Simulation of spatiotemporal light dynamics based on the time-dependent Schrödinger equation.

We establish a first-principle model for the simulation of spatiotemporal light pulse dynamics based on the combination of the time-dependent Schrödinger equation and the unidirectional propagation equation. The proposed numerical scheme enables computationally efficient simulation while being stable and accurate. We use the new model to examine self-focusing of a short pulse in atomic hydrogen and show that an accurate description of the excited-levels dynamics can only be achieved by a propagation model with an ab-initio description of the light-matter interaction, which accounts for the laser-dressed multilevel structure of the system, including bound and free states, and its sub-cycle response.

Tunable in situ near-UV pulses by transient plasmonic resonance in nanocomposites.

We propose a concept for generation of ultrashort pulses based on transient field-induced plasmonic resonance in nanoparticle composites. Photoionization and free-carrier plasma generation change the susceptibility of nanoparticles on a few-femtosecond scale under the action of the pump pulse. This opens a narrow time window when the system is in plasmonic resonance, which is accompanied by a short burst of the local field. During this process, frequency-tunable few-fs pulses can be emitted. This paves a way to ultra-compact yet efficient generation of ultrashort pulses at short wavelengths.

Non-instantaneous third-order optical response of gases in low-frequency fields.

It is commonly assumed that for low-intensity short optical pulses far from resonance, the third-order optical nonlinear response is instantaneous. We solve the three-dimensional time-dependent Schrödinger equation for the hydrogen atom and show that this is not the case: the polarization is not simply proportional to the cube of the electric field even at low intensities. We analyze the fundamental-frequency and third-harmonic nonlinear susceptibilities of hydrogen, investigate their dependence on intensity, and find that the delays in the Kerr response rapidly approach the femtosecond time-scale at higher intensities, while the delays in the third harmonic generation remain much lower. We also propose an experimental scheme to detect and characterize the above effects.

Propagator operator for pulse propagation in resonant media.

We show that, for the case of resonant media, the available models for unidirectional propagation of short pulses can face serious challenges with respect to numerical efficiency, accuracy, or numerical artifacts. We propose an alternative approach based on a propagator operator defined in the time domain. This approach enables precise simulations using short time windows even for resonant media and facilitates coupling of the propagation equation with first-principle methods such as the time-dependent Schödinger equation. Additionally, we develop a numerically efficient recipe to construct and apply such a propagator operator.

Sub-4 fs laser pulses at high average power and high repetition rate from an all-solid-state setup.

The generation of high average power, carrier-envelope phase (CEP) stable, near-single-cycle pulses at a repetition rate of 100 kHz is demonstrated using an all solid-state setup. By exploiting self-phase modulation in thin quartz plates and air, the spectrum of intense pulses from a high-power, high repetition rate non-collinear optical parametric chirped pulse amplifier (NOPCPA) is extended to beyond one octave, and pulse compression down to 3.7 fs is achieved. The octave-spanning spectrum furthermore allows performing straightforward f-to-2f interferometry by frequency-doubling the long-wavelength part of the spectrum. Excellent CEP-stability is demonstrated for extended periods of time. A full spatio-spectral characterization of the compressed pulses shows only minor asymmetries between the two perpendicular beam axes. We believe that the completed system represents the first laser system satisfying all requirements for performing high repetition rate attosecond pump-probe experiments with fully correlated detection of all ions and electrons produced in the experiment.

Application of mid-infrared pulses for quasi-phase-matching of high-order harmonics in silver plasma.

We demonstrate the quasi-phase-matching of a group of harmonics generated in Ag multi-jet plasma using tunable pulses in the region of 1160 - 1540 nm and their second harmonic emission. The numerical treatment of this effect includes microscopic description of the harmonic generation, propagation of the pump pulse, and the propagation of the generated harmonics. We obtained more than 30-fold growth of harmonics at the conditions of quasi-phase-matching in the region of 35 nm using eight-jet plasma compared with the case of imperforated plasma.

Combined action of the bound-electron nonlinearity and the tunnel-ionization current in low-order harmonic generation in noble gases.

We study numerically low-order harmonic generation in noble gases pumped by intense femtosecond laser pulses in the tunneling ionization regime. We analyze the influence of the phase-mismatching on this process, caused by the generated plasma, and study in dependence on the pump intensity the origin of harmonic generation arising either from the bound-electron nonlinearity or the tunnel-ionization current. It is shown that in argon the optimum pump intensity of about 100 TW/cm² leads to the maximum efficiency, where the main contribution to low-order harmonics originates from the bound-electron third and fifth order susceptibilities, while for intensities higher than 300 TW/cm² the tunnel-ionization current plays the dominant role. Besides, we predict that VUV pulses at 133 nm can be generated with relatively high efficiency of about 1.5 × 10⁻³ by 400 nm pump pulses.

High-harmonic and single attosecond pulse generation using plasmonic field enhancement in ordered arrays of gold nanoparticles with chirped laser pulses.

Coherent XUV sources, which may operate at MHz repetition rate, could find applications in high-precision spectroscopy and for spatio-time-resolved measurements of collective electron dynamics on nanostructured surfaces. We theoretically investigate utilizing the enhanced plasmonic fields in an ordered array of gold nanoparticles for the generation of high-harmonic, extreme-ultraviolet (XUV) radiation. By optimization of the chirp of ultrashort laser pulses incident on the array, our simulations indicate a potential route towards the temporal shaping of the plasmonic near-field and, in turn, the generation of single attosecond pulses. The inherent effects of inhomogeneity of the local fields on the high-harmonic generation are analyzed and discussed. While taking the inhomogeneity into account does not affect the optimal chirp for the generation of a single attosecond pulse, the cut-off energy of the high-harmonic spectrum is enhanced by about a factor of two.

Slow light in dielectric composite materials of metal nanoparticles.

We propose a method for slowing down light pulses by using composites doped with metal nanoparticles. The underlying mechanism is related to the saturable absorption near the plasmon resonance in a pump-probe regime, leading to strong dispersion of the probe refractive index and significantly reduced group velocities. By using a non-collinear scheme, we predict a total fractional delay of 43. This scheme promises simple and compact slow-light on-chip devices with tunable delay and THz bandwidth.

Theory of plasmonic femtosecond pulse generation by mode-locking of long-range surface plasmon polariton lasers.

We develop a semiclassical theory of passively mode-locked surface plasmon polariton (SPP) lasers based on a SPP Bragg resonator with a metal film deposited on a polymer host and adjacent layers of a slow saturable absorber and a slow saturable gain medium. The mode-locked laser dynamics is studied for the case that both the gain medium and the saturable absorber are solid-state dyes. The SPP laser pulse parameters are calculated in dependence on layer thicknesses of the metal film and pump parameters. We predict the possibility of SPP pulse generation with ∼ 100 fs pulse duration.

High-order harmonic generation employing field enhancement by metallic fractal rough surfaces.

We numerically investigate high-order harmonic generation (HHG) in noble gases in the vicinity of fractal structures of metallic rough surfaces described by the restricted solid-on-solid model. The calculated intensity enhancement factors in the range of 10³ enables HHG up to the 50-th order with low pump intensity down to tens of GW/cm². The increased interaction volume of "hot spots" in the case of grazing incidence of s-polarized pump pulses leads to an efficiency of harmonics in the plateau region of about 10⁻7.

Saturable absorption in composites doped with metal nanoparticles.

We study saturable absorption and the nonlinear contribution to the refractive index of metal-nanoparticle composites by using a modifie self-consistent Maxwell-Garnett formalism for spherical nanoparticles and a generalization of the discrete-dipole formalism for particles of arbitrary shape and size. The results for fused silica doped with silver nanoparticles show that the saturation of loss of the composites is strongest near the surface plasmon resonance and the saturation intensity is in the range of 10 MW/cm(2). The nonlinear refraction index decrease with increasing intensity and its sign depends on frequency and fillin factor. The predictions show that metal-nanoparticle composites can be used for mode locking of lasers in a broad spectral range down to 400 nm, where attractive saturable absorbers are still missing.

High-power soliton-induced supercontinuum generation and tunable sub-10-fs VUV pulses from kagome-lattice HC-PCFs.

We theoretically study a novel approach for soliton-induced high-power supercontinuum generation by using kagome lattice HC-PCFs filled with a noble gas. Anomalous dispersion and broad-band low loss of these fibers enable the generation of two-octave broad spectra by fs pulses, with high coherence and high spectral peak power densities up to five orders of magnitude larger than in standard PCFs. In addition, up to 20% of the output radiation energy forms a narrow UV/VUV band, which can be tuned by controlling the pressure in the range from 350 nm to 120 nm. In the temporal domain this corresponds to sub-10-fs UV/VUV pulses with pulse energy of few tens of microJ, caused by the formation of a high-order soliton emitting non-solitonic radiation.

Linear and nonlinear optical characteristics of composites containing metal nanoparticles with different sizes and shapes.

We study the effective linear and nonlinear optical parameters of composites containing noble metal nanoparticles and their dependence on the shape and size of the particles. Our numerical approach is based on the effective medium approximation combined with discrete dipole approximation, which results in a fast and accurate numerical method. The results demonstrate the possibility to achieve large enhancements of the linear and nonlinear optical parameters by tuning the plasmon resonance to a desired frequency by changing the size and the shape of the nanoparticles.

Low-threshold supercontinuum generation in glasses doped with silver nanoparticles.

We present a comprehensive study of low-threshold supercontinuum generation using the large frequency-dependent enhancement of the nonlinearity in glasses doped with silver nanoparticles. We predict octave-spanning asymmetric, blue-shifted spectral broadening of fs pulses with intensity in the range of tens of GW/cm(2). We also demonstrate the dependence of the spectral broadening on different physical parameters such as central operating wavelength, pulse duration, input power and the filling factor of the nanoparticles.

Guiding properties and dispersion control of kagome lattice hollow-core photonic crystal fibers.

Dispersion properties, loss and optimum design of kagome lattice hollow-core photonic crystal fibers filled with argon are studied for the purpose of possible applications in ultrafast nonlinear optics. As will be shown numerically and by using an approximate analytical formula these fibers exhibit anomalous dispersion for visible or UV wavelengths both for a 1-cell-core as well for a 3-ring-core which can be controlled by the gas pressure and do not suffer from high loss. It is shown that while the loss is mainly influenced by the strut thickness of the kagome lattice the group velocity dispersion is almost independently controlled by the core size. These results demonstrate that kagome lattice hollow fibers have a promising potential in ultrashort pulse delivering of high-energy pulses and in several interesting applications in ultrafast nonlinear optics.

High-power fifth-harmonic generation of femtosecond pulses in the vacuum ultraviolet using a Ti:sapphire laser.

We demonstrate the generation of fifth-harmonic pulses at 161 nm, with an energy of up to 600 nJ and 160 fs pulse duration from a Ti:sapphire laser at 1 kHz repetition rate by four-wave difference-frequency mixing in argon-filled waveguides. The efficiency is greatly improved by coupling to higher-order transverse modes, as well as by coating the inner surface of the waveguide. A numerical model of the process yields an understanding of the main effects influencing the harmonic generation.