We induce ultrafast magneto-photocurrents in a GaAs crystal employing interband excitation with femtosecond laser pulses at room temperature and non-invasively separate surface and bulk contributions to the overall current response. The separation between the different symmetry contributions is achieved by measuring the simultaneously emitted terahertz radiation for different sample orientations. Excitation intensity and photon energy dependences of the magneto-photocurrents for linearly and circularly polarized excitations reveal an involvement of different microscopic origins, one of which we believe is the inverse Spin-Hall effect. Our experiments are important for a better understanding of the complex momentum-space carrier dynamics in magnetic fields.
We induce ultrafast photocurrents in a GaAs crystal exposed to a magnetic field by optical femtosecond excitation. The magneto-photocurrents are studied by time-resolved detection of the simultaneously emitted THz radiation. We find that their dynamics differ considerably from the dynamics of other photocurrents which are expected to follow the temporal shape of the optical intensity. We attribute this difference to the influence of carrier-anisotropy relaxation on the magneto-photocurrents. Our measurements show that the anisotropy relaxation for carrier densities ranging between $10^{16}$ cm…
Carrier-envelope phase control of ultrafast photocurrents in layered MoS$_2$
Walter Schottky Institute and Physics Department, Technical University of Munich（慕尼黑工业大学瓦尔特·肖特基研究所和物理系）；Munich Center of Quantum Science and Technology (MCQST)（慕尼黑量子科学与技术中心）
A microscopic approach that is based on the multisubband semiconductor Bloch equations formulated in the basis of a 14-band ${\mathbf k} \cdot {\mathbf p}$ model is employed to compute the temporal dynamics of photocurrents in GaAs quantum wells following the excitation with femtosecond laser pulses. This approach provides a transparent description of the interband, intersubband, and intraband excitations, fully includes all resonant as well as off-resonant excitations, and treats the light-matter interaction non-perturbatively. For linearly polarized excitations the photocurrents contain cont…
We use the terahertz (THz) emission spectroscopy to study femtosecond photocurrent dynamics in the prototypical 2D semiconductor, transition metal dichalcogenide MoSe$_2$. We identify several distinct mechanisms producing THz radiation in response to an ultrashort ($30\,$fs) optical excitation in a bilayer (BL) and a multilayer (ML) sample. In the ML, the THz radiation is generated at a picosecond timescale by out-of-plane currents due to the drift of photoexcited charge carriers in the surface electric field. The BL emission is generated by an in-plane shift current. Finally, we observe oscil…
We show that, by monitoring the free carrier reservoir in a GaAs-based quantum well microcavity under nonresonant pulsed optical pumping, lasing supported by a fermionic reservoir (photon lasing) can be distinguished from lasing supported by a reservoir of bosons (polariton lasing). Carrier densities are probed by measuring the photocurrent between lateral contacts deposited directly on the quantum wells of a microcavity that are partially exposed by wet chemical etching. We identify two clear thresholds in the input-output characteristic of the photoluminescence signal which can be attributed…
Strong Coulomb interaction in monolayer semiconductors allows them to host optically active large many-body states, such as the five-particle state, charged biexciton. Strong nonlinear light absorption by the charged biexciton under spectral resonance, coupled with its charged nature, makes it intriguing for nonlinear photodetection - an area that is hitherto unexplored. Using the high built-in vertical electric field in an asymmetrically designed few-layer graphene encapsulated 1L-WS$_2$ heterostructure, here we report a large, highly nonlinear photocurrent arising from the strong absorption …
It is demonstrated that the non-instantaneous response of the optically induced coherent polarization tremendously influences the real-space shift of electronic charges in semiconductors. The possibility to coherently control this real-space shift with temporally non-overlapping excitation pulses allows for the observation of a new type of shift current, which only exists for certain polarization-shaped excitation pulses and vanishes in the continuous-wave limit. In contrast to previously studied shift currents, the new current requires a phase mismatch between two orthogonal transition dipole…
We performed non-degenerate pump-probe experiments on a GaAs/AlAs photonic structure. We switched the photonic properties using the optical Kerr effect and free carriers excited by three photon absorption. From these measurements we extracted the non-degenerate Kerr coefficients over a broad wavelength range and we extracted the three photon absorption coefficient for GaAs at three wavelengths in the near infrared. We show that the optical Kerr effect is large enough to switch a cavity resonance with a high \emph{Q} ($Q>1000$) photonic cavity.
We compute the jerk current tensor of GaAs, Si, and ferroelectric single-layer GeS, GeSe, SnS, and SnSe. We find peak values of the order of $10^{14}$ mA/V$^3$s$^2$ in GaAs and Si within the visible energy spectrum and an order of magnitude larger in single-layer GeS, GeSe, SnSe and SnS. We show that the detailed knowledge of this tensor and its large value in single-layer GeS, GeSe, SnSe and SnS make it possible to predict the magnitude and angle of rotation of polarization of intense terahertz pulses generated in photoconductive switches and point to alternative functionalities of these devi…
We study ultrafast photocurrents in thin films of a model ferromagnetic metal with broken bulk inversion symmetry, the half-metallic Heusler compound NiMnSb, following excitation with an optical pump pulse with photon energy 1.55 eV. Remarkably, in terms of the direction of the sample magnetization M, all photocurrents are found to be a superposition of a component with Rashba- and Dresselhaus-type symmetry. We explain the Dresselhaus bulk photocurrent as follows: Pump-induced electron heating induces an excess of spin μ_s||M, which transfers spin angular momentum into states with Dresselhaus-…
We study the time-resolved reflectivity spectrum of a switched planar GaAs-AlAs microcavity. Between 5 and 40 ps after the switching (pump) pulse we observe a strong excess probe reflectivity and a change of the frequency of light trapped in the cavity up to 5 linewidths away from the cavity resonance. This frequency change does not adiabatically follow the fast-changing cavity resonance. The frequency change is attributed to an accumulated phase change due to the time-dependent refractive index. An analytical model predicts dynamics in qualitative agreement with the experiments, and points to…
We explore a planar GaAs/AlAs photonic microcavity using pump-probe spectroscopy. Free carriers are excited in the GaAs with short pump pulses. The time-resolved reflectivity is spectrally resolved short probe pulses. We show experimentally that the cavity resonance and its width depend on the dynamic refractive index of both the lambda-slab and the lambda/4 GaAs mirrors. We clearly observe a double exponential relaxation of both the the cavity resonance and its width, which is due to the different recombination timescales in the lambda-slab and the mirrors. In particular, the relaxation time …
Spatiotemporal Terahertz Emission Nanoscopy of Spintronic Photocurrents
RPTU Kaiserslautern-Landau（凯泽斯劳滕-兰道莱布尼茨理工学院）；Fraunhofer Institute for Industrial Mathematics ITWM（弗劳恩霍夫工业数学研究所）；Freie Universität Berlin（柏林自由大学）；Hangzhou International Innovation Institute, Beihang University（北京航空航天大学杭州国际创新学院）；School of Electronic and Information Engineering, Beihang University（北京航空航天大学电子与信息工程学院）；School of Engineering, Brown University（布朗大学工程学院）；University of Lille, CNRS, Centrale Lille, Université Polytechnique Hauts-de-France（里尔大学、法国国家科学研究中心、中央里尔理工学院、上法兰西高等工业大学联合实验室）；Zhangjiang Laboratory（张江实验室）
The authors study the ultrafast switching-on and -off of planar GaAs/AlAs microcavities. Up to 0.8% refractive index changes are achieved by optically exciting free carriers at 1720 nm and a pulse energy of 1.8 micro Joules. The cavity resonance is dynamically tracked by measuring reflectivity versus time delay with tunable laser pulses, and is found to shift by as much as 3.3 linewidths within a few picoseconds. The switching-off occurs with a decay time of around 50 ps. The authors derive the dynamic behavior of the carrier density and of the complex refractive index. They propose that the i…
We demonstrate optical coherent control of the emission direction of THz radiation. Femtosecond laser pulses are used to excite different types of ultrafast photocurrents along different directions in a bulk GaAs sample. The overall emission pattern can be modified by changing the phase of the optical excitation. With this method, THz beam steering of about 8 degrees is realized. A simple dipole-based model allows us to relate the size of the steering effect to the amplitude ratio between the different photocurrent contributions and to diffraction effects resulting from the excitation spot siz…
We employ polarization-shaped ultrafast optical pulses to generate photocurrents which only arise if the optically induced coherent polarization is frequency modulated. This frequency modulation is obtained via detuned excitation of light-hole excitons in (110)-oriented GaAs quantum wells. The observed photocurrents vanish for resonant excitation of excitons and reverse their direction with a change of the sign of detuning. Moreover, the currents do not exist for continuous-wave excitation. Our work reveals the existence of a new class of photocurrents and visualizes the complexity of current …
As a fascinating topological phase of matter, Weyl semimetals host chiral fermions with distinct chiralities and spin textures. Optical excitations involving those chiral fermions can induce exotic carrier responses, and in turn lead to novel optical phenomena. Here, we discover strong coherent chiral terahertz emission from the Weyl semimetal TaAs and demonstrate unprecedented manipulation over its polarization on a femtosecond timescale. Such polarization control is achieved via the colossal ultrafast photocurrents in TaAs arising from the circular or linear photogalvanic effect. We unravel …
In this work, we investigate multiphoton and optical-field tunneling emission from metallic surfaces with nanoscale vacuum gaps. Using time-dependent Schrodinger equation (TDSE) simulations, we find that the properties of the emitted photocurrent in such systems can be greatly altered by the application of only a few-volt DC bias. We find that when coupled with expected plasmonic enhancements within the nanometer-scale metallic gaps, the application of this DC bias significantly reduces the threshold for the transition to optical-field-driven tunneling from the metal surface, and could suffici…
We demonstrate a new, nonlinear optical effect of electric currents. First, a steady current is generated by applying a voltage on a doped GaAs crystal. We demonstrate that this current induces second-harmonic generation of a probe laser pulse. Second, we optically inject a transient current in an undoped GaAs crystal by using a pair of ultrafast laser pulses, and demonstrate that it induces the same second-harmonic generation. In both cases, the induced second-order nonlinear susceptibility is proportional to the current density. This effect can be used for nondestructive, noninvasive, and ul…
We have previously demonstrated that in the context of two-dimensional (2D) coherent electronic spectroscopy measured by phase modulation and phase-sensitive detection, an \emph{incoherent} nonlinear response, due to pairs of photoexcitations produced via linear excitation pathways, contribute to the measured signal as unexpected background [Grégoire et al., J.\ Chem.\ Phys. \textbf{147}, 114201 (2017)]. Here, we simulate the effect of such incoherent population mixing in the photocurrent signal collected from a GaAs solar cell by acting externally on the transimpedance amplifier circuit used …
We report on the generation of bulk photocurrents in materials driven by non-resonant bi-chromatic fields that are circularly polarized and co-rotating. The nonlinear photocurrents have a fully controllable directionality and amplitude without requiring carrier-envelope-phase stabilization or few-cycle pulses, and are generated with photon energies much smaller than the band gap (reducing heating in the photo-conversion process). We demonstrate with ab-initio calculations that the photocurrent generation mechanism is universal and arises in gaped materials (Si, diamond, MgO, hBN), in semi-meta…
We have performed ultrafast pump-probe experiments on a GaAs-AlAs microcavity with a resonance near 1300 nm in the "original" telecom band. We exploit the virtually instantaneous electronic Kerr effect to repeatedly and reproducibly switch a GaAs-AlAs planar microcavity. We achieve repetition times as fast as 300 fs, thereby breaking the THz modulation barrier. The rate of the switching in our experiments is only determined by optics and not by material related relaxation. Our results offer novel opportunities for fundamental studies of cavity-QED and optical information processing in sub-pico…
