Nanostructured metal oxides, such as Cu2O, CeO2, α-Fe2O3, and TiO2, can efficiently mediate photocatalysis for solar-to-chemical energy conversion and pollution remediation. In this contribution, we report a novel approach, dielectric Mie resonance-enhanced photocatalysis, to enhance the catalytic activity of metal oxide photocatalysts. Specifically, we demonstrate that Cu2O nanostructures exhibiting dielectric Mie resonances can exhibit up to an order of magnitude higher photocatalytic rate as compared with Cu2O nanostructures not exhibiting dielectric Mie resonances. Our finite-difference time-domain (FDTD) simulation and experimental results predict a volcano-type relationship between the photocatalytic rate and the size of Cu2O nanospheres and nanocubes. Using transient absorption measurements, we reveal that a coherent electronic process associated with dielectric Mie resonance-mediated charge carrier generation is dominant in Cu2O nanostructures that exhibit higher photocatalytic rates. Although we experimentally demonstrate dielectric Mie resonance-enhanced photocatalysis with only Cu2O nanoparticles here, based on our FDTD simulations, we anticipate the same can be achieved with other metal oxide photocatalysts, including CeO2, α-Fe2O3, and TiO2.

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A type-II InAs/AlAs$$_{0.16}$$ 0.16 Sb$$_{0.84}$$ 0.84 multiple-quantum well sample is investigated for the photoexcited carrier dynamics as a function of excitation photon energy and lattice temperature. Time-resolved measurements are performed using a near-infrared pump pulse, with photon energies near to and above the band gap, probed with a terahertz probe pulse. The transient terahertz absorption is characterized by a multi-rise, multi-decay function that captures long-lived decay times and a metastable state for an excess-photon energy of $$>100$$ > 100 meV. For sufficient excess-photon energy, excitation of the metastable state is followed by a transition to the long-lived states. Excitation dependence of the long-lived states map onto a nearly-direct band gap ($$E{_g}$$ E g ) density of states with an Urbach tail below $$E{_g}$$ E g . As temperature increases, the long-lived decay times increase $$<E{_g}$$ < E g , due to the increased phonon interaction of the unintentional defect states, and by phonon stabilization of the hot carriers $$>E{_g}$$ > E g . Additionally, Auger (and/or trap-assisted Auger) scattering above the onset of the plateau may also contribute to longer hot-carrier lifetimes. Meanwhile, the initial decay component shows strong dependence on excitation energy and temperature, reflecting the complicated initial transfer of energy between valence-band and defect states, indicating methods to further prolong hot carriers for technological applications.

The downscaling of nonlinear optical devices is significantly hindered by the inherently weak nonlinearity in regular materials. Here, we report a giant third-harmonic generation discovered in epitaxial thin films of V−VI chalcogenide topological insulators. Using a tailored substrate and capping layer, a single reflection from a 13 nm film can produce a nonlinear conversion efficiency of nearly 0.01%, a performance that rivals micron-scale waveguides made from conventional materials or metasurfaces with far more complex structures. Such strong nonlinear optical emission, absent from the topologically trivial member in the same compound family, is found to be generated by the same bulk band characteristics that are responsible for producing the band inversion and the nontrivial topological ordering. This finding reveals the possibility of obtaining superior optical nonlinearity by examining the large pool of newly discovered topological materials with similar band characteristics.