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We report on a combined experimental and numerical study of photoelectron circular dichroism (PECD) induced by intense few-cycle laser pulses, using methyloxirane as the molecular example. Our experiments reveal a remarkably pronounced sensitivity of the PECD strength of double-ionization on the carrier-envelope phase (CEP) of the laser pulses. By comparison to the simulations, which reproduce the measured CEP-dependence for specific orientations of the molecules in the lab frame, we attribute the origin of the observed CEP-dependence of PECD to the CEP-induced modulation of ionization from different areas of the wave functions of three dominant orbitals.

All-optical switching of 75 fs pulses centered at 1560 nm, driven by 270 fs, 1030 nm pulses in a dual-core optical fiber exhibiting high index contrast is presented. The fiber is made of a thermally matched pair of lead silicate and borosilicate glasses used as core and cladding material, respectively. The novel switching approach is based on nonlinear balancing of dual-core asymmetry, by control pulse intensity induced group velocity reduction of the fast fiber channel. Due to the fiber core made of soft glass with high nonlinearity high switching contrast exceeding 20 dB is reached by using control pulses of only few nanojoule energy. The optimum fiber length is 14 mm, which closely match the calculated coupling length at the signal wavelength. The results express significant progress in comparison to similar studies based on self-switching of solitonic pulses in dual-core fibers and represent high application potential.

Next-generation high-speed optical networks demand the development of ultrafast optical interconnects capable of Tbit s(-1) data rates. By utilizing colloidal CdSe/CdS core/shell quantum dots, gated by intense THz pulses, a proof of concept of an all-optical femtosecond electro-absorption switch is presented in this work. Without any additional enhancement of the THz electric field, an extinction contrast of more than 6 dB and transmission changes in the visible of more than 15% are achieved, with the latter setting a new record for solution-processed electro-absorption materials at room temperature. The absence of physical artifacts, originating from electrodes and field enhancing structures, allows to employ a simple and intuitive numerical model, which rationalizes the large field-induced electro-absorption response. Supported by theoretical calculations, the importance of the energy band alignment of heterostructure quantum dots are discussed for the first time and suggest that further improvement of the modulation depth and contrast may be achieved with Type-II quantum dots., Advanced Optical Materials, 10 (9), ISSN:2195-1071

We investigate experimentally and theoretically effects of the inter-core propagation mismatch on nonlinear switching in dual-core high-index-contrast soft-glass optical fibers. Incident femtosecond pulses of various energy are fed into a single ("straight") core, to identify transitions between different dynamical regimes, viz., inter-core oscillations, self-trapping in the cross core, and retaining the pulse in the straight core. The transfer between channels, which has solitonic character, is controlled by the pulse's energy. A model based on the system of coupled nonlinear Schr\"{o}dinger equations reveals the effect of the mismatch parameter and pulse duration on the diagram of the various energy dependent dynamical regimes. Optimal values of the mismatch and pulse width, which ensure stable performance of the nonlinear switching, are identified. The theoretical predictions are in agreement with experimental findings., Comment: 25 pages, 9 figures. To be published in "Chaos, Solitons & Fractals"

We introduce a new approach to reduce uncorrelated background signals from fluorescence imaging data, using real-time subtraction of background light. This approach takes advantage of the short fluorescence lifetime of most popular fluorescent activity reporters, and the low duty-cycle of ultrafast lasers. By synchronizing excitation and recording, laser-induced multiphoton fluorescence can be discriminated from background light levels with each laser pulse. We demonstrate the ability of our method to – in real-time – remove image artifacts that in a conventional imaging setup lead to clipping of the signal. In other words, our method enables imaging under conditions that in a conventional setup would yield corrupted data from which no accurate information can be extracted. This is advantageous in experimental setups requiring additional light sources for applications such as optogenetic stimulation.

Extreme nonlinear interactions of THz electromagnetic fields with matter are the next frontier in nonlinear optics. However, reaching this frontier in free space is limited by the existing lack of appropriate powerful THz sources. Here, we experimentally demonstrate that two-color filamentation of femtosecond mid-infrared laser pulses at 3.9 μm allows one to generate ultrashort sub-cycle THz pulses with sub-milijoule energy and THz conversion efficiency of 2.36%, resulting in THz field amplitudes above 100 MV cm−1. Our numerical simulations predict that the observed THz yield can be significantly upscaled by further optimizing the experimental setup. Finally, in order to demonstrate the strength of our THz source, we show that the generated THz pulses are powerful enough to induce nonlinear cross-phase modulation in electro-optic crystals. Our work paves the way toward free space extreme nonlinear THz optics using affordable table-top laser systems., Powerful terahertz pulses are generated during the nonlinear propagation of ultrashort laser pulses in gases. Here, the authors demonstrate efficient sub-cycle THz pulse generation by using two-color midinfrared femtosecond laser filaments in ambient air.

We demonstrate bright, narrow-bandwidth, high order harmonics driven by VIS lasers, continuously tunable towards higher and lower EUV – X-ray photon energies, ideal for resonant, ultrafast, coherent diffractive imaging at the absorption edges of ferromagnets.

We report on direct ultrafast electro-absorption switching in colloidal CdSe/CdS core/shell quantum dots driven by intense THz pulses without a field enhancing structure, and suggest a route to optimize electro-absorption modulators with respect to the energy band alignment of the heterostructure material.

We present a complex study of pulse-energy-controlled solitonic self-switching of femtosecond pulses at wavelengths of 1700 and 1560 nm in two nonlinear high-index contrast dual-core fibers having different levels of slight asymmetry. In the case of the fiber with higher dual-core asymmetry excited by 1700 nm pulses, the highest switching contrast of 20.8 dB at 40 mm fiber length was demonstrated. It was accompanied by multiple exchanges of the dominant core at the fiber output, which is a strong signature of the soliton-based switching process. In the case of the fiber with lower dual-core asymmetry, excited by 1560 nm pulses, the highest switching contrast of 21.4 dB at 35 mm fiber length was achieved with a broadband character of the switching in the spectral range of 1450–1650 nm. Both demonstrations represent progress in all-optical switching studies at these particular wavelengths thanks to a comparison between their results, which reveals the requirement of a higher level of dual-core symmetry for applicable C-band operation.

We present a robust fiber-based setup for Bessel-like beam extended depth-of-focus Fourier-domain optical coherence microscopy, where the Bessel-like beam is generated in a higher order mode fiber module. In this module a stable guided LP02 core mode is selectively excited by a long period grating written in the higher order mode fiber. Imaging performance of this system in terms of lateral resolution and depth of focus was analyzed using samples of suspended microbeads and compared to the case where illumination is provided by the fundamental LP01 mode of a single mode fiber. Illumination with the LP02 mode allowed for a lateral resolution down to 2.5 µm as compared to 4.5 µm achieved with the LP01 mode of the single mode fiber. A three-fold enhancement of the depth of focus compared to a Gaussian beam with equally tight focus is achieved with the LP02 mode. Analysis of the theoretical lateral point spread functions for the case of LP01 and LP02 illumination agrees well with the experimental data. As the design space of waveguides and long-period gratings allows for further optimization of the beam parameters of the generated Bessel-like beams in an all-fiber module, this approach offers a robust and yet flexible alternative to free-space optics approaches or the use of conical fiber tips.

The use of ultrashort laser pulses with long wavelengths as drivers is a relevant strategy for scaling high harmonic generation (HHG) to higher photon energies. Here, stimulated Raman scattering enhanced by the formation of multidimensional solitary states in a molecular gas‐filled hollow‐core fiber as the mechanism to produce a versatile HHG driver is reported on. This recently discovered method allows to red shift and to compress conventional subpicosecond laser pulses with a simple experimental apparatus, ultimately increasing the generated photon energy, while assuring a high photon flux. The adaptability, simplicity, and stability of this method make it attractive for tailoring HHG sources to individual applications at specific photon energies. Measurements of resonant magnetic scattering in a cobalt/platinum multilayer sample are presented as a demonstration of the relevance of this approach for photon‐hungry applications in the extreme ultraviolet.

Multidimensional solitary states generated by intermodal stimulated Raman scattering in a gas-filled hollow-core fiber form red-shifted, few-cycle pulses after propagation thought glass. These pulses, when used to drive the high harmonic generation process, allow for tailoring the extreme ultraviolet source to specific photon-demanding applications.

The interaction of laser pulses with condensed matter forms the basis of light-wave-driven electronics potentially enabling tera- and petahertz switching rate applications. Carrier control using near- and midinfrared pulses is appealing for integration into existing platforms. Toward this end, a fundamental understanding of the complexity of phenomena concerning sub-band-gap driven semiconductors such as high harmonic generation, carrier excitation due to multiphoton absorption, and interband tunneling as well as carrier-carrier interactions due to strong acceleration in infrared transients is important. Here, stimulated emission from polycrystalline ZnO thin films for pump wavelengths between 1.2 \ensuremath{\mu}m (1 eV) and 10 \ensuremath{\mu}m (0.12 eV) is observed. Contrary to the expected higher intensity threshold for longer wavelengths, the lowest threshold pump intensity for stimulated emission is obtained for the longest pump wavelength corroborating the importance of collisional excitation upon intraband electron acceleration.

Nonlinear self-channeling (filamentation) of intense, ultrashort laser pulses in air has been extensively studied with ultrafast, near-infrared and visible laser sources [1] . Recently these investigations advanced to longer wavelengths, as well as to the regime of few-cycle pulses, where the effects associated with the carrier-envelope phase (CEP) of the laser pulse become important. It has been shown that spectral interference in the white light generated on filamentation of an ultrafast, short-wave infrared laser source carries CEP information [2] . Here, we report using this spectral interference for single-shot characterization of the CEP of an ultrafast, mid-infrared (MIR) laser source at 3.9 µm wavelength.

Due to numerous unique properties, such as the capability of resonantly exciting crystal lattice vibrations, molecular rotations and other low energy transitions in solids, liquids and gases, terahertz radiation belongs to one of the most interesting but yet less explored spectral regions. Recently, a considerable progress has been demonstrated in THz generation by optical rectification (OR) in organic crystals, conventionally driven by near-IR fs-pulses centred at the telecommunication wavelength of 1.5 µm. Although high optical- to THz conversion efficiencies of 1-3% with pulse energies of up to 0.9 mJ [1] can be achieved, the conversion efficiency is nevertheless deteriorated by multiphoton absorption and is fundamentally limited by the damage threshold of the crystal. This restricts the applicable pump fluence to nothing more than 20 mJ/cm 2 .

Within the last decades, electro-optic (EO) modulators based on the quantum confined Stark effect (QCSE) in quantum well structures came to prominence for high-speed optical networks. When an external electric field is applied to such a quantum structure, it bends the energy levels and shifts the absorption edge to smaller energies. In addition, the overlap between electron and hole wave functions decreases, which diminishes the amount of absorption [1] . This technique is ultimately limited to the time scale necessary to change the electric field on the attached electrodes. Moreover, largest modulation of the energy levels can be achieved for structures with a strong confinement and large excition binding energies. Hence, low dimensional materials like quantum dots (QDs) in combination with intense THz pulses which provide the electric field driver, are promising candidates for sub-picosecond all-optical switching of optical absorption. Pioneering work has been performed by Pein and co-workers [2] wherein they report on a THz-field induced QCSE in CdSe/CdS colloidal QDs. However, due to difficulties to generate THz radiation with the electric field in the MV/cm range, necessary to alter the optical transmission, THz field enhancing structures have been employed.

High harmonic generation (HHG) in gasses has become a method of choice among table-top extreme ultraviolet (XUV) sources. In order to push the harmonic cut-off towards higher photon energies, many strategies can be implemented, including red-shifting and compressing the driver pulses. Here, we propose a new approach for tuning the red-shift of sub-picosecond driver pulses and compressing them to few-cycle durations in a single stage. This method uses newly discovered multidimensional solitary states (MDSS) pulses as a spatio-temporal engineered source based on the nonlinear Raman process in gas-filled hollow-core fibres (HCF) [1] . It has a few key advantages: 1) The MDSS pulses exhibit a negative quadratic spectral phase and can be compressed by simple propagation through glass. 2) In contrast with commonly-used optical parametric amplifiers, a small redshift can be obtained, allowing to reach a target XUV photon energy while minimizing the detrimental effects of long driver wavelengths on HHG efficiency. We apply our method to X-ray Resonant Magnetic Scattering (XRMS) measurements on a cobalt/platinum ferromagnet, an application that requires a high photon flux at the M 2,3 edge of cobalt (60 eV).

In this paper, we present an iterative learning algorithm for pulse-shape control applications of optical chirped pulse amplifiers for ultra-short, high-energy light pulses. For this, we first introduce a general nonlinear and infinite-dimensional mathematical model of chirped pulse amplifiers. By reducing the complexity of this detailed model and reformulating the control task, we are subsequently able to apply inversion-based iterative learning control to track desired output pulses. Using the reduced model to estimate both internal states and unknown parameters yields a fast and simple way of consistently estimating the input–output behavior without relying on a calibrated system model. The effectiveness of the resulting adaptive algorithm is finally illustrated with simulation scenarios on an experimentally validated mathematical model.

We demonstrate a time-domain method to quantitatively retrieve the angular dependence of laser-induced electron rescattering from the measured rotational half-revival signals of molecules with a reaction microscope. The method is based on the measured channel-resolved ion yields of single ionization and electron-rescattering-induced double ionization and the in situ measured alignment distribution of molecules. From the measured data for ${\mathrm{CO}}_{2}$, we retrieve the angular dependence of electron rescattering in nonsequential double ionization for both nondissociative and dissociative cases. The results imply that the angular dependence of electron rescattering is affected by the state of the parent ion populated during the first ionization step. The method demonstrated here opens up the possibility to quantitatively retrieve from measured data which molecular orbitals are involved in the interaction of strong laser fields with molecules.

We report on the observation of quantum confined stark effect (QCSE) in CdSe/CdS core/shell quantum dots (QDs) directly driven by an intense THz field, generated in the organic crystal DAST, which is pumped with multi-millijoule mid-IR pulses.

The generation of ultrashort laser pulse bursts has already contributed to many applications such as materials processing [1] , pulsed laser deposition [2] , laser induced breakdown spectroscopy (LIBS) [3] and seeding of free electron lasers [4] . Currently, there is a rising demand on burst sources providing terahertz (THz) intraburst repetition rates or higher corresponding to pulse spacings in the order of a few picoseconds, given by applications such as resonant driving of optical nonlinearities [5] , time-resolved nonlinear spectroscopies [6] , coherent control of quantum systems [7] or as driver for secondary radiation sources, e.g. generation of THz bursts [8] . However, the amplification of bursts to multi-millijoule energies at THz intraburst repetition rates is highly problematic. This is given by the appearance of spectral modes that are mapped into the time-domain, formed by spectral interference of closely spaced pulses which are overlapping when applying Chirped Pulse Amplification (CPA). This leads to insufficient energy extraction in an amplifier and, if pulse spacing is not stabilized on an interferometric scale, to temporally unstable burst generation. Recently, we have successfully demonstrated energy-safe, stabilized CPA of ultrashort pulse bursts with THz intraburst frequencies up to multi-millijoules by applying Vernier-enabled phase-modulation techniques, breaking the mentioned energy-limiting barrier [8] . In this contribution, we demonstrate a new version of our burst-generation technique, which drastically lowers system complexity compared to our previous approach, allowing its application to any master-oscillator regenerative-amplifier combination setup with only minor modifications.

A pair of sub-mJ femtosecond pulses separated by 110 ns, generated in a single cw-pumped Yb regenerative amplifier, is employed as a frontend for mid-IR OPCPA operating in the atmospheric transparency window.

By exploiting stimulated Raman scattering in long nitrogen-filled capillary fibers, we demonstrate continuous tunability of Yb laser systems over the 1.0-1.7 μm range, with conversion efficiency up to 82%, and an up to 10-fold pulse compression.

The generation of high order harmonics from femtosecond mid-IR laser pulses in ZnO has shown great potential to reveal new insight into the ultrafast electron dynamics on a few femtosecond timescale. In this work we report on the experimental investigation of photoluminescence and high-order harmonic generation (HHG) in a ZnO single crystal and polycrystalline thin film irradiated with intense femtosecond mid-IR laser pulses. The ellipticity dependence of the HHG process is experimentally studied up to the 17th harmonic order for various driving laser wavelengths in the spectral range 3&ndash, 4 &micro, m. Interband Zener tunneling is found to exhibit a significant excitation efficiency drop for circularly polarized strong-field pump pulses. For higher harmonics with energies larger than the bandgap, the measured ellipticity dependence can be quantitatively described by numerical simulations based on the density matrix equations. The ellipticity dependence of the below and above ZnO band gap harmonics as a function of the laser wavelength provides an efficient method for distinguishing the dominant HHG mechanism for different harmonic orders.

Generating intense ultrashort pulses with high-quality spatial modes is crucial for ultrafast and strong-field science and can be achieved by nonlinear supercontinuum generation (SCG) and pulse compression. In this work, we propose that the generation of quasi-stationary solitons in periodic layered Kerr media can greatly enhance the nonlinear light-matter interaction and fundamentally improve the performance of SCG and pulse compression in condensed media. With both experimental and theoretical studies, we successfully identify these solitary modes and reveal their unified condition for stability. Space-time coupling is shown to strongly influence the stability of solitons, leading to variations in the spectral, spatial and temporal profiles of femtosecond pulses. Taking advantage of the unique characteristics of these solitary modes, we first demonstrate single-stage SCG and the compression of femtosecond pulses from 170 to 22 fs with an efficiency >85%. The high spatiotemporal quality of the compressed pulses is further confirmed by high-harmonic generation. We also provide evidence of efficient mode self-cleaning, which suggests rich spatiotemporal self-organization of the laser beams in a nonlinear resonator. This work offers a route towards highly efficient, simple, stable and highly flexible SCG and pulse compression solutions for state-of-the-art ytterbium laser technology.

Optical rectification in lithium niobate and semiconductor nonlinear optical materials, utilizing the tilted-pulse-front technique, has become a versatile source of intense single- and multicycle THz pulses. Novel approaches recently proposed, and some of them demonstrated, are promising to scale the technology to unprecedented field strengths by enabling uniform interaction length for THz generation across a large beam. The generation of continuously-tunable, narrowband THz pulses from phase-locked multi-millijoule femtosecond pulse bursts by optical rectification is demonstrated.

We experimentally demonstrate that temporally confined spatial solitons can be realized by space-time coupled propagation of strong femtosecond pulses in a nonlinear optical resonator, consisting of periodic layered Kerr media (PLKM). A universal relationship between the characteristic beam size and the critical nonlinear phase of the solitary modes is revealed, defining different regions of soliton stability. Taking advantage of the unique characters of these solitary modes, we demonstrate supercontinuum generation and pulse compression of initially 260 μJ, 170 fs pulses down to 22 fs in a single-stage PLKM resonator with an efficiency >90%.

We demonstrate a pulse energy-governed nonlinear self-switching of femtosecond pulses at the wavelengths of 1700 nm and 1560 nm in a highly nonlinear high index contrast dual-core fiber. The improved technology process allowed the first-time registration of the switching effect in the communication C-band.

We describe the results of experiments and simulations performed with the aim of extending photoelectron spectroscopy with intense laser pulses to the case of molecular compounds. Dimer frame photoelectron angular distributions generated by double ionization of ${\mathrm{N}}_{2}\ensuremath{-}{\mathrm{N}}_{2}$ and ${\mathrm{N}}_{2}\ensuremath{-}{\mathrm{O}}_{2}$ van der Waals dimers with ultrashort, intense laser pulses are measured using four-body coincidence imaging with a reaction microscope. To study the influence of the first-generated molecular ion on the ionization behavior of the remaining neutral molecule we employ a two-pulse sequence comprising of a linearly polarized and a delayed elliptically polarized laser pulse that allows distinguishing the two ionization steps. By analysis of the obtained electron momentum distributions we show that scattering of the photoelectron on the neighboring molecular potential leads to a deformation and rotation of the photoelectron angular distribution as compared to that measured for an isolated molecule. Based on this result we demonstrate that the electron momentum space in the dimer case can be separated, allowing us to extract information about the ionization pathway from the photoelectron angular distributions. Our work, when implemented with a variable pulse delay, opens up the possibility of investigating light-induced electronic dynamics in molecular dimers using angularly resolved photoelectron spectroscopy with intense laser pulses.

Ultrashort high-energy pulses at wavelengths longer than 1 µm are now desirable for a vast variety of applications in ultrafast and strong-field physics. To date, the main answer to the wavelength tunability for energetic, broadband pulses still relies on optical parametric amplification (OPA), which often requires multiple and complex stages, may feature imperfect beam quality, and has limited conversion efficiency into one of the amplified waves. In this work, we present a completely different strategy to realize an energy-efficient and scalable laser frequency shifter. This relies on the continuous red shift provided by stimulated Raman scattering (SRS) over a long propagation distance in nitrogen-filled hollow-core fibers (HCF). We show a continuous tunability of the laser wavelength from 1030 nm up to 1730 nm with a conversion efficiency higher than 70% and high beam quality. The highly asymmetric spectral broadening, arising from the spatiotemporal nonlinear interplay between higher-order modes of the HCF, can be readily employed to generate pulses ( ∼ 20 f s ) significantly shorter than the pump ones ( ∼ 200 f s ) with high beam quality, and the pulse energy can further be scaled up to tens of millijoules. We envision that this technique, coupled with the emerging high-power Yb laser technology, has the potential to answer the increasing demand for energetic multi-TW few-cycle sources tunable in the near-IR.

We establish a generalized picture of the phase sensitivity of laser-induced directional bond breaking using the H_{2} molecule as the example. We show that the well-known proton ejection anisotropy measured with few-cycle pulses as a function of their carrier-envelope phases arises as an amplitude modulation of an intrinsic anisotropy that is sensitive to the laser phase at the ionization time and determined by the molecule's electronic structure. Our work furthermore reveals a strong electron-proton correlation that may open up a new approach to experimentally accessing the laser-sub-cycle intramolecular electron dynamics also in larger molecules.

All-optical switching of 77 fs pulses centered at 1550 nm, driven by 270 fs, 1030 nm pulses in dual-core optical fibre exhibiting high index contrast is presented. The switching is achieved by nonlinear balancing of dual-core asymmetry. High switching contrast exceeding 20 dB is attained with driving pulses of only few nanojoule energy, which is due to the fibre core made of soft glass possessing high nonlinearity.

We demonstrate an efficient approach for enhancing the spectral broadening of long laser pulses and for efficient frequency redshifting by exploiting the intrinsic temporal properties of molecular alignment inside a gas-filled hollow-core fiber (HCF). We find that laser-induced alignment with durations comparable to the characteristic rotational time scale T R o t A l i g n enhances the efficiency of redshifted spectral broadening compared to noble gases. The applicability of this approach to Yb lasers with (few hundred femtoseconds) long pulse duration is illustrated, for which efficient broadening based on conventional Kerr nonlinearity is challenging to achieve. Furthermore, this approach proposes a practical solution for high energy broadband long-wavelength light sources, and it is attractive for many strong field applications.

Extreme nonlinear interactions of THz electromagnetic fields with matter are the next frontier in nonlinear optics. However, reaching this frontier in free space is limited by the existing lack of appropriate powerful THz sources. Here we demonstrate both theoretically and experimentally the realization of a novel THz source with high peak power performance based on two-color filamentation of femtosecond mid-infrared laser pulses at 3.9 μm. Our theory predicts that under this scheme sub-cycle THz pulses with multi-millijoule energies and record conversion efficiencies can be produced. Besides, we elucidate the origin of this high efficiency, which is made up of several factors, including a novel mechanism where the harmonics produced by the mid-infrared pulses strongly contribute to the field symmetry breaking and enhance the THz generation. In our experiments we verify the theoretical predictions by demonstrating ultrashort sub-cycle THz pulses with sub-millijoule energy and THz conversion efficiency of 2.36%, resulting in THz field amplitudes above 100 MV cm-1. Moreover, we show that these intense THz fields can drive nonlinear effects in bulk semiconductors (ZnSe and ZnTe) in free space and at room temperature. Our numerical simulations indicate that the observed THz yield can be significantly upscaled by further optimizing the experimental setup leading to even higher field strengths. Such intense THz pulses enable extreme field science, including into other, relativistic phenomena.