It has been recently shown that the orbital angular momentum (OAM) and temporal degrees of freedom in ultrafast (few-cycle) vortices are coupled. This coupling manifests itself with different effects in different parts of the vortex, as has been shown for the ring surrounding the vortex where the pulse energy is maximum, and also in the immediate vicinity of the vortex center. In may applications, however, the ring of maximum energy is not of primary interest, but that where the pulse peak intensity is maximum, which is particularly true in nonlinear optics applications such as the experiments with ultrafast vortices exciting high harmonics and attosecond pulses carrying also OAM. This article describes the effects of the OAM-temporal coupling at the ring of maximum pulse peak intensity, which does not always coincide with the ring of maximum pulse energy. We find that there exists an upper bound to the magnitude of the topological charge that an ultrafast vortex with prescribed pulse shape at its most intense ring can carry, and vice versa, a lower bound to the duration of the pulse at the most intense ring for a given magnitude of the topological charge. These bounds imply that with a given laser source spectrum, the duration of the synthesized ultrafast vortex increases with the magnitude of the topological charge. Explicit analytical expressions of ultrafast vortices containing these OAM-temporal couplings are given that can be of interest in a variety of applications, particularly in the study of their propagation and interaction with matter.
We report on efficient nonlinear generation of ultrafast, higher order "perfect" vortices at the green wavelength. Based on Fourier transformation of the higher order Bessel-Gauss beam generated through the combination of spiral phase plate and axicon we have transformed the Gaussian beam of the ultrafast Yb-fiber laser at 1060 nm into perfect vortices of power 4.4 W and order up to 6. Using single-pass second harmonic generation (SHG) of such vortices in 5-mm long chirped MgO-doped, periodically poled congruent LiNbO$_3$ crystal we have generated perfect vortices at green wavelength with outp…
Ultrafast lasers ($< 500$ fs) have enabled laser-matter interactions at intensities exceeding $10^{18} \rm{Wcm}^{-2}$ with only millijoules of laser energy. However, as pulse durations become shorter, larger spectral bandwidths are required. Increasing the bandwidth causes the temporal structure to be increasingly sensitive to spectral phase, yet measuring the spectral phase of a laser pulse is nontrivial. While direct measurements of the spectral phase cannot be done using square-integrable detectors, phase information can be reconstructed by measuring the spectral response of a nonlinear opt…
In any form of wave propagation, strong spatiotemporal coupling appears when non-elementary, three-dimensional wave-packets are composed by superimposing pure plane waves, or spontaneously generated by light-matter interaction and nonlinear processes. Ultrashort pulses with orbital angular momentum (OAM), or ultrashort vortices, furnish a critical paradigm in which the analysis of the spatiotemporal coupling in the form of temporal-OAM coupling can be carried out accurately by analytical tools. By generalizing and unifying previously reported results, we show that universal and spatially heter…
We conduct a theoretical study of the propagation of few-cycle, ultrafast vortices (UFVs) carrying orbital angular momentum (OAM) in free space. Our analysis reveals much more complex temporal dynamics than that of few-cycle fundamental Gaussian-like beams, particularly when approaching the single-cycle regime and the magnitude of the topological charge $l$ is high. The recently described lower bound $\sqrt{|l|}$ to the number of oscillations of UFVs with propagation-invariant temporal shape (isodiffracting UFVs) is found to hold on average also for UFVs of general type, with variations along …
Optically generated electron-hole plasma in high-index dielectric nanostructures was demonstrated as a means of tuning of their optical properties. However, until now an ultrafast operation regime of such plasma driven nanostructures has not been attained. Here, we perform pump-probe experiments with resonant silicon nanoparticles and report on dense optical plasma generation near the magnetic dipole resonance with ultrafast (about 2.5 ps) relaxation rate. Basing on experimental results, we develop an analytical model describing transient response of a nanocrystalline silicon nanoparticle to a…
We introduce a simple and practical method to create ultrashort intense optical vortices for applications involving high-intensity lasers. Our method utilizes femtosecond laser pulses to laser-etch grating lines into laser-quality gold mirrors. These grating lines holographically encode an optical vortex. We derive mathematical equations for each individual grating line to be etched, for any desired (integer) topological charge. We investigate the smoothness of the etched grooves. We show that they are smooth enough to produce optical vortices with an intensity that is only a few percent lower…
Strongly-coupled quantum fields, such as multi-component atomic condensates, optical fields and polaritons, are remarkable systems where the simple dynamics of coupled oscillators can meet the intricate phenomenology of quantum fluids. When the coupling between the components is coherent, not only the particles number, but also their phase texture that maps the linear and angular momentum, can be exchanged. Here, on a system of exciton-polaritons, we have realized a so-called full-Bloch beam: a configuration in which all superpositions of the upper and the lower polariton -- all quantum states…
Carrier envelope phase (CEP) stabilized pulses of intense 800 nm light of 5 fs duration are used to probe the dissociation dynamics of dications of isotopically-substituted water, HOD. HOD$^{2+}$ dissociates into either H$^+$ + OD$^+$ or D$^+$ + OH$^+$. The branching ratio for these two channels is CEP-dependent; the OD$^+$/OH$^+$ ratio (relative to that measured with CEP-unstabilized pulses) varies from 150% to over 300% at different CEP values, opening prospects of isotope-dependent control over molecular bond breakage. The kinetic energy released as HOD$^{2+}$ Coulomb explodes is also CEP-d…
A scheme for generating intense high-harmonic optical vortices is proposed. It relies on spin-orbit interaction of light when a relativistically-strong circularly polarized laser pulse irradiates a micro-plasma-waveguide. The intense laser field drives a strong surface wave at the inner boundary of the waveguide, which leads to high-order harmonic generation as the laser traveling inside. For a circularly polarized drive laser, the optical chirality is imprinted to the surface wave, which facilitates conversion of spin angular momentum of the fundamental light into orbital angular momenta of t…
Recently, a spatiotemporal optical vortex (STOV) with a transverse orbital angular momentum (OAM) has been generated from coherent ultrafast pulses using mode-locked lasers. In contrast, we demonstrate theoretically and experimentally that a STOV can be generated from a light source with partial temporal coherence with fluctuating temporal phase. By eliminating the need of mode-locked laser sources, the partially coherent STOV will serve as a convenient and cost-effective transverse OAM source.
The spectrum of resonance fluorescence is calculated for a two-level system excited by an intense, ultrashort x-ray pulse made available for instance by free-electron lasers such as the Linac Coherent Light Source. We allow for inner-shell hole decay widths and destruction of the system by further photoionization. This two-level description is employed to model neon cations strongly driven by x rays tuned to the 1s 2p-1 --> 1s-1 2p transition at 848 eV; the x rays induce Rabi oscillations which are so fast that they compete with Ne 1s-hole decay. We predict resonance fluorescence spectra for t…
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…
Optical quadratic nonlinearity is ultrafast in nature, while parametric interaction usually manifests only the broadband characteristic. Enormous progress has been made toward broadband phase-matching for parametric amplification and wide applications. In existing devices of broadband parametric amplification, the power efficiency of conversion is restricted to approximately the energy efficiency, and the desire for the signal power enhancement necessitates additional pulse compression after amplification. Here, we demonstrate ultrafast parametric amplification having an extraordinary power ef…
We use an open-aperture Z-scan technique to show how intense few-cycle terahertz pulses can experience a nonlinear bleaching of absorption in an n-doped semiconductor due to terahertz-electric-field-driven intervalley scattering of electrons in the conduction band. Coherent detection of the transmitted terahertz pulse waveform also allows the nonlinear conductivity dynamics to be followed with sub-picosecond time resolution. Both the Z-scan and time-domain results are found to be in agreement with our theoretical analysis.
We report on the experimental evidence of magnetic helicoidal dichroism, observed in the interaction of an extreme ultraviolet vortex beam carrying orbital angular momentum with a magnetic vortex. Numerical simulations based on classical electromagnetic theory show that this dichroism is based on the interference of light modes with different orbital angular momenta, which are populated after the interaction between the light phase chirality and the magnetic topology. This observation gives insight into the interplay between orbital angular momentum and magnetism, and sets the framework for th…
The additional degree of freedom as introduced by the orbital angular momentum (OAM) of light has revolutionized the various technological applications. Optical pulses with OAM have applications in the generation of twisted attosecond pulses, ultrafast spectroscopy, telecommunication, high harmonic generation and in many other areas of physics as well. In this paper, we present a numerical investigation of the propagation dynamics of ultrashort Laguerre Gauss (LG) vortices using nonlinear envelope equation (NEE) in a dispersive and nonlinear medium. Asymmetric splitting of ultrashort LG vortic…
Infrared and visible light beams carrying orbital angular momentum (OAM) are currently thoroughly studied for their extremely broad applicative prospects, among which are quantum information, micromachining and diagnostic tools. Here we extend these prospects, presenting a comprehensive study for the synthesis and full characterization of optical vortices carrying OAM in the extreme ultraviolet (XUV) domain. We confirm the upconversion rules of a femtosecond infrared helically phased beam into its high-order harmonics, showing that each harmonic order carries the total number of OAM units abso…
We have demonstrated for the first time that an array of nanoantennas (central nanotips inside sub-micron pits) on an aluminum surface, fabricated using a specific double-pulse femtosecond laser irradiation scheme, results in a 28-fold enhancement of the non-linear (three-photon) electron photoemission yield, driven by a third intense IR femtosecond laser pulse. The supporting numerical electrodynamic modeling indicates that the electron emission is increased not owing to a larger effective aluminum surface, but due to instant local electromagnetic field enhancement near the nanoantenna, contr…
In this work using three-dimensional particle-in-cell simulations and analytical considerations we demonstrate intense high-order plasma surface harmonics carrying a time-varying orbital angular momentum (OAM) -- the self-torque. We show that by using two laser beams with different OAMs $l_1$ and $l_2$ and a certain delay between each other and shooting them obliquely on an overdense plasma target, one can generate harmonics with OAM spanning $nl_1$ to $nl_2$, where $n$ is the order of the harmonic. Such intense self-torqued harmonics can offer new possibilities in ultrafast spectroscopy.
Nanophotonic platforms such as metasurfaces, achieving arbitrary phase profiles within ultrathin thickness, emerge as miniaturized, ultracompact and kaleidoscopic optical vortex generators. However, it is often required to segment or interleave independent subarray metasurfaces to multiplex optical vortices in a single nano device, which in turn affects the compactness and channel capacity of the device. Here, inspired by phyllotaxis patterns in pine cones and sunflowers, we theoretically prove and experimentally report that multiple optical vortices can be produced in a single compact phyllot…
Nonlinear propagation of intense femtosecond laser pulses in bulk transparent media leads to a specific propagation regime, termed femtosecond filamentation, which in turn produces dramatic spectral broadening, or superbroadening, termed supercontinuum generation. Femtosecond supercontinuum generation in transparent solids represents a compact, efficient and alignment-insensitive technique for generation of coherent broadband radiation at various parts of the optical spectrum, which finds numerous applications in diverse fields of modern ultrafast science. During recent years, this research fi…
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…
Irradiation of isolated water molecules by few-cycle pulses of intense infrared laser light can give rise to ultrafast rearrangement resulting in formation of the H2+ ion. Such unimolecular reactions occur on the potential energy surface of the H2O2+ dication that is accessed when peak laser intensities in the 1015 W cm-2 range and pulse durations as short as 9-10 fs are used; ion yields of ~1.5% are measured. We also study such reactions by means of time-dependent wavepacket dynamics on an ab initio potential energy surface of the dication and show that a proton, generated from O-H bond ruptu…
We report on a novel experimental scheme to generate continuous-wave (cw), high power, and higher-order optical vortices tunable across mid-IR wavelength range. Using cw, two-crystal, singly resonant optical parametric oscillator (T-SRO) and pumping one of the crystals with Gaussian beam and the other crystal with optical vortices of orders, lp = 1 to 6, we have directly transferred the vortices at near-IR to the mid-IR wavelength range. The idler vortices of orders, li = 1 to 6, are tunable across 2276-3576 nm with a maximum output power of 6.8 W at order of, li = 1, for the pump power of 25 …
We report on tunnel ionization of Xe by 2-cycle, intense, infrared laser pulses and its dependence on carrier-envelope-phase (CEP). At low values of optical field ($E$), the ionization yield is maximum for cos-like pulses with the dependence becoming stronger for higher charge states. At higher $E$-values, the CEP dependence either washes out or flips. A simple phenomenological model is developed that predicts and confirms the observed results. CEP effects are seen to persist for 8-cycle pulses. Unexpectedly, electron rescattering plays an unimportant role in the observed CEP dependence. Our r…
Many important ultrafast phenomena take place in the liquid phase. However, there is no practical theory to predict how liquids respond to intense light. Here, we propose an $ab~initio$ accurate method to study the non-perturbative interaction of intense pulses with a liquid target to investigate its high-harmonic emission. We consider the case of liquid water, but the method can be applied to any other liquid or amorphous system. The liquid water structure is reproduced using Car-Parrinello molecular dynamics simulations in a periodic supercell. Then, we employ real-time time-dependent densit…
Bright Ar K-shell x-ray with very little background has been generated using an Ar clustering gas jet target irradiated with an 800 mJ, 30 fs ultra-high contrast laser, with the measured flux of 1.1 x 10^4 photons/mrad^2/pulse. This intense x-ray source critically depends on the laser contrast and the laser energy and the optimization of this source with interaction is addressed. Electron driven by laser electric field directly via nonlinear resonant is proved in simulation, resulting in effective electron heating and the enhancement of x-ray emission. The x-ray pulse duration is demonstrated …
We investigate the ultrafast electron dynamics triggered by terahertz and optical pulses in thin platinum and gold films by probing their transient optical reflectivity. The response of the platinum film to an intense terahertz pulse is similar to the optically-induced dynamics of both films and can be described by a two-temperature model. Surprisingly, gold can exhibit a much smaller terahertz pulse-induced reflectivity change and with opposite sign. For platinum, we estimate a 20% larger electron-phonon coupling for the terahertz-driven dynamics compared to the optically-induced one, which w…
Starting from first principles, we theoretically model the nonlinear temporal dynamics of gold-based plasmonic devices resulting from the heating of their metallic components. At optical frequencies, the gold susceptibility is determined by the interband transitions around the X,L points in the first Brillouin zone and thermo-modulational effects ensue from Fermi smearing of the electronic energy distribution in the conduction band. As a consequence of light-induced heating of the conduction electrons, the optical susceptibility becomes nonlinear. In this paper we describe, for the first time …
Terahertz (THz) radiation is a powerful tool with widespread applications ranging from imaging, sensing, and broadband communications to spectroscopy and nonlinear control of materials. Future progress in THz technology depends on the development of efficient, structurally simple THz emitters that can be implemented in advanced miniaturized devices. Here we show how the natural electronic anisotropy of layered conducting transition metal oxides enables the generation of intense terahertz radiation via the transverse thermoelectric effect. In thin films grown on offcut substrates, femtosecond l…
The non-linear response of dielectrics to intense, ultrashort electric fields has been a sustained topic of interest for decades with one of its most important applications being femtosecond laser micro/nano-machining. More recently, renewed interests in strong field physics of solids were raised with the advent of mid-infrared femtosecond laser pulses, such as high-order harmonic generation, optical-field-induced currents, etc. All these processes are underpinned by photoionization (PI), namely the electron transfer from the valence to the conduction bands, on a time scale too short for phono…
Bistability is widely exploited to demonstrate all-optical signal processing and light-based computing. The standard paradigm of switching between two steady states corresponding to '0" and '1" bits is based on the rule that a transition occurs when the signal pulse intensity overcomes the bistability threshold, and otherwise, the system remains in the initial state. Here, we break with this concept by revealing the phenomenon of indefinite switching in which the eventual steady state of a resonant bistable system is transformed into a nontrivial function of signal pulse parameters for moderat…
Inverse Compton scattering (ICS) is an elemental radiation process that produces high-energy photons both in nature and in the laboratory. Non-linear ICS is a process in which multiple photons are converted to a single high-energy photon. Here, we theoretically show that the photon produced by non-linear ICS of circularly polarized photons is a vortex, which means that it possesses a helical wave front and carries orbital angular momentum. Our work explains a recent experimental result regarding non-linear Compton scattering that clearly shows an annular intensity distribution as a remarkable …
Future information technology demands ultimately fast, low-loss quantum control. Intense light fields have facilitated important milestones, such as inducing novel states of matter, accelerating electrons ballistically, or coherently flipping the valley pseudospin. These dynamics leave unique signatures, such as characteristic bandgaps or high-order harmonic radiation. The fastest and least dissipative way of switching the technologically most important quantum attribute - the spin - between two states separated by a potential barrier is to trigger an all-coherent precession. Pioneering experi…
