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.

Photonic molecule state transition by collision.

We investigate the impact of collisions with two-frequency photonic molecules aiming to observe internal dynamic behavior and challenge their strong robustness. Versatile interaction scenarios show intriguing state changes expressed through modifications of the resulting state such as temporal compression and unknown collision-induced spectral tunneling. These processes show potential for efficient coherent supercontinuum generation and all-optical manipulation.

Third and fifth order nonlinear susceptibilities in thin HfO2 layers.

Third harmonic generation (THG) from dielectric layers is investigated. By forming a thin gradient of HfO2 with continuously increasing thickness, we are able to study this process in detail. This technique allows us to elucidate the influence of the substrate and to quantify the layered materials third χ(3)(3ω: ω, ω, ω) and even fifth order χ(5)(3ω: ω, ω, ω, ω, - ω) nonlinear susceptibility at the fundamental wavelength of 1030 nm. This is to the best of our knowledge the first measurement of the fifth order nonlinear susceptibility in thin dielectric layers.

Direct time-resolved plasma characterization with broadband terahertz light pulses.

We report here the results of comprehensive plasma characterization and diagnostics by analyzing time-resolved absorption spectra of short ultrabroadband (0.1-50 THz) pulses propagated through the test plasma. Spectral analysis of plasma-induced absorption of such THz pulses provides very direct, in situ, high dynamical range, potentially single-shot access to the plasma density, plasma decay time, electron temperature, and ballistic dynamics of the plasma expansion. We have demonstrated a proof-of-principle measurement of plasma created by an intense laser beam. In particular, we showed a reliable measurement of plasma densities from around 10^{16} to 10^{20}cm^{-3}. Apart from the plasma parameters, this method allowed us to reconstruct peak intensity inside the plasma spot and to observe a very early stage of plasma evolution after its excitation.

Onset of Bloch oscillations in the almost-strong-field regime.

In the field of high-order harmonic generation from solids, the electron motion typically exceeds the edge of the first Brillouin zone. In conventional nonlinear optics, on the other hand, the excursion of band electrons is negligible. Here, we investigate the transition from conventional nonlinear optics to the regime where the crystal electrons begin to explore the first Brillouin zone. It is found that the nonlinear optical response changes abruptly already before intraband currents due to ionization become dominant. This is observed by an interference structure in the third-order harmonic generation of few-cycle pulses in a non-collinear geometry. Although approaching Keldysh parameter γ = 1, this is not a strong-field effect in the original sense, because the iterative series still converges and reproduces the interference structure. The change of the nonlinear interband response is attributed to Bloch motion of the reversible (or transient or virtual) population, similar to the Bloch motion of the irreversible (or real) population which affects the intraband currents that have been observed in high-order harmonic generation.

Self-Stopping of Light.

Here, we show that light can bring itself to a complete standstill (self-stop) via self-interaction mediated by the resonant nonlinearity in a fully homogeneous medium. An intense few-cycle pulse, entering the medium, may reshape to form a strongly coupled light-matter bundle, in which the energy is transferred from light to the medium and back periodically on the single-cycle scale. Such oscillating structure can decelerate, alter its propagation direction, and even completely stop, depending on the state of its internal degrees of freedom. This phenomenon is expected to occur in the few-cycle strong-field regime when the Rabi oscillation frequency becomes comparable with the frequency of the incoming light.

Role of frequency dependence of the nonlinearity on a soliton's evolution in photonic crystal fibers.

We reveal the crucial role played by the frequency dependence of the nonlinear parameter on the evolution of femtosecond solitons inside photonic crystal fibers (PCFs). We show that the conventional approach based on the self-steepening effect is not appropriate when such fibers have two zero-dispersion wavelengths, and several higher-order nonlinear terms must be included for realistic modeling of the nonlinear phenomena in PCFs. These terms affect not only the Raman-induced wavelength shift of a soliton but also impact its shedding of dispersive radiation.

Single-cycle pulse compression in dense resonant media.

We propose here a new approach for compression and frequency up-conversion of short optical pulses in the regime of extreme nonlinear optics in optically dense absorbing media, providing an alternative route to attosecond-scale pulses at high frequencies. This method is based on dynamics of self-induced transparency (SIT) pulses of nearly single cycle duration, leading to single-cycle-scale Rabi oscillations in the medium. The sub-cycle components of an incident pulse behave as separate SIT-pulses, approaching each other and self-compressing, resulting in the threefold compression in time and frequency up-conversion by the same factor. As we show, the scheme can be cascaded, staying at the subsequent stage with nearly the same compression and up-conversion ratio. In this way, as our simulations show, after only few micrometers of propagation, a 700 nm wavelength single cycle pulse can be compressed to a pulse of 200 attoseconds duration located in XUV frequency range.

Population difference gratings created on vibrational transitions by nonoverlapping subcycle THz pulses.

We study theoretically a possibility of creation and ultrafast control (erasing, spatial frequency multiplication) of population density gratings in a multi-level resonant medium having a resonance transition frequency in the THz range. These gratings are produced by subcycle THz pulses coherently interacting with a nonlinear medium, without any need for pulses to overlap, thereby utilizing an indirect pulse interaction via an induced coherent polarization grating. High values of dipole moments of the transitions in the THz range facilitate low field strength of the needed THz excitation. Our results clearly show this possibility in multi-level resonant media. Our theoretical approach is based on an approximate analytical solution of time-dependent Schrödinger equation (TDSE) using perturbation theory. Remarkably, as we show here, quasi-unipolar subcycle pulses allow more efficient excitation of higher quantum levels, leading to gratings with a stronger modulation depth. Numerical simulations, performed for THz resonances of the [Formula: see text] molecule using Bloch equations for density matrix elements, are in agreement with analytical results in the perturbative regime. In the strong-field non-perturbative regime, the spatial shape of the gratings becomes non-harmonic. A possibility of THz radiation control using such gratings is discussed. The predicted phenomena open novel avenues in THz spectroscopy of molecules with unipolar and quasi-unipolar THz light bursts and allow for better control of ultra-short THz pulses.

Stable coherent mode-locking based on [Formula: see text] pulse formation in single-section lasers.

Here we consider coherent mode-locking (CML) regimes in single-section cavity lasers, taking place for pulse durations less than atomic population and phase relaxation times, which arise due to coherent Rabi oscillations of the atomic inversion. Typically, CML is introduced for lasers with two sections, the gain and absorber ones. Here we show that, for certain combination of the cavity length and relaxation parameters, a very stable CML in a laser, containing only gain section, may arise. The mode-locking is unconditionally self-starting and appears due to balance of intra-pulse de-excitation and slow interpulse-scale pump-induced relaxation processes. We also discuss the scaling of the system to shorter pulse durations, showing a possibility of mode-locking for few-cycle pulses.

Influence of tunnel ionization to third-harmonic generation of infrared femtosecond laser pulses in air.

Here we present an experimental as well as theoretical study of third-harmonic generation in tightly focused femtosecond filaments in air at the wavelength of [Formula: see text]. At low intensities, longitudinal phase matching is dominating in the formation of 3rd harmonics, whereas at higher intensities locked X-waves are formed. We provide the arguments that the X-wave formation is governed mainly by the tunnel-like ionization dynamics rather than by the multiphoton one. Despite of this fact, the impact of the ionization-induced nonlinearity is lower than the one from bound-bound transitions at all intensities.

Higher-order dispersion and the spectral behavior in a doubly resonant optical parametric oscillator.

In doubly resonant optical parametric oscillators (DROPOs), it is possible to generate, enhance, and phase lock two frequencies at once. Following intracavity phase conditions, a complex tuning behavior of the signal and idler spectra takes place in DROPOs, cumulating into degeneracy with phase self-locking and coherent wavelength doubling. In this work, we identify group delay matching as the important parameter determining the global tuning behavior and demonstrate the key role of higher-order dispersion in the spectral dependencies. Applicationwise, we suggest a simple way to control the phase self-locking region by varying the intracavity third-order dispersion.

Selective ultrafast control of multi-level quantum systems by subcycle and unipolar pulses.

The most typical way to optically control population of atomic and molecular systems is to illuminate them with radiation, resonant to the relevant transitions. Here we consider a possibility to control populations with the subcycle and even unipolar pulses, containing less than one oscillation of electric field. Despite the spectrum of such pulses covers several levels at once, we show that it is possible to selectively excite the levels of our choice by varying the driving pulse shape, duration or time delay between consecutive pulses. The pulses which are not unipolar, but have a peak of electric field of one polarity much higher (and shorter) than of the opposite one, are also capable for such control.

Generating Ultrabroadband Deep-UV Radiation and Sub-10 nm Gap by Hybrid-Morphology Gold Antennas.

We experimentally investigate the interaction between hybrid-morphology gold optical antennas and a few-cycle Ti:sapphire laser up to ablative intensities, demonstrating rich nonlinear plasmonic effects and promising applications in coherent frequency upconversion and nanofabrication technology. The two-dimensional array of hybrid antennas consists of elliptical apertures combined with bowties in its minor axis. The plasmonic resonance frequency of the bowties is red-shifted with respect to the laser central frequency and thus mainly enhances the third harmonic spectrum at long wavelengths. The gold film between two neighboring elliptical apertures forms an hourglass-shaped structure, which acts as a "plasmonic lens" and thus strongly reinforces surface currents into a small area. This enhanced surface current produces a rotating magnetic field that deeply penetrates into the substrate. At resonant frequency, the magnetic field is further intensified by the bowties. The resonant frequency of the hourglass is blueshifted with respect to the laser central frequency. Consequently, it spectacularly extends the third harmonic spectrum toward short wavelengths. The resultant third harmonic signal ranges from 230 to 300 nm, much broader than the emission from a sapphire crystal. In addition, the concentration of surface current within the neck of the hourglass antenna results in a structural modification through laser ablation, producing sub-10 nm sharp metallic gaps. Moreover, after laser illumination the optical field hotspots are imprinted around the antennas, allowing us to confirm the subwavelength enhancement of the electric near-field intensity.

Soliton Molecules with Two Frequencies.

We demonstrate a peculiar mechanism for the formation of bound states of light pulses of substantially different optical frequencies, in which pulses are strongly bound across a vast frequency gap. This is enabled by a propagation constant with two separate regions of anomalous dispersion. The resulting soliton compound exhibits moleculelike binding energy, vibration, and radiation and can be understood as a mutual trapping providing a striking analogy to quantum mechanics. The phenomenon constitutes an intriguing case of two light waves mutually affecting and controlling each other.

Regularizing Aperiodic Cycles of Resonant Radiation in Filament Light Bullets.

We demonstrate an up to now unrecognized and very effective mechanism which prevents filament collapse and allows persistent self-guiding propagation retaining a large portion of the optical energy on axis over unexpected long distances. The key ingredient is the possibility of continuously leaking energy into the normal dispersion regime via the emission of resonant radiation. The frequency of the radiation is determined by the dispersion dynamically modified by photogenerated plasma, thus allowing us to excite new frequencies in spectral ranges which are otherwise difficult to access.

Simple route toward efficient frequency conversion for generation of fully coherent supercontinua in the mid-IR and UV range.

Fiber supercontinua represent light sources of pivotal importance for a wide range of applications, ranging from optical communications to frequency metrology. Although spectra encompassing more than three octaves can be produced, the applicability of such spectra is strongly hampered due to coherence degradation during spectral broadening. Assuming pulse parameters at the cutting edge of currently available laser technology, we demonstrate the possibility of strongly coherent supercontinuum generation. In a fiber with two zero-dispersion wavelengths a higher-order soliton experiences a temporal breakdown, without any compression or splitting behavior, which leads to nearly complete conversion of input solitonic radiation into resonant nonsolitonic radiation in the dispersive wave regime. As the process is completely deterministic and shows little sensitivity to input noise, the resulting pulses appear to be compressible down to the sub-cycle level and may thus hold a new opportunity for direct generation of attosecond pulses in the visible to near ultraviolet wavelength range.

Controlling formation and suppression of fiber-optical rogue waves.

Fiber-optical rogue waves appear as rare but extreme events during optical supercontinuum generation in photonic crystal fibers. This process is typically initiated by the decay of a high-order fundamental soliton into fundamental solitons. Collisions between these solitons as well as with dispersive radiation affect the soliton trajectory in frequency and time upon further propagation. Launching an additional dispersive wave at carefully chosen delay and wavelength enables statistical manipulation of the soliton trajectory in such a way that the probability of rogue wave formation is either enhanced or reduced. To enable efficient control, parameters of the dispersive wave have to be chosen to allow trapping of dispersive radiation in the nonlinear index depression created by the soliton. Under certain conditions, direct manipulation of soliton properties is possible by the dispersive wave. In other more complex scenarios, control is possible via increasing or decreasing the number of intersoliton collisions. The control mechanism reaches a remarkable efficiency, enabling control of relatively large soliton energies. This scenario appears promising for highly dynamic all-optical control of supercontinua.

3D numerical simulations of THz generation by two-color laser filaments.

Terahertz (THz) radiation produced by the filamentation of two-color pulses over long distances in argon is numerically investigated using a comprehensive model in full space-time-resolved geometry. We show that the dominant physical mechanism for THz generation in the filamentation regime at clamping intensity is based on quasi-dc plasma currents. The calculated THz spectra for different pump pulse energies and pulse durations are in agreement with previously reported experimental observations. For the same pulse parameters, near-infrared pump pulses at 2 µm are shown to generate a more than 1 order of magnitude greater THz yield than pumps centered at 800 nm.

Accelerated rogue waves generated by soliton fusion at the advanced stage of supercontinuum formation in photonic-crystal fibers.

Soliton fusion is a fascinating and delicate phenomenon that manifests itself in optical fibers in case of interaction between copropagating solitons with small temporal and wavelength separation. We show that the mechanism of acceleration of a trailing soliton by dispersive waves radiated from the preceding one provides necessary conditions for soliton fusion at the advanced stage of supercontinuum generation in photonic-crystal fibers. As a result of fusion, large-intensity robust light structures arise and propagate over significant distances. In the presence of small random noise the delicate condition for the effective fusion between solitons can easily be broken, making the fusion-induced giant waves a rare statistical event. Thus oblong-shaped giant accelerated waves become excellent candidates for optical rogue waves.