No Arabic abstract
Polar metals are an intriguing class of materials that simultaneously host free carriers and polar structural distortions. Despite the name polar metal, however, most well-studied polar metals are poor electrical conductors. Here, we demonstrate the molecular beam epitaxial (MBE) growth of LaPtSb and LaAuGe, two polar metal compounds whose electrical resistivity is an order of magnitude lower than the well studied oxide polar metals. These materials belong to a broad family of $ABC$ intermetallics adopting the stuffed wurtzite structure, also known as hexagonal Heusler compounds. Scanning transmission electron microscopy (STEM) reveals a polar structure with unidirectionally buckled $BC$ (PtSb, AuGe) planes. Magnetotransport measurements demonstrate good metallic behavior with low residual resistivity ($rho_{LaAuGe}=59.05$ $muOmegacdot$cm and $rho_{LaAPtSb}=27.81$ $muOmegacdot$cm at 2K) and high carrier density ($n_hsim 10^{21}$ cm$^{-3}$). Photoemission spectroscopy measurements confirm the band metallicity and are in quantitative agreement with density functional theory (DFT) calculations. Through DFT-Chemical Pressure and Crystal Orbital Hamilton Population analyses, the atomic packing factor is found to support the polar buckling of the structure, though the degree of direct interlayer $B-C$ bonding is limited by repulsion at the $A-C$ contacts. When combined with insulating hexagonal Heuslers, these materials provide a new platform for fully epitaxial, multiferroic heterostructures.
We have fabricated Pt-containing granular metals by focused electron beam induced deposition from the $(CH_3)_3CH_3C_5H_4Pt$ precursor gas. The granular metals are made of platinum nanocrystallites embedded in a carbonaceous matrix. We have exposed the as-grown nanocomposites to low energy electron beam irradiation and we have measured the electrical conductivity as a function of the irradiation dose. Postgrowth electron beam irradiation transforms the matrix microstructure and thus the strength of the tunneling coupling between Pt nanocrystallites. For as-grown samples (weak tunnel coupling regime) we find that the temperature dependence of the electrical conductivity follows the stretched exponential behavior characteristic of the correlated variable-range hopping transport regime. For briefly irradiated samples (strong tunnel coupling regime) the electrical conductivity is tuned across the metal-insulator transition. For long-time irradiated samples the electrical conductivity behaves like that of a metal. In order to further analyze changes of the microstructure as a function of the electron irradiation dose we have carried out transmission electron microscope (TEM), micro-Raman and atomic force microscopy (AFM) investigations. TEM pictures reveal that the crystallites size of long-time irradiated samples is larger than that of as-grown samples. Furthermore we do not have evidence of microstructural changes in briefly irradiated samples. By means of micro-Raman we find that by increasing the irradiation dose the matrix changes following a graphitization trajectory between amorphous carbon and nanocrystalline graphite. Finally, by means of AFM measurements we observe a reduction of the volume of the samples with increasing irradiation time which we attribute to the removal of carbon molecules.
Precise control of lattice mismatch accommodation and cation interdiffusion across the interface is critical to modulate correlated functionalities in epitaxial heterostructures, particularly when the interface composition is positioned near a compositional phase transition boundary. Here we select La1-xSrxMnO3 (LSMO) as a prototypical phase transition material and establish vertical epitaxial interfaces with NiO to explore the strong interplay between strain accommodation, stoichiometry modification, and localized electron transport across the interface. It is found that localized stoichiometry modification overcomes the plaguing dead layer problem in LSMO and leads to strongly directional conductivity, as manifested by more than three orders of magnitude difference between out-of-plane to in-plane conductivity. Comprehensive structural characterization and transport measurements reveal that this emerging behavior is related to a compositional change produced by directional cation diffusion that pushes the LSMO phase transition from insulating into metallic within an ultrathin interface region. This study explores the nature of unusual electric conductivity at vertical epitaxial interfaces and establishes an effective route for engineering nanoscale electron transport for oxide electronics.
The use of oxide glasses is pervasive throughout everyday amenities and commodities. Such glasses are typically electrical insulators, and endowing them with electrical conductivity without changing their salutary mechanical properties, weight, or thermoformability enables new applications in multifunctional utensils, smart windows, and automotive parts. Previous strategies to impart electrical conductivity include modifying the glass composition or forming a solid-in-solid composite of the glass and a conductive phase. Here we demonstrate using the latter strategy the highest reported room-temperature electrical conductivity in a bulk oxide glass 1800 S/m corresponding to the theoretical limit for the loading fraction of the conductive phase. This is achieved through glass-sintering of a mixture of carbon nanofibers and oxide flint F2 or soda lime glasses, with the bulk conductivity further enhanced by a polyethylene-block-poly(ethylene glycol) additive. A theoretical model provides predictions that are in excellent agreement with the dependence of conductivity of these composites on the carbon-loading fraction. Moreover, nanoscale electrical characterization of the composite samples provides evidence for the existence of a connected network of carbon nanofibers throughout the bulk. Our results establish a potentially low-cost approach for producing large volumes of highly conductive glass independently of the glass composition.
The possibility of reconciliation between seemingly mutually exclusive properties in one system can not only lead to theoretical breakthroughs but also potential novel applications. The research on the coexistence of two purportedly contra-indicated properties, ferroelectricity/polarity and conductivity, proposed by Anderson and Blount over 50 years ago was recently revitalized by the discovery of the first unambiguous polar metal LiOsO3 and further fueled by the demonstration of the first switchable ferroelectric metal WTe2. In this review, we first discuss the reasons why the coexistence of ferroelectricity/polarity and conductivity have been deemed incompatible, followed by a review on the history of ferroelectric/polar metals. Secondly, we review the important milestones along with the corresponding mechanisms for the ferroelectric/polar metallic phases in these materials. Thirdly, we summarize the design approaches for ferroelectric/polar metals. Finally, we discuss the future prospects and potential applications of ferroelectric/polar metals.
The electronic and transport properties of the half-Heusler compound LaPtSb are investigated by performing first-principles calculations combined with semi-classical Boltzmann theory and deformation potential theory. Compared with many typical half-Heusler compounds, the LaPtSb exhibits obviously larger power factor at room temperature, especially for the n-type system. Together with the very low lattice thermal conductivity, the thermoelectric figure of merit (ZT) of LaPtSb can be optimized to a record high value of 2.2 by fine tuning the carrier concentration.