to evaluate its carrier transport and defect properties. We find that Ba Zr S 3 has a phonon-limited electron mobility of 37 cm 2 / V s, which is comparable to that in halide perovskites, but lower hole mobility of 11 cm 2 / V s. The defect computations indicate that Ba Zr S 3 is intrinsically n -type due to shallow sulfur vacancies, but that strong compensation by sulfur vacancies will prevent attempts to make it p -type. We also establish that Ba Zr S 3 shows some degree of defect tolerance, presenting only few low formation energy, deep intrinsic defects. Among the deep defects, sulfur interstitials are the dominant nonradiative recombination centers but exhibit a moderate capture coefficient. Our work highlights the material’s intrinsic limitations in carrier mobility and p -type doping, and suggests focusing on suppressing the formation of sulfur interstitials to achieve longer carrier lifetime. Published by the American Physical Society 2024

Yuan, Zhenkun (ORCID:0000000272005973)↗
NASA NTRS2008

Three-Stage InP Submillimeter-Wave MMIC Amplifier

A submillimeter-wave monolithic integrated- circuit (S-MMIC) amplifier has been designed and fabricated using an indium phosphide (InP) 35-nm gate-length high electron mobility transistor (HEMT) device, developed at Northrop Grumman Corporation. The HEMT device employs two fingers each 15 micrometers wide. The HEMT wafers are grown by molecular beam epitaxy (MBE) and make use of a pseudomorphic In0.75Ga0.25As channel, a silicon delta-doping layer as the electron supply, an In0.52Al0.48As buffer layer, and an InP substrate. The three-stage design uses coplanar waveguide topology with a very narrow ground-to-ground spacing of 14 micrometers. Quarter-wave matching transmission lines, on-chip metal-insulator-metal shunt capacitors, series thin-film resistors, and matching stubs were used in the design. Series resistors in the shunt branch arm provide the basic circuit stabilization. The S-MMIC amplifier was measured for S-parameters and found to be centered at 320 GHz with 13-15-dB gain from 300-345 GHz. This chip was developed as part of the DARPA Submillimeter Wave Imaging Focal Plane Technology (SWIFT) program (see figure). Submillimeter-wave amplifiers could enable more sensitive receivers for earth science, planetary remote sensing, and astrophysics telescopes, particularly in radio astronomy, both from the ground and in space. A small atmospheric window at 340 GHz exists and could enable ground-based observations. However, the submillimeter-wave regime (above 300 GHz) is best used for space telescopes as Earth s atmosphere attenuates most of the signal through water and oxygen absorption. Future radio telescopes could make use of S-MMIC amplifiers for wideband, low noise, instantaneous frequency coverage, particularly in the case of heterodyne array receivers.

Pukala, David↗
DOE OSTI2021

Mitigation of the internal p-n junction in CoS 2 -contacted FeS 2 single crystals: Accessing bulk semiconducting transport

Pyrite FeS 2 is an outstanding candidate for a low-cost, nontoxic, sustainable photovoltaic material, but efficient pyrite-based solar cells are yet to materialize. Recent studies of single crystals have shed much light on this by uncovering a p-type surface inversion layer on n-type (S-vacancy doped) crystals, and the resulting internal p-n junction. This leaky internal junction likely plays a key role in limiting efficiency in pyrite-based photovoltaic devices, also obscuring the true bulk semiconducting transport properties of pyrite crystals. Here, we demonstrate complete mitigation of the internal p-n junction in FeS 2 crystals by fabricating metallic CoS 2 contacts via a process that simultaneously diffuses Co (a shallow donor) into the crystal, the resulting heavy n doping yielding direct Ohmic contact to the interior. Low-temperature bulk transport studies of controllably Co- and S-vacancy doped semiconducting crystals then enable a host of previously inaccessible observations and measurements, including determination of donor activation energies (which are as low as 5 meV for Co), observation of an unexpected second activated transport regime, realization of electron mobility up to 2100 cm 2 V –1 s –1 , elucidation of very different mobilities in Co- and S-vacancy-doped cases, and observation of an abrupt temperaturedependent crossover to bulk Efros-Shklovskii variable-range hopping, accompanied by an unusual form of nonlinear Hall effect. Aspects of the results are interpreted with the aid of first-principles electronic structure calculations on both Co- and S-vacancy-doped FeS 2 . Furthermore, this work thus demonstrates unequivocal mitigation of the internal p-n junction in pyrite single crystals, with important implications for both future fundamental studies and photovoltaic devices

36 MATERIALS SCIENCE↗
DOE OSTI2023

Role of aggregates and microstructure of mixed-ionic–electronic-conductors on charge transport in electrochemical transistors

Synthetic efforts have delivered a library of organic mixed ionic–electronic conductors (OMIECs) with high performance in electrochemical transistors. The most promising materials are redox-active conjugated polymers with hydrophilic side chains that reach high transconductances in aqueous electrolytes due to volumetric electrochemical charging. Current approaches to improve transconductance and device stability focus mostly on materials chemistry including backbone and side chain design. However, other parameters such as the initial microstructure and microstructural rearrangements during electrochemical charging are equally important and are influenced by backbone and side chain chemistry. In this study, we employ a polymer system to investigate the fundamental electrochemical charging mechanisms of OMIECs. We couple in situ electronic charge transport measurements and spectroelectrochemistry with ex situ X-ray scattering electrochemical charging experiments and find that polymer chains planarize during electrochemical charging. Our work shows that the most effective conductivity modulation is related to electrochemical accessibility of well-ordered, interconnected aggregates that host high mobility electronic charge carriers. Electrochemical stress cycling induces microstructural changes, but we find that these aggregates can largely maintain order, providing insights on the structural stability and reversibility of electrochemical charging in these systems. Finally, this work shows the importance of material design for creating OMIECs that undergo structural rearrangements to accommodate ions and electronic charge carriers during which percolating networks are formed for efficient electronic charge transport.

36 MATERIALS SCIENCE↗
DOE OSTI2022

GaN HEMT Fabrication for Radiation-Hardened Sensing and Communications Electronics

Gallium nitride (GaN), a wide bandgap semiconductor, has vast potential to address two environment conditions associated with the application of electronics to nuclear power: elevated temperatures, and high levels of radiation. A process was developed at The Ohio State University (OSU) to enable fabrication of complex digital and analog electronics circuits for application to nuclear power environments such as locations near or in the reactor core or in spent nuclear fuel casks. Radio frequency (RF)-grade GaN high electron mobility transistor (HEMT) devices were fabricated as part of this process. These were fabricated as depletion mode and enhancement mode devices. They have been electrically characterized and have demonstrated the expected performance. Behavioral models (Verilog-A) were developed from these device measurements to enable electrical simulation of GaN HEMT devices and circuits using common electronics simulation tools based on Simulation Program with Integrated Circuit Emphasis (SPICE). A similar set of GaN HEMT devices is being developed to provide lower speed devices for logic and analog functions. These accomplishments position this technology for effective application to sensor interfacing, signal processing, and data communications in nuclear power plants, including operation in or near the reactor core.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2023

Low-thermal-budget synthesis of monolayer molybdenum disulfide for silicon back-end-of-line integration on a 200 mm platform

Two-dimensional (2D) materials are promising candidates for future electronics due to their excellent electrical and photonic properties. Although promising results on the wafer-scale synthesis (≤150 mm diameter) of monolayer molybdenum disulfide (MoS 2 ) have already been reported, the high-quality synthesis of 2D materials on wafers of 200 mm or larger, which are typically used in commercial silicon foundries, remains difficult. The back-end-of-line (BEOL) integration of directly grown 2D materials on silicon complementary metal–oxide–semiconductor (CMOS) circuits is also unavailable due to the high thermal budget required, which far exceeds the limits of silicon BEOL integration (<400 °C). This high temperature forces the use of challenging transfer processes, which tend to introduce defects and contamination to both the 2D materials and the BEOL circuits. Here we report a low-thermal-budget synthesis method (growth temperature < 300 °C, growth time ≤ 60 min) for monolayer MoS 2 films, which enables the 2D material to be synthesized at a temperature below the precursor decomposition temperature and grown directly on silicon CMOS circuits without requiring any transfer process. We designed a metal–organic chemical vapour deposition reactor to separate the low-temperature growth region from the high-temperature chalcogenide-precursor-decomposition region. We obtain monolayer MoS 2 with electrical uniformity on 200 mm wafers, as well as a high material quality with an electron mobility of ~35.9 cm 2 V -1 s -1 . Finally, we demonstrate a silicon-CMOS-compatible BEOL fabrication process flow for MoS 2 transistors; the performance of these silicon devices shows negligible degradation (current variation < 0.5%, threshold voltage shift < 20 mV). We believe that this is an important step towards monolithic 3D integration for future electronics.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2021

Phonon- and defect-limited electron and hole mobility of diamond and cubic boron nitride: A critical comparison

Diamond and cBN are two of the most promising ultra-wide bandgap semiconductors for applications in high-power high-frequency electronic devices. Despite extensive studies on carrier transport in these materials, there are large discrepancies in their reported carrier mobilities. In this work, we investigate the phonon- and dopant-limited electron and hole mobilities of cBN and diamond with atomistic first-principles calculations in order to understand their fundamental upper bounds to carrier transport. Our results show that although the phonon-limited electron mobilities are comparable between cBN and diamond, the hole mobility is significantly lower in cBN due to its heavier hole effective mass. Moreover, although lattice scattering dominates the mobility at low doping, neutral impurity scattering becomes the dominant scattering mechanism at higher dopant concentrations due to the high dopant ionization energies. Our analysis provides critical insights and reveals the intrinsic upper limits to the carrier mobilities of diamond and cBN as a function of doping and temperature for applications in high-power electronic devices.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗