Twisted Nonlinear Optics in Monolayer van der Waals Crystals.

In addition to a plethora of emergent phenomena, the spatial topology of optical vortices enables an array of applications in optical communications and quantum information science. Multibeam nonlinear optical processes, augmented by optical vortices, are essential in this context, providing robust access to an infinitely large set of quantum states associated with the orbital angular momentum of light. Here, we push the boundaries of vortex nonlinear optics to the ultimate limits of material dimensionality.

Electrodynamics of photo-carriers in multiferroic EuYMnO.

Understanding and controlling the antiferromagnetic order in multiferroic materials on an ultrafast time scale is a long standing area of interest, due to their potential applications in spintronics and ultrafast magnetoelectric switching. We present an optical pump-terahertz (THz) probe study on multiferroic EuYMnO. The optical pump predominantly excites the d-d transitions of the Mn ions, and the temporal evolution of the pump-induced transient conductivity is measured with a subsequent THz pulse.

Creation, stabilization, and investigation at ambient pressure of pressure-induced superconductivity in BiSbTe.

In light of breakthroughs in superconductivity under high pressure, and considering that record critical temperatures (Ts) across various systems have been achieved under high pressure, the primary challenge for higher T should no longer solely be to increase T under extreme conditions but also to reduce, or ideally eliminate, the need for applied pressure in retaining pressure-induced or -enhanced superconductivity. The topological semiconductor BiSbTe (BST) was chosen to demonstrate our approach to addressing this challenge and exploring its intriguing physics. Under pressures up to ~50 GPa, three superconducting phases (BST-I, -II, and -III) were observed.

Feasible Route to High-Temperature Ambient-Pressure Hydride Superconductivity.

A key challenge in materials discovery is to find high-temperature superconductors. Hydrogen and hydride materials have long been considered promising materials displaying conventional phonon-mediated superconductivity. However, the high pressures required to stabilize these materials have restricted their application.

Light-driven nanoscale vectorial currents.

Controlled charge flows are fundamental to many areas of science and technology, serving as carriers of energy and information, as probes of material properties and dynamics and as a means of revealing or even inducing broken symmetries. Emerging methods for light-based current control offer particularly promising routes beyond the speed and adaptability limitations of conventional voltage-driven systems. However, optical generation and manipulation of currents at nanometre spatial scales remains a basic challenge and a crucial step towards scalable optoelectronic systems for microelectronics and information science.

Ultrafast terahertz emission from emerging symmetry-broken materials.

Nonlinear optical spectroscopies are powerful tools for investigating both static material properties and light-induced dynamics. Terahertz (THz) emission spectroscopy has emerged in the past several decades as a versatile method for directly tracking the ultrafast evolution of physical properties, quasiparticle distributions, and order parameters within bulk materials and nanoscale interfaces. Ultrafast optically-induced THz radiation is often analyzed mechanistically in terms of relative contributions from nonlinear polarization, magnetization, and various transient free charge currents.

Revealing charge carrier dynamics and transport in Te-doped GaAsSb and GaAsSbN nanowires by correlating ultrafast terahertz spectroscopy and optoelectronic characterization.

Recent advances in the growth of III-V semiconductor nanowires (NWs) hold great promise for nanoscale optoelectronic device applications. It is established that a small amount of nitrogen (N) incorporation in III-V semiconductor NWs can effectively red-shift their wavelength of operation and tailor their electronic properties for specific applications. However, understanding the impact of N incorporation on non-equilibrium charge carrier dynamics and transport in semiconducting NWs is critical in achieving efficient semiconducting NW devices.

High Entropy Oxide Relaxor Ferroelectrics.

Relaxor ferroelectrics are important in technological applications due to strong electromechanical response, energy storage capacity, electrocaloric effect, and pyroelectric energy conversion properties. Current efforts to discover and design materials in this class generally rely on substitutional doping as slight changes to local compositional order can significantly affect the Curie temperature, morphotropic phase boundary, and electromechanical responses. In this work, we demonstrate that moving to the strong limit of compositional complexity in an O perovskite allows stabilization of relaxor responses that do not rely on a single narrow phase transition region.

Manipulation of Exciton Dynamics in Single-Layer WSe Using a Toroidal Dielectric Metasurface.

Recent advances in emerging atomically thin transition metal dichalcogenide semiconductors with strong light-matter interactions and tunable optical properties provide novel approaches for realizing new material functionalities. Coupling two-dimensional semiconductors with all-dielectric resonant nanostructures represents an especially attractive opportunity for manipulating optical properties in both the near-field and far-field regimes. Here, by integrating single-layer WSe and titanium oxide (TiO) dielectric metasurfaces with toroidal resonances, we realized robust exciton emission enhancement over 1 order of magnitude at both room and low temperatures.

Hot Carrier Cooling and Recombination Dynamics of Chlorine-Doped Hybrid Perovskite Single Crystals.

Controlling the photoexcited properties and behavior of hybrid perovskites by halide doping has the potential to impact a wide range of emerging technologies, including solar cells and radiation detectors. Crystalline samples of methylammonium lead bromide substituted with chlorine (MAPbBrCl) were examined by transient reflectivity spectroscopy and nonadiabatic molecular dynamics simulations. At picosecond time scales, the addition of chlorine to the perovskite crystal increased the observed rate of hot carrier cooling and the calculated electron-phonon coupling constants.

Induced ferroelectric phases in SrTiO by a nanocomposite approach.

Inducing new phases in thick films via vertical lattice strain is one of the critical advantages of vertically aligned nanocomposites (VANs). In SrTiO (STO), the ground state is ferroelastic, and the ferroelectricity in STO is suppressed by the orthorhombic transition. Here, we explore whether vertical lattice strain in three-dimensional VANs can be used to induce new ferroelectric phases in SrTiO:MgO (STO:MgO) VAN thin films.

Ultrafast relaxation dynamics in bimetallic plasmonic catalysts.

Combining a plasmonic metal, such as gold, with other popular catalysts, such as Ni or Pt, can extend its benefits to many energy-extensive reactions catalyzed by those metals. The efficiency of a plasmon-enhanced catalytic reaction is mainly determined by the light absorption cross section and the photoexcited charge carrier relaxation dynamics of the nanoparticles. We have investigated the charge carrier relaxation dynamics of gold/nickel (Au/Ni) and gold/platinum (Au/Pt) bimetallic nanoparticles.

Competing Interface and Bulk Effect-Driven Magnetoelectric Coupling in Vertically Aligned Nanocomposites.

Room-temperature magnetoelectric (ME) coupling is developed in artificial multilayers and nanocomposites composed of magnetostrictive and electrostrictive materials. While the coupling mechanisms and strengths in multilayers are widely studied, they are largely unexplored in vertically aligned nanocomposites (VANs), even though theory has predicted that VANs exhibit much larger ME coupling coefficients than multilayer structures. Here, strong transverse and longitudinal ME coupling in epitaxial BaTiO:CoFeO VANs measured by both optical second harmonic generation and piezoresponse force microscopy under magnetic fields is reported.

Nanoscale Artificial Plasmonic Lattice in Self-Assembled Vertically Aligned Nitride-Metal Hybrid Metamaterials.

Nanoscale metamaterials exhibit extraordinary optical properties and are proposed for various technological applications. Here, a new class of novel nanoscale two-phase hybrid metamaterials is achieved by combining two major classes of traditional plasmonic materials, metals (e.g.

Magnetoelastoelectric coupling in core-shell nanoparticles enabling directional and mode-selective magnetic control of THz beam propagation.

Magnetoelastoelectric coupling in an engineered biphasic multiferroic nanocomposite enables a novel magnetic field direction-defined propagation control of terahertz (THz) waves. These core-shell nanoparticles are comprised of a ferromagnetic cobalt ferrite core and a ferroelectric barium titanate shell. An assembly of these nanoparticles, when operated in external magnetic fields, exhibits a controllable amplitude modulation when the magnetic field is applied antiparallel to the THz wave propagation direction; yet the same assembly displays an additional phase modulation when the magnetic field is applied along the propagation direction.

Conducting Interface in Oxide Homojunction: Understanding of Superior Properties in Black TiO2.

Black TiO2 nanoparticles with a crystalline core and amorphous-shell structure exhibit superior optoelectronic properties in comparison with pristine TiO2. The fundamental mechanisms underlying these enhancements, however, remain unclear, largely due to the inherent complexities and limitations of powder materials. Here, we fabricate TiO2 homojunction films consisting of an oxygen-deficient amorphous layer on top of a highly crystalline layer, to simulate the structural/functional configuration of black TiO2 nanoparticles.

Heterogeneous nucleation and growth dynamics in the light-induced phase transition in vanadium dioxide.

We report on ultrafast optical investigations of the light-induced insulator-to-metal phase transition in vanadium dioxide with controlled disorder generated by substrate mismatch. These results reveal common dynamics of this optically-induced phase transition that are independent of this disorder. Above the fluence threshold for completing the transition to the rutile crystalline phase, we find a common time scale, independent of sample morphology, of 40.

Ultrafast Optical Microscopy of Single Monolayer Molybdenum Disulfide Flakes.

We have performed ultrafast optical microscopy on single flakes of atomically thin CVD-grown molybdenum disulfide, using non-degenerate femtosecond pump-probe spectroscopy to excite and probe carriers above and below the indirect and direct band gaps. These measurements reveal the influence of layer thickness on carrier dynamics when probing near the band gap. Furthermore, fluence-dependent measurements indicate that carrier relaxation is primarily influenced by surface-related defect and trap states after above-bandgap photoexcitation.

Ultrafast phase transition via catastrophic phonon collapse driven by plasmonic hot-electron injection.

Ultrafast photoinduced phase transitions could revolutionize data-storage and telecommunications technologies by modulating signals in integrated nanocircuits at terahertz speeds. In quantum phase-changing materials (PCMs), microscopic charge, lattice, and orbital degrees of freedom interact cooperatively to modify macroscopic electrical and optical properties. Although these interactions are well documented for bulk single crystals and thin films, little is known about the ultrafast dynamics of nanostructured PCMs when interfaced to another class of materials as in this case to active plasmonic elements.

Ultrafast nonlinear optical spectroscopy of a dual-band negative index metamaterial all-optical switching device.

We study the nonlinear optical response of a fishnet structure-metamaterial all-optical switching device that exhibits two near-infrared negative-index resonances. We study and compare the nonlinear optical response at both resonances and identify transient spectral features associated with the negative index resonance. We see a significantly stronger response at the longer wavelength resonance, but identical temporal dynamics at both resonances, providing insight into separately engineering the switching time and switching ratio of such a fishnet structure metamaterial all-optical switch.

Subpicosecond optical switching with a negative index metamaterial.

We demonstrate a nanoscale, subpicosecond (ps) metamaterial device capable of terabit/second all-optical communication in the near-IR. The 600 fs response, 2 orders of magnitude faster than previously reported, is achieved by accessing a previously unused regime of high-injection level, subpicosecond carrier dynamics in the alpha-Si dielectric layer of the metamaterial. Further, we utilize a previously unrecognized, higher-order, shorter-wavelength negative-index resonance in the fishnet structure, thereby extending device functionality (via structural tuning of device dimensions) over 1.

Ultrafast spectroscopy of the uranium(IV) and thorium(IV) bis(ketimide) complexes (C5Me5)2An[-N=C(Ph)(CH2Ph)]2 (An = Th, U).

Ultrafast pump-probe spectroscopic studies have been performed on (C 5Me 5) 2U[- N=C(Ph)(CH 2Ph)] 2 and (C 5Me 5) 2Th[- N=C(Ph)(CH 2Ph)] 2 including, for the uranium complex, the first direct measurement of dynamics of electronic deactivation within a 5f-electron manifold. Evidence has been found for strong coupling between the electronic ground state and the f-electron manifold which dominates the dynamics of the excited states of the bis(ketimide) uranium complex. These also demonstrate strong singlet-f manifold coupling, which assists in the deactivation of the photoexcited state of the uranium complex, and provide information on intersystem crossing and internal conversion processes in both complexes.