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 dynamics1 and as a means of revealing2,3 or even inducing4,5 broken symmetries. Emerging methods for light-based current control5-16 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. Here we introduce vectorial optoelectronic metasurfaces in which ultrafast light pulses induce local directional charge flows around symmetry-broken plasmonic nanostructures, with tunable responses and arbitrary patterning down to subdiffractive nanometre scales. Local symmetries and vectorial currents are revealed by polarization-dependent and wavelength-sensitive electrical readout and terahertz (THz) emission, whereas spatially tailored global currents are demonstrated in the direct generation of elusive broadband THz vector beams17. We show that, in graphene, a detailed interplay between electrodynamic, thermodynamic and hydrodynamic degrees of freedom gives rise to rapidly evolving nanoscale driving forces and charge flows under the extremely spatially and temporally localized excitation. These results set the stage for versatile patterning and optical control over nanoscale currents in materials diagnostics, THz spectroscopies, nanomagnetism and ultrafast information processing.

Highly Mobile Excitons in Single Crystal Methylammonium Lead Tribromide Perovskite Microribbons.

Excitons are often given negative connotation in solar energy harvesting in part due to their presumed short diffusion lengths. We investigate exciton transport in single-crystal methylammonium lead tribromide (MAPbBr3) microribbons via spectrally, spatially, and temporally resolved photocurrent and photoluminescence measurements. Distinct peaks in the photocurrent spectra unambiguously confirm exciton formation and allow for accurate extraction of the low temperature exciton binding energy (39 meV). Photocurrent decays within a few µm at room temperature, while a gate-tunable long-range photocurrent component appears at lower temperatures (about 100 µm below 140 K). Carrier lifetimes of 1.2 µs or shorter exclude the possibility of the long decay length arising from slow trapped-carrier hopping. Free carrier diffusion is also an unlikely source of the highly nonlocal photocurrent, due to their small fraction at low temperatures. We attribute the long-distance transport to high-mobility excitons, which may open up new opportunities for novel exciton-based photovoltaic applications.

Transport Modeling of Locally Photogenerated Excitons in Halide Perovskites.

Excitons have fundamental impacts on optoelectronic properties of semiconductors. Halide perovskites, with long carrier lifetimes and ionic crystal structures, may support highly mobile excitons because the dipolar nature of excitons suppresses phonon scattering. Inspired by recent experimental progress, we perform device modeling to rigorously analyze exciton formation and transport in methylammonium lead triiodide under local photoexcitation by using a finite element method. Mobile excitons, coexisting with free carriers, can dominate photocurrent generation at low temperatures. The simulation results are in excellent agreement with the experimentally observed strong temperature and gate dependence of carrier diffusion. This work signifies that efficient exciton transport can substantially influence charge transport in the family of perovskite materials.

Temperature and Gate Dependence of Carrier Diffusion in Single Crystal Methylammonium Lead Iodide Perovskite Microstructures.

We investigate temperature-dependent photogenerated carrier diffusion in single-crystal methylammonium lead iodide microstuctures via scanning photocurrent microscopy. Carrier diffusion lengths increased abruptly across the tetragonal to orthorhombic phase transition and reached 200 ± 50 µm at 80 K. In combination with the microsecond carrier lifetime measured by a transient photocurrent method, an enormous carrier mobility value of 3 × 104 cm2/V s was extracted at 80 K. The observed highly nonlocal photocurrent and the rapid increase of the carrier diffusion length at low temperatures can be understood by the formation and efficient transport of free excitons in the orthorhombic phase as a result of reduced optical phonon scattering due to the dipolar nature of the excitons. Carrier diffusion lengths were tuned by a factor of 8 by gate voltage and increased with increasing majority carrier (electron) concentration, consistent with the exciton model.

Millimetre-long transport of photogenerated carriers in topological insulators.

Excitons are spin integer particles that are predicted to condense into a coherent quantum state at sufficiently low temperature. Here by using photocurrent imaging we report experimental evidence of formation and efficient transport of non-equilibrium excitons in Bi2-xSbxSe3 nanoribbons. The photocurrent distributions are independent of electric field, indicating that photoexcited electrons and holes form excitons. Remarkably, these excitons can transport over hundreds of micrometers along the topological insulator (TI) nanoribbons before recombination at up to 40 K. The macroscopic transport distance, combined with short carrier lifetime obtained from transient photocurrent measurements, indicates an exciton diffusion coefficient at least 36 m2 s-1, which corresponds to a mobility of 6 × 104 m2 V-1 s-1 at 7 K and is four order of magnitude higher than the value reported for free carriers in TIs. The observation of highly dissipationless exciton transport implies the formation of superfluid-like exciton condensate at the surface of TIs.

Broadband ultrafast terahertz spectroscopy in the 25 T Split Florida-Helix.

We describe the development of a broadband (0.3-10 THz) optical pump-terahertz probe spectrometer with an unprecedented combination of temporal resolution (≤200 fs) operating in external magnetic fields as high as 25 T using the new Split Florida-Helix magnet system. Using this new instrument, we measure the transient dynamics in a gallium arsenide four-quantum well sample after photoexcitation at 800 nm.

Ultrafast pump-probe spectroscopy in gallium arsenide at 25 T.

We have performed high-fluence, nondegenerate pump-probe spectroscopy in the Split Florida-Helix magnet at 25 T and 15 K. The electronic component of our ultrafast differential reflectivity can be described with a simplified four-level approximation to determine the scattering and recombination rates. Ultrafast oscillations are well described by a coherent acoustic phonon model. Our free-space ultrafast spectroscopic technique will permit future experimental investigations to study novel photoinduced phase transitions and complex interactions in correlated electron systems, which will require the high pulse energies of our free-space alternative.