Rotation of the plane of the polarization of light in the presence of a magnetic-field, known as the Faraday rotation, is a consequence of the electromagnetic nature of light and has been utilized in many optical devices. Current efforts aim to realize the ultrafast Faraday rotation on a sub-picosecond time scale. Thereby, the Faraday medium should allow an ultrafast process by which in the presence of an ultrashort intense magnetic-field, the light polarization rotates. We meet these criteria by applying an intense single cycle THz magnetic-field to simple molecular liquids and demonstrate the rotation of the plane of polarization of an optical pulse traversing the liquids on a sub-picosecond time scale. The effect is attributed to the deflection of an optically induced instantaneous electric polarization under the influence the THz magnetic-field. The resolved Faraday rotation scales linearly with the THz magnetic-field and quadratically with the molecular polarizability.
We report on a giant Faraday effect in an electron plasma in n-InSb probed via polarization-resolved terahertz (THz) time-domain spectroscopy. Polarization rotation angles and ellipticities reach as large as π/2 and 1, respectively, over a wide frequency range (0.3-2.5 THz) at magnetic fields of a few Tesla. The experimental results together with theoretical simulations show its promising ability to construct broadband and tunable THz polarization optics, such as a circular polarizer, half-wave plate, and polarization modulators.
The transition frequency between nonthermal coherent magnetic precessions and ultrafast demagnetization is arguably the most sought after answer in magnetism science and technology nowadays. So far, it is believed to be in the terahertz (THz) range. Here, using an ultra-intense low frequency THz bullet, and thin magnetic layers, we report on experimental evidences that fully coherent nonthermal THz magnetic switching may never be reachable in conventional ferromagnetic thin films. At high excitation intensities, while the spins still coherently precess with the THz magnetic field, the deposite…
We predict a strong-field ultrafast optical Faraday effect, where a circularly polarized ultrashort optical pulse induces transient chirality in an achiral transparent dielectric. This effect is attractive for time-resolved measurements because it gives access to the non-instantaneity of the nonlinear medium response, and also because it represents relaxation of time-reversal symmetry by all-optical means. We propose probing the induced transient chirality with a weak linearly polarized ultraviolet pulse that is shorter than the near-infrared pump pulse. The predicted effects are ultrafast: th…
We demonstrate ultrafast resonance switching of terahertz metamaterials through optical excitation of radiation damaged silicon placed in the gap of single split gap ring resonator. We observe the dynamic switching OFF of the fundamental resonance mode on a time scale of 4 picoseconds (ps) followed by the switching ON of the same resonance after 20 ps. Electric field distributions in the metamaterials unit cell derived through numerical simulations clearly support our experimental observations, showing that the high electric field at the resonator gaps, responsible for inductive-capacitive res…
Terahertz (THz)-based electron manipulation has recently been shown to hold tremendous promise as a technology for manipulating and driving the next-generation of compact ultrafast electron sources. Here, we demonstrate an ultrafast electron diffractometer with THz-driven pulse compression. The electron bunches from a conventional DC gun are compressed by a factor of 10 and reach a duration of ~180 fs (FWHM) with 10,000 electrons/pulse at a 1 kHz repetition rate. The resulting ultrafast electron source is used in a proof-of-principle experiment to probe the photoinduced dynamics of single-crys…
We use an open-aperture Z-scan technique to show how intense few-cycle terahertz pulses can experience a nonlinear bleaching of absorption in an n-doped semiconductor due to terahertz-electric-field-driven intervalley scattering of electrons in the conduction band. Coherent detection of the transmitted terahertz pulse waveform also allows the nonlinear conductivity dynamics to be followed with sub-picosecond time resolution. Both the Z-scan and time-domain results are found to be in agreement with our theoretical analysis.
We study ultrafast magnetization quenching of ferromagnetic iron following excitation by an optical vs a terahertz pump pulse. While the optical pump (photon energy of 3.1 eV) induces a strongly nonthermal electron distribution, terahertz excitation (~4 meV) results in a quasi-thermal perturbation of the electron population. The pump-induced spin and electron dynamics are interrogated by the magneto-optic Kerr effect (MOKE). A deconvolution procedure allows us to push the time resolution down to 130 fs, even though the driving terahertz pulse is more than 0.5 ps long. Remarkably, the MOKE sign…
We present a combined theoretical and experimental study of spatio-temporal propagation effects in terahertz (THz) generation in gases using two-color ionizing laser pulses. The observed strong broadening of the THz spectra with increasing gas pressure reveals the prominent role of spatio-temporal reshaping and of a plasma-induced blue-shift of the pump pulses in the generation process. Results obtained from (3+1)-dimensional simulations are in good agreement with experimental findings and clarify the mechanisms responsible for THz emission.
We demonstrate theoretically that ultrafast heating of metal nanoparticles by the laser pulse should lead to the generation of coherent terahertz (THz) radiation during the heat redistribution process. It is shown that after the femtosecond laser pulse action the time-dependent gradient of the electronic temperature induces low-frequency particle polarization with the characteristic timescale of about fractions of picosecond. In the case of the directed metallic pattern, the THz pulse waveform can be controlled by changing geometry of the individual particle. The generation mechanism proposed …
We investigate the ultrafast electron dynamics triggered by terahertz and optical pulses in thin platinum and gold films by probing their transient optical reflectivity. The response of the platinum film to an intense terahertz pulse is similar to the optically-induced dynamics of both films and can be described by a two-temperature model. Surprisingly, gold can exhibit a much smaller terahertz pulse-induced reflectivity change and with opposite sign. For platinum, we estimate a 20% larger electron-phonon coupling for the terahertz-driven dynamics compared to the optically-induced one, which w…
Rapid evolutions of microscopic fields govern the majority of elementary excitations in condensed matter and drive microelectronic currents at increasing frequencies. Beyond nominal "radio frequencies", however, access to local electric waveforms remains a challenge. Several imaging schemes resolve sub-wavelength fields up to multi-Terahertz (THz) frequencies - including scanning-probe techniques, electro-optic sampling or recent ultrafast electron microscopy. Yet, various constraints on sample geometries, acquisition speed and maximum fields limit applications. Here, we introduce ubiquitous f…
The ultrafast switching of magnetization in multiferroic materials by a femtosecond laser could provide various advantages in photonics and magnonics. An efficient approach to control the light matter interaction is the modulation of ultrafast coherent magnons and phonons in the high frequency range. Spontaneous Raman and infrared spectra reveal the excitation of magnons and optical phonons in multiferroic BiFeO3 in the sub few terahertz range. However, coherent control of such quasiparticles has not been achieved yet. In this study, we demonstrate that linearly polarized laser pulses simultan…
For the purposes of measuring the high-frequency complex conductivity of correlated-electron materials at low temperatures and high magnetic fields, a method is introduced for performing coherent time-domain terahertz spectroscopy directly in the cryogenic bore of existing dc and pulsed magnets. Miniature fiber-coupled THz emitters and receivers are constructed and are demonstrated to work down to 1.5 Kelvin and up to 17 Tesla, for eventual use in higher-field magnets. Maintaining the sub-micron alignment between fiber and antenna during thermal cycling, obtaining ultrafast (${<200}$~fs) optic…
As a key component for next-generation wireless communications (6G and beyond), terahertz (THz) electronic oscillators are being actively developed. Precise and dynamic phase control of ultrafast THz waveforms is essential for high-speed beam steering and high-capacity data transmission. However, measurement of such ultrafast dynamic process is beyond the scope of electronics due to the limited bandwidth of the electrical measuring instruments. Here we surpass this limit by applying photonic technology. Using a femtosecond laser, we generate offset-free THz pulses to phase-lock the electronic …
Terahertz (THz) emission spectroscopy is a powerful method that allows one to measure the ultrafast dynamics of polarization, current, or magnetization in a material based on THz emission from the material. However, the practical implementation of this method can be challenging, and can result in significant errors in the reconstruction of the quantity of interest. Here, we experimentally and theoretically demonstrate a rigorous method of signal reconstruction in THz emission spectroscopy, and describe the main experimental and theoretical sources of reconstruction error. We identify the linea…
Dirac Fermion, which is the low energy collective excitation near the Dirac cone in monolayer graphene, have gained great attention by low energy Terahertz probe. In the case of undoped graphene, it has been generally understood that the ultrafast terahertz thermal relaxation is mostly driven by the electron-phonon coupling (EOP), which can be prolonged to tens and hundreds of picoseconds. However, for the high doped graphene, which manifests the negative photoinduced terahertz conductivity, there is still no consensus on the dominant aspects of the cooling process on a time scale of a few pic…
Controlling light polarization is one of the most essential routines in modern optical technology. Since the demonstration of optical pulse shaping by spatial light modulators and its potential in controlling the quantum reaction pathways, it paved the way for many applications as a coherent control of the photoionization process or as polarization shaping of terahertz (THz) pulses. Here, we evidenced efficient nonresonant and noncollinear $χ^{(2)}$-type light-matter interaction in femtosecond polarization-sensitive time-resolved optical measurements. Such nonlinear optical interaction of visi…
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…
Visualizing ultrafast dynamics at the atomic scale requires time-resolved pump-probe characterization with femtosecond temporal resolution. For single-shot ultrafast electron diffraction (UED) with fully relativistic electron bunch probes, existing techniques are limited by the achievable electron probe bunch length, charge, and timing jitter. We present the first experimental demonstration of pump-probe UED with THz-driven compression and time-stamping that enable UED probes with unprecedented temporal resolution. This technique utilizes two counter-propagating quasi-single-cycle THz pulses g…
Ultrashort photoemitted electron bunches can provide high electron currents within sub-picosecond timeframes, enabling time-resolved investigations of ultrafast physical processes with nanoscale resolution. Non-resonant conductive nanotips are typically employed to realize nanoscale photoelectron sources with high brightness. However, such emitters require complex non-scalable fabrication procedures featuring poor reproducibility. Planar resonant antennas fabricated via photolithography have been recently investigated, also because of their superior field enhancement properties. Nevertheless, …
Although Gigahertz-scale free-carrier modulators have been previously demonstrated in silicon, intensity modulators operating at Terahertz speeds have not been reported because of silicon's weak ultrafast optical nonlinearity. We have demonstrated intensity modulation of light with light in a silicon-polymer integrated waveguide device, based on the all-optical Kerr effect - the same ultrafast effect used in four-wave mixing. Direct measurements of time-domain intensity modulation are made at speeds of 10 GHz. We showed experimentally that the ultrafast mechanism of this modulation functions a…
For terahertz (THz) wave applications, tunable and rapid modulation is highly required. When studied by means of optical pump-terahertz probe spectroscopy, single-walled carbon nanotubes (SWCNTs) thin films demonstrated ultrafast carrier recombination lifetimes with a high relative change in the signal under optical excitation, making them promising candidates for high-speed modulators. Here, combination of SWCNTthin films and stretchable substrates facilitated studies of the SWCNT mechanical properties under strain,and enabled the development of a new type of an opto-mechanical modulator. By …
Intersubband (ISB) transitions in semiconductor multi-quantum well (MQW) structures are promising candidates for the development of saturable absorbers at terahertz (THz) frequencies. Here, we exploit amplitude and phase-resolved two-dimensional (2D) THz spectroscopy on the sub-cycle time scale to observe directly the saturation dynamics and coherent control of ISB transitions in a metal-insulator MQW structure. Clear signatures of incoherent pump-probe and coherent four-wave mixing signals are recorded as a function of the peak electric field of the single-cycle THz pulses. All nonlinear sign…
We predict a new type of ultrafast third-order nonlinearity of surface plasmon polaritons (SPP) in planar magneto-plasmonic structures caused by the inverse Faraday effect (IFE). Planar SPPs with a significant longitudinal component of the electric field act via the IFE as an effective transverse magnetic field. Its response to the plasmon propagation leads to strong ultrafast self-action which manifests itself through a third-order nonlinearity. We derive a general formula and analytical expressions for the IFE-related nonlinear susceptibility for two specific planar magneto-plasmonic structu…
Flexible manipulation of terahertz-wave polarization during the generation process is very important for terahertz applications, especially for the next-generation on-chip functional terahertz sources. However, current terahertz emitters could not satisfy such demand, hence calling for new mechanism and conceptually new terahertz source. Here we demonstrate a magnetic-field-controlled, highly-efficient, cost-effective, and broadband terahertz source with flexible switch of terahertz polarization states in ferromagnetic heterostructures driven by femtosecond laser pulses. We verify that the chi…
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…
Ultrafast Terahertz and Optical Spectroscopy under Synergetic Extreme Conditions
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所凝聚态物理国家实验室）；School of Physical Sciences, University of Chinese Academy of Sciences（中国科学院大学物理科学学院）；Tsung-Dao Lee Institute, Department of Physics and Astronomy, Shanghai Jiao Tong University（上海交通大学物理与天文学院紫江研究院）；International Center for Quantum Materials, School of Physics, Peking University（北京大学物理学院量子材料科学中心）
Ferroelectric materials offer unprecedented ultrafast responses and are of great interest for the development of new polarizable media under the influence of an electromagnetic field. Recent research efforts have demonstrated the role of optical excitation and intense terahertz (THz) pulses in inducing a polar order and revealing a hidden phase transition in SrTiO3 (STO), respectively. Here we show that the surface of STO crystals at room temperature act as ultrafast sensors that enable sub-picosecond switching through the Kerr effect and multi-ps recording of polar THz intensity with spatial …
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）
Ultrafast two-dimensional spectroscopy utilizes correlated multiple light-matter interactions for retrieving dynamic features that may otherwise be hidden under the linear spectrum. Its extension to the terahertz regime of the electromagnetic spectrum, where a rich variety of material degrees of freedom reside, remains an experimental challenge. Here we report ultrafast two-dimensional terahertz spectroscopy of gas-phase molecular rotors at room temperature. Using time-delayed terahertz pulse pairs, we observe photon echoes and other nonlinear signals resulting from molecular dipole orientatio…
The thermoelectric effects of topological semimetals have attracted tremendous research interest because many topological semimetals are excellent thermoelectric materials and thermoelectricity serves as one of their most important potential applications. In this work, we reveal the transient photothermoelectric response of Dirac semimetallic Cd3As2, namely the photo-Seebeck effect and photo-Nernst effect, by studying the terahertz (THz) emission from the transient photocurrent induced by these effects. Our excitation polarization and power dependence confirm that the observed THz emission is …
Magneto-terahertz phenomena are the main focus of the thesis. This work started as supporting research for the science of an X-ray laser (SwissFEL). X-ray lasers have recently drawn great attention as an unprecedented tool for scientific research on the ultrafast scale..... To answer this fundamental question, we performed original numerical simulations using a coupled Landau- Lifshitz-Gilbert Maxwell model. ... Those requirements were the motivations for the experiments performed in the second part of the thesis. To shape the terahertz pulses, .... Regarding the field intensities, we followed…
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 …
Excitation of antiferromagnetic spin waves in HoFeO$_{3}$ crystal combined with a split ring resonator (SRR) is studied using terahertz (THz) electromagnetic pulses. The magnetic field in the vicinity of the SRR induced by the incident THz electric field component excites and the Faraday rotation of the polarization of a near-infrared probe pulse directly measures oscillations that correspond to the antiferromagnetic spin resonance mode. The good agreement of the temperature-dependent magnetization dynamics with the calculation using the two-lattice Landau-Lifshitz-Gilbert equation confirms th…
We report the development of new terahertz techniques for rapidly measuring the complex Faraday angle in systems with broken time-reversal symmetry using the cyclotron resonance of a GaAs two-dimensional electron gas in a magnetic field as a system for demonstration of performance. We have made polarization modulation, high sensitivity (< 1 mrad) narrow band rotation measurements with a CW optically pumped molecular gas laser, and by combining the distinct advantages of terahertz (THz) time domain spectroscopy and polarization modulation techniques, we have demonstrated rapid broadband rotatio…
We use finite element simulations in both the frequency and the time-domain to study the terahertz resonance characteristics of a metamaterial (MM) comprising a spiral connected to a straight arm. The MM acts as a RLC circuit whose resonance frequency can be precisely tuned by varying the characteristic geometrical parameters of the spiral: inner and outer radius, width and number of turns. We provide a simple analytical model that uses these geometrical parameters as input to give accurate estimates of the resonance frequency. Finite element simulations show that linearly polarized terahertz …
Quantum cascade lasers (QCLs) represent a fascinating accomplishment of quantum engineering and enable the direct generation of terahertz (THz) frequency radiation from an electrically-biased semiconductor heterostructure. Their large spectral bandwidth, high output powers and quantum-limited linewidths have facilitated the realization of THz pulses by active mode-locking and passive generation of optical frequency combs (FCs) through intracavity four-wave-mixing, albeit over a restricted operational regime. Here, we conceive an integrated architecture for the generation of high power (10 mW) …
We report about the anomalous Hall effect in 4f 3d metallic alloys measured using terahertz time-domain spectroscopy. The strength of the observed terahertz spin-dependent transport phenomenon is in good agreement with expectations based on electronic transport measurements. Employing this effect, we succeeded to reveal ultrafast dynamics of the anomalous Hall effect which accompanies the sub-100 picosecond optically induced magnetization reversal in a GdFeCo alloy. The experiments demonstrate the ability to control currents at terahertz frequencies in spintronic devices magnetically and ultra…
Strong coupling between light and matter occurs when the two interact strongly enough to form new hybrid modes called polaritons. Here we report on the strong coupling of both the electric and magnetic degrees of freedom to an ultrafast terahertz (THz) frequency electromagnetic wave. In our system, optical phonons in a slab of ferroelectric lithium niobate (LiNbO$_3$) are strongly coupled to a THz electric field to form phonon-polaritons, which are simultaneously strongly coupled to magnons in an adjacent slab of canted antiferromagnetic erbium orthoferrite (ErFeO$_3$) via the THz magnetic fie…
In this Letter we study the generation of quasi-static magnetic fields by the plasmon-induced inverse Faraday effect and propose a magneto-optical waveguide structure for achieving magnetization switching at sub-ps time in a nano-confined magneto-optical structure. In particular we show that the direction of the generated quasi-static field in a magneto-optical dielectric cavity side-coupled to a metal-insulator-metal (MIM) waveguide depends sensitively on the wavelength of the surface plasmon polaritions (SPP). This phenomenon could open up a new energy-efficient ultrafast method for nano-con…
We demonstrate an ultrafast reversible modulation of resonant terahertz (THz) response in strongly photoexcited metamaterials. The transient spectral-temporal response of the dipole transition ~1.6 THz exhibits a distinct non-monotonic variation as a function of pump fluence. The transition energy shift, strength, spectral width and density-dependent ultrafast relaxation manifest a remarkable re-emergence of the resonances after initial quenching. Our simulation, incorporating the first-order diffraction from the photoinduced transient grating, reproduces the salient features, providing a new …
