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

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Thermoelectrics: From longitudinal to transverse

Thermoelectric power generation is a promising technology to realize a sustainable society because it directly converts thermal energy into electricity in a solid. Conventional thermoelectric generation is driven by the Seebeck effect, discovered by T.J. Seebeck in 1821, in which a charge current J c is generated in the direction parallel to a temperature gradient ∇T, the longitudinal geometry. Here, the ratio between the generated longitudinal electromotive force and applied ∇T is defined as the Seebeck coefficient. As shown in Figure 1A, a thermoelectric module based on the Seebeck effect typically consists of many pairs (128 for a 12V unit) of p-type and n-type conductors alternately arranged and connected in series. Since the Seebeck coefficient of a p-type (n-type) conductor is positive (negative), the thermopower in each element adds to the total output in the Seebeck module. This configuration is needed to achieve a practical voltage because each element only supplies millivolts but limits the use of thermoelectric generators. The efficiency of thermoelectric generators is characterized by the thermoelectric figure of merit, zT. Despite a 3-fold improvement in zT resulting from materials research over the last two decades, little progress has been made in their practical use; this is ascribed to the technological challenges in contact technology. The contacts on the hot side are subject to thermal degradation. All contacts (512 for a 12V unit) add electrical and thermal contact resistances that reduce the device efficiency to a fraction of that promised by the materials.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2023

Designing transparent conductors using forbidden optical transitions

Many semiconductors present weak or forbidden transitions at their fundamental band gaps, inducing a widened region of transparency. This occurs in high-performing n-type transparent conductors (TCs) such as Sn-doped In 2 O 3 (ITO); however, thus far, the presence of forbidden transitions has been neglected in the search for new p-type TCs. To address this, we first compute high-throughput absorption spectra across ~18, 000 semiconductors, showing that over half exhibit forbidden or weak optical transitions at their band edges. Next, we demonstrate that compounds with highly localized band-edge states are more likely to present forbidden transitions. Lastly, we search this set for p-type and n-type TCs with forbidden transitions and, by performing defect calculations, propose unexplored TC candidates such as ambipolar BeSiP 2 , p-type wurtzite BAs, and n-type Ba 2 InGaO 5 , among others. In conclusion, we share our dataset and recommend that future screenings for optical properties consider the impact of forbidden transitions.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Transport properties of the SnBi{sub 2}Te{sub 4}–PbBi{sub 2}Te{sub 4} solid solution

We report on the electrical and thermal transport properties of the Sn{sub 1−x}Pb{sub x}Bi{sub 2}Te{sub 4} series and we discuss the potential of these materials for thermoelectric conversion applications. From the evolution of the XRD patterns, we can confidently conclude that a complete solid solution exists between SnBi{sub 2}Te{sub 4} and PbBi{sub 2}Te{sub 4}, with no miscibility gap. A crossover from p-type conduction in Sn-rich samples to n-type conduction in Pb-rich ones has been observed, with a transition between x=0.3 and 0.4. A concomitant increase of the electrical resistivity and of the Seebeck coefficient has been observed in the solid solution, which leads to almost constant values of the thermoelectric power factor. Moreover, the thermal conductivity is slightly reduced in the solid solution. The best figure of merit ZT values at room temperature have been observed for p-type Sn{sub 0.8}Pb{sub 0.2}Bi{sub 2}Te{sub 4} with ZT=0.25 and for n-type Sn{sub 0.3}Pb{sub 0.7}Bi{sub 2}Te{sub 4} with ZT=0.15. - Graphical abstract: Seebeck coefficient in (Pb/Sn)Bi{sub 2}Te{sub 4} solid solution. - Highlights: • A complete solid solution exists between PbBi{sub 2}Te{sub 4} and SnBi{sub 2}Te{sub 4.} • A crossover between p-type and n-type is observed for 0.3<Pb fraction <0.4. • The lattice thermal conductivity is hardly reduced in the solid solution.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Nonequilibrium Green's function formulation of intersubband absorption for nonparabolic single-band effective mass Hamiltonian

The formulas are derived that enable calculations of intersubband absorption coefficient within nonequilibrium Green's function method applied to a single-band effective-mass Hamiltonian with the energy dependent effective mass. The derivation provides also the formulas for the virtual valence band components of the two-band Green's functions which can be used for more exact estimation of the density of states and electrons and more reliable treatment of electronic transport in unipolar n-type heterostructure semiconductor devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Growth temperature dependence of Si doping efficiency and compensating deep level defect incorporation in Al{sub 0.7}Ga{sub 0.3}N

The growth temperature dependence of Si doping efficiency and deep level defect formation was investigated for n-type Al{sub 0.7}Ga{sub 0.3}N. It was observed that dopant compensation was greatly reduced with reduced growth temperature. Deep level optical spectroscopy and lighted capacitance-voltage were used to understand the role of acceptor-like deep level defects on doping efficiency. Deep level defects were observed at 2.34 eV, 3.56 eV, and 4.74 eV below the conduction band minimum. The latter two deep levels were identified as the major compensators because the reduction in their concentrations at reduced growth temperature correlated closely with the concomitant increase in free electron concentration. Possible mechanisms for the strong growth temperature dependence of deep level formation are considered, including thermodynamically driven compensating defect formation that can arise for a semiconductor with very large band gap energy, such as Al{sub 0.7}Ga{sub 0.3}N.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Metal-interconnection-free integration of InGaN/GaN light emitting diodes with AlGaN/GaN high electron mobility transistors

We report a metal-interconnection-free integration scheme for InGaN/GaN light emitting diodes (LEDs) and AlGaN/GaN high electron mobility transistors (HEMTs) by combining selective epi removal (SER) and selective epitaxial growth (SEG) techniques. SER of HEMT epi was carried out first to expose the bottom unintentionally doped GaN buffer and the sidewall GaN channel. A LED structure was regrown in the SER region with the bottom n-type GaN layer (n-electrode of the LED) connected to the HEMTs laterally, enabling monolithic integration of the HEMTs and LEDs (HEMT-LED) without metal-interconnection. In addition to saving substrate real estate, minimal interface resistance between the regrown n-type GaN and the HEMT channel is a significant improvement over metal-interconnection. Furthermore, excellent off-state leakage characteristics of the driving transistor can also be guaranteed in such an integration scheme.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Facile fabrication of a ultraviolet tunable MoS{sub 2}/p-Si junction diode

Chemical vapor deposition grown MoS{sub 2} single crystals were transferred onto the edge of a p-Si/SiO{sub 2} wafer, forming an abrupt heterogeneous junction diode at the MoS{sub 2}/p-Si interface. When electrically characterized as a field effect transistor, MoS{sub 2} exhibits an n-type response and can be doped in the presence of ultraviolet (UV) light. As a diode, it operates satisfactorily in air, but has higher currents in vacuum with a turn on voltage of ∼1.3 V and an on/off ratio of 20 at ±2 V. UV irradiation increases the diode on state current, decreases the turn-on voltage, and reduces the ideality parameter below 2. These changes are reversible after annealing in air as desorption of electron trapping species like O{sub 2}{sup −} and H{sub 2}O{sup −} are believed responsible for this effect. A circuit integrating this diode was used to rectify a 1 kHz signal with an efficiency of 12%. Its simple design, coupled with the ability to clip AC signals, sense UV light, and reversibly tune these diodes, makes them inexpensive, multifunctional, and usable as active or passive circuit components in complex electronics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Interfacial electronic structure at the CH{sub 3}NH{sub 3}PbI{sub 3}/MoO{sub x} interface

Interfacial electronic properties of the CH{sub 3}NH{sub 3}PbI{sub 3} (MAPbI{sub 3})/MoO{sub x} interface are investigated using ultraviolet photoemission spectroscopy and X-ray photoemission spectroscopy. It is found that the pristine MAPbI{sub 3} film coated onto the substrate of poly (3,4-ethylenedioxythiophene) poly(styrenesulfonate)/indium tin oxide by two-step method behaves as an n-type semiconductor, with a band gap of ∼1.7 eV and a valence band edge of 1.40 eV below the Fermi energy (E{sub F}). With the MoO{sub x} deposition of 64 Å upon MAPbI{sub 3}, the energy levels of MAPbI{sub 3} shift toward higher binding energy by 0.25 eV due to electron transfer from MAPbI{sub 3} to MoO{sub x}. Its conduction band edge is observed to almost pin to the E{sub F}, indicating a significant enhancement of conductivity. Meanwhile, the energy levels of MoO{sub x} shift toward lower binding energy by ∼0.30 eV, and an interface dipole of 2.13 eV is observed at the interface of MAPbI{sub 3}/MoO{sub x}. Most importantly, the chemical reaction taking place at this interface results in unfavorable interface energy level alignment for hole extraction. A potential barrier of ∼1.36 eV observed for hole transport will impede the hole extraction from MAPbI{sub 3} to MoO{sub x}. On the other hand, a potential barrier of ∼0.14 eV for electron extraction is too small to efficiently suppress electrons extracted from MAPbI{sub 3} to MoO{sub x}. Therefore, such an interface is not an ideal choice for hole extraction in organic photovoltaic devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Silicon vacancy-related centers in non-irradiated 6H-SiC nanostructure

We present the first findings of the silicon vacancy related centers identified in the non-irradiated 6H-SiC nanostructure using the electron spin resonance (ESR) and electrically-detected (ED) ESR technique. This planar 6H-SiC nanostructure represents the ultra-narrow p-type quantum well confined by the δ-barriers heavily doped with boron on the surface of the n-type 6H-SiC(0001) wafer. The new EDESR technique by measuring the only magnetoresistance of the 6H-SiC nanostructure under the high frequency generation from the δ-barriers appears to allow the identification of the isolated silicon vacancy centers as well as the triplet center with spin state S = 1. The same triplet center that is characterized by the large value of the zero-field splitting constant D and anisotropic g-factor is revealed by the ESR (X-band) method. The hyperfine (HF) lines in the ESR and EDESR spectra originating from the HF interaction with the {sup 14}N nucleus seem to attribute this triplet center to the N-V{sub Si} defect.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Effect of Intermediate Semiconducting TiOx Thin Films on Nanoparticle-Mediated Electron Transfer: Electrooxidation of CO

The concept of nanoparticle-mediated electron transfer (eT) across insulating thin films was elucidated theoretically by Allongue and Chazalviel in 2011. In their model, metal nanoparticles (NPs) are immobilized atop passivating, self-assembled monolayers (SAMs). They found that under certain conditions, related to the thickness of the SAM and the size of the NPs, efficient faradaic oxidation and reduction reactions could proceed at the NP surface. In the absence of NPs, however, eT was suppressed by the insulating SAM thin films. Allongue and Chazalviel concluded that, within certain bounds, eT is mediated by fast tunneling between the conductive electrode and the metal NPs, while the kinetics of the redox reaction are controlled by the NPs. This understanding has been confirmed using a variety of experimental models. The theory is based on electron tunneling; therefore, the nature of the intervening medium (the insulator in prior studies) should not affect the eT rate. In the present manuscript, however, we show that the theory breaks down under certain electrochemical conditions when the medium between conductors is an n-type semiconductor. Specifically, we find that in the presence of either Au or Pt NPs immobilized on a thin film of TiOx, CO electrooxidation does not proceed. In contrast, the exact same systems lead to the efficient reduction of oxygen. At present, we are unable to explain this finding within the context of the model of Allongue and Chazalviel.

Galyamova, Aigerim↗
DOE OSTI2022

From p- to n-Type Mixed Conduction in Isoindigo-Based Polymers through Molecular Design

Organic mixed ionic and electronic conductors are of significant interest for bioelectronic applications. Here, we use three different isoindigoid building blocks to obtain polymeric mixed conductors with vastly different structural and electronic properties which can be further fine-tuned through the choice of comonomer unit. We show how careful design of the isoindigoid scaffold can afford highly planar polymer structures with high degrees of electronic delocalization, while subtle structural modifications can control the dominant charge carrier (hole or electron) when probed in organic electrochemical transistors. We employ a combination of experimental and computational techniques to probe electrochemical, structural and mixed ionic and electronic properties of the polymer series which in turn allows us to derive important structure-property relations for this promising class of materials in the context of organic bioelectronics. Ultimately, we use these findings to outline robust molecular design strategies for isoindigo-based mixed conductors that can support efficient p-type, n-type and ambipolar transistor operation in an aqueous environment.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Synthetic Nuances to Maximize n-Type Organic Electrochemical Transistor and Thermoelectric Performance in Fused Lactam Polymers

A series of fully fused n-type mixed conduction lactam polymers p(g 7 NC n N), systematically increasing the alkyl side chain content, are synthesized via an inexpensive, nontoxic, precious-metal-free aldol polycondensation. Employing these polymers as channel materials in organic electrochemical transistors (OECTs) affords state-of-the-art n-type performance with p(g 7 NC 10 N) recording an OECT electron mobility of 1.20 x 10 -2 cm 2 V -1 s -1 and a μC* figure of merit of 1.83 F cm -1 V -1 s -1. In parallel to high OECT performance, upon solution doping with (4-(1,3-dimethyl-2,3-dihydro-1H-benzoimidazol-2-yl)phenyl)dimethylamine (N-DMBI), the highest thermoelectric performance is observed for p(g 7 NC 4 N), with a maximum electrical conductivity of 7.67 S cm -1 and a power factor of 10.4 μWm -1 K -2 . These results are among the highest reported for n-type polymers. Importantly, while this series of fused polylactam organic mixed ionic-electronic conductors (OMIECs) highlights that synthetic molecular design strategies to bolster OECT performance can be translated to also achieve high organic thermoelectric (OTE) performance, a nuanced synthetic approach must be used to optimize performance. Herein, we outline the performance metrics and provide new insights into the molecular design guidelines for the next generation of high-performance n-type materials for mixed conduction applications, presenting for the first time the results of a single polymer series within both OECT and OTE applications.

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

Side chain engineering in indacenodithiophene- co -benzothiadiazole and its impact on mixed ionic–electronic transport properties

Organic semiconductors are increasingly being decorated with hydrophilic solubilising chains to create materials that can function as mixed ionic–electronic conductors, which are promising candidates for interfacing biological systems with organic electronics. While numerous organic semiconductors, including p- and n-type materials, small molecules and polymers, have been successfully tailored to encompass mixed conduction properties, common to all these systems is that they have been semicrystalline materials. Here, we explore how side chain engineering in the nano-crystalline indacenodithiophene-co-benzothiadiazole (IDTBT) polymer can be used to instil ionic transport properties and how this in turn influences the electronic transport properties. This allows us to ultimately assess the mixed ionic–electronic transport properties of these new IDTBT polymers using the organic electrochemical transistor as the testing platform. Using a complementary experimental and computational approach, we find that polar IDTBT derivatives can be infiltrated by water and solvated ions, they can be electrochemically doped efficiently in aqueous electrolyte with fast doping kinetics, and upon aqueous swelling there is no deterioration of the close interchain contacts that are vital for efficient charge transport in the IDTBT system. Despite these promising attributes, mixed ionic–electronic charge transport properties are surprisingly poor in all the polar IDTBT derivatives. Albeit a “negative” result, this finding clearly contradicts established side chain engineering rules for mixed ionic–electronic conductors, which motivated our continued investigation of this system. We eventually find this anomalous behaviour to be caused by increasing energetic disorder in the polymers with increasing polar side chain content. We have investigated computationally how the polar side chain motifs contribute to this detrimental energetic inhomogeneity and ultimately use the learnings to propose new molecular design criteria for side chains that can facilitate ion transport without impeding electronic transport.

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

The effect of residual palladium on the performance of organic electrochemical transistors

Organic electrochemical transistors are a promising technology for bioelectronic devices, with applications in neuromorphic computing and healthcare. The active component enabling an organic electrochemical transistor is the organic mixed ionic-electronic conductor whose optimization is critical for realizing high-performing devices. In this study, the influence of purity and molecular weight is examined for a p-type polythiophene and an n-type naphthalene diimide-based polymer in improving the performance and safety of organic electrochemical transistors. Our preparative GPC purification reduced the Pd content in the polymers and improved their organic electrochemical transistor mobility by ~60% and 80% for the p- and n-type materials, respectively. These findings demonstrate the paramount importance of removing residual Pd, which was concluded to be more critical than optimization of a polymer’s molecular weight, to improve organic electrochemical transistor performance and that there is readily available improvement in performance and stability of many of the reported organic mixed ionic-electronic conductors.

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

N-type molecular doping of a semicrystalline conjugated polymer through cation exchange

Control of electrical doping is indispensable in any semiconductor device, and both efficient hole and electron doping are required for many devices. In organic semiconductors, however, electron doping has been essentially more problematic compared to hole doping because in general organic semiconductors have low electron affinities and require dopants with low ionization potentials that are often air-sensitive. Here, we adapt an efficient molecular doping method, so-called ion-exchange doping, to dope electrons in a polymeric semiconductor. We initially reduce the polymeric semiconductor using one electron transfer from molecular dopants, and then the ionized dopants in the resulting air-unstable films are replaced with secondary ions via cation exchange. Improved ambient stability and crystallinity of the doped polymeric semiconductors are achieved when a specific bulky molecular cation was chosen as the secondary ion, compared to conventional methods. The presented strategy can overcome the trade-off relationship between reducing capability and ambient stability in molecular dopants, and a wider selection of dopant ions will help to realize ambient-stable electron conductors.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Electrical, structural and thermomechanical properties of doped-LaCrO3 ceramics for high temperature electronics and sensing applications.

Many important electrical and sensor applications require stable conductors under working temperatures up to 1500oC various redox environments. Common high temperature conductors such as nitrides and carbides are not stable under oxidizing atmospheres, for this reason low redox behavior materials would be more attractive. In this work, further dopant studies of the LaCrO3 system were completed in order to control the electronic and ionic conductivity, as well as the relative chemical and microstructural stability. Neodymium and Niobium dopants were initially studied to control the p-type, and potentially n-type conductive mechanisms, respectively, but other dopants strategies were also investigated. The electrical conductivity and Seebeck coefficient were characterized up to 1500oC under varying oxygen partial pressures. The phase and microstructural evolution of each material was also investigated for these compositions by XRD and SEM. The materials showing the best electrical and thermomechanical performance were included within thick films sensors and were tested.

20 FOSSIL-FUELED POWER PLANTS↗