The time-resolved detection of ultrashort pulsed THz-band electric field temporal profiles without an ultrashort laser probe is demonstrated. A non-linear interaction between a narrow-bandwidth optical probe and the THz pulse transposes the THz spectral intensity and phase information to the optical region, thereby generating an optical pulse whose temporal electric field envelope replicates the temporal profile of the real THz electric field. This optical envelope is characterised via an autocorrelation based FROG measurement, hence revealing the THz temporal profile. The combination of a narrow-bandwidth, long duration, optical probe and self-referenced FROG makes the technique inherently immune to timing jitter between the optical probe and THz pulse, and may find particular application where the THz field is not initially generated via ultrashort laser methods, such as the measurement of longitudinal electron bunch profiles in particle accelerators.
Most transmission and detection channels fail to faithfully support broadband wave packets because of physical limitations, like chromatic dispersion and absorption. We explore the case of lossy detection of ultrashort THz pulses using the widespread electro-optic detection scheme. We demonstrate that one can fully recover the original THz pulse shape, duration and amplitude, using a simple experimental procedure and a reconstruction algorithm which encodes the physical properties of the detection system.
Optical rectification of ultrashort laser pulses in LiNbO3 by tilted-pulse-front excitation is a powerful way to generate near single-cycle terahertz (THz) pulses. Motivated by various applications, calculations were carried out to optimize the THz peak electric field strength. The results predict THz output with peak electric field strength on the MV/cm level in the 0.3-1.5 THz frequency range by using optimal pump pulse duration of about 500 fs, optimal crystal length, and cryogenic temperatures for reducing THz absorption in LiNbO3. The THz electric field strength can be increased further t…
Recently, there has been growing interest in terahertz (THz) wave generation from liquids under optical excitation. Here, we propose and demonstrate the use of liquid lines in place of liquid films as THz emitters to boost THz signals. The geometry of the emitter eliminates the total internal reflection at the flat liquid-air interface. In addition, we observe that the polarity of the liquid has a significant influence on the THz wave generation. Alpha-pinene, a nonpolar liquid, offers much stronger THz radiation than water does. Besides paving the way to develop intense liquid THz sources, ou…
The tremendous applications of terahertz (THz) spectroscopy and imaging require THz sources in different parameters. We propose a novel scheme to generate single-cycle powerful THz pulses by ultrashort intense laser pulses incident obliquely on a tenuous plasma slab of few THz wavelengths in thickness. This is made possible by driving a large amplitude electron plasma wave in the plasma slab, thus producing a net transient current at the plasma surfaces. Theory and simulations show that such a THz source is capable of providing megawatt power and field strength of MV/cm, which may open up new …
Transient field-resolved spectroscopy enables studies of ultrafast dynamics in molecules, nanostructures, or solids with sub-cycle resolution, but previous work has so far concentrated on extracting the dielectric response at frequencies below 50\,THz. Here, we implemented transient field-resolved reflectometry at 50-100\,THz (3-6\,$μ$m) with MHz repetition rate employing 800\,nm few-cycle excitation pulses that provide sub-10\,fs temporal resolution. The capabilities of the technique are demonstrated in studies of ultrafast photorefractive changes in the semiconductors Ge and GaAs, where the …
By combining a tilted-pulse-intensity-front scheme using a LiNbO3 crystal and a chirped-pulse-beating method, we generated a narrowband intense terahertz (THz) pulse, which had a maximum electric field of more than 10 kV/cm at around 2 THz, a bandwidth of about 50 GHz,and frequency tunability from 0.5 to 2 THz. By performing THz-pump and near-infrared-probe experiments on GaAs quantum wells, we observed that the resonant excitation of the intraexcitonic 1s-2p transition induces a clear and large Autler-Townes splitting. Our time-resolved measurements show that the splitting energy observed in …
Nonlinear THz photonics is probably the last frontier of nonlinear optics. The strength of both the electric and the magnetic fields of these ultrashort low frequency light bunches opens the way to exciting science and applications. Progress in the field though is slow because of the deficiency in suitable sources. Here we show that two-color filamentation of mid-infrared 3.9 um laser pulses allows one to generate single cycle THz pulses with multi-millijoule energies and extreme conversion efficiencies. Moreover, the focused THz peak electric and magnetic fields reach values of GV/cm and kT, …
The intense terahertz (THz) pulses facilitate the observation of various nonlinear optical effects and manipulation of material properties. In this work, we report a convenient approach that can produce strong broadband terahertz pulses with center frequency tunable between 2-4 THz. The coherent THz light source with pulse energy of 1.2 microjoule can be generated from a low-cost crystalline quartz pumped by an ultrashort tilted wave-front pulse. Thanks to the wide transparent spectral window and high damage threshold, our theoretical analysis and experiment show that the optical rectification…
Fundamental interactions induced by lattice vibrations on ultrafast time scales become increasingly important for modern nanoscience and technology. Experimental access to the physical properties of acoustic phonons in the THz frequency range and over the entire Brillouin zone is crucial for understanding electric and thermal transport in solids and their compounds. Here, we report on the generation and nonlinear propagation of giant (1 percent) acoustic strain pulses in hybrid gold/cobalt bilayer structures probed with ultrafast surface plasmon interferometry. This new technique allows for un…
We developed THz-resonant scanning probe tips, yielding strongly enhanced and nanoscale confined THz near fields at their tip apex. The tips with length in the order of the THz wavelength (λ = 96.5 μm) were fabricated by focused ion beam (FIB) machining and attached to standard atomic force microscopy (AFM) cantilevers. Measurements of the near-field intensity at the very tip apex (25 nm radius) as a function of tip length, via graphene-based (thermoelectric) near-field detection, indicate their first and second order geometrical antenna resonances for tip length of 33 and 78 μm, respectively.…
Characterization of spatially inhomogeneous chirp in ultrashort multielectron beams via femtosecond hole burning
RIKEN Center for Advanced Photonics (RAP), RIKEN（理化学研究所先进光子学中心）；Department of Physics, Tokyo University of Science（东京科学大学物理系）；RIKEN Pioneering Research Institute (PRI), RIKEN（理化学研究所开创性研究本部）
Generation of few-cycle optical vortex pulses is challenging due to the large spectral bandwidths, as most vortex generation techniques are designed for monochromatic light. In this work, we use a spiral phase plate to generate few-cycle optical vortices from an ultrafast titanium:sapphire oscillator, and characterize them in the spatiotemporal domain using a recently introduced technique based on spatially resolved Fourier transform spectrometry. The performance of this simple approach to the generation of optical vortices is analyzed from a wavelength dependent perspective, as well as in the…
The active control of matter by strong electromagnetic fields is of growing importance, with applications all across the optical spectrum from the extreme-ultraviolet to the far-infrared. In recent years, phase-stable terahertz (THz) fields have shown tremendous potential in the observation and manipulation of elementary excitations in complex systems. The combination of concepts from attosecond science with advanced THz technology facilitates novel spectroscopic schemes, such as THz streaking. In general, driving charges at lower frequency enhances interaction energies and can promote drastic…
A wide range of ultrafast phenomena in various atomic, molecular and condense matter systems is governed by electron dynamics. Therefore, the ability to image electronic motion in real space and real time would provide a deeper understanding of such processes and guide developments of tools to control them. Ultrashort light pulses, which can provide unprecedented time resolution approaching subfemtosecond time scale, are perspective to achieve real-time imaging of electron dynamics. This task is challenging not only from an experimental view, but also from a theory perspective, since standard …
Quantum Cascade Lasers (QCL) constitute an intriguing opportunity for the production of on-chip optical Dissipative Kerr Solitons (DKS): self-organized optical waves which can travel while preserving their shape thanks to the interplay between Kerr effect and dispersion. Originally demonstrated in passive microresonators, DKS were recently observed in mid-IR ring QCL paving the way for their achievement even at longer wavelengths. To this end we realized defect-less THz ring QCLs featuring anomalous dispersion leveraging on a technological platform based on waveguide planarization. A concentri…
We introduce THz Stark spectroscopy by using intense single-cycle terahertz pulses as the electric field source and monitoring the induced spectral response of an isotropic molecular ensemble with a coincident femtosecond supercontinuum pulse. THz Stark spectroscopy offers several advantages over conventional Stark spectroscopy and opens previously inaccessible perspectives. Most importantly, THz pulses oscillate faster than typical molecular rotations and consequently eliminate the requirement to freeze the samples to prevent poling effects. Hence, THz Stark spectroscopy allows for time-resol…
Electro-optical sampling of Terahertz fields with ultrashort pulsed probes is a well-established approach for directly measuring the electric field of THz radiation. This technique usually relies on balanced detection to record the optical phase shift brought by THz-induced birefringence. The sensitivity of electro-optical sampling is, therefore, limited by the shot noise of the probe pulse, and improvements could be achieved using quantum metrology approaches using, e.g., NOON states for Heisenberg-limited phase estimation. We report on our experiments on THz electro-optical sampling using si…
We report a simple fiber-implemented technique for complete reconstruction of intensity profile and phase of ultrashort laser pulses based on processing only pulse spectrum and two self-phase modulated spectra measured after a short piece of optical fiber. Its applicability is shown on an example of a fiber optical system in the telecommunication range. A retrieval algorithm in a dispersionless approximation and with considering dispersion effects is developed. The obtained results are confirmed by independent measurements using the second-harmonic generation frequency-resolved optical gating …
There are implementations and proposals for using microwave or optical radiation for electron acceleration, undulation, deflection, and spatial as well as temporal focusing. Using terahertz (THz) radiation in such applications can be superior to microwave or optical radiation since THz pulses can be generated with significantly smaller temporal jitter to the electron bunch to be manipulated as compared to microwave pulses, and contrary to the optical pulses, the much larger wavelength of THz pulses compares well with typical sizes of electron bunches. Recently generation of ultrashort THz puls…
Broadband ultrashort terahertz (THz) pulses can be produced using plasma generation in a noble gas ionized by femtosecond two-color pulses. Here we demonstrate that, by using multiple-frequency laser pulses, one can obtain a waveform which optimizes the free electron trajectories in such a way that they reach the highest velocity at the electric field extrema. This allows to increase the THz conversion efficiency to the percent level, an unprecedented performance for THz generation in gases. Besides the analytical study of THz generation using a local current model, we perform comprehensive 3D…
We present a technique for the single-shot measurement of the space- and time-resolved spatiotemporal amplitude and phase of an ultrashort laser pulse. The method, transient-grating single-shot supercontinuum spectral interferometry (TG- SSSI), is demonstrated by the space-time imaging of short pulses carrying spatiotemporal optical vortices (STOVs). TG-SSSI is well-suited for characterizing ultrashort laser pulses that contain singularities associated with spin/orbital angular momentum or polarization.
We demonstrate that full temporal characterisation of few-cycle electromagnetic pulses, including retrieval of the carrier envelope phase (CEP), can be directly obtained from Frequency Resolved Optical Gating (FROG) techniques in which the interference between non-linear frequency mixing processes is resolved. We derive a framework for this scheme, defined Real Domain-FROG (ReD-FROG), as applied to the cases of interference between sum and difference frequency components and between fundamental and sum/difference frequency components. A successful numerical demonstration of ReD-FROG as applied…
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…
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 …
We theoretically study how time- and angle-resolved photoemission spectroscopy can be applied for imaging coherent electron dynamics in molecules. We consider a process in which a pump pulse triggers coherent electronic dynamics in a molecule by creating a valence electron hole. An ultrashort extreme ultraviolet (XUV) probe pulse creates a second electron hole in the molecule. Information about the electron dynamics is accessed by analyzing angular distributions of photoemission probabilities at a fixed photoelectron energy. We demonstrate that a rigorous theoretical analysis, which takes into…
We report a method to characterize the propagation of an ultrashort pulse of light through a multiple scattering medium by measuring its time-resolved transmission matrix. This method is based on the use of a spatial light modulator together with a coherent time-gated detection of the transmitted speckle field. Using this matrix, we demonstrate the focusing of the scattered pulse at any arbitrary position in space and time after the medium. Our approach opens new perspectives for both fundamental studies and applications in imaging and coherent control in disordered media.
Given the wide range of applications of time-domain spectroscopy, and particularly THz time-domain spectroscopy, the modelling of a probe pulse propagating through a multilayered structure is often required. Due to the fact that the multilayers are usually grown on a substrate much thicker than the other layers, the transmission of a probe pulse includes a series of echo pulses caused by the multiple reflections at the substrate interfaces. Experiments often measure the time profile and construct the transmitted spectrum only from the first transmitted pulse. Due to the fact that typical subst…
Imaging with ultrashort exposure times is generally achieved with a crossed-beam geometry. In the usual arrangement, an off-axis gating pulse induces birefringence in a medium exhibiting a strong Kerr response (commonly carbon disulfide) which is followed by a polarizer aligned to fully attenuate the on-axis imaging beam. By properly timing the gate pulse, imaging light experiences a polarization change allowing time-dependent transmission through the polarizer to form an ultrashort image. The crossed-beam system is effective in generating short gate times, however, signal transmission through…
All-Optical Field-Resolved Spectroscopy With Interferometric Nonlinear Cross-Correlations
Massachusetts Institute of Technology（麻省理工学院）；Deutsches Elektronen Synchrotron (DESY)（德国电子同步加速器）；Center for Free-Electron Laserscience (CFEL)（自由电子激光科学中心）
Coherent Raman scattering spectroscopy is studied purposely, with the Gaussian ultrashort pulses as a hands-on elucidatory extraction tool of the clean coherent Raman resonant spectra from the overall measured data contaminated with the non-resonant four wave mixing background. The integral formulae for both the coherent anti-Stokes and Stokes Raman scattering are given in the semiclassical picture, and the closed-form solutions in terms of a complex error function are obtained. An analytic form of maximum enhancement of pure coherent Raman spectra at threshold time delay depending on bandwidt…
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…
Manipulating the atomic and electronic structure of matter with strong terahertz (THz) fields while probing the response with ultrafast pulses at x-ray free electron lasers (FELs) has offered unique insights into a multitude of physical phenomena in solid state and atomic physics. Recent upgrades of x-ray FEL facilities are pushing to much higher repetition rates, enabling unprecedented signal to noise for pump probe experiments. This requires the development of suitable THz pump sources that are able to deliver intense pulses at compatible repetition rates. Here we present a high power laser-…
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 th…
Massachusetts Institute of Technology（麻省理工学院）；Georgia Institute of Technology（佐治亚理工学院）
Heavy sweep distortion induced by alignments and inter-reflections of layers of a sample is a major burden in recovering 2D and 3D information in time resolved spectral imaging. This problem cannot be addressed by conventional denoising and signal processing techniques as it heavily depends on the physics of the acquisition. Here we propose and implement an algorithmic framework based on low-rank matrix recovery and alternating minimization that exploits the forward model for THz acquisition. The method allows recovering the original signal in spite of the presence of temporal-spatial distorti…
We present a common pulse retrieval algorithm (COPRA) that can be used for a broad category of ultrashort laser pulse measurement schemes including frequency-resolved optical gating (FROG), interferometric FROG, dispersion scan, time domain ptychography, and pulse shaper assisted techniques such as multiphoton intrapulse interference phase scan (MIIPS). We demonstrate its properties in comprehensive numerical tests and show that it is fast, reliable and accurate in the presence of Gaussian noise. For FROG it outperforms retrieval algorithms based on generalized projections and ptychography. Fu…
We apply terahertz (THz) near-field streaking in a nanofocusing geometry to investigate plasmon polariton propagation on the shaft of a conical nanotip. By evaluating the delay between a streaking spectrogram for plasmon-induced photoemission with a measurement for direct apex excitation, we obtain an average plasmon group velocity, which is in agreement with numerical simulations. Combining plasmon-induced photoemission with THz near-field streaking facilitates extensive control over localized photoelectron sources for time-resolved imaging and diffraction.
In this research, we employ accurate time-dependent density functional calculations for ultrashort laser spectroscopy of nitrogen molecule. Laser pulses with different frequencies, intensities, and durations are applied to the molecule and the resulting photoelectron spectra are analyzed. It is argued that relative orientation of the molecule in the laser pulse significantly influence the orbital character of the emitted photoelectrons. Moreover, the duration of the laser pulse is also found to be very effective in controlling the orbital resolution and intensity of photoelectrons. Angular res…
Ultrashort electron beams with narrow energy spread, high charge, and low jitter are essential for resolving phase transitions in metals, semiconductors, and molecular crystals. These semirelativistic beams, produced by phototriggered electron guns, are also injected into accelerators for x-ray light sources. The achievable resolution of these time-resolved electron diffraction or x-ray experiments has been hindered by surface field and timing jitter limitations in conventional RF guns, which thus far are <200 MV/m and >96 fs, respectively. A gun driven by optically-generated single-cycle THz …
We demonstrate generation of 7.6 fs near-UV pulses centered at 400 nm via 8-fold soliton-effect self-compression in an Ar-filled hollow-core kagomé-style photonic crystal fiber with ultrathin core walls. Analytical calculations of the effective compression length and soliton order permit adjustment of the experimental parameters, and numerical modelling of the nonlinear pulse dynamics in the fiber accurately predict the spectro-temporal profiles of the self-compressed pulses. After compensation of phase distortion introduced by the optical elements along the beam path from the fiber to the dia…
We present a real-time THz imaging method using a commercial fiber coupled photo conductive antenna as the THz source and an uncooled microbolometer camera for detection. Compared to other THz imaging setups, this concept is very adaptable due to its compact and uncooled radiation source, whose fiber coupling allows for a flexible placement. Using a camera with high sensitivity renders real-time imaging possible. As a proof-of-concept, the beam shape of a THz Time Domain Spectrometer was measured. We also demonstrate the potential for practical applications in transmission geometry, covering m…
