skip to main content


Title: Full Control of Polarization in Ferroelectric Thin Films Using Growth Temperature to Modulate Defects
Abstract

Deterministic control of the intrinsic polarization state of ferroelectric thin films is essential for device applications. Independently of the well‐established role of electrostatic boundary conditions and epitaxial strain, the importance of growth temperature as a tool to stabilize a target polarization state during thin film growth is shown here. Full control of the intrinsic polarization orientation of PbTiO3thin films is demonstrated—from monodomain up, through polydomain, to monodomain down as imaged by piezoresponse force microscopy—using changes in the film growth temperature. X‐ray diffraction and scanning transmission electron microscopy reveal a variation ofc‐axis related to out‐of‐plane strain gradients. These measurements, supported by Ginzburg–Landau–Devonshire free energy calculations and Rutherford backscattering spectroscopy, point to a defect mediated polarization gradient initiated by a temperature dependent effective built‐in field during growth, allowing polarization control not only under specific growth conditions, but ex‐situ, for subsequent processing and device applications.

 
more » « less
Award ID(s):
1708615
NSF-PAR ID:
10454256
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Electronic Materials
Volume:
6
Issue:
12
ISSN:
2199-160X
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    BaTiO3is a technologically relevant material in the perovskite oxide class with above‐room‐temperature ferroelectricity and a very large electro‐optical coefficient, making it highly suitable for emerging electronic and photonic devices. An easy, robust, straightforward, and scalable growth method is required to synthesize epitaxial BaTiO3thin films with sufficient control over the film's stoichiometry to achieve reproducible thin film properties. Here the growth of BaTiO3thin films by hybrid molecular beam epitaxy is reported. A self‐regulated growth window is identified using complementary information obtained from reflection high energy electron diffraction, the intrinsic film lattice parameter, film surface morphology, and scanning transmission electron microscopy. Subsequent optical characterization of the BaTiO3films by spectroscopic ellipsometry revealed refractive index and extinction coefficient values closely resembling those of stoichiometric bulk BaTiO3crystals for films grown inside the growth window. Even in the absence of a lattice parameter change of BaTiO3thin films, degradation of optical properties is observed, accompanied by the appearance of a wide optical absorption peak in the IR spectrum, attributed to optical transitions involving defect states present. Therefore, the optical properties of BaTiO3can be utilized as a much finer and more straightforward probe to determine the stoichiometry level present in BaTiO3films.

     
    more » « less
  2. Abstract

    While induced spin polarization of a palladium (Pd) overlayer on antiferromagnetic and magneto-electric Cr2O3(0001) is possible because of the boundary polarization at the Cr2O3(0001), in the single domain state, the Pd thin film appears to be ferromagnetic on its own, likely as a result of strain. In the conduction band, we find the experimental evidence of ferromagnetic spin polarized in Pd thin films on a Cr2O3(0001) single crystal, especially in the thin limit, Pd thickness of around 1–4 nm. Indeed there is significant spin polarization in 10 Å thick Pd films on Cr2O3(0001) at 310 K, i.e. above the Néel temperature of bulk Cr2O3. While Cr2O3(0001) has surface moments that tend to align along the surface normal, for Pd on Cr2O3, the spin polarization contains an in-plane component. Strain in the Pd adlayer on Cr2O3(0001) appears correlated to the spin polarization measured in spin polarized inverse photoemission spectroscopy. Further evidence for magnetization of Pd on Cr2O3is provided by measurement of the exchange bias fields in Cr2O3/Pd(buffer)/[Co/Pd]nexchange bias systems. The magnitude of the exchange bias field is, over a wide temperature range, virtually unaffected by the Pd thickness variation between 1 and 2 nm.

     
    more » « less
  3. Bi2NiMnO6(BNMO) epitaxial thin films with a layered supercell (LSC) structure have emerged as a promising single‐phase multiferroic material recently. Because of the required strain state for the formation of the LSC structures, most of the previous BNMO films are demonstrated on rigid oxide substrates such as SrTiO3and LaAlO3. Here, the potential of BNMO films grown on muscovite mica substrates via van der Waals epitaxy, spotlighting their suitability for cutting‐edge flexible device applications is delved. Comprehensive scanning transmission electron microscopy/energy‐dispersive X‐ray analyses reveal a layered structure in the BNMO film and a pristine interface with the mica substrate, indicating high‐quality deposition and minimal interfacial defects. Capitalizing on its unique property of easily cleavable layers due to weak van der Waals forces in mica substrates, flexible BNMO/mica samples are fixed. A standout feature of the BNMO film grown on mica substrate is its consistent multiferroic properties across varied mechanical conditions. A novel technique is introduced for thinning the mica substrate and subsequent transfer of the sample, with post‐transfer analyses validating the preserved structural and magnetic attributes of the film. Overall, this study illuminates the resilient multiferroic properties of BNMO films on mica, offering promising avenues for their integration for next‐generation flexible electronics.

     
    more » « less
  4. Abstract

    The ability to actively regulate heat flow at the nanoscale could be a game changer for applications in thermal management and energy harvesting. Such a breakthrough could also enable the control of heat flow using thermal circuits, in a manner analogous to electronic circuits. Here we demonstrate switchable thermal transistors with an order of magnitude thermal on/off ratio, based on reversible electrochemical lithium intercalation in MoS2thin films. We use spatially-resolved time-domain thermoreflectance to map the lithium ion distribution during device operation, and atomic force microscopy to show that the lithiated state correlates with increased thickness and surface roughness. First principles calculations reveal that the thermal conductance modulation is due to phonon scattering by lithium rattler modes,c-axis strain, and stacking disorder. This study lays the foundation for electrochemically-driven nanoscale thermal regulators, and establishes thermal metrology as a useful probe of spatio-temporal intercalant dynamics in nanomaterials.

     
    more » « less
  5.  
    more » « less