Observation of large Rashba spin–orbit coupling at room temperature in compositionally engineered perovskite single crystals and application in high performance photodetectors

This is the author accepted manuscript. The final version is available from Elsevier via the DOI in this recordIndirect absorption extended below the direct transition edge and increase in carrier lifetime derived from Rashba spin-orbit coupling may advance the optoelectronic applications of metal halide perovskites. Spin-orbit coupling in halide perovskites is due to the presence of heavy elements in their structure. However, when these materials lack an inversion symmetry, for example by the application of strain, spin-orbit coupling becomes odd in the electron’s momentum giving rise to a splitting in the electronic energy bands. Here we report on the observation of a large Rashba splitting of 117 meV at room temperature through a facile compositional engineering approach in halide perovskite single crystals, as predicted by relativistic first-principles calculations. Partial substitution of organic cations by rubidium ions in single crystals induces significant indirect absorption and dual emission as a result of a large Rashba splitting. We measured significant magneto-photocurrent, magneto-electroluminescence and magneto-photoluminescence responses in perovskite single crystal devices and thin films. They originate from the significant spin-momentum locking that leads to different precession frequencies of their respective spins about the applied magnetic field. A hybrid perovskite single crystal photodetector achieved record figures of merit, including detectivity of more than 1.3×1018 Jones which represents a three orders of magnitude improvement compared to the to date record. These findings show that facile compositional engineering of perovskite single crystals holds great promise for further advancing the optoelectronic properties of existing materials.European Regional Development Fund (ERDF)European Union Horizon 2020Ministero dell’Istruzione dell’Universitàe della Ricerca (MIUR)Università degli Studi di PerugiaCNPq, Brazi

Tunable Microwave Conductance of Nanodomains in Ferroelectric PbZr0.2Ti0.8O3 Thin Film

Ferroelectric materials exhibit spontaneous polarization that can be switched by electric field. Beyond traditional applications as nonvolatile capacitive elements, the interplay between polarization and electronic transport in ferroelectric thin films has enabled a path to neuromorphic device applications involving resistive switching. A fundamental challenge, however, is that finite electronic conductivity may introduce considerable power dissipation and perhaps destabilize ferroelectricity itself. Here, tunable microwave frequency electronic response of domain walls injected into ferroelectric lead zirconate titanate (PbZr0.2Ti0.8O3) on the level of a single nanodomain is revealed. Tunable microwave response is detected through first-order reversal curve spectroscopy combined with scanning microwave impedance microscopy measurements taken near 3 GHz. Contributions of film interfaces to the measured AC conduction through subtractive milling, where the film exhibited improved conduction properties after removal of surface layers, are investigated. Using statistical analysis and finite element modeling, we inferred that the mechanism of tunable microwave conductance is the variable area of the domain wall in the switching volume. These observations open the possibilities for ferroelectric memristors or volatile resistive switches, localized to several tens of nanometers and operating according to well-defined dynamics under an applied field

Automated Interpretation and Extraction of Topographic Information from Time of Flight Secondary Ion Mass Spectrometry Data

Abstract Time of flight secondary ion mass spectrometry (ToF-SIMS) is a powerful surface-sensitive characterization tool allowing the imaging of chemical properties over a wide range of organic and inorganic material systems. This technique allows precise studies of chemical composition with sub-100-nm lateral and nanometer depth spatial resolution. However, comprehensive interpretation of ToF-SIMS results is challenging because of the very large data volume and high dimensionality. Furthermore, investigation of samples with pronounced topographical features is complicated by systematic and measureable shifts in the mass spectrum. In this work we developed an approach for the interpretation of the ToF-SIMS data, based on the advanced data analytics. Along with characterization of the chemical composition, our approach allows extraction of the sample surface morphology from a time of flight registration technique. This approach allows one to perform correlated investigations of surface morphology, biological function, and chemical composition of Arabidopsis roots