Electron-electron (e-e) interaction is known as a source of logarithmic renormalizations for Dirac fermions in quantum field theory. The renormalization of electron--optical phonon coupling (EPC) by e-e interaction, which plays a pivotal role in hot carrier and phonon dynamics, has been discussed after the discovery of graphene. We investigate the hot carrier dynamics and the EPC strength using time-resolved ultrabroadband terahertz (THz) spectroscopy combined with numerical simulation based on the Boltzmann transport equation and comprehensive temperature model. The large negative photoconductivity and the non-Drude behavior of THz conductivity spectra appear under high pump fluence and can be attributed to the temporal variation of the hot carrier distribution and scattering rate. We successfully estimate the dimensionless EPC matrix element of the $A_1^{\prime}$ optical phonon mode near the $\mathbf{K}$ point as $λ_{\mathbf{K}} \approx$0.09 from the fitting of THz conductivity spectra and temporal evolution of transient THz reflectivity, which is slightly larger than the prediction of the renormalization group.
Terahertz electromagnetic radiation is extremely useful for numerous applications such as imaging and spectroscopy. Therefore, it is highly desirable to have an efficient table-top emitter covering the 1-to-30-THz window whilst being driven by a low-cost, low-power femtosecond laser oscillator. So far, all solid-state emitters solely exploit physics related to the electron charge and deliver emission spectra with substantial gaps. Here, we take advantage of the electron spin to realize a conceptually new terahertz source which relies on tailored fundamental spintronic and photonic phenomena in…
We study the generation of THz radiation from the acceleration of ultrafast photoexcited charge carriers in graphene in the presence of a DC electric field. Our model is based on calculating the transient current density from the time-dependent distribution function which is determined using the Boltzmann transport equation within a relaxation time approximation. We include the time-dependent generation of carriers by the pump pulse by solving for the carrier generation rate using the Bloch equations in the rotating wave approximation (RWA). The linearly polarized pump pulse generates an aniso…
Phase-locked ultrashort pulses in the rich terahertz (THz) spectral range have provided key insights into phenomena as diverse as quantum confinement, first-order phase transitions, high-temperature superconductivity, and carrier transport in nanomaterials. Ultrabroadband electro-optic sampling of few-cycle field transients can even reveal novel dynamics that occur faster than a single oscillation cycle of light. However, conventional THz spectroscopy is intrinsically restricted to ensemble measurements by the diffraction limit. As a result, it measures dielectric functions averaged over the s…
The efficient modulation and control of ultrafast signals on-chip is of central importance in terahertz (THz) communications and a promising route toward sub-diffraction limit THz spectroscopy. Two-dimensional (2D) materials may provide a platform for these endeavors. We explore this potential, integrating high-quality graphene p-n junctions within two types of planar transmission line circuits to modulate and emit picosecond pulses. In a coplanar stripline geometry, we demonstrate electrical modulation of THz signal transmission by 95%. In a Goubau waveguide geometry, we achieve complete gate…
Coupling phase-stable single-cycle terahertz (THz) pulses to scanning tunneling microscope (STM) junctions enables spatio-temporal imaging with femtosecond temporal and Ångstrom spatial resolution. The time resolution achieved in such THz-gated STM is ultimately limited by the sub-cycle temporal variation of the tip-enhanced THz field acting as an ultrafast voltage pulse, and hence by the ability to feed high-frequency, broadband THz pulses into the junction. Here, we report on the coupling of ultrabroadband (1-30 THz) single-cycle THz pulses from a spintronic THz emitter(STE) into a metallic …
We present a numerical study on the intraband optical conductivity of hot carriers at quasi-equilibria in photoexcited graphene based on the semiclassical Boltzmann transport equations (BTE) with the aim of understanding the effects of intrinsic optical phonon and extrinsic coulomb scattering caused by charged impurities at the graphene--substrate interface. Instead of using full-BTE solutions, we employ iterative solutions of the BTE and the comprehensive model for the temporal evolutions of hot-carrier temperature and hot-optical-phonon occupations to reduce computational costs. Undoped grap…
Terahertz emission spectroscopy of ultrathin multilayers of magnetic and heavy metals has recently attracted much interest. This method not only provides fundamental insights into photoinduced spin transport and spin-orbit interaction at highest frequencies but has also paved the way to applications such as efficient and ultrabroadband emitters of terahertz electromagnetic radiation. So far, predominantly standard ferromagnetic materials have been exploited. Here, by introducing a suitable figure of merit, we systematically compare the strength of terahertz emission from X/Pt bilayers with X b…
We have performed time-resolved terahertz absorption measurements on photoexcited electron-hole pairs in undoped GaAs quantum wells in magnetic fields. We probed both unbound- and bound-carrier responses via cyclotron resonance and intraexciton resonance, respectively. The stability of excitons, monitored as the pair density was systematically increased, was found to dramatically increase with increasing magnetic field. Specifically, the 1$s$-2$p_-$ intraexciton transition at 9 T persisted up to the highest density, whereas the 1$s$-2$p$ feature at 0 T was quickly replaced by a free-carrier Dr…
For many of the envisioned optoelectronic applications of graphene it is crucial to understand the sub-picosecond carrier dynamics immediately following photoexcitation, as well as the effect on the electrical conductivity - the photoconductivity. Whereas these topics have been studied using various ultrafast experiments and theoretical approaches, controversial and incomplete explanations have been put forward concerning the sign of the photoconductivity, the occurrence and significance of the creation of additional electron-hole pairs, and, in particular, how the relevant processes depend on…
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 probe the electron transport properties in the shell of GaAs/In0.2Ga0.8As core/shell nanowires at high electric fields using optical pump / THz probe spectroscopy with broadband THz pulses and peak electric fields up to 0.6 MV/cm. The plasmon resonance of the photoexcited charge carriers exhibits a systematic redshift and a suppression of its spectral weight for THz driving fields exceeding 0.4 MV/cm. This behavior is attributed to the intervalley electron scattering resulting in the increase of the average electron effective mass and the corresponding decrease of the electron mobility by a…
The photoelectric effect consists in the photoexcitation of electrons above a potential barrier at a material interface and is exploited for photodetection over a wide frequency range. This three-dimensional process has an inherent inefficiency: photoexcited electrons gain momenta predominantly parallel to the interface, while to leave the material they have to move perpendicular to it. Here, we report on the discovery of an in-plane photoelectric effect occurring within a two-dimensional electron gas. In this purely quantum-mechanical, scattering-free process, photo-electron momenta are perfe…
We study the momentum alignment of photoexcited carriers and the optical control of valley population in gapless and gapped two-dimensional Dirac materials. The trigonal warping effect leads to the spatial separation of charge carriers belonging to different valleys upon linearly polarized high-frequency photoexcitation. Valley separation in gapped materials can be detected by measuring the degree of circular polarization of band-edge photoluminescence at different sides of the sample or light spot (optical valley Hall effect). We demonstrate that the celebrated Rashba effect, caused by substr…
Dielectric control of ultrafast carrier dynamics and transport in graphene
Max Planck Institute for Polymer Research（马克斯·普朗克聚合物研究所）；Debye Institute for Nanomaterials Science, Utrecht University（乌得勒支大学德拜纳米科学研究所）；Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST（加泰罗尼亚纳米科学与纳米技术研究所（ICN2，西班牙高等科学研究委员会和巴塞罗那独立科学与技术基金会））；School of Physics and Astronomy, University of Manchester（曼彻斯特大学物理与天文学学院）；Department of Applied Physics, TU Eindhoven（埃因霍温理工大学应用物理系）
