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 anisotropic distribution of photoexcited carriers in the $k_x-k_y$ plane. The collision integral in the Boltzmann equation includes a term that leads to the \textit{thermalization} of carriers via carrier-carrier scattering to an effective temperature above the lattice temperature, as well as a \textit{cooling} term which leads to energy relaxation via inelastic carrier-phonon scattering. The radiated signal is proportional to the time derivative of the transient current density. In spite of the fact that the magnitude of the velocity is the same for all the carriers in graphene, there is still emitted radiation from the photoexcited charge carriers with frequency components in the THz range due to a change in the \textit{direction} of velocity of the photoexcited carriers in the external electric field as well as \textit{cooling} of the photoexcited carriers on a sub-picosecond time scale.
We theoretically study the population inversion and negative dynamic conductivity in intrinsic graphene in the terahertz (THz) frequency range upon pulse photoexcitation with near-/mid-infrared wavelength. The threshold pulse energy required for the population inversion and negative dynamic conductivity can be orders-of-magnitude lower when the pulse photon energy is lower, due to the inverse proportionality of the photoexcited carrier concentration to the pulse photon energy and to the weaker carrier heating. We also investigate the dependence of the dynamic conductivity on the momentum relax…
We theoretically investigate the ultrafast terahertz(THz) properties of monolayer graphene. The analytical formulations of the photon carrier, electric polarization and optical current are obtained by solving the Bloch-equations in present of the ultrafast THz Gaussian pulse. Graphene shows a large nonlinear and ultrafast optical response at THz frequencies due to the gapless and relativistic Dirac particles with nearly linear energy dispersion. It is found that the photon carrier density, electric polarization and optical current density increase with increasing the frequency of the THz pulse…
We have measured the ultrafast anisotropic optical response of highly doped graphene to an intense single cycle terahertz pulse. The time profile of the terahertz-induced anisotropy signal at 800 nm has minima and maxima repeating those of the pump terahertz electric field modulus. It grows with increasing carrier density and demonstrates a specific nonlinear dependence on the electric field strength. To describe the signal, we have developed a theoretical model that is based on the energy and momentum balance equations and takes into account optical phonons of graphene and substrate. Accordin…
Laser-induced terahertz spin transport (TST) and ultrafast demagnetization (UDM) are central but so far disconnected phenomena in femtomagnetism and terahertz spintronics. Here, we use broadband terahertz emission spectroscopy to reliably measure both processes in one setup. We find that the rate of UDM of a single ferromagnetic metal film F has the same time evolution as the flux of TST from F into an adjacent normal-metal layer N. This remarkable agreement shows that UDM and TST are driven by the same force, which is fully determined by the state of the ferromagnet. An analytical model consi…
Through the integration of semiconductors or complex oxides into metal resonators, tunable metamaterials have been achieved by a change of environment using an external stimulus. Metals provide high conductivity to realize a strong resonant response in metamaterials; however, they contribute very little to the tunability. The complex conductivity in high-temperature superconducting films is highly sensitive to external perturbations, which provides new opportunities in achieving tunable metamaterials resulting directly from the resonant elements. Here we demonstrate ultrafast dynamical tuning …
Black phosphorus has recently emerged as a promising material for high performance electronic and optoelectronic device for its high mobility, tunable mid-infrared bandgap and anisotropic electronic properties. Dynamical evolution of photo excited carriers and its induced change of transient electronic properties are critical for materials' high field performance, but remains to be explored for black phosphorus. In this work, we perform angle resolved transient reflection spectroscopy to study the dynamical evolution of anisotropic properties of black phosphorus under photo excitation. We find…
Ultrafast optical pump-probe spectroscopy measurement on monolayer graphene observes significant optical nonlinearities. We show that strongly photoexcited graphene monolayers with 35 fs pulses quasi-instantaneously build up a broadband, inverted Dirac fermion population. Optical gain emerges and directly manifests itself via a negative conductivity at the near-infrared region for the first 200fs, where stimulated emission completely compensates absorption loss in the graphene layer. To quantitatively investigate this transient, extremely dense photoexcited Dirac-fermion state, we construct a …
Electric control of magnetic vortex dynamics in a reproducible way and on an ultrafast time scale is key element in the quest for efficient spintronic devices with low-energy consumption. To be useful the control scheme should ideally be swift, scalable, non-invasive, and resulting in reliable magnetic switching. Such requirements and in particular the reproducibility of altering the vortex chirality and/or polarity are not yet met by magnetic vortex switching via external magnetic fields, spin-polarized currents, spin waves, or laser pulses. Here we demonstrate a novel packaged-skyrmion media…
We present a detailed investigation of ultrafast (subpicosecond) exciton dynamics in the lattice model of a donor/acceptor heterojunction. Exciton generation by means of a photoexcitation, exciton dissociation, and further charge separation are treated on equal footing. The experimentally observed presence of space-separated charges at $\lesssim 100$ fs after the photoexcitation is usually attributed to ultrafast transitions from excitons in the donor to charge transfer and charge separated states. Here, we show, however, that the space-separated charges appearing on $\lesssim 100$-fs time sca…
Upon the discovery of the superatom states in endohedral metallofullerenes (EMFs), the superatom properties have become attractive, because ultrafast motion of the trapped atom modifies the charge distribution in the fullerene cage. However, the observation of ultrafast atom motion in the fullerene cage is very challenging, since dynamical processes take place in the terahertz (THz) frequency range in a picometer region. Here, we report on the THz spectroscopy of single Ce@C82 EMF molecules by using the single molecule transistor geometry. Due to the vibron-assisted tunneling process, two broa…
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…
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…
Probing topological Floquet states in graphene with ultrafast terahertz scanning tunneling microscopy
University of Bremen（不来梅大学）；Max Planck Institute for the Structure and Dynamics of Matter（马普物质结构与动力学研究所）；Paul Scherrer Institute（保罗谢尔研究所）；University of Fribourg（弗里堡大学）；The Flatiron Institute（_flatiron研究所）；Fritz Haber Institute of the Max Planck Society（马克斯·普朗克学会弗里茨·哈伯研究所）
Recent advances in the growth of III-V semiconductor nanowires (NWs) hold great promise for nanoscale optoelectronic device applications. Recently, it was found that a small amount of nitrogen (N) incorporation in III-V semiconductor NWs can effectively red-shift their wavelength of operation and tailor their electronic properties for specific applications. However, understanding the impact of N incorporation on non-equilibrium charge carrier dynamics and transport in semiconducting NWs is critical in achieving efficient semiconducting NW devices. In this work, ultrafast optical pump-terahertz…
We investigate the role of polarization-photon coupling (specifically, polarization-oscillation-induced radiation electric field) in the excitation of ferroelectric thin films by an ultrafast terahertz (THz) electric-field pulse. Analytical theory is developed to predict how the frequencies and relaxation time of three-dimensional soft mode phonons (intrinsic polarization oscillation) are modulated by radiation electric field and epitaxial strain. Ultrafast THz-pulse-driven excitation of harmonic polarization oscillation in strained single-domain ferroelectric thin film is then simulated using…
We use optical pump--THz probe spectroscopy at low temperatures to study the hot carrier response in thin Bi$_2$Se$_3$ films of several thicknesses, allowing us to separate the bulk from the surface transient response. We find that for thinner films the photoexcitation changes the transport scattering rate and reduces the THz conductivity, which relaxes within 10 picoseconds (ps). For thicker films, the conductivity increases upon photoexcitation and scales with increasing both the film thickness and the optical fluence, with a decay time of approximately 5 ps as well as a much higher scatteri…
We investigate the non-linear response and energy absorption in bulk silicon irradiated by intense 12-fs near-infrared laser pulses. Depending on the laser intensity, we distinguish two regimes of non-linear absorption of the laser energy: for low intensities, energy deposition and photoionization involve perturbative three-photon transition through the direct bandgap of silicon. For laser intensities near and above 10$^{14}$ W/cm$^2$, corresponding to photocarrier density of order 10$^{22}$ cm$^{-3}$, we find that absorption at near-infrared wavelengths is greatly enhanced due to excitation o…
The highly efficient, easy-to-implement, long-ranged and non-destructive way to realize active pumping has been still a great challenge. Here, using molecular dynamics simulations, terahertz electromagnetic wave (TEW) is firstly employed to stimulate an active pump for water transportation by biasedly irradiated in a (6,6) single-walled carbon nanotube (SWCNT) under no external pressure gradient. It is found that an ultrafast conductivity (up to 9.5 /ns) through the pump around a characteristic frequency of 14 THz. The excellent pumping ability is attributed to the resonance coupling between t…
In a semiconductor illuminated by a strong terahertz field, optically excited electron-hole pairs can recombine to emit light in a broad frequency comb evenly spaced by twice the terahertz frequency. Such high-order terahertz sideband generation is of interest both as an example of extreme nonlinear optics and also as a method for ultrafast electro-optical modulation. So far, this phenomenon has only been observed with large field strengths (~10 kVcm-1), an obstacle for technological applications. Here we predict that bi-layer graphene generates high-order sidebands at much weaker terahertz fi…
Terahertz (THz) Faraday rotation measurements were performed to investigate carrier dynamics in p-type CVD graphene. We used static and time-resolved polarization-sensitive THz transmission measurements in a magnetic field to probe free carriers in GaAs, InP and Graphene. Static measurements probe the equilibrium carrier density and momentum scattering rate. Time-resolved (optical pump/THz probe) measurements probe the change in these quantities following photoexcitation. In a typical CVD graphene sample we found that 0.5ps following photoexcitation with 1*10^13 photons/cm2 pulses at 800nm the…
We analyze ultrafast tunneling experiments in which electron transport through a localized orbital is induced by a single cycle THz pulse. We include both electron-electron and electron-phonon interactions on the localized orbital using the Anderson-Holstein model and consider two possible filling factors, the singly occupied Kondo regime and the doubly occupied regime relevant to recent experiments with a pentacene molecule. Our analysis is based on variational non-Gaussian states and provides the accurate description of the degrees of freedom at very different energies, from the high microsc…
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$6 meV. An analytical model reproduces the response which enables quantitative analysis of transient densities of dark excitons and {\em e-h} plasma, oscillator strength, transition energy renormalization and dynamics. %excitation-induced renormalization. Non-equilibrium, yet stable, quasi-1D quantum states with dark excitonic correlations rapidly emerge even with increasing off-resonan…
We investigated ultrafast carrier dynamics in graphene with near-infrared transient absorption measurement after intense half-cycle terahertz pulse excitation. The terahertz electric field efficiently drives the carriers, inducing large transparency in the near-infrared region. Theoretical calculations using the Boltzmann transport equation quantitatively reproduce the experimental findings. This good agreement suggests that the intense terahertz field should promote remarkable impact ioniza- tion process, which leads to suppression of optical phonon emission and results in efficient carrier t…
Dirac Fermion, which is the low energy collective excitation near the Dirac cone in monolayer graphene, have gained great attention by low energy Terahertz probe. In the case of undoped graphene, it has been generally understood that the ultrafast terahertz thermal relaxation is mostly driven by the electron-phonon coupling (EOP), which can be prolonged to tens and hundreds of picoseconds. However, for the high doped graphene, which manifests the negative photoinduced terahertz conductivity, there is still no consensus on the dominant aspects of the cooling process on a time scale of a few pic…
Terahertz spin waves could be generated on-demand via all-optical manipulation of magnetization by femtosecond laser pulse. Here, we present an energy balance model, which explains the energy transfer rates from laser pulse to electron bath coupled with phonon, spin, and magnetization of five different magnetic metallic thin films: Iron, Cobalt, Nickel, Gadolinium and Ni$_{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…
Collective vibrations of proteins, rotations of small molecules, excitations of high-temperature superconductors, and electronic transitions in semiconductor nanostructures occur with characteristic frequencies between 1 and 10 THz. Applications to medicine, communications, security and other fields are emerging. However, mapping the coldest parts of the universe has been the largest driver for developing THz detectors. The result is a family of exquisitely-sensitive detectors requiring sub-4K temperatures. For earthbound THz science and technology, sensitivity remains important but many appli…
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 diverse applications of terahertz radiation and its importance to fundamental science makes finding ways to generate, manipulate, and detect terahertz radiation one of the key areas of modern applied physics. One approach is to utilize carbon nanomaterials, in particular, single-wall carbon nanotubes and graphene. Their novel optical and electronic properties offer much promise to the field of terahertz science and technology. This article describes the past, current, and future of the terahertz science and technology of carbon nanotubes and graphene. We will review fundamental studies suc…
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 …
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…
In spin-based electronics, information is encoded by the spin state of electron bunches. Processing this information requires the controlled transport of spin angular momentum through a solid, preferably at frequencies reaching the so far unexplored terahertz (THz) regime. Here, we demonstrate, by experiment and theory, that the temporal shape of femtosecond spin-current bursts can be manipulated by using specifically designed magnetic heterostructures. A laser pulse is employed to drive spins from a ferromagnetic Fe thin film into a nonmagnetic cap layer that has either low (Ru) or high (Au) …
We present optically tunable magnetic 3D metamaterials at terahertz (THz) frequencies which exhibit a tuning range of ~30% of the resonance frequency. This is accomplished by fabricating 3D array structures consisting of double-split-ring resonators (DSRRs) on silicon-on-sapphire, fabricated using multilayer electroplating. Photoexcitation of free carriers in the silicon within the capacitive region of the DSRR results in a red-shift of the resonant frequency from 1.74 THz to 1.16 THz. The observed frequency shift leads to a transition from a magnetic-to-bianisotropic response as verified thro…
We have used a femtosecond pump-probe impulsive Raman technique to explore the ultrafast dynamics of micelle suspended single walled carbon nanotubes (SWNTs) in various pH environments. The structures of coherent phonon spectra of the radial breathing modes (RBMs) exhibit significant pH dependence, to which we attribute the effect of the protonation at the surface of SWNTs, resulting in the modification of electronic properties of semiconductor SWNTs. Analysis of the time-domain data using a time-frequency transformation uncovers also a second transient longitudinal breathing mode, which vanis…
We investigate the hot carrier dynamics of ZrTe$_5$ by ultrafast time-resolved optical reflectivity. Our results reveal a phonon-mediated across-gap recombination, consistent with its temperature-dependent gap nature as observed previously by photoemission. In addition, two distinct relaxations with a kink feature right after initial photoexcitation are well resolved, suggesting the complexity of electron thermalization process. Our findings indicate that correlated many-body effects play important role for the transient dynamics of ZrTe$_5$.
Ultrafast and sensitive (noise equivalent power <1 nWHz-1/2) light-detection in the Terahertz (THz) frequency range (0.1-10 THz) and at room-temperature is key for applications such as time-resolved THz spectroscopy of gases, complex molecules and cold samples, imaging, metrology, ultra-high-speed data communications, coherent control of quantum systems, quantum optics and for capturing snapshots of ultrafast dynamics, in materials and devices, at the nanoscale. Here, we report room-temperature THz nano-receivers exploiting antenna-coupled graphene field effect transistors integrated with lith…
Solution-processable two-dimensional (2D) semiconductors with chemically tunable thickness and associated tunable band gaps are highly promising materials for ultrathin optoelectronics. Here, the properties of free charge carriers and excitons in 2D PbS nanosheets of different thickness are investigated by means of optical pump-terahertz probe spectroscopy. By analyzing the frequency-dependent THz response, a large quantum yield of excitons is found. The scattering time of free charge carriers increases with nanosheet thickness, which is ascribed to reduced effects of surface defects and ligan…
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…
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…
Oscillator-strength sum rule in light-induced transitions is one general form of quantum-mechanical identities. Although this sum rule is well established in equilibrium photo-physics, an experimental corroboration for the validation of the sum rule in a nonequilibrium regime has been a long-standing unexplored question. The simple band structure of graphene is an ideal system for investigating this question due to the linear Dirac-like energy dispersion. Here, we employed both ultrafast terahertz and optical spectroscopy to directly monitor the transient oscillator-strength balancing between …
