RESUMEN
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.
RESUMEN
A type-II InAs/AlAs[Formula: see text]Sb[Formula: see text] 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 [Formula: see text] 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 ([Formula: see text]) density of states with an Urbach tail below [Formula: see text]. As temperature increases, the long-lived decay times increase [Formula: see text], due to the increased phonon interaction of the unintentional defect states, and by phonon stabilization of the hot carriers [Formula: see text]. 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.
RESUMEN
Solar-driven production of renewable energy (e.g., H2) has been investigated for decades. To date, the applications are limited by low efficiency due to rapid charge recombination (both radiative and nonradiative modes) and slow reaction rates. Tremendous efforts have been focused on reducing the radiative recombination and enhancing the interfacial charge transfer by engineering the geometric and electronic structure of the photocatalysts. However, fine-tuning of nonradiative recombination processes and optimization of target reaction paths still lack effective control. Here we show that minimizing the nonradiative relaxation and the adsorption energy of photogenerated surface-adsorbed hydrogen atoms are essential to achieve a longer lifetime of the charge carriers and a faster reaction rate, respectively. Such control results in a 16-fold enhancement in photocatalytic H2 evolution and a 15-fold increase in photocurrent of the crystalline g-C3N4 compared to that of the amorphous g-C3N4.
RESUMEN
Optical rectification of near-infrared laser pulses generates broadband terahertz radiation in chalcopyrite crystals CdGeP2, ZnGeP2 and CdSiP2. The emission is characterized using linear-polarized excitation from 0.8 eV to 1.55 eV (1550 nm - 800 nm). All three crystals are (110)-cut and polished to 0.5 mm, thinner than the coherence length across most of the excitation photon energy range, such that they all produce a bandwidth ~2.5 THz when excited with ~100 fs pulses. It is found that CdGeP2 produced the strongest emission at telecoms wavelengths, while CdSiP2 is generally the strongest source. Pump-intensity dependence provides the nonlinear coefficients for each crystal.