Ultrafast exciton fluid flow in an atomically thin MoS2 semiconductor.

Excitons (coupled electron-hole pairs) in semiconductors can form collective states that sometimes exhibit spectacular nonlinear properties. Here, we show experimental evidence of a collective state of short-lived excitons in a direct-bandgap, atomically thin MoS2 semiconductor whose propagation resembles that of a classical liquid as suggested by the nearly uniform photoluminescence through the MoS2 monolayer regardless of crystallographic defects and geometric constraints. The exciton fluid flows over ultralong distances (at least 60 µm) at a speed of ~1.8 × 107 m s-1 (~6% the speed of light). The collective phase emerges above a critical laser power, in the absence of free charges and below a critical temperature (usually Tc ≈ 150 K) approaching room temperature in hexagonal-boron-nitride-encapsulated devices. Our theoretical simulations suggest that momentum is conserved and local equilibrium is achieved among excitons; both these features are compatible with a fluid dynamics description of the exciton transport.

Transition from Diffusive to Superdiffusive Transport in Carbon Nanotube Networks via Nematic Order Control.

The one-dimensional confinement of quasiparticles in individual carbon nanotubes (CNTs) leads to extremely anisotropic electronic and optical properties. In a macroscopic ensemble of randomly oriented CNTs, this anisotropy disappears together with other properties that make them attractive for certain device applications. The question however remains if not only anisotropy but also other types of behaviors are suppressed by disorder. Here, we compare the dynamics of quasiparticles under strong electric fields in aligned and random CNT networks using a combination of terahertz emission and photocurrent experiments and out-of-equilibrium numerical simulations. We find that the degree of alignment strongly influences the excited quasiparticles' dynamics, rerouting the thermalization pathways. This is, in particular, evidenced in the high-energy, high-momentum electronic population (probed through the formation of low energy excitons via exciton impact ionization) and the transport regime evolving from diffusive to superdiffusive.

Zero-field quantum beats and spin decoherence mechanisms in CsPbBr3 perovskite nanocrystals.

Coherent optical manipulation of exciton states provides a fascinating approach for quantum gating and ultrafast switching. However, their coherence time for incumbent semiconductors is highly susceptible to thermal decoherence and inhomogeneous broadening effects. Here, we uncover zero-field exciton quantum beating and anomalous temperature dependence of the exciton spin lifetimes in CsPbBr3 perovskite nanocrystals (NCs) ensembles. The quantum beating between two exciton fine-structure splitting (FSS) levels enables coherent ultrafast optical control of the excitonic degree of freedom. From the anomalous temperature dependence, we identify and fully parametrize all the regimes of exciton spin depolarization, finding that approaching room temperature, it is dominated by a motional narrowing process governed by the exciton multilevel coherence. Importantly, our results present an unambiguous full physical picture of the complex interplay of the underlying spin decoherence mechanisms. These intrinsic exciton FSS states in perovskite NCs present fresh opportunities for spin-based photonic quantum technologies.

From rogue wave solution to solitons.

Using a generalized nonlinear Schrödinger equation, we investigate the transformation of a fundamental rogue wave solution to a collection of solitons. Taking the third-order dispersion, self-steepening, and Raman-induced self-frequency shift as the generalizing effects, we systematically observe how a fundamental rogue wave has an impact on its surrounding continuous wave background and reshapes its own characteristics while a group of solitons are created. Applying a local inverse scattering technique based on the periodization of an isolated structure, we show that the third-order dispersion and Raman-induced self-frequency shift generates a group of solitons in the neighborhood where the rogue wave solution emerges. Using a volume interpretation, we show that the self-steepening effect stretches the rogue wave solution by reducing its volume. Also, we find that with the Raman-induced self-frequency shift, a decelerating rogue wave generates a red-shifted Raman radiation while the rogue wave itself turns into a slow-moving soliton. We show that when third-order dispersion, self-steepening, and Raman-induced self-frequency shift act together on the rogue wave solution, each of these effects favor the rogue wave to generate a group of solitons near where it first emerges while the rogue wave itself also becomes one of these solitons.

Ultrafast Thermalization Pathways of Excited Bulk and Surface States in the Ferroelectric Rashba Semiconductor GeTe.

A large Rashba effect is essential for future applications in spintronics. Particularly attractive is understanding and controlling nonequilibrium properties of ferroelectric Rashba semiconductors. Here, time- and angle-resolved photoemission is utilized to access the ultrafast dynamics of bulk and surface transient Rashba states after femtosecond optical excitation of GeTe. A complex thermalization pathway is observed, wherein three different timescales can be clearly distinguished: intraband thermalization, interband equilibration, and electronic cooling. These dynamics exhibit an unconventional temperature dependence: while the cooling phase speeds up with increasing sample temperature, the opposite happens for interband thermalization. It is demonstrated how, due to the Rashba effect, an interdependence of these timescales on the relative strength of both electron-electron and electron-phonon interactions is responsible for the counterintuitive temperature dependence, with spin-selection constrained interband electron-electron scatterings found both to dominate dynamics away from the Fermi level, and to weaken with increasing temperature. These findings are supported by theoretical calculations within the Boltzmann approach explicitly showing the opposite behavior of all relevant electron-electron and electron-phonon scattering channels with temperature, thus confirming the microscopic mechanism of the experimental findings. The present results are important for future applications of ferroelectric Rashba semiconductors and their excitations in ultrafast spintronics.

Electro-Ionic Control of Surface Plasmons in Graphene-Layered Heterostructures.

Precise control of light is indispensable to modern optical communication devices especially as the size of such devices approaches the subwavelength scale. Plasmonic devices are suitable for the development of these optical devices due to the extreme field confinement and its ability to be controlled by tuning the carrier density at the metal/dielectric interface. Here, an electro-ionic controlled plasmonic device consisting of Au/graphene/ion-gel is demonstrated as an optical switch, where an external electric field modulates the real part of the electrical conductivity. The graphene layer enhances charge penetration and charge separation at the Au/graphene interface resulting in an increased photoinduced voltage. The ion-gel immobilized on the Au/graphene further enables the electrical tunability of plasmons which modulates the intensity of the reflected laser light. This work paves the way for developing novel plasmonic electro-optic switches for potential applications such as integrated optical devices.

Terahertz Excitonics in Carbon Nanotubes: Exciton Autoionization and Multiplication.

Excitons play major roles in optical processes in modern semiconductors, such as single-wall carbon nanotubes (CNTs), transition metal dichalcogenides, and 2D perovskite quantum wells. They possess extremely large binding energies (>100 meV), dominating absorption and emission spectra even at high temperatures. The large binding energies imply that they are stable, that is, hard to ionize, rendering them seemingly unsuited for optoelectronic devices that require mobile charge carriers, especially terahertz emitters and solar cells. Here, we have conducted terahertz emission and photocurrent studies on films of aligned single-chirality semiconducting CNTs and find that excitons autoionize, i.e., spontaneously dissociate into electrons and holes. This process naturally occurs ultrafast (<1 ps) while conserving energy and momentum. The created carriers can then be accelerated to emit a burst of terahertz radiation when a dc bias is applied, with promising efficiency in comparison to standard GaAs-based emitters. Furthermore, at high bias, the accelerated carriers acquire high enough kinetic energy to create secondary excitons through impact exciton generation, again in a fully energy and momentum conserving fashion. This exciton multiplication process leads to a nonlinear photocurrent increase as a function of bias. Our theoretical simulations based on nonequilibrium Boltzmann transport equations, taking into account all possible scattering pathways and a realistic band structure, reproduce all of our experimental data semiquantitatively. These results not only elucidate the momentum-dependent ultrafast dynamics of excitons and carriers in CNTs but also suggest promising routes toward terahertz excitonics despite the orders-of-magnitude mismatch between the exciton binding energies and the terahertz photon energies.

Effect of Strong Electric Fields on Material Responses: The Bloch Oscillation Resonance in High Field Conductivities.

In this paper, we investigated the effect of strong electric fields on material responses and the Bloch oscillation resonance in high field conductivities. For this purpose, a high-order accurate explicit modal discontinuous Galerkin (DG) solver is employed for solving the quantum Boltzmann transport equation (BTE) in the context of electron transport at nanoscales under strongly out-of-equilibrium conditions. Here, we study the transient behavior and the convergence of a steady-state response to an external oscillating electric field switched on at time zero. We first benchmark our numerical results with known analytic steady-state responses at low fields. The computational results show that the present DG scheme is in excellent agreement with analytic solutions over the whole range of parameters and to an extremely high precision, allowing us to achieve good agreement even for the fifth-order response at low fields. We then extend the method to strong electric fields and show how the responses are deviated from the low-field ones and the transition to a dampened Bloch oscillation regime. Most importantly, we report the observation of a new regime induced by the resonance between the standard low-field response and Bloch oscillations.

Modification of spintronic terahertz emitter performance through defect engineering.

Spintronic ferromagnetic/non-magnetic heterostructures are novel sources for the generation of THz radiation based on spin-to-charge conversion in the layers. The key technological and scientific challenge of THz spintronic emitters is to increase their intensity and frequency bandwidth. Our work reveals the factors to engineer spintronic Terahertz generation by introducing the scattering lifetime and the interface transmission for spin polarized, non-equilibrium electrons. We clarify the influence of the electron-defect scattering lifetime on the spectral shape and the interface transmission on the THz amplitude, and how this is linked to structural defects of bilayer emitters. The results of our study define a roadmap of the properties of emitted as well as detected THz-pulse shapes and spectra that is essential for future applications of metallic spintronic THz emitters.

Ultrafast Spin-to-Charge Conversion at the Surface of Topological Insulator Thin Films.

Strong spin-orbit coupling, resulting in the formation of spin-momentum-locked surface states, endows topological insulators with superior spin-to-charge conversion characteristics, though the dynamics that govern it have remained elusive. Here, an all-optical method is presented, which enables unprecedented tracking of the ultrafast dynamics of spin-to-charge conversion in a prototypical topological insulator Bi2 Se3 /ferromagnetic Co heterostructure, down to the sub-picosecond timescale. Compared to pure Bi2 Se3 or Co, a giant terahertz emission is observed in the heterostructure that originates from spin-to-charge conversion, in which the topological surface states play a crucial role. A 0.12 ps timescale is identified that sets a technological speed limit of spin-to-charge conversion processes in topological insulators. In addition, it is shown that the spin-to-charge conversion efficiency is temperature independent in Bi2 Se3 as expected from the nature of the surface states, paving the way for designing next-generation high-speed optospintronic devices based on topological insulators at room temperature.

Generalized GW+Boltzmann Approach for the Description of Ultrafast Electron Dynamics in Topological Insulators.

Quantum-phase transitions between trivial insulators and topological insulators differ from ordinary metal-insulator transitions in that they arise from the inversion of the bulk band structure due to strong spin-orbit coupling. Such topological phase transitions are unique in nature as they lead to the emergence of topological surface states which are characterized by a peculiar spin texture that is believed to play a central role in the generation and manipulation of dissipationless surface spin currents on ultrafast timescales. Here, we provide a generalized G W +Boltzmann approach for the description of ultrafast dynamics in topological insulators driven by electron-electron and electron-phonon scatterings. Taking the prototypical insulator Bi 2 Te 3 as an example, we test the robustness of our approach by comparing the theoretical prediction to results of time- and angle-resolved photoemission experiments. From this comparison, we are able to demonstrate the crucial role of the excited spin texture in the subpicosecond relaxation of transient electrons, as well as to accurately obtain the magnitude and strength of electron-electron and electron-phonon couplings. Our approach could be used as a generalized theory for three-dimensional topological insulators in the bulk-conducting transport regime, paving the way for the realization of a unified theory of ultrafast dynamics in topological materials.

Ultrafast magnetization enhancement in metallic multilayers driven by superdiffusive spin current.

Uncovering the physical mechanisms that govern ultrafast charge and spin dynamics is crucial for understanding correlated matter as well as the fundamental limits of ultrafast spin-based electronics. Spin dynamics in magnetic materials can be driven by ultrashort light pulses, resulting in a transient drop in magnetization within a few hundred femtoseconds. However, a full understanding of femtosecond spin dynamics remains elusive. Here we spatially separate the spin dynamics using Ni/Ru/Fe magnetic trilayers, where the Ni and Fe layers can be ferro- or antiferromagnetically coupled. By exciting the layers with a laser pulse and probing the magnetization response simultaneously but separately in Ni and Fe, we surprisingly find that optically induced demagnetization of the Ni layer transiently enhances the magnetization of the Fe layer when the two layer magnetizations are initially aligned parallel. Our observations are explained by a laser-generated superdiffusive spin current between the layers.