Terahertz spin waves could be generated on-demand via all-optical manipulation of magnetization by femtosecond laser pulse. Here, we present an energy balance model, which explains the energy transfer rates from laser pulse to electron bath coupled with phonon, spin, and magnetization of five different magnetic metallic thin films: Iron, Cobalt, Nickel, Gadolinium and Ni$_{2}$MnSn Heusler alloy. Two types of transient magnetization dynamics emerge in metallic magnetic thin films based on their Curie temperatures (T$_{C}$): type I (Fe, Co, and Ni with T$_{C}$ > room temperature, RT) and type II films (Gd and Ni$_{2}$MnSn with T$_{C}$ $\approx$ RT). We study the effect of laser fluence and pulse width for single Gaussian laser pulses and the effect of metal film thickness on magnetization dynamics. Spectral dynamics show that broadband spin waves up to 24 THz could be generated by all-optical manipulation of magnetization in these nanofilms.
The ultrafast relaxation and recombination dynamics of photogenerated electrons and holes in epitaxial graphene are studied using optical-pump Terahertz-probe spectroscopy. The conductivity in graphene at Terahertz frequencies depends on the carrier concentration as well as the carrier distribution in energy. Time-resolved studies of the conductivity can therefore be used to probe the dynamics associated with carrier intraband relaxation and interband recombination. We report the electron-hole recombination times in epitaxial graphene for the first time. Our results show that carrier cooling o…
The terahertz spectral regime, ranging from about 0.1 to 15 THz, is one of the least explored yet most technologically transformative spectral regions. One current challenge is to develop efficient and compact terahertz emitters/detectors with a broadband and gapless spectrum that can be tailored for various pump photon energies. Here we demonstrate efficient single-cycle broadband THz generation, ranging from about 0.1 to 4 THz, from a thin layer of split-ring resonators with few tens of nanometers thickness by pumping at the telecommunications wavelength of 1.5 micrometer (200 THz). The tera…
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 report a terahertz optical modulator consisting of randomly stacked trilayer graphene (TLG) deposited on an oxidized silicon substrate by means of THz- Time Domain Spectroscopy (THz-TDS). Here, the gate tuning of the Fermi level of the TLG provides the fundamental basis for the modulation of THz transmission. We measured a 15% change in the THz transmission of this device over a broad frequency range (0.6-1.6THz). We also observed a strong absorption >80% in the time-domain signals and a frequency independence of the conductivity. Furthermore, unlike previous studies, we find that the under…
Ultrafast terahertz spectroscopy accesses the {\em dark} excitonic ground state in resonantly-excited (6,5) SWNTs via internal, direct dipole-allowed transitions between lowest lying dark-bright pair state $\sim$6 meV. An analytical model reproduces the response which enables quantitative analysis of transient densities of dark excitons and {\em e-h} plasma, oscillator strength, transition energy renormalization and dynamics. %excitation-induced renormalization. Non-equilibrium, yet stable, quasi-1D quantum states with dark excitonic correlations rapidly emerge even with increasing off-resonan…
We use ultrafast x-ray pulses to characterize the lattice response of SrTiO3 when driven by strong terahertz (THz) fields. We observe transient changes in the diffraction intensity with a delayed onset with respect to the driving field. Fourier analysis reveals two frequency components corresponding to the two lowest energy zone-center optical modes in SrTiO3. The lower frequency mode exhibits clear softening as the temperature is decreased while the higher frequency mode shows slight temperature dependence.
Simultaneous detection of THz emission and transient magneto-optical response is employed to study ultrafast laser-induced magnetization dynamics in multisublattice magnets NdFeCo and GdFeCo amorphous alloys with in-plane magnetic anisotropy. A satisfactory quantitative agreement between the dynamics revealed with the help of these two techniques is obtained for GdFeCo. For NdFeCo the THz emission reveals faster dynamics than the magneto-optical response. This indicates that in addition to spin dynamics of Fe ultrafast laser excitation triggers faster magnetization dynamics of Nd.
The anisotropic effective mass of electrons is directly measured using time-resolved THz- pump/THz-probe techniques in a n-doped InGaAs semiconductor thin film. A microscopic theory is used to attribute this anisotropy in the THz probe transmission to the nonparabolicity of the conduction band. Self-consistent light-matter coupling is shown to contribute significantly to the THz response.
Intense, few-cycle pulses in the terahertz frequency range have strong potential for schemes of control over vibrational modes in solid-state materials in the electronic ground-state. Here we report an experiment using single cycle terahertz pulses to directly excite lattice vibrations in the ferroelectric material $\mathrm{Sn_2P_2S_6}$ and ultrafast x-ray diffraction to quantify the resulting structural dynamics. A model of a damped harmonic oscillator driven by the transient electric field of the terahertz pulses describes well the movement of the Sn$^{2+}$ ion along the ferroelectric soft m…
Optical rectification is demonstrated in (110)-cut ZnGeP_2 (ZGP) providing broadband terahertz (THz) generation. The source is compared to both GaP and GaAs over a wavelength range of 1150 nm to 1600 nm and peak intensity range of 0.5 GW/cm^2 to 40 GW/cm^2. ZGP peak-to-peak field amplitude is larger than in the other materials due to either lower nonlinear absorption or larger second order nonlinearity. This material is well suited for broadband THz generation across a wide range of infrared excitation wavelengths.
Terahertz (THz) radiation has been observed from multiferroic BiFeO$_3$ thin films via ultrafast modulation of spontaneous polarization upon carrier excitation with illumination of femtosecond laser pulses. The radiated THz pulses from BiFeO$_3$ thin films were clarified to directly reflect the spontaneous polarization state, giving rise to a memory effect in a unique style and enabling THz radiation even at zero-bias electric field. On the basis of our findings, we demonstrate potential approaches to ferroelectric nonvolatile random access memory with nondestructive readability and ferroelect…
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…
The carrier dynamics of photoexcited electrons in the vicinity of the surface of (NH4)2S-passivated GaAs were studied via terahertz (THz) emission spectroscopy and optical-pump THz-probe spectroscopy. THz emission spectroscopy measurements, coupled with Monte Carlo simulations of THz emission, revealed that the surface electric field of GaAs reverses after passivation. The conductivity of photoexcited electrons was determined via optical-pump THz-probe spectroscopy, and was found to double after passivation. These experiments demonstrate that passivation significantly reduces the surface state…
We investigate the dynamical formation of excitons from photoexcited electron-hole plasma and its subsequent decay dynamics in monolayer MoS2 grown by chemical vapor deposition using ultrafast pump and terahertz probe spectroscopy. Different photoexcited electron-hole states are resolved based on their distinct responses to THz photon and decay lifetime. The observed transient THz transmission can be fit with two decay components: a fast component with decay lifetime of 20 ps, which is attributed to exciton life time including the exciton formation and subsequent intraexciton relaxation; a slo…
Novel mechanisms for electromagnetic wave emission in the terahertz (THz) frequency regime emerging at the nanometer scale have recently attracted intense attention for the purpose of searching next-generation broadband THz emitters. Here, we report a new mechanism for broadband THz emission, utilizing the interface inverse Rashba-Edelstein effect. By engineering the symmetry of the Ag/Bi Rashba interface, we demonstrate a controllable THz radiation (~0.1-5 THz) waveform emitted from metallic Fe/Ag/Bi heterostructures following photo-excitation. We further reveal that this type of THz radiatio…
Measuring terahertz (THz) conductivity on an ultrafast time scale is an excellent way to observe charge-carrier dynamics in semiconductors as a function of time after photoexcitation. However, a conductivity measurement alone cannot separate the effects of charge-carrier recombination from effective mass changes as charges cool and experience different regions of the electronic band structure. Here we present a form of time-resolved magneto-THz spectroscopy which allows us to measure cyclotron effective mass on a picosecond time scale. We demonstrate this technique by observing electron coolin…
Methylammonium lead iodide (MAPI) is a benchmark hybrid organic perovskite material, which is used for the low-cost, printed solar cells with over 20 percent power conversion efficiency. Yet, the nature of light-matter interaction in MAPI as well as the exact physical mechanism behind device operation is currently debated. Here we report room temperature, ultrafast photocurrent and freespace terahertz (THz) emission generation from unbiased MAPI induced by 150 fs light pulses. Polarization dependence of the observed photoresponse is consistent with the Bulk Photovoltaic Effect (BPVE) caused by…
We study the broadband optical conductivity and ultrafast carrier dynamics of epitaxial graphene in the few-layer limit. Equilibrium spectra of nominally buffer, monolayer, and multilayer graphene exhibit significant terahertz and near-infrared absorption, consistent with a model of intra- and interband transitions in a dense Dirac electron plasma. Non-equilibrium terahertz transmission changes after photoexcitation are shown to be dominated by excess hole carriers, with a 1.2-ps mono-exponential decay that reflects the minority-carrier recombination time.
In this article, we reconnoiter the differential reflection signal of a Bi2Se3 single crystal flake, using ultrafast transient absorption spectroscopy in the femtosecond time domain and thereby explore the experimental data in terms of terahertz frequency generated in the sample. An exfoliated flake of a well characterized self-flux grown bulk Bi2Se3 single crystal having rhombohedral structure and layered morphology is used in the present study. The kinetic profile of the same being generated through a reflection signal by a pump laser of 650 nm at an average power of 0.5 mW is studied utiliz…
We are reporting on terahertz generation from organic crystal BNA using a 1.15 to 1.55 um near infrared pump. We observed a very large emission spectrum extending up to 7 THz, compared to 2.5 THz from Ti:Sa pump in previous reports. The maximum optical-to-THz conversion efficiency in our experiment was 0.8% at 1 kHz repetition rate and without saturation leading to a peak electric field of 1 GV/m. Our results show pronounced phase matching privilege for intense terahertz generation using a pump in the 1.15 to 1.25 um range where high energy near infrared pump sources operate.
We report a study of the complex AC impedance of CVD grown graphene. We measure the explicit frequency dependence of the complex impedance and conductance over the microwave and terahertz range of frequencies using our recently developed broadband microwave Corbino and time domain terahertz spectrometers (TDTS). We demonstrate how one may resolve a number of technical difficulties in measuring the intrinsic impedance of the graphene layer that this frequency range presents, such as distinguishing contributions to the impedance from the substrate. From our microwave measurements, the AC impedan…
Spintronic terahertz emitters are novel, broadband and efficient sources of terahertz radiation, which emerged at the intersection of ultrafast spintronics and terahertz photonics. They are based on efficient spin-current generation, spin-to-charge-current and current-to-field conversion at terahertz rates. In this review, we address the recent developments and applications, the current understanding of the physical processes as well as the future challenges and perspectives of broadband spintronic terahertz emitters.
Tin iodide phosphide (SnIP), an inorganic double-helix material, is a quasi-1D van der Waals semiconductor that shows promise in photocatalysis and flexible electronics. However, our understanding of the fundamental photophysics and charge transport dynamics of this new material is limited. Here, we use time-resolved terahertz (THz) spectroscopy to probe the transient photoconductivity of SnIP nanowire films and, with insight into the highly anisotropic electronic structure from quantum chemical calculations, measure an electron mobility as high as 280 $cm^2V^{-1}s^{-1}$. Additionally, the THz…
Here we show how time-resolved broadband optical spectroscopy can be used to quantify, with femtometer resolution, the oscillation amplitudes of coherent phonons through a displacive model without free tuning parameters, except an overall scaling factor determined by comparison between experimental data and density functional theory calculations. $WTe_2$ is used to benchmark this approach. In this semimetal, the response is anisotropic and provides the spectral fingerprints of two $A_1$ optical phonons at $\sim$8 and $\sim$80 $cm^-$$^1$. In principle, this methodology can be extended to any ma…
Spin-to-charge conversion (SCC) involving topological surface states (TSS) is one of the most promising routes for highly efficient spintronic devices for terahertz (THz) emission. Here, the THz generation generally occurs mainly via SCC consisting in efficient dynamical spin injection into spin-locked TSS. In this work, we demonstrate sizable THz emission from a nanometric thick topological insultator (TI)/ferromagnetic junction - SnBi$_2$Te$_4$/Co - specifically designed to avoid bulk band crossing with the TSS at the Fermi level, unlike its parent material Bi$_2$Te$_3$. THz emission time do…
Carbon nanomaterials such as carbon nanotubes and graphene have proved to be efficient building blocks for active optoelectronic devices. Especially, the exotic properties of crystalline graphene, such as a linear/gapless energy dispersion, offer a generic route to the development of active photonic modulator at the infrared (IR) and terahertz (THz) regime with large modulation depth. Here, we show that graphene oxide (GO), an oxygenated derivative of graphene with randomly distributed molecular defects (e.g., adsorbed water molecules and punched holes), can provide a different way to effectiv…
The recent discovery of topology-protected charge transport of ultimate thinness on surfaces of three-dimensional topological insulators (TIs) are breaking new ground in fundamental quantum science and transformative technology. Yet a challenge remains on how to isolate and disentangle helical spin transport on the surface from bulk conduction. Here we show that selective midinfrared femtosecond photoexcitation of exclusive intraband electronic transitions at low temperature underpins topological enhancement of terahertz (THz) surface transport in doped Bi2Se3, with no complication from interb…
The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here we apply sub-picosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO$_3$ ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large amplitude displacements of the titanium…
Topologically-protected surface states present rich physics and promising spintronic, optoelectronic and photonic applications that require a proper understanding of their ultrafast carrier dynamics. Here, we investigate these dynamics in topological insulators (TIs) of the bismuth and antimony chalcogenide family, where we isolate the response of Dirac fermions at the surface from the response of bulk carriers by combining photoexcitation with below-bandgap terahertz (THz) photons with TI samples with varying Fermi level, including one sample with the Fermi level located within the bandgap. W…
The electromagnetic response of Dirac semimetals in the infrared and terahertz frequency ranges is attracting growing interest for potential applications in optoelectronics and nonlinear optics. The interplay between the free-carrier response and interband transitions in the gapless, linear dispersion relation plays a key role in enabling novel functionalities. Here we investigate ultrafast dynamics in thin films of a photoexcited Dirac semimetal Cd$_3$As$_2$ by probing the broadband response functions as complex quantities in the multiterahertz region (10-45 THz, 40-180 meV, or 7-30 $μ$m), wh…
Light-matter interactions are key in providing fundamental information about materials. Even in the linear-response regime, the spectroscopic response of a material encodes in it many properties of the ground state as well as of its excitations. This knowledge has been critical in our understanding of novel quantum materials, and the further improvement and extensions of linear spectroscopy will continue to be key in the exploration of novel states of matter. We report the development of broadband circular polarization spectroscopy in the terahertz range of the electromagnetic spectrum. We tak…
We report the low-energy electrodynamics of a moderately clean A15 superconductor (SC) following ultrafast excitation to understand and manipulate terahertz (THz) quasi--particle (QP) transport by tuning pump photoexcitation of from competing orders. Using 35-fs optical pulses, we observe a non-thermal enhancement in the low frequency conductivity, opposite to that observed for THz pump, which persists up to an additional critical temperature, above the SC one, from an electronic order in the Martensitic normal state. In the SC state, the fluence dependence of pair breaking kinetics together w…
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 …
"Hidden phases" are metastable collective states of matter that are typically not accessible on equilibrium phase diagrams. These phases can host exotic properties in otherwise conventional materials and hence may enable novel functionality and applications, but their discovery and access are still in early stages. Using intense terahertz electric field excitation, we show that an ultrafast phase transition into a hidden ferroelectric phase can be dynamically induced in the quantum paraelectric SrTiO$_3$. The induced lowering in crystal symmetry yields dramatic changes in the phonon excitation…
This review discusses the ultrafast magnetization dynamics within the gigahertz to terahertz frequency range in ferrimagnetic rare-earth iron garnets with different substitutions. In these garnets, the roles of spin-orbit and exchange interactions have been detected using femtosecond laser pulses via the inverse Faraday effect. The all-optical control of spin-wave and Kaplan-Kittel exchange resonance modes in different frequency ranges is shown. Generation and localization of the electric field distribution inside the garnet through the metal-bound surface plasmon-polariton strongly enhance th…
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 …
Ultrafast broadband transient reflectivity experiments are performed to study the interplay between the non-equilibrium dynamics of the pseudogap and the superconducting phases in Bi$_{2}$Sr$_{2}$Ca$_{0.92}$Y$_{0.08}$Cu$_{2}$O$_{8+δ}$. Once superconductivity is established the relaxation of the pseudogap proceeds $\sim$ 2 times faster than in the normal state, and the corresponding transient reflectivity variation changes sign after $\sim$ 0.5 ps. The results can be described by a set of coupled differential equations for the pseudogap and for the superconducting order parameter. The sign and …
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 …
The availability of high-frequency pulsed emitters in the $2-2.5\,μ$m wavelength range paved the way for a wealth of new applications in ultrafast spectroscopy, free-space and fiber-optical communications, surveillance and recognition, artificial intelligence, and medical imaging. However, developing these emerging technologies and their large-scale use depend on the availability of high-speed, low-noise, and cost-effective photodetectors. With this perspective, here we demonstrate GeSn photodiodes grown on silicon wafers featuring a high broadband operation covering the extended-SWIR range wi…
