The two-dimensional (2D) Ruddlesden−Popper organic-inorganic halide perovskites such as (2D)-phenethylammonium lead iodide (2D-PEPI) have layered structure that resembles multiple quantum wells (MQW). The heavy atoms in 2D-PEPI contribute a large spin-orbit coupling that influences the electronic band structure. Upon breaking the inversion symmetry, a spin splitting ('Rashba splitting') occurs in the electronic bands. We have studied the spin splitting in 2D-PEPI single crystals using the circular photogalvanic effect (CPGE). We confirm the existence of Rashba splitting at the electronic band extrema of 35±10 meV, and identify the main inversion symmetry breaking direction perpendicular to the MQW planes. The CPGE action spectrum above the bandgap reveals spin-polarized photocurrent generated by ultrafast relaxation of excited photocarriers separated in momentum space. Whereas the helicity dependent photocurrent with below-gap excitation is due to spin-galvanic effect of the ionized spin-polarized excitons, where spin polarization occurs in the spin-split bands due to asymmetric spin-flip.
We demonstrate new capabilities for frequency-agile terahertz devices using perovskites.
Boiling, a dynamic and multiscale process, has been studied for several decades; however, a comprehensive understanding of the process is still lacking. The bubble ebullition cycle, which occurs over millisecond time-span, makes it extremely challenging to study near-surface interfacial characteristics of a single bubble. Here, we create a steady-state vapor bubble that can remain stable for hours in a pool of sub-cooled water using a femtosecond laser source. The stability of the bubble allows us to measure the contact-angle and perform in-situ imaging of the contact-line region and the microlayer, on hydrophilic and hydrophobic surfaces and in both degassed and regular (with dissolved air) water. The early growth stage of vapor bubble in degassed water shows a completely wetted bubble base with the microlayer, and the bubble does not depart from the surface due to reduced liquid pressure in the microlayer. Using experimental data and numerical simulations, we obtain permissible range of maximum heat transfer coefficient possible in nucleate boiling and the width of the evaporating layer in the contact-line region. This technique of creating and measuring fundamental characteristics of a stable vapor bubble will facilitate rational design of nanostructures for boiling enhancement and advance thermal management in electronics.
Three-dimensional (3D) semimetals have been predicted and demonstrated to have a wide variety of interesting properties associated with its linear energy dispersion. In analogy to twodimensional (2D) Dirac semimetals, such as graphene, Cd3As2, a 3D semimetal, has shown ultrahigh mobility, large Fermi velocity, and has been hypothesized to support plasmons at terahertz frequencies. In this work, we demonstrate synthesis of high-quality large-area Cd3As2 thin-films through thermal evaporation as well as the experimental realization of plasmonic structures consisting of periodic arrays of Cd3As2 stripes. These arrays exhibit sharp resonances at terahertz frequencies with associated quality-factors (Q) as high as ~ 3.7. Such spectrally-narrow resonances can be understood on the basis of a large kinetic-inductance, resulting from a long momentum scattering time, which in our films can approach ~1 ps at room-temperature.Moreover, we demonstrate an ultrafast tunable response through excitation of photo-induced 2 carriers in optical pump / terahertz probe experiments. Our results evidence that the intrinsic 3D nature of Cd3As2 provides for a very robust platform for terahertz plasmonic applications. Overall, our observations pave a way for the development of myriad terahertz (opto) electronic devices based on Cd3As2 and other 3D Dirac semimetals, benefiting from strong coupling of terahertz radiation, ultrafast transient response, magneto-plasmon properties, etc. Moreover, the long momentum scattering time, thus large kinetic inductance in Cd3As2, also holds enormous potential for the re-design of passive elements such as inductors and hence can have a profound impact in the field of RF integrated circuits.
Utilizing the spin degree of freedom of photoexcitations in hybrid organic inorganic perovskites for quantum information science applications has been recently proposed and explored. However, it is still unclear whether the stable photoexcitations in these compounds correspond to excitons, free/trapped electron-hole pairs, or charged exciton complexes such as trions. Here we investigate quantum beating oscillations in the picosecond time-resolved circularly polarized photoinduced reflection of single crystal methyl-ammonium tri-iodine perovskite (MAPbI3) measured at cryogenic temperatures. We observe two quantum beating oscillations (fast and slow) whose frequencies increase linearly with B with slopes that depend on the crystal orientation with respect to the applied magnetic field. We assign the quantum beatings to positive and negative trions whose Landé g-factors are determined by those of the electron and hole, respectively, or by the carriers left behind after trion recombination. These are $${g}_{[001]}^{e}$$ g [ 001 ] e = 2.52 and $${g}_{[1\bar{1}0]}^{e}\,$$ g [ 1 1 ¯ 0 ] e = 2.63 for electrons, whereas $$\big|{g}_{[001]}^{h}\big|\,$$ g [ 001 ] h = 0.28 and $$\big|{g}_{[1\bar{1}0]}^{h}\big|\,$$ g [ 1 1 ¯ 0 ] h = 0.57 for holes. The obtained g-values are in excellent agreement with an 8-band K.P calculation for orthorhombic MAPbI3. Using the technique of resonant spin amplification of the quantum beatings we measure a relatively long spin coherence time of ~ 11 (6) nanoseconds for electrons (holes) at 4 K.
The fullerene C60, C70, and C84 molecules, that are composed of ∼99% naturally abundant 12C having spinless nuclei, are considered to have miniature hyperfine interaction and also weak intrinsic spin-orbit coupling (SOC) due to the light carbon atoms. However, it has been theoretically predicted that the curvature of the fullerene molecules may increase the SOC due to the induced hybridization of the π and σ electrons on the carbon atoms that reside on the fullerene molecule surface. In this work, we have measured the spin diffusion length in films of C60, C70, and C84 in NiFe/fullerene/Pt trilayer devices, where pure spin current is injected into the fullerene film at the NiFe/fullerene interface via spin pumping induced by microwave absorption at ferromagnet resonance conditions, and subsequently detected at the fullerene/Pt interface as electrical current via the inverse spin-Hall effect. The obtained spin diffusion lengths in the fullerene films are of the order of 10 nm and increase from C60 to C84 in which the fullerene molecule’s curvature decreases; this finding validates the existence of curvature-induced SOC in the fullerenes. Our results deepen the understanding of spin transport in fullerene films and may benefit the design of molecular spintronic devices.
We report on terahertz characterization of La-doped BaSnO3 (BSO) thin-films. BSO is a transparent complex oxide material, which has attracted substantial interest due to its large electrical conductivity and wide bandgap. The complex refractive index of these films is extracted in the 0.3 to 1.5 THz frequency range, which shows a metal-like response across this broad frequency window. The large optical conductivity found in these films at terahertz wavelengths makes this material an interesting platform for developing electromagnetic structures having a strong response at terahertz wavelengths, i.e. terahertz-functional, while being transparent at visible and near-IR wavelengths. As an example of such application, we demonstrate a visible-transparent terahertz polarizer.
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