skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


  • NSF Public Access
  • Search Results
  • Graphene/Strontium Titanate: Approaching Single Crystal–Like Charge Transport in Polycrystalline Oxide Perovskite Nanocomposites through Grain Boundary Engineering
Title: Graphene/Strontium Titanate: Approaching Single Crystal–Like Charge Transport in Polycrystalline Oxide Perovskite Nanocomposites through Grain Boundary Engineering
Abstract Grain boundaries critically limit the electronic performance of oxide perovskites. These interfaces lower the carrier mobilities of polycrystalline materials by several orders of magnitude compared to single crystals. Despite extensive effort, improving the mobility of polycrystalline materials (to meet the performance of single crystals) is still a severe challenge. In this work, the grain boundary effect is eliminated in perovskite strontium titanate (STO) by incorporating graphene into the polycrystalline microstructure. An effective mass model provides strong evidence that polycrystalline graphene/strontium titanate (G/STO) nanocomposites approach single crystal‐like charge transport. This phenomenological model reduces the complexity of analyzing charge transport properties so that a quantitative comparison can be made between the nanocomposites and STO single crystals. In other related works, graphene composites also optimize the thermal transport properties of thermoelectric materials. Therefore, decorating grain boundaries with graphene appears to be a robust strategy to achieve “phonon glass–electron crystal” behavior in oxide perovskites.  more » « less
Award ID(s):
1729487
PAR ID:
10457954
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Functional Materials
Volume:
30
Issue:
12
ISSN:
1616-301X
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; ; ; ; ; ; ; ; (, Science Advances)
    null (Ed.)
    In recent years, lanthanum aluminate/strontium titanate (LAO/STO) heterointerfaces have been used to create a growing family of nanoelectronic devices based on nanoscale control of LAO/STO metal-to-insulator transition. The properties of these devices are wide-ranging, but they are restricted by nature of the underlying thick STO substrate. Here, single-crystal freestanding membranes based on LAO/STO heterostructures were fabricated, which can be directly integrated with other materials via van der Waals stacking. The key properties of LAO/STO are preserved when LAO/STO membranes are formed. Conductive atomic force microscope lithography is shown to successfully create reversible patterns of nanoscale conducting regions, which survive to millikelvin temperatures. The ability to form reconfigurable conducting nanostructures on LAO/STO membranes opens opportunities to integrate a variety of nanoelectronics with silicon-based architectures and flexible, magnetic, or superconducting materials. 
    more » « less
  2. ; ; ; ; (, Modelling and Simulation in Materials Science and Engineering)
    Abstract Grain boundaries can greatly affect the transport properties of polycrystalline materials, particularly when the grain size approaches the nanoscale. While grain boundaries often enhance diffusion by providing a fast pathway for chemical transport, some material systems, such as those of solid oxide fuel cells and battery cathode particles, exhibit the opposite behavior, where grain boundaries act to hinder diffusion. To facilitate the study of systems with hindered grain boundary diffusion, we propose a model that utilizes the smoothed boundary method to simulate the dynamic concentration evolution in polycrystalline systems. The model employs domain parameters with diffuse interfaces to describe the grains, thereby enabling solutions with explicit consideration of their complex geometries. The intrinsic error arising from the diffuse interface approach employed in our proposed model is explored by comparing the results against a sharp interface model for a variety of parameter sets. Finally, two case studies are considered to demonstrate potential applications of the model. First, a nanocrystalline yttria-stabilized zirconia solid oxide fuel cell system is investigated, and the effective diffusivities are extracted from the simulation results and are compared to the values obtained through mean-field approximations. Second, the concentration evolution during lithiation of a polycrystalline battery cathode particle is simulated to demonstrate the method’s capability. 
    more » « less
  3. ; ; ; ; ; ; ; ; ; ; et al (, Advanced Functional Materials)
    Abstract Highly crystalline thin films in organic semiconductors are important for applications in high‐performance organic optoelectronics. Here, the effect of grain boundaries on the Hall effect and charge transport properties of organic transistors based on two exemplary benchmark systems is elucidated: (1) solution‐processed blends of 2,7‐dioctyl[1]benzothieno[3,2‐b][1]benzothiophene (C8‐BTBT) small molecule and indacenodithiophene‐benzothiadiazole (C16IDT‐BT) conjugated polymer, and (2) large‐area vacuum evaporated polycrystalline thin films of rubrene (C42H28). It is discovered that, despite the high field‐effect mobilities of up to 6 cm2V−1s−1and the evidence of a delocalized band‐like charge transport, the Hall effect in polycrystalline organic transistors is systematically and significantly underdeveloped, with the carrier coherence factor α < 1 (i.e., yields an underestimated Hall mobility and an overestimated carrier density). A model based on capacitively charged grain boundaries explaining this unusual behavior is described. This work significantly advances the understanding of magneto‐transport properties of organic semiconductor thin films. 
    more » « less
  4. ; ; ; ; ; ; ; ; (, Journal of Vacuum Science & Technology A)
    Perovskite materials, of which strontium titanate (STO) and its thin films are an example, have attracted significant scientific interest because of their desirable properties and the potential to tune thermal conductivity by employing several techniques. Notably, strontium titanate thin films on silicon (Si) substrates serve as a fundamental platform for integrating various oxides onto Si substrates, making it crucial to understand the thermal properties of STO on Si. This work investigates the thermal conductivity of STO thin films on an Si substrate for varying film thicknesses (12, 50, 80, and 200 nm) at room temperature (∼300 K). The thin films are deposited using molecular beam epitaxy on the Si substrate and their thermal conductivity is characterized using the frequency domain thermoreflectance (FDTR) method. The measured values range from 7.4 ± 0.74 for the 200 nm thick film to 0.8 ± 0.1 W m−1 K−1 for the 12 nm thick film, showing a large effect of the film thickness on the thermal conductivity values. The trend of the values is diminishing with the corresponding decrease in the thin film thickness, with a reduction of 38%–93% in the thermal conductivity values, for film thicknesses ranging from 200 to 12 nm. This reduction in the values is relative to the bulk single crystal values of STO, which may range from 11 to 13.5 W m−1 K−1 [Yu et al., Appl. Phys. Lett. 92, 191911 (2008) and Fumega et al., Phys. Rev. Mater. 4, 033606 (2020)], as measured by our FDTR-based experiment. The study also explores the evaluation of volumetric heat capacity (Cp). The measured volumetric heat capacity for the 200 nm thin film is 3.07 MJ m−3 K−1, which is in reasonable agreement with the values available in the literature. 
    more » « less
  5. ; ; ; ; ; ; ; ; ; ; et al (, Nature Communications)
    Abstract Architecting grain crystallographic orientation can modulate charge distribution and chemomechanical properties for enhancing the performance of polycrystalline battery materials. However, probing the interplay between charge distribution, grain crystallographic orientation, and performance remains a daunting challenge. Herein, we elucidate the spatially resolved charge distribution in lithium layered oxides with different grain crystallographic arrangements and establish a model to quantify their charge distributions. While the holistic “surface-to-bulk” charge distribution prevails in polycrystalline particles, the crystallographic orientation-guided redox reaction governs the charge distribution in the local charged nanodomains. Compared to the randomly oriented grains, the radially aligned grains exhibit a lower cell polarization and higher capacity retention upon battery cycling. The radially aligned grains create less tortuous lithium ion pathways, thus improving the charge homogeneity as statistically quantified from over 20 million nanodomains in polycrystalline particles. This study provides an improved understanding of the charge distribution and chemomechanical properties of polycrystalline battery materials. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Save / Share this Record
  • Send to Email