We describe a unified numerical model which allows fast and accurate simulation of nonlinear light propagation in nanoparticle composites, including various effects such as group velocity dispersion, second- and third-order nonlinearity, quasi-free-carrier formation and plasma contribution, exciton dynamics, scattering and so on. The developed software package SOLPIC is made available for the community. Using this model, we analyze and optimize efficient generation of THz radiation by two-color pulses in ZnO/fused silica composite, predicting an efficiency of 3\%. We compare the role of various nonlinear effects contributing to the frequency conversion, and show that optimum conditions of THz generation differ from those expected intuitively.
Using the tilted-pulse-intensity-front scheme, we generate single-cycle terahertz (THz) pulses by optical rectification of femtosecond laser pulses in LiNbO3. In the THz generation setup, the condition that the image of the grating coincides with the tilted-optical-pulse front is fulfilled to obtain optimal THz beam characteristics and pump-to-THz conversion efficiency. The designed focusing geometry enables tight focus of the collimated THz beam with a spot size close to the diffraction limit, and the maximum THz electric field of 1.2 MV/cm is obtained.
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…
High-order harmonic generation in the presence of a chirped THz pulse is investigated numerically with a complete 3D non-adiabatic model. The assisting THz pulse illuminates the HHG gas cell laterally inducing quasi-phase-matching. We demonstrate that it is possible to compensate the phase mismatch during propagation and extend the macroscopic cutoff of a propagated strong IR pulse to the single-dipole cutoff. We obtain two orders of magnitude increase in the harmonic efficiency of cutoff harmonics ($\approx$170 eV) using a THz pulse of constant wavelength, and a further factor of 3 enhancemen…
In Terahertz (THz) technology, one of the long-standing challenges has been the formation of intense pulses covering the hard-to-access frequency range of 1-15 THz (so-called THz gap). This frequency band, lying between the electronically (<1 THz) and optically (>15 THz) accessible spectrum hosts a series of important collective modes and molecular fingerprints which cannot be fully accessed by present THz sources. While present high-energy THz sources are limited to 0.1-4 THz the accessibility to the entire THz gap with intense THz pulses would substantially broaden THz applications like live…
Transmission through photoexcited semiconductors is used to temporally and spectrally shape a Terahertz pulse. By adjusting the optical pump-THz probe delay, we experimentally introduce a polar asymmetry in the pulse profile as high as 92%. To shape the spectrum, we apply the same technique after strongly chirping the Terahertz pulse. This led to significant reshaping of the spectrum with a 52% upshift of spectrum median. Pulse shaping techniques introduced here are of particular importance for temporal and spectral shape-sensitive THz nonlinear experiments.
The main effects of an intense THz pulse on gas high harmonic generation are studied via trajectory analysis on the single atom level. Spectral and temporal modifications to the generated radiation are highlighted.
We report the synthesis of arbitrary optical waveforms by manipulating the spectral phases of Raman sidebands with a wide frequency spacing line-by-line. Trains of rectangular and triangular pulses are stably produced at an ultrahigh repetition rate of 10.6229 THz, reminiscent of an ultrafast function generator.
We present a study on THz generation in lithium niobate pumped by a powerful and versatile Yb:CaF2 laser. The unique laser system delivers transform-limited pulses of variable duration (0.38-0.65 ps) with pulse energy of up to 15 mJ at a center wavelength of 1030 nm. From theoretical investigations it is expected that those laser parameters are ideally suited for efficient THz generation. Here we present experimental results on both the conversion efficiency and the THz spectral shape for variable pump pulse durations and for different crystal temperatures down to 25 K. We experimentally verif…
The evolution of THz waveform generated in air plasma provides a sensitive probe to the variation of the carrier envelope phase (CEP) of propagating intense few-cycle pulses. Our experimental observation and calculation reveal that the number and positions of the inversion of THz waveform are dependent on the initial CEP, which is near 0.5π constantly under varied input pulse energies when two inversions of THz waveform in air plasma become one. This provides a method of measuring the initial CEP in an accuracy that is only limited by the stability of the driving few-cycle pulses.
We present a numerical parametric study of single-cycle electromagnetic pulse generation in a DAST/SiO2 multilayer structure via collinear optical rectification of 800 nm femtosecond laser pulses. It is shown that modifications of the thicknesses of the DAST and SiO2 layers allow tuning of the average frequency of the generated THz pulses in the frequency range from 3 to 6 THz. The laser-to-THz energy conversion efficiency in the proposed structures is compared with that in a bulk DAST crystal and a quasi-phase-matching periodically poled DAST crystal and shows significant enhancement.
Short mode-locked pulses from planarized Y-coupled THz lasers
Quantum Optoelectronics Group, Institute of Quantum Electronics, ETH Zürich（苏黎世联邦理工学院量子电子学研究所）；John A. Paulson School of Engineering and Applied Sciences, Harvard University（哈佛大学约翰·保尔森工程与应用科学学院）；Institute of Physics and Center for Quantum Science and Engineering, Ecole Polytechnique Fédérale de Lausanne（洛桑联邦理工学院物理系与量子科学与工程中心）；Istituto di Fotonica e Nanotecnologie, CNR（意大利国家研究委员会光子学与纳米技术研究所）
The effect of terahertz (THz) pulse generation has revolutionized broadband coherent spectroscopy and imaging at THz frequencies. However, THz pulses typically lack spatial structure, whereas structured beams are becoming essential for advanced spectroscopy applications. Non-linear optical metasurfaces with nanoscale THz emitters can provide a solution by defining the beam structure at the generation stage. We develop a non-linear InAs metasurface consisting of nanoscale optical resonators for simultaneous generation and structuring of THz beams. We find that THz pulse generation in the resona…
The speed of magnetization reversal is a key feature in magnetic data storage. Magnetic fields from intense THz pulses have been recently shown to induce small magnetization dynamics in Cobalt thin film on the sub-picosecond time scale. Here, we show that at higher field intensities, the THz electric field starts playing a role, strongly changing the dielectric properties of the cobalt thin film. Both the electronic and magnetic responses are found to occur simultaneously, with the electric field response persistent on a time scale orders of magnitude longer than the THz stimulus
The development of multiplexing information transmission technology in the THz band may accelerate the arrival of the 6G era. In this paper, has demonstrated the feasibility of forming a sequence of subpulses in the temporal domain and the corresponding quasidiscrete spectrum in the THz frequency range. It is shown that despite the fact that the THz pulse has an exponential chirp, there is a "linkage relation" between spectrum and temporal structures of the THz pulse train. This fact can be used for encoding information in THz pulses for implementation in 6G communication systems in the future…
We report fabrication method and THz characterization of composite films containing either aligned metallic (tin alloy) microwires or chalcogenide As2Se3 microwires. The microwire arrays are made by stack-and-draw fiber fabrication technique using multi-step co-drawing of low-melting-temperature metals or semiconductor glasses together with polymers. Fibers are then stacked together and pressed into composite films. Transmission through metamaterial films is studied in the whole THz range (0.1-20 THz) using a combination of FTIR and TDS. Metal containing metamaterials are found to have strong …
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 …
A model for THz generation by optical rectification using tilted-pulse-fronts is developed. It simultaneously accounts for (i) the spatio-temporal distortions of the optical pump pulse, (ii) the nonlinear coupled interaction of THz and optical radiation in two spatial dimensions (2-D), (iii) self-phase modulation and (iv) stimulated Raman scattering. The model is validated by quantitative agreement with experiments and analytic calculations. We show that the optical pump beam is significantly broadened in the transverse-momentum (kx) domain as a consequence of the spectral broadening caused by…
We report on the global temporal pulse characteristics of individual harmonics in an attosecond pulse train by means of photo-electron streaking in a strong low-frequency transient. The scheme allows direct retrieval of pulse durations and first order chirp of individual harmonics without the need of temporal scanning. The measurements were performed using an intense THz field generated by tilted phase front technique in LiNbO_3 . Pulse properties for harmonics of order 23, 25 and 27 show that the individual pulse durations and linear chirp are decreasing by the harmonic order.
We report optical parametric amplification (OPA) of low-frequency infrared pulses in the intermediate region between terahertz (THz) frequency and mid-infrared (MIR), i.e., from 16.9 to 44.8 THz. The 255-fs laser output of the Yb:KGW regenerative amplifier is compressed to 11-fs pulses using a multi-plate broadening scheme, which generates THz-to-MIR pulses with a spectrum extending to approximately 50 THz by intra-p1ulse differential frequency generation (DFG) in GaSe. The THz-to-MIR pulses are further amplified using a two-stage OPA in GaSe. The temporal dynamics and photocarrier effects dur…
Few-cycle THz Pulse Generation in DSTMS Crystal Pumped by a 8.3-MHz Amplified Mamyshev Oscillator
Istituto di Fotonica e Nanotecnologie, Consiglio Nazionale delle Ricerche（意大利国家研究委员会光子学与纳米技术研究所）；Dipartimento di Fisica, Politecnico di Milano（米兰理工大学物理系）；Dipartimento di Ingegneria Industriale e dell’Informazione, Università di Pavia（帕维亚大学工业与信息工程系）；Dipartimento di Fisica, Università degli Studi di Roma ”La Sapienza”（罗马第一大学物理系）；Istituto Nazionale di Fisica Nucleare, Sezione di Roma（意大利国家核物理研究所罗马分部）
Although the THz spectral range experiences a tremendous grow of interest for at least two decades, it is still one of the least explored but most exciting areas to study light-matter interaction. Due to the small photon energy of THz radiation, it can propagate through non-conductive materials and resonantly interact with low-energy excitations, leading to a plethora of applications. The THz pulse is thereby primarily used as a probe while an optical pulse excites the material that is examined. In contrast, intense strong-field THz transients would allow on-demand control of the properties of…
Terahertz (THz) generation by optical rectification (OR) using tilted-pulse-fronts is studied. One-dimensional (1-D) and 2-D spatial models, which simultaneously account for (i) the nonlinear coupled interaction of the THz and optical radiation, (ii) angular and material dispersion, (iii) absorption, iv) self-phase modulation and (v) stimulated Raman scattering are presented. We numerically show that the large experimentally observed cascaded frequency down-shift and spectral broadening (cascading effects) of the optical pump pulse is a direct consequence of THz generation. In the presence of …
Air turns into a nonlinear medium for electromagnetic waves under exceptionally strong fields. However up to present, its minuscule nonlinear response has limited the exploration to the optical frequency regime owing to the availability of intense near-infrared lasers. Here, we report on the observation of large-amplitude nonlinearity in air induced by an extremely intense light bullet at Terahertz frequencies (0.1-10 THz) provoking strong air birefringence. The observed nonlinearity manifests itself as third order susceptibility. The presented nonlinear observations break the barrier for the …
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, …
We theoretically and numerically study the influence of both instantaneous and Raman-delayed Kerr nonlinearities as well as a long-wavelength pump in the terahertz (THz) emissions produced by two-color femtosecond filaments in air. Although the Raman-delayed nonlinearity induced by air molecules weakens THz generation, four-wave mixing is found to impact the THz spectra accumulated upon propagation via self-, cross-phase modulations and self-steepening. Besides, using the local current theory, we show that the scaling of laser-to-THz conversion efficiency with the fundamental laser wavelength …
Pulsed terahertz (THz) radiation, generated through optical rectification (OR) by exciting [110] ZnTe crystal with ultrafast optical pulses, typically consists of only a few cycles of electromagnetic field oscillations with a duration about a couple of picoseconds. However, it is possible, under appropriate conditions, to generate a long damped oscillation tail (LDOT) following the main cycles. The LDOT can last tens of picoseconds and its Fourier transform shows a higher and narrower frequency peak than that of the main pulse. We have demonstrated that the generation of the LDOT depends on bo…
We present a novel method for THz generation in lithium niobate using a reflective stair-step echelon structure. The echelon produces a discretely tilted pulse front with less angular dispersion compared to a high groove-density grating. The THz output was characterized using both a 1-lens and 3-lens imaging system to set the tilt angle at room and cryogenic temperatures. Using broadband 800 nm pulses with a pulse energy of 0.95 mJ and a pulse duration of 70 fs (24 nm FWHM bandwidth, 39 fs transform limited width), we produced THz pulses with field strengths as high as 500 kV/cm and pulse ener…
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-…
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…
We present a comprehensive experimental and numerical study of photoelectron streaking at metallic nanotips using single-cycle Terahertz (THz) transients and a static bias voltage as an external control parameter. Analyzing bias voltage dependent streaking spectrograms, we explore the THz-induced reshaping of photoelectron energy spectra, governed by the superimposed static field. Numerical simulations are employed to determine the local field strengths and spatial decay lengths of the field contributions, demonstrating electron trajectory control and the manipulation of the phase space distri…
A whole class of two-color experiments involves intense, short Terahertz radiation pulses. A fast detector that is sensitive and able to resolve both near-infrared and Terahertz pulses at the same time is highly desirable. Here we present the first detector of this kind. The detector element is a GaAs-based field effect transistor operated at room temperature. THz detection is successfully demonstrated at frequencies up to 4.9 THz. The THz detection time constant is shorter than 30 ps, the optical time constant is 150 ps. This detector is ideally suited for precise, simultaneous resolution of …
Coherent control is an optical technique to manipulate quantum states of matter. The coherent control of 40-THz optical phonons in diamond was demonstrated by using a pair of sub-10-fs optical pulses. The optical phonons were detected via transient transmittance using a pump and probe protocol. The optical and phonon interferences were observed in the transient transmittance change and its behavior was well reproduced by quantum mechanical calculations with a simple model which consists of two electronic levels and shifted harmonic oscillators.
We experimentally investigate the limits to 800 nm-to-terahertz (THz) energy conversion in lithium niobate at room temperature driven by amplified Ti:Sapphire laser pulses with tilted-pulse-front. The influence of the pump central wavelength, pulse duration, and fluence on THz generation is studied. We achieved a high peak efficiency of 0.12% using transform limited 150 fs pulses and observed saturation of the optical to THz conversion efficiency at a fluence of 15 mJ/cm2. We experimentally identify two main limitations for the scaling of optical-to-THz conversion efficiencies: (i) the large s…
The generation of single-cycle attosecond pulses based on Thomson scattering of terahertz (THz) pulses is proposed. In the scheme, a high-quality relativistic electron beam produced by a laser-plasma wakefield accelerator (LPWA), is sent through suitable magnetic devices to produce ultrathin electron layers for coherent Thomson backscattering of intense THz pulses. According to numerical simulations, single-cycle attosecond pulse generation is possible with up to 1 nJ energy. The waveform of the attosecond pulses closely resembles that of the THz pulses. This allows for a flexible waveform con…
We theoretically study the generation of terahertz (THz) radiation by two-color filamentation of ultrashort laser pulses with different wavelengths. We consider wavelengths in the range from 0.6 to 10.6 $μ$m, thus covering the whole range of existing and future powerful laser sources in the near, mid and far-infrared. We show how different parameters of two-color filaments and generated THz pulses depend on the laser wavelength. We demonstrate that there is an optimal laser wavelength for two-color filamentation that provides the highest THz conversion efficiency and results in generation of e…
Femtosecond laser filament generates strong terahertz (THz) pulse in air. In this paper, THz pulse waveform generated by femtosecond laser filament has been experimentally investigated as a function of the length of the filament. Superluminal propagation of THz pulse has been uncovered, indicating that the filament creates a THz waveguide in air. Numerical simulation has confirmed that the waveguide is formed because of the radially non-uniform refractive index distribution inside the filament. The underlying physical mechanisms and the control techniques of this type THz pulse generation meth…
We report multicycle, narrowband, terahertz radiation at 14.8 THz produced by phase-matched optical rectification of femtosecond laser pulses in bulk lithium niobate (LiNbO$_3$) crystals. Our experiment and simulation show that the output terahertz energy greatly enhances when the input laser pulse is highly chirped, contrary to a common optical rectification process. We find this abnormal behavior is attributed to a linear electro-optic (or Pockels) effect, in which the laser pulse propagating in LiNbO$_3$ is modulated by the terahertz field it produces, and this in turn drives optical rectif…
A new type of tilted-pulse-front pumped terahertz (THz) source has been demonstrated, which is based on a lithium niobate plane-parallel slab with an echelon structure on its input surface. Single-cycle pulses of 1 microjoule energy and 0.30 THz central frequency have been generated with 0.05% efficiency from such a source. One order-of-magnitude increase in efficiency is expected by pumping a cryogenically cooled echelon of increased size and thickness with a Ti:sapphire laser. The use of a plane-parallel nonlinear optical crystal slab enables straightforward scaling to high THz pulse energie…
We demonstrate efficient multicycle terahertz pulse generation at 14.6 THz from large-area lithium niobate crystals by using high-energy (up to 2 J) femtosecond Ti:sapphire laser pulses. Such terahertz radiation is produced by phase-matched optical rectification in lithium niobate. Experimentally, we achieve maximal terahertz energy of 0.71 mJ with conversion efficiency of $\sim$0.04%. We also find that the effective interaction length for optimal terahertz conversion is fundamentally limited by terahertz absorption, laser pulse stretching by material dispersion, and terahertz-induced nonlinea…
Polymer compounds from titania-doped polyethylene are fabricated and their linear optical properties characterized by THz-TDS. We show that high concentration of dopants not only enhances the refractive index of the composite material, but also can dramatically raise its absorption coefficient. We demonstrate that the design of Bragg reflectors based on lossy composite polymers depends on finding a compromise between index contrast and corresponding losses. A small absorption value is also shown to be favorable, compared to an ideal lossless reflector, as it enables to smooth the transmission …
A composite plasmonic slab based on double-layer metallic gratings and a dielectric film is experimentally and numerically demonstrated in terahertz (THz) regions, which can support two resonance modes and then form a broad bandgap (40%). As compared to the double-layer metal grating, the dielectric film in composite THz slabs significantly enhances the transmission of the transverse magnetic (TM) mode. Electric field vector proved that the low-frequency resonance mode originates from the symmetric plasmonic mode and the high-frequency resonance mode is induced by the hybrid mode of plasmonic …
Applications ranging from nonlinear terahertz spectroscopy to remote sensing require broadband and intense THz radiation which can be generated by focusing two-color laser pulses into a gas. In this setup, THz radiation originates from the buildup of the electron density in sharp steps of attosecond duration due to tunnel ionization, and subsequent acceleration of free electrons in the laser field. We show that the spectral shape of the THz pulses generated by this mechanism is determined by superposition of contributions from individual ionization events. This provides a straightforward analo…
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…
We studied the effects of cryogenic cooling of a 2-[3-(4-hydroxystyryl)-5, 5-dimethylcyclohex-2-enylidene] malononitrile (OH1) crystal on the generation of broadband THz pulses via collinear optical rectification of 1350 nm femtosecond laser pulses. Cooling of the OH1 crystal from room temperature to 10 K leads to a ~10% increase of the pump-to-THz energy conversion efficiency and a shift of the THz pulse spectra to a higher frequency range. Both effects are due the temperature variation of THz absorption and the refractive index of the OH1 crystal. This conclusion has been verified by tempera…
Nanoscale pulsed light is highly desirable in nano-integrated optics. In this letter, we obtained femtosecond pulses with THz repetition frequency via the strong coupling between quantum emitters (QEs) and plasmonic resonators. Our structure consists of a V-groove (VG) plasmonic resonator and a nanowire embedded with two-level QEs. The influences of the incident light intensity and QE number density on the transmission response for this hybrid system are investigated through semi-classical theory and simulation. It is found that the transmission response can be modulated to the pulse form. The…
We obtained an optical-to-terahertz (THz) energy conversion efficiency of 0.5% using the tilted-pulse-front technique in lithium niobate at a cryogenically cooled temperature of 100 K pumped by amplified Ti:sapphire laser pulses with ~150 fs pulse duration at 800 nm wavelength. Compared with the optimized conversion efficiency of 0.18% achieved at room temperature, we achieved more than 2.5 times enhancement in conversion efficiency upon cryogenically cooling the crystal due to reduction of THz absorption. Further improvements to the conversion efficiency can be made by optimizing the out-coup…
We numerically investigate the use of strong THz radiation in assisting single attosecond pulse generation by few-cycle, 800 nm laser pulses. We optimize focusing conditions to generate short and powerful single attosecond pulses of high-energy photons by keeping the parameters of the THz field within the limits achieved experimentally. We show that using optimal focusing geometry isolated attosecond pulses shorter than 100 as can be obtained even in the absence of further gating or XUV compression techniques, using an 8 fs generating pulse. Furthermore, quantum path control of short- and long…
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.
Free-space super-strong terahertz (THz) electromagnetic fields offer multifaceted capabilities for reaching extreme nonlinear THz optics, accelerating and manipulating charged particles, and realizing other fascinating applications. However, the lack of powerful solid-state THz sources with single pulse energy >1 mJ is impeding the proliferation of extreme THz applications. The fundamental challenge lies in hard to achieve high efficiency due to high intensity pumping caused crystal damage, linear absorption and nonlinear distortion induced short effective interaction length, and so on. Here, …
Broadband THz spectroscopy system beyond 25 THz using BNA crystals and a tunable single-ring-fiber compressor
University of Ottawa（渥太华大学）；Max Planck Institute for the Science of Light（马克斯·普朗克光科学研究所）；University of Erlangen-Nürnberg（埃尔朗根-纽伦堡大学）；National Research Council Canada（加拿大国家研究委员会）
A new difference-frequency method based on electro-optic phase modulators and two free-running lasers is reported to perform THz dual-comb spectroscopy.
