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Results for “charge-carrier doping”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Controllable Formation of Threefold-Coordinated Oxygen in Graphene by Low-Energy Ion Implantation

The atomically precise engineering of impurities in graphene and the understanding of their structural and carrier-dependent electronic properties at the nanoscale are crucial for advancing graphene-based nanoelectronics, catalysis, and energy technologies. Here, we demonstrate controllable incorporation of the elusive 3-fold-coordinated O substitutions into graphene using low-energy O + ion implantation under ultrahigh-vacuum conditions. By combining high-resolution scanning tunneling microscopy and spectroscopy (STM/S), bond-resolved noncontact atomic force microscopy techniques, and density functional theory (DFT) calculations, we resolve both the structural and electronic properties of the O-related defects. The STM/S measurements, corroborated by DFT calculations, uncover a characteristic impurity state that is energetically pinned to the Dirac point across different charge-carrier doping regimes. Molecular dynamics simulations further reveal the distribution of implantation-induced configurations and identify the formation of 3-fold-coordinated O dopants. Furthermore, this work provides a viable route to incorporate 3-fold-coordinated O dopants and opens new opportunities for controlled defect engineering in graphene.

3-fold-coordinated oxygen↗
DOE OSTI2020

Hund's metal physics: From SrNiO 2 to LaNiO 2

We study the normal state electronic structure of the recently discovered infinite-layer nickelate superconductor, Nd 1-x Sr x NiO 2 , using density functional theory plus dynamical mean-field theory calculations. Starting with the multiorbital compound SrNiO 2 , our calculations show that despite large charge-carrier doping from SrNiO 2 to LaNiO 2 , the Ni-3d total occupancy is barely changed due to the decreased hybridization with the occupied oxygen-2p states and increased hybridization with the unoccupied La-5d states. Thus, using SrNiO 2 as a reference, La 1-x Sr x NiO 2 is naturally and conclusively found to be a multiorbital electronic system with characteristic Hund's metal behaviors, such as metallicity, the importance of high-spin configurations, tendency towards orbital differentiation, and the absence of magnetism in regimes which are ordered according to static mean-field theories. Finally, our results are in good agreement with the existing spectroscopic studies and make an essential step towards an understanding of the electronic structures of Nd 1-x Sr x NiO 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

High-performance carbon nanotube electronic ratchets

The rapid advancements in low-power portable/wearable electronic devices require concurrent development of technologies that can provide power without the need for bulky, heavy battery storage. Electronic ratchets, asymmetric transistor-based devices that can convert AC signals or electronic noise into DC power, have been proposed as one solution to this growing need. Here, the recent demonstration of conjugated polymer-based electronic ratchets offers a route toward lightweight, flexible power sources for portable applications. Here we demonstrate the fabrication of the first electronic ratchets where the active channel component consists of semiconducting single-walled carbon nanotubes (s-SWCNTs), which can transform electronic noise or AC signals to a stable DC current with higher output power (up to ca. 14 mW for a chemically doped device) than their polymer-based analogs. We also show that patterning of the dopant profile in the s-SWCNT channel enables reasonable power conversion performance (ca. 3.5 mW) with improved stability relative to homogeneously doped devices. Our findings demonstrate the promise for s-SWCNT electronic ratchets as energy harvesting devices for portable, low-power applications.

ENGINEERING,MATERIALS SCIENCE,NANOSCIENCE AND NANO↗
DOE OSTI2022

Establishing Self-Dopant Design Principles from Structure–Function Relationships in Self-n-Doped Perylene Diimide Organic Semiconductors

Self-doping is a particular doping method that has been applied to a wide range of organic semiconductors. However, there is a lack of understanding regarding the relationship between dopant structure and function. A structurally diverse series of self-n-doped perylene diimides (PDIs) is investigated to study the impact of steric encumbrance, counterion selection, and dopant/PDI tether distance on functional parameters such as doping, stability, morphology, and charge-carrier mobility. The studies show that self-n-doping is best enabled by the use of sterically encumbered ammoniums with short tethers and Lewis basic counterions. Additionally, water is found to inhibit doping, which concludes that thermal degradation is merely a phenomenological feature of certain dopants, and that residual solvent evaporation is the primary driver of thermally activated doping. In situ grazing-incidence wide-angle X-ray scattering studies show that sample annealing increases the π–π stacking distance and shrinks grain boundaries for improved long-range ordering. These features are then correlated to contactless carrier-mobility measurements with time-resolved microwave conductivity before and after thermal annealing. In conclusion, the collective relationships between structural features and functionality are finally used to establish explicit self-n-dopant design principles for the future design of materials with improved functionality.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Pinhole electrical conductivity in polycrystalline Si on locally etched SiN$_y$/SiO$_x$ passivating contacts for Si solar cells

State-of-the-art monocrystalline Si (c-Si) solar cells require passivating contacts to achieve a high degree of charge-carrier separation and collection. In this work, we focus on boron-doped polycrystalline Si on locally etched silicon nitride/silicon oxide (PLENO) passivating contacts. In PLENO contacts, excellent surface passivation is provided by the ~10 nm dielectric bilayer, while pinholes in the dielectric bilayer, that are filled with doped polycrystalline Si, provide charge-carrier selectivity and transport. During PLENO fabrication, etch undercut in the dielectric bilayer occurs. Here, using electrical characterization and microscopies, we show that undercut causes pinholes to be electrically resistive in PLENO. A processing sequence that eliminates the undercut in the final PLENO structure results in electrically conductive pinholes with low contact resistivity.

14 SOLAR ENERGY↗
DOE OSTI2022

A laser-assisted chlorination process for reversible writing of doping patterns in graphene

Chemical doping can be used to control the charge-carrier polarity and concentration in two-dimensional van der Waals materials. However, conventional methods based on substitutional doping or surface functionalization result in the degradation of electrical mobility due to structural disorder, and the maximum doping density is set by the solubility limit of dopants. Here we show that a reversible laser-assisted chlorination process can be used to create high doping concentrations (above 3 × 10 13 cm -2 ) in graphene monolayers with minimal drops in mobility. The approach uses two lasers—with distinct photon energies and geometric configurations—that are designed for chlorination and subsequent chlorine removal, allowing highly doped patterns to be written and erased without damaging the graphene. To illustrate the capabilities of our approach, we use it to create rewritable photoactive junctions for graphene-based photodetectors.

42 ENGINEERING↗
DOE OSTI2023

High-Performance Passivating Contacts for Si PV Based on Engineered, Doped Nanopinholes through Dielectric Layers

We present a novel, industrially relevant method to fabricate high-performance poly-Si passivating contacts for Si PV. Passivating contacts based on SiOx/poly-Si layer stacks have been implemented in record-efficiency homojunction Si solar cells. In this technology, the carrier transport through a surface-passivating SiOx is enabled either by quantum-tunneling or nanopinholes. The doped poly-Si layer provides charge-carrier selectivity. Previously, the ISFH research group demonstrated a record 26.1% efficient Si homojunction cell, where transport pinholes in ~2 nm SiOx were produced by thermal breakdown at > 1000 degrees C, which is hard to control and is surface morphology-dependent. At room temperature, our new process uses electroless plating of Ag nanoparticles, followed by metal-assisted chemical etching. Nanogalvanic corrosion yields < 20 nm-wide nanopinholes in an insulating > 2 nm SiOx layer. The nanopinholes are filled by a heavily doped a-Si:H overlayer. We drive in the dopants into the Si wafer with subsequent high-temperature annealing. Preferential incorporation of dopants at pinhole locations results in nanoscale p+/n or n+/n junctions near the wafer interface. Each heavily-doped nanoscale pinhole junction collects and transports photogenerated carriers to the cell metal contacts. The density of the engineered nanopinholes can be tuned over a wide range which is critical for optimization of device performance. The same nanogalvanic corrosion principles can be applied to produce doped transport pinholes in well-passivating thick dielectric SiOx/SiNy stacks. Importantly, our process does not rely on thermal breakdown of the dielectric layers and can be applied to textured wafers resulting in Si solar cells with > 20% conversion efficiency.

dielectric layer↗
NASA NTRS1989

Piezoresistive silicon pressure sensors in cryogenic environment

This paper presents data on low-temperature measurements of silicon pressure sensors. It was found that both the piezoresistance coefficients and the charge-carrier mobility increase with decreasing temperature. For lightly doped semiconductor materials, the density of free charge carriers decreases with temperature and can freeze out eventually. However, the effect of carrier freeze-out can be minimized by increasing the impurity content to higher levels, at which the temperature dependency of piezoresistance coefficients is reduced. An impurity density of 1 x 10 to the 19th/cu cm was found to be optimal for cryogenic applications of pressure sensor dies.

Kahng, Seun K.↗
DOE OSTI2021

Correlation between antiferromagnetic and Mott states in spin orbit coupled Sr 2 Ir O 4 : A study of Sr 2 Ir 1 – x M x O 4 ( M = Fe or Co)

Sr 2 IrO 4 is an archetypal spin-orbit-coupled Mott insulator with an antiferromagnetic state below 240 K. Here we report results of our study on single crystals of Sr 2 Ir 1–x Fe x O 4 (0 ≤ x < 0.32) and Sr 2 Ir 1–x Co x O 4 (0 ≤ x < 0.22). Fe doping retains the antiferromagnetic state but simultaneously precipitates an emergent metallic state whereas Co doping causes a rapid collapse of both the antiferromagnetic and Mott states, giving rise to a confined metallic state featuring a pronounced linearity of the basal-plane resistivity up to 700 K. The results indicate tetravalent Fe 4+ (3d 4 ) ions in the intermediate spin state with S = 1 and Co 4+ (3d 5 ) ions in the high spin state with S = 5/2 substituting for Ir 4+ (5d 5 ) ions in Sr 2 IrO 4 , respectively. The effective magnetic moment closely tracks the Néel temperature as doping increases, suggesting that the spin state of the dopant predominately determines the magnetic properties in doped Sr 2 IrO 4 . Furthermore, all relevant properties including charge-carrier density (e.g., 10 28 /m 3 ), Sommerfeld coefficient (e.g., 19 mJ / mole K 2 ), and Wilson ratio (e.g., 2.6) consistently demonstrate an emergent metallic state that is both robust and highly correlated in the two systems, arising from the percolation of bound states and the weakening of structural distortions. Furthermore, this study strongly indicates that the antiferromagnetic and Mott states are correlated in an unconventional manner in Sr 2 IrO 4 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Non-covalent planarizing interactions yield highly ordered and thermotropic liquid crystalline conjugated polymers

Controlling the multi-level assembly and morphological properties of conjugated polymers through structural manipulation has contributed significantly to the advancement of organic electronics. In this work, a redox active conjugated polymer, TPT–TT, composed of alternating 1,4-(2-thienyl)-2,5-dialkoxyphenylene (TPT) and thienothiophene (TT) units is reported with non-covalent intramolecular S⋯O and S⋯H–C interactions that induce controlled main-chain planarity and solid-state order. As confirmed by density functional theory (DFT) calculations, these intramolecular interactions influence the main chain conformation, promoting backbone planarization, while still allowing dihedral rotations at higher kinetic energies (higher temperature), and give rise to temperature-dependent aggregation properties. Thermotropic liquid crystalline (LC) behavior is confirmed by cross-polarized optical microscopy (CPOM) and closely correlated with multiple thermal transitions observed by differential scanning calorimetry (DSC). This LC behavior allows us to develop and utilize a thermal annealing treatment that results in thin films with notable long-range order, as shown by grazing-incidence X-ray diffraction (GIXD). Specifically, we identified a first LC phase, ranging from 218 °C to 107 °C, as a nematic phase featuring preferential face-on π–π stacking and edge-on lamellar stacking exhibiting a large extent of disorder and broad orientation distribution. A second LC phase is observed from 107 °C to 48 °C, as a smectic A phase featuring sharp, highly ordered out-of-plane lamellar stacking features and sharp tilted backbone stacking peaks, while the structure of a third LC phase with a transition at 48 °C remains unclear, but resembles that of the solid state at ambient temperature. Furthermore, the significance of thermal annealing is evident in the ∼3-fold enhancement of the electrical conductivity of ferric tosylate-doped annealed films reaching 55 S cm −1 . More importantly, thermally annealed TPT–TT films exhibit both a narrow distribution of charge-carrier mobilities (1.4 ± 0.1) × 10 −2 cm 2 V −1 s −1 along with a remarkable device yield of 100% in an organic field-effect transistor (OFET) configuration. This molecular design approach to obtain highly ordered conjugated polymers in the solid state affords a deeper understanding of how intramolecular interactions and repeat-unit symmetry impact liquid crystallinity, solution aggregation, solution to solid-state transformation, solid-state morphology, and ultimately device applications.

Chemistry↗
DOE OSTI2021

Controlled n –Doping of Naphthalene Diimide–Based Two–Dimensional Polymers

Two-dimensional polymers (2DPs) are promising as structurally well-defined, permanently porous, organic semiconductors. However, 2DPs are nearly always isolated as closed shell organic species with limited charge carriers, which leads to low bulk conductivities. Here, we enhance the bulk conductivity of two naphthalene diimide (NDI)-containing 2DP semiconductors by controllably n-doping the NDI units using cobaltocene (CoCp 2 ). Optical and transient microwave spectroscopy reveals that both as-prepared NDI-containing 2DPs are semiconducting with sub-2 eV optical bandgaps and photoexcited charge-carrier lifetimes of tens of nanoseconds. Following reduction with CoCp 2 , both 2DPs largely retain their periodic structures and exhibit optical and electron-spin resonance spectroscopic features consistent with the presence of NDI-radical anions. Here, while the native NDI-based 2DPs are electronically insulating, maximum bulk conductivities of >10 –4 S cm –1 are achieved by substoichiometric levels of n-doping. Density functional theory calculations show that the strongest electronic couplings in these 2DPs exist in the out-of-plane (π-stacking) crystallographic directions, which indicates that cross-plane electronic transport through NDI stacks is primarily responsible for the observed electronic conductivity. Taken together, this study underlines that controlled molecular doping is a useful approach to access structurally well-defined, paramagnetic, 2DP n-type semiconductors with measurable bulk electronic conductivities of interest for electronic or spintronic devices.

2D polymers↗
DOE OSTI2026

Quantitative Infrared-to-Terahertz Nanospectroscopy of Semiconductors

Semiconductor technology now employs few-nanometer features, necessitating tools probing electronic properties on the same length scale. While the concentration of free charge carriers is routinely measured, the scattering rate remains challenging to access at the nanoscale. Here, we present ultrabroadband (5–50 THz) synchrotron infrared nanospectroscopy as a quantitative metrology tool for semiconductors. This technique can determine both the charge carrier concentration and scattering rate with percent-level accuracy, and it is inherently capable of ∼10 nm spatial resolution. We study silicon with different doping levels and confirm the method’s accuracy by statistical analysis and comparison with established far-field infrared spectroscopy. Near-field measurements systematically reveal charge-carrier concentrations ∼30% lower than far-field values, consistent with increased surface sensitivity and surface depletion. Our work establishes synchrotron infrared nanospectroscopy as a precise tool for quantitative nanoscale semiconductor characterization and paves the way toward all-optical characterization of surface depletion effects.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Synthesis, Hole Doping, and Electrical Properties of a Semiconducting Azatriangulene-Based Covalent Organic Framework

Two-dimensional covalent organic frameworks (2D COFs) containing heterotriangulenes have been theoretically identified as semiconductors with tunable, Dirac-cone-like band structures, which are expected to afford high charge-carrier mobilities ideal for next-generation flexible electronics. However, few bulk syntheses of these materials have been reported, and existing synthetic methods provide limited control of network purity and morphology. Here, we report transimination reactions between benzophenone-imine-protected azatriangulenes (OTPA) and benzodithiophene dialdehydes (BDT), which afforded a new semiconducting COF network, OTPA-BDT. The COFs were prepared as both polycrystalline powders and thin films with controlled crystallite orientation. Here, the azatriangulene nodes are readily oxidized to stable radical cations upon exposure to an appropriate p type dopant, tris(4-bromophenyl)ammoniumyl hexachloroantimonate, after which the network’s crystallinity and orientation are maintained. Oriented, hole-doped OTPA-BDT COF films exhibit electrical conductivities of up to 1.2 × 10 –1 S cm –1 , which are among the highest reported for imine-linked 2D COFs to date.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Optically controllable magnetism in atomically thin semiconductors

We report evidence that ferromagnetic order in electrostatically doped, monolayer transition metal dichalcogenide (TMD) semiconductors can be stabilized and controlled at zero magnetic field by local optical pumping. We use circular dichroism (CD) in reflectivity from excitonic states as a spatially resolved probe of charge-carrier spin polarization. At electron densities $n_e$ ~ 10 12 cm -2 , a diffraction-limited, circularly polarized optical pump breaks symmetry between oppositely polarized magnetic states and stabilizes long-range magnetic order, with carrier polarization exceeding 80% over an 8 μm by 5 μm extent. In time-resolved measurements with pulsed optical excitation, we observe that magnetic interactions amplify the initial pump-induced spin polarization by more than an order of magnitude. The optical control of magnetism with local optical pumps will unlock advancements in spin and optical technologies and provides a versatile tool in the study of correlated phases in two-dimensional electron gases.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Revealing Micro-Scale Doping Variations in Thin-Films via Simultaneous Luminescence and Current Collection Measurements

Doping thin films used for photovoltaic absorbers is both critical to maximize device voltage and challenging due to complex interactions between point defects in these materials. Such interactions can result in compensation of the intended dopant species, meaning that the active charge-carrier concentration is lower than the concentration incorporated dopants. Charge-carrier compensation is directly related to the open-circuit voltage (VOC) deficit, or magnitude of VOC relative to the theoretical limit. Understanding how the carrier concentration varies within thin-films is necessary to design material processing schedules to minimize this VOC deficit and produce more efficient devices. Unfortunately, measurements of the free carrier concentration are generally relevant at the device level and cannot resolve local differences. Resolving local doping differences in thin-films such as Cd(Se,Te), CZTS, and CIGSe requires techniques with micron or sub-micron spatial resolution due to the polycrystalline structure as well as intended and unintended composition variations in these materials. In this contribution, we show how simultaneous measurement of cathodoluminescence (CL) and electron-beam-induced current (EBIC) can be used to expose doping variations in Cd(Se,Te) thin-films. Simultaneous collection of these signals reveals unexpected differences in the electric field strength through the device thickness due to spatial variation in the carrier concentration.

41 EE - Solar Energy Technologies Office (EE-4S)↗
DOE OSTI2026

Thermoelectric Behavior of Structurally Disordered Lanthanide and Actinide Silicides

Lanthanide and actinide intermetallic materials exhibit intriguing electronic, structural, and magnetic properties arising from their partially filled f orbitals. Strong f-electron correlations can significantly modify the electronic density of states, carrier scattering, and transport behavior, making these systems promising candidates for unconventional thermoelectric materials. In previous studies, single crystals of A1.33T4Al8Si2 (A = Ce, Th, U, Np; T = Co, Ni) were synthesized. This structure consists of ordered TAl2 corrugated double layers separated by disordered An–Si monolayers. The inherent disorder within the An–Si layers has been linked to unusual magnetic behavior, such as spin-glass phenomena, and is expected to strongly influence phonon scattering and charge-carrier transport relevant to thermoelectric performance. However, the thermoelectric properties of this material family have not previously been explored. In this work, DFT calculations were performed to evaluate the electronic density of states, band structures, and thermoelectric properties, including the effects of doping. To validate these predictions, Ce1.33Co4Al8Si2 single crystals were grown and experimentally characterized. Additionally, a new Yb1.33Co4Al8Si2 phase was synthesized and characterized using single-crystal XRD, SEM-EDS, magnetization measurements, and thermoelectric measurements. These results provide insight into structure–property relationships governing thermoelectric behavior in f-electron intermetallics and offer guidance for future thermoelectric materials.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C↗
DOE OSTI2022

Electrically controllable chirality in a nanophotonic interface with a two-dimensional semiconductor

Chiral nanophotonic interfaces enable propagation direction-dependent interactions between guided optical modes and circularly dichroic materials. Electrical tuning of interface chirality would aid active, switchable non-reciprocity in on-chip optoelectronic and photonic circuitry, but remains an outstanding challenge. Here, in this paper, we report electrically controllable chirality in a nanophotonic interface with atomically thin monolayer tungsten diselenide (WSe 2 ). Titanium dioxide waveguides are directly fabricated on the surface of low-disorder, boron nitride-encapsulated WSe 2 . Following integration, photoluminescence from excitonic states into the waveguide can be electrically switched between balanced and directionally biased emission. The operational principle leverages the doping-dependent valley polarization of excitonic states in WSe 2 . Furthermore, the nanophotonic waveguide can function as a near-field source for diffusive exciton fluxes, which display valley and spin polarizations that are inherited from the interface chirality. Our versatile fabrication approach enables the deterministic integration of photonics with van der Waals heterostructures and could provide optical control over their excitonic and charge-carrier behaviour.

42 ENGINEERING↗
DOE OSTI2021

Fabrication of Poly-Si on Locally Etched SiOx as Passivating Contacts for c-Si Solar Cells

Polysilicon on silicon oxide (poly-Si/SiO x ) passivating contacts with predominant charge-carrier transport via pinholes were prepared with room temperature metal-assisted chemical etching. Pinhole areal densities in the range of 2.8 x 10^4 to 4.5 x 10^7 cm^-2 were imaged by SEM. Contact resistivity of 32 m-ohm-cm^2 and implied open circuit voltage of 729 mV were obtained for symmetric n+ poly-Si/SiOx grown onto randomly textured n-Cz. We also show preliminary data pertaining boron-doped polysilicon on nitride/oxide passivating contacts, with which we achieved implied open circuit voltage above 730 mV and recombination current of 0.2 fA/cm^2.

amorphous Si↗