Browse
Submit Data
Databases
API
Help

Dataset Information

20 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Modulation of Charge Transport at Grain Boundaries in SrTiO₃: Toward a High Thermoelectric Power Factor at Room Temperature.

ABSTRACT: Modulation of the grain boundary properties in thermoelectric materials that have thermally activated electrical conductivity is crucial in order to achieve high performance at low temperatures. In this work, we show directly that the modulation of the potential barrier at the grain boundaries in perovskite SrTiO₃ changes the low-temperature dependency of the bulk material's electrical conductivity. By sintering samples in a reducing environment of increasing strength, we produced La_0.08Sr_0.9TiO₃ (LSTO) ceramics that gradually change their electrical conductivity behavior from thermally activated to single-crystal-like, with only minor variations in the Seebeck coefficient. Imaging of the surface potential by Kelvin probe force microscopy found lower potential barriers at the grain boundaries in the LSTO samples that had been processed in the more reducing environments. A theoretical model using the band offset at the grain boundary to represent the potential barrier agreed well with the measured grain boundary potential dependency of conductivity. The present work showed an order of magnitude enhancement in electrical conductivity (from 85 to 1287 S cm^-1) and power factor (from 143 to 1745 μW m^-1 K^-2) at 330 K by this modulation of charge transport at grain boundaries. This significant reduction in the impact of grain boundaries on charge transport in SrTiO₃ provides an opportunity to achieve the ultimate "phonon glass electron crystal" by appropriate experimental design and processing.

SUBMITTER: Cao J

PROVIDER: S-EPMC8023519 | biostudies-literature |

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Similar Datasets

Defect segregation facilitates oxygen transport at fluorite UO2 grain boundaries.

Project description:An important challenge for modelling transport in materials for energy applications is that in most applications they are polycrystalline, and hence it is critical to understand the properties in the presence of grain boundaries. Moreover, most grain boundaries are not pristine stoichiometric interfaces and hence dopants are likely to play a significant role. In this paper, we describe our recent work on using atomistic molecular dynamics simulations to model the effect of doped grain boundaries on oxygen transport of fluorite structured UO2. UO2, much like other fluorite grain boundaries, are found to be sinks for oxygen vacancy segregation relative to the grain interior, thus facilitating oxygen transport. Fission products further enhance diffusivity via strong interactions between the impurities and oxygen defects. Doping produces a striking structural alteration in the Σ5 class of grain boundaries that enhances oxygen diffusivity even further. This article is part of a discussion meeting issue 'Energy materials for a low carbon future'.

| S-EPMC6635626 | biostudies-literature

Energy barriers at grain boundaries dominate charge carrier transport in an electron-conductive organic semiconductor.

Project description:Semiconducting organic films that are at the heart of light-emitting diodes, solar cells and transistors frequently contain a large number of morphological defects, most prominently at the interconnects between crystalline regions. These grain boundaries can dominate the overall (opto-)electronic properties of the entire device and their exact morphological and energetic nature is still under current debate. Here, we explore in detail the energetics at the grain boundaries of a novel electron conductive perylene diimide thin film. Via a combination of temperature dependent charge transport measurements and ab-initio simulations at atomistic resolution, we identify that energetic barriers at grain boundaries dominate charge transport in our system. This novel aspect of physics at the grain boundary is distinct from previously identified grain-boundary defects that had been explained by trapping of charges. We furthermore derive molecular design criteria to suppress such energetic barriers at grain boundaries in future, more efficient organic semiconductors.

| S-EPMC6173704 | biostudies-literature

Thermoelectric fabrics: toward power generating clothing.

Project description:Herein, we demonstrate that a flexible, air-permeable, thermoelectric (TE) power generator can be prepared by applying a TE polymer (e.g. poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate)) coated commercial fabric and subsequently by linking the coated strips with a conductive connection (e.g. using fine metal wires). The poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate) coated fabric shows very stable TE properties from 300 K to 390 K. The fabric device can generate a TE voltage output (V) of 4.3 mV at a temperature difference (ΔT) of 75.2 K. The potential for using fabric TE devices to harvest body temperature energy has been discussed. Fabric-based TE devices may be useful for the development of new power generating clothing and self-powered wearable electronics.

| S-EPMC4372730 | biostudies-literature

Enhanced thermoelectric properties of lightly Nb doped SrTiO3 thin films.

Project description:Novel thermoelectric materials developed for operation at room temperature must have similar or better performance along with being as ecofriendly as those commercially used, e.g., Bi2Te3, in terms of their toxicity and cost. In this work, we present an in-depth study of the thermoelectric properties of epitaxial Nb-doped strontium titanate (SrTi1-x Nb x O3) thin films as a function of (i) doping concentration, (ii) film thickness and (iii) substrate type. The excellent crystal quality was confirmed by high resolution transmission electron microscopy and X-ray diffraction analysis. The thermoelectric properties were measured by the three-omega method (thermal conductivity) and van der Pauw method (electrical resistivity), complemented by Seebeck coefficient measurements. A maximum power factor of 8.9 × 10-3 W m-1 K-2 and a thermoelectric figure of merit of 0.49 were measured at room temperature in 50 nm-thick films grown on lanthanum strontium aluminate. The mechanisms behind this high figure of merit are discussed in terms of a possible two-dimensional electron gas, increase of the effective mass of the electrons, electron filtering and change in strain due to different substrates. The overall enhancement of the thermoelectric properties suggests that SrTi1-x Nb x O3 is a very promising n-type candidate for room- to high-temperature applications.

| S-EPMC9419777 | biostudies-literature

Strain-induced room-temperature ferroelectricity in SrTiO3 membranes.

Project description:Advances in complex oxide heteroepitaxy have highlighted the enormous potential of utilizing strain engineering via lattice mismatch to control ferroelectricity in thin-film heterostructures. This approach, however, lacks the ability to produce large and continuously variable strain states, thus limiting the potential for designing and tuning the desired properties of ferroelectric films. Here, we observe and explore dynamic strain-induced ferroelectricity in SrTiO3 by laminating freestanding oxide films onto a stretchable polymer substrate. Using a combination of scanning probe microscopy, optical second harmonic generation measurements, and atomistic modeling, we demonstrate robust room-temperature ferroelectricity in SrTiO3 with 2.0% uniaxial tensile strain, corroborated by the notable features of 180° ferroelectric domains and an extrapolated transition temperature of 400?K. Our work reveals the enormous potential of employing oxide membranes to create and enhance ferroelectricity in environmentally benign lead-free oxides, which hold great promise for applications ranging from non-volatile memories and microwave electronics.

| S-EPMC7305178 | biostudies-literature

Thermoelectric response from grain boundaries and lattice distortions in crystalline gold devices.

Project description:The electronic Seebeck response in a conductor involves the energy-dependent mean free path of the charge carriers and is affected by crystal structure, scattering from boundaries and defects, and strain. Previous photothermoelectric (PTE) studies have suggested that the thermoelectric properties of polycrystalline metal nanowires are related to grain structure, although direct evidence linking crystal microstructure to the PTE response is difficult to elucidate. Here, we show that room temperature scanning PTE measurements are sensitive probes that can detect subtle changes in the local Seebeck coefficient of gold tied to the underlying defects and strain that mediate crystal deformation. This connection is revealed through a combination of scanning PTE and electron microscopy measurements of single-crystal and bicrystal gold microscale devices. Unexpectedly, the photovoltage maps strongly correlate with gradually varying crystallographic misorientations detected by electron backscatter diffraction. The effects of individual grain boundaries and differing grain orientations on the PTE signal are minimal. This scanning PTE technique shows promise for identifying minor structural distortions in nanoscale materials and devices.

| S-EPMC7519306 | biostudies-literature

In-situ four-tip STM investigation of the transition from 2D to 3D charge transport in SrTiO3.

Project description:The electrical properties of SrTiO3(100) single crystals were investigated in-situ at different stages of thermal reduction by means of a 4-tip STM. Using the tips of the STM as electrical probes, distance-dependent four-point measurements were performed at the surface of the crystal at room temperature after reduction by thermal treatment. For annealing temperatures T ≤ 700 °C, charge transport is confined to a surface region <3 μm below the surface. For reduction at T ≥ 900 °C a transition from a conducting 2D sheet with insulating bulk to a system with dominant 3D bulk conductivity is found. At an intermediate reduction temperature of T = 800 °C, a regime with mixed 2D/3D contributions is observed in the distance-dependent resistance measurements. Describing the depth-dependent conductivity with an analytical N-layer model, this regime of mixed 2D/3D conductivity is evaluated quantitatively under the assumption of an exponentially decaying conductivity profile, correlated with the previously observed depth-dependent dislocation density in the sample. A non-monotonous temperature dependence of the 3D conductivity in the respective conducting layer is found and possible underlying mechanisms are discussed, particularly with regard to non-intrinsic material properties depending on details of the sample preparation.

| S-EPMC6384903 | biostudies-literature

Unraveling the Impact of Graphene Addition to Thermoelectric SrTiO3 and La-Doped SrTiO3 Materials: A Density Functional Theory Study.

Project description:We present a detailed theoretical investigation of the interaction of graphene with the SrO-terminated (001) surface of pristine and La-doped SrTiO3. The adsorption of graphene is thermodynamically favorable with interfacial adsorption energies of -0.08 and -0.32 J/m2 to pristine SrTiO3 and La-doped SrTiO3 surfaces, respectively. We find that graphene introduces C 2p states at the Fermi level, rendering the composite semimetallic, and thus the electrical properties are predicted to be highly sensitive to the amount and quality of the graphene. An investigation of the lattice dynamics predicts that graphene adsorption may lead to a 60-90% reduction in the thermal conductivity due to a reduction in the phonon group velocities, accounting for the reduced thermal conductivity of the composite materials observed experimentally. This effect is enhanced by La doping. We also find evidence that both La dopant ions and adsorbed graphene introduce low-frequency modes that may scatter heat-carrying acoustic phonons, and that, if present, these effects likely arise from stronger phonon-phonon interactions.

| S-EPMC8414480 | biostudies-literature

Phononic Thermal Transport along Graphene Grain Boundaries: A Hidden Vulnerability.

Project description:While graphene grain boundaries (GBs) are well characterized experimentally, their influence on transport properties is less understood. As revealed here, phononic thermal transport is vulnerable to GBs even when they are ultra-narrow and aligned along the temperature gradient direction. Non-equilibrium molecular dynamics simulations uncover large reductions in the phononic thermal conductivity (κp ) along linear GBs comprising periodically repeating pentagon-heptagon dislocations. Green's function calculations and spectral energy density analysis indicate that the origin of the κp reduction is hidden in the periodic GB strain field, which behaves as a reflective diffraction grating with either diffuse or specular phonon reflections, and represents a source of anharmonic phonon-phonon scattering. The non-monotonic dependence with dislocation density of κp uncovered here is unaccounted for by the classical Klemens theory. It can help identify GB structures that can best preserve the integrity of the phononic transport.

| S-EPMC8456227 | biostudies-literature

Microscale Liquid Transport in Polycrystalline Inverse Opals across Grain Boundaries.

Project description:Delivering liquid through the void spaces in porous metals is a daunting challenge for a variety of emerging interface technologies ranging from battery electrodes to evaporation surfaces. Hydraulic transport characteristics of well-ordered porous media are governed by the pore distribution, porosity, and morphology. Much like energy transport in polycrystalline solids, hydraulic transport in semi-ordered porous media is predominantly limited by defects and grain boundaries. Here, we report the wicking performances for porous copper inverse opals having pore diameters from 300 to 1000 nm by measuring the capillary-driven liquid rise. The capillary performance parameter within single crystal domain (K ij /R eff = 10-3 to 10-2 µm) is an order of magnitude greater than the collective polycrystal (K eff /R eff = ~10-5 to 10-3 µm) due to the hydraulic resistances (i.e. grain boundaries between individual grains). Inspired by the heterogeneity found in biological systems, we report that the capillary performance parameter of gradient porous copper (K eff /R eff = ~10-3 µm), comparable to that of single crystals, overcomes hydraulic resistances through providing additional hydraulic routes in three dimensions. The understanding of microscopic liquid transport physics through porous crystals and across grain boundaries will help to pave the way for the spatial design of next-generation heterogeneous porous media.

| S-EPMC5585244 | biostudies-literature