Using a 3D fully-vectorial nonlinear time-domain analysis we numerically investigate the generation of terahertz radiation by pumping a photonic crystal microcavity out of resonance. High quality factors and a quadratic susceptibility lead to few-cycle terahertz pulses via optical rectification. Material dispersion as well as linear and nonlinear anisotropy is fully accounted for.
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…
We demonstrate high-energy terahertz generation from a large-aperture (75 mm diameter) lithium niobate wafer by using a femtosecond laser with energy up to 2 J. This scheme utilizes optical rectification in a bulk lithium niobate crystal, where most terahertz energy is emitted from a thin layer of the rear surface. Despite its simple setup, this scheme can yield 0.19 mJ of terahertz energy with laser-to-terahertz conversion efficiencies of ~0.01%, about 3 times better than ZnTe when pumped at 800 nm. The experimental setup is up-scalable for multi-mJ terahertz generation with petawatt laser pu…
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…
We propose a scheme for efficient cavity-enhanced nonlinear THz generation via difference-frequency generation (DFG) processes using a triply resonant system based on photonic crystal cavities. We show that high nonlinear overlap can be achieved by coupling a THz cavity to a doubly-resonant, dual-polarization near-infrared (e.g. telecom band) photonic-crystal nanobeam cavity, allowing the mixing of three mutually orthogonal fundamental cavity modes through a chi(2) nonlinearity. We demonstrate through coupled-mode theory that complete depletion of the pump frequency - i.e., quantum-limited con…
The angular dependence of terahertz (THz) emission from birefringent crystals can differ significantly from that of cubic crystals. Here we consider optical rectification in uniaxial birefringent materials, such as chalcopyrite crystals. The analysis is verified in (110)-cut ZnGeP_2 and compared to (zincblende) GaP. Although the crystals share the same nonzero second-order tensor elements, the birefringence in chalcopyrite crystals cause the pump pulse polarization to evolve as it propagates through the crystal, resulting in a drastically different angular dependence in chalcopyrite crystals. …
Using an affordable ytterbium laser with sub-mJ of energy combined with a novel pulse compression technique, we demonstrate an extremely competitive state-of-the-art terahertz (THz) source with 53 mW of average power and 310 kV/cm at focus from the tilted-pulse front pumping scheme in lithium niobate at room temperature. Key points of this demonstration include the use of a pump pulse duration of 280 fs in combination with an echelon mirror. Our results present unmatched combined characteristics and are highly competitive with the existing THz sources pumped at the mJ range. This demonstration…
Terahertz radiation by optical rectification has been observed at room temperature in a hydrogen-bonded organic molecular ferroelectric crystal, 2-phenyl malondialdehyde (PhMDA). The radiated electromagnetic wave consisted of a single-cycle terahertz pulse with a temporal width of $\sim$ 0.5 ps. The terahertz radiation amplitude divided by the sample thickness in PhMDA was nearly equivalent to that in a typical terahertz wave emitter ZnTe. This is attributable to a long coherence length in the range of 130 $\sim$ 800 $μ$m for the terahertz radiation from PhMDA. We also discussed the possibilit…
Using a canonical pump-probe experimental technique, we studied the terahertz (THz) waves generation and detection via optical rectification and mixing in Czochralski-grown periodically poled Mg:Y:LiNbO3 (PPLN) crystals. THz waves with frequencies at 1.37 THz and 0.68 THz as well as 1.8 THz were obtained for PPLN with nonlinear grating periods of 0.03 and 0.06 mm, respectively. A general theoretical model was developed by considering the dispersion and damping of low frequency phonon-polariton mode. Our results show that THz waves are generated in forward and backward directions via pumping pu…
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.
High energy terahertz pulses are produced by optical rectification (OR) in organic crystals DAST and DSTMS by a Ti:sapphire amplifier system centered at 0.8 microns. The simple scheme provides broadband spectra between 1 and 5 THz, when pumped by collimated 60 fs near-infrared pump pulse and it is scalable in energy. Fluence-dependent conversion efficiency and damage threshold are reported as well as optimized OR at visible wavelength.
A 2-D spatio-temporal analysis of terahertz generation by optical rectification of tilted-pulse-fronts is presented. Closed form expressions of terahertz transients and spectra in two spatial dimensions are furnished in the undepleted limit. Importantly, the analysis incorporates spatio-temporal distortions of the optical pump pulse such as angular dispersion, group-velocity dispersion due to angular dispersion, spatial and temporal chirp as well as beam curvature. The importance of the radius of curvature to the tilt-angle and group-velocity dispersion due to angular dispersion to terahertz f…
Bridging the "terahertz (THz) gap" relies upon synthesizing arbitrary waveforms in the THz domain enabling applications that require both narrow band sources for sensing and few-cycle drives for classical and quantum objects. However, realization of custom-tailored waveforms needed for these applications is currently hindered due to limited flexibility for optical rectification of femtosecond pulses in bulk crystals. Here, we experimentally demonstrate that thin-film lithium niobate (TFLN) circuits provide a versatile solution for such waveform synthesis through combining the merits of complex…
The nonlinear metamaterials have been shown to provide nonlinear properties with high nonlinear conversion efficiency and in a myriad of light manipulation. Here we study terahertz generation from nonlinear metasurface consisting of single layer nanoscale split-ring resonator array. The terahertz generation due to optical rectification by the second-order nonlinearity of the split-ring resonator is investigated by a time-domain implementation of the hydrodynamic model for electron dynamics in metal. The results show that the nonlinear metasurface enables us to generate broadband terahertz radi…
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…
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…
The ideal laser source for the emerging research field of nonlinear Terahertz (THz) spectroscopy should offer radiation with a large versatility and deliver both ultra-intense multi-octave spanning single-cycle pulses and user-selectable multi-cycle pulses at narrow linewidth. The absence of such a table-top source has hampered advances in numerous THz disciplines including imaging, nonlinear photonics and spectroscopy, selective out-of-equilibrium excitation of condensed matter and quantum systems. Here we introduce a highly versatile table-top THz laser platform providing single-cycle GV/m t…
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 …
Polar liquids are strong absorbers of electromagnetic waves in the terahertz range, therefore, historically such liquids have not been considered as good candidates for terahertz sources. However, flowing liquid medium has explicit advantages, such as a higher damage threshold compared to solid-state sources and more efficient ionization process compared to gases. Here we report systematic study of efficient generation of terahertz radiation in flat liquid jets under sub-picosecond single-color optical excitation. We demonstrate how medium parameters such as molecular density, ionization energ…
To achieve high efficiency and good performance of spintronic terahertz sources, we propose and corroborate a remnant magnetization method to radiate continuously and stably terahertz pulses from W/CoFeB/Pt magnetic nanofilms without carrying magnets on the transmitters driven by femtosecond laser pulses. We systematically investigate the influences of the pumping central wavelength and find out the optimal wavelength for a fixed sample thickness. We also optimize the incidence angle of the pumping laser and find the emission efficiency is enhanced under oblique incidence. Combing the aforemen…
Achieving efficient terahertz (THz) generation using compact turn-key sources operating at room temperature and modest power levels represents one of the critical challeges that must be overcome to realize truly practical applications based on THz. Up to now, the most efficient approaches to THz generation at room temperature -- relying mainly on optical rectification schemes -- require intricate phase-matching set-ups and powerful lasers. Here we show how the unique light-confining properties of triply-resonant photonic resonators can be tailored to enable dramatic enhancements of the convers…
Amplified bursts of laser pulses are sought for various machining, deposition, spectroscopic and strong-field applications. Standard frequency- and time-domain techniques for pulse division become inadequate when intraburst repetition rates reach the terahertz (THz) range as a consequence of inaccessible spectral resolution, requirement for interferometric stability, and collapse of the chirped pulse amplification (CPA) concept due to the loss of usable bandwidth needed for safe temporal stretching. Avoiding the burst amplification challenge and resorting to a lossy post-division of an isolate…
The sub-luminal phase velocity of electromagnetic waves in free space is generally unobtainable, being closely linked to forbidden faster than light group velocities. The requirement of effective sub-luminal phase-velocity in laser-driven particle acceleration schemes imposes a fundamental limit on the total acceleration achievable in free-space, and necessitates the use of dielectric structures and waveguides for extending the field-particle interaction. Here we demonstrate a new travelling-source and free space propagation approach to overcoming the sub-luminal propagation limits. The approa…
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…
Collinear phase-matched optical rectification is studied in ZnGeP$_{2}$ pumped with near-infrared light. The pump-intensity dependence is presented for three crystal lengths (0.3, 1.0 and 3.0 mm) to determine the effects of linear optical absorption, nonlinear optical absorption and terahertz free-carrier absorption on the generation. Critical parameters such as the coherence length (for velocity matching), dispersion length (for linear pulse broadening) and nonlinear length (for self-phase modulation) are determined for this material. These parameters provide insight into the upper limit of p…
The availability of few-cycle optical pulses opens a window to physical phenomena occurring on the attosecond time scale. In order to take full advantage of such pulses, it is crucial to measure and stabilise their carrier-envelope (CE) phase, i.e., the phase difference between the carrier wave and the envelope function. We introduce a novel approach to determine the CE phase by down-conversion of the laser light to the terahertz (THz) frequency range via plasma generation in ambient air, an isotropic medium where optical rectification (down-conversion) in the forward direction is only possibl…
We present designs of all-optical computing circuits, namely, half-full adder/subtractor, de-multiplexer, multiplexer, and an arithmetic unit, based on bacteriorhodopsin (BR) protein coated microcavity switch in a tree architecture. The basic all-optical switch consists of an input infrared (IR) laser beam at 1310 nm in a single mode fiber (SMF-28) switched by a control pulsed laser beam at 532 nm, which triggers the change in the resonance condition on a silica bead coated with BR between two tapered fibers. We show that fast switching of 50 us can be achieved by injecting a blue laser beam a…
Giant enhancement of terahertz high-harmonic generation by cavity engineering of a three-dimensional Dirac semimetal
TU Dortmund University（多特蒙德工业大学）；CNR-Istituto Nanoscienze（国家研究委员会纳米科学研究所）；Scuola Normale Superiore（比萨高等师范学院）；University of Basel（巴塞尔大学）；Fudan University（复旦大学）；Shanghai Research Center for Quantum Sciences（上海量子科学研究中心）；Beijing Academy of Quantum Information Sciences（北京量子信息科学研究院）
We report on high energy terahertz pulses by optical rectification (OR) in the organic crystal N-benzyl-2-methyl-4-nitroaniline (BNA) directly pumped by a conventional Ti:Sapphire (Ti:Sa) amplifier. The simple scheme provides an optical to terahertz conversion efficiency of 0.25% when pumped by a collimated laser pulses with duration of 50 fs and central wavelength of 800nm. The generated radiation spans frequencies between 0.2 and 3 THz. We measured the damage threshold as well as the dependency of the conversion efficiency on the pump fluence, pump wavelength, and pulse duration.
Nonlinear couplings between photons and electrons in new materials give rise to a wealth of interesting nonlinear phenomena. This includes frequency mixing, optical rectification or nonlinear current generation, which are of particular interest for generating radiation in spectral regions that are difficult to access, such as the terahertz gap. Owing to its specific linear dispersion and high electron mobility at room temperature, graphene is particularly attractive for realizing strong nonlinear effects. However, since graphene is a centrosymmetric material, second-order nonlinearities a prio…
We study the use of exciton-polaritons in semiconductor microcavities to generate radiation spanning the infrared to terahertz regions of the spectrum by exploiting transitions between upper and lower polariton branches. The process, which is analogous to difference-frequency generation (DFG), relies on the use of semiconductors with a nonvanishing second-order susceptibility. For an organic microcavity composed of a nonlinear optical polymer, we predict a DFG irradiance enhancement of $2.8\cdot10^2$, as compared to a bare nonlinear polymer film, when triple resonance with the fundamental cavi…
We refine the method towards extraction of sub-cycle transients in the 0.1-1 THz frequency (mm-wavelength) range from optical rectification in lithium niobate using tilted pulse fronts. Our scheme exploits previously unexplored spatio-temporal shaping of the pump pulses, resulting in highly efficient and near diffraction-limited sub-THz transients reaching 0.2 GV/m electric field strengths in free-space using only mJ-level optical ps-pulses. We address experimentally and theoretically the means to producing above-GV/m relativistic sub-THz transients with proper beam confinement and under moder…
Electromagnetic pulses with tilted pulse fronts are instrumental in enhancing the efficiency of many light-matter interaction processes, with prominent examples including terahertz generation by optical rectification, dielectric laser acceleration, ultrafast electron imaging and X-ray generation from free electron lasers. Here, we find closed-form expressions for tilted-pulse-front pulses that capture their exact propagation dynamics even in deeply nonparaxial and sub-single-cycle regimes. By studying the zero-bandwidth counterparts of these pulses, we further obtain classes of nondiffracting …
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…
Deriving single or few cycle terahertz pulse (THz) by intense femtosecond laser through cascaded optical rectification in electro-optic crystals is a crucial technique in cutting-edge time-resolved spectroscopy to characterize micro-scale structures and ultrafast dynamics. In the past decade, lithium niobate (LN) crystal implementation of wave-front tilt scheme has been prevalently used, while painstaking efforts have been invested in order to achieve higher THz conversion efficiency. In this research we developed a brand new type of LN crystal possessing dual-face-cut and Brewster coupling, a…
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-…
