Ultrafast charge carrier dynamics in quantum confined 2D perovskite.

We studied the charge carrier dynamics in 2D perovskite NBT2PbI4 by ultrafast optical pump-THz probe spectroscopy. We observed a few ps long relaxation dynamics that can be ascribed to the band to band carrier recombination, in the absence of any contribution from many-body and trap assisted processes. The transient conductivity spectra show that the polaron dynamics is strongly modulated by the presence of a rich exciton population. The polarization field resulting from the exciton formation acts as the source of a restoring force that localizes polarons. This is revealed by the presence of a negative imaginary conductivity. Our results show that the dynamics of excitons in 2D perovskites at room temperature can be detected by monitoring their effect on the conductivity of the photoinduced polaronic carrier.

Femtosecond Laser-Micromachining of Glass Micro-Chip for High Order Harmonic Generation in Gases.

We report on the application of femtosecond laser micromachining to the fabrication of complex glass microdevices, for high-order harmonic generation in gas. The three-dimensional capabilities and extreme flexibility of femtosecond laser micromachining allow us to achieve accurate control of gas density inside the micrometer interaction channel. This device gives a considerable increase in harmonics' generation efficiency if compared with traditional harmonic generation in gas jets. We propose different chip geometries that allow the control of the gas density and driving field intensity inside the interaction channel to achieve quasi phase-matching conditions in the harmonic generation process. We believe that these glass micro-devices will pave the way to future downscaling of high-order harmonic generation beamlines.

Ultrafast THz Probe of Photoinduced Polarons in Lead-Halide Perovskites.

We study the nature of photoexcited charge carriers in CsPbBr_{3} nanocrystal thin films by ultrafast optical pump-THz probe spectroscopy. We observe a deviation from a pure Drude dispersion of the THz dielectric response that is ascribed to the polaronic nature of carriers; a transient blueshift of observed phonon frequencies is indicative of the coupling between photogenerated charges and stretching-bending modes of the deformed inorganic sublattice, as confirmed by DFT calculations.

Generation of deep ultraviolet sub-2-fs pulses.

We demonstrate the generation of few-cycle deep ultraviolet pulses via frequency upconversion of 5-fs near-infrared pulses in argon using a laser-fabricated gas cell. The measured spectrum extends from 210 to 340 nm, corresponding to a transform-limited pulse duration of 1.45 fs. We extract from a dispersion-free second-order cross-correlation measurement a pulse duration of 1.9 fs, defining a new record in the deep ultraviolet spectral range.

Fast stabilization of a high-energy ultrafast OPA with adaptive lenses.

The use of fast closed-loop adaptive optics has improved the performance of optical systems since its first application. Here we demonstrate the amplitude and carrier-envelope phase stabilization of a high energy IR optical parametric amplifier devoted to Attosecond Science exploiting two high speed adaptive optical systems for the correction of static and dynamic instabilities. The exploitation of multi actuator adaptive lenses allowed for a minimal impact on the optical setup.

Laser induced strong-field ionization gas jet tomography.

We introduce a novel in-situ strong field ionization tomography approach for characterizing the spatial density distribution of gas jets. We show that for typical intensities in high harmonic generation experiments, the strong field ionization mechanism used in our approach provides an improvement in the resolution close to factor of 2 (resolving about 8 times smaller voxel volume), when compared to linear/single-photon imaging modalities. We find, that while the depth of scan in linear tomography is limited by resolution loss due to the divergence of the driving laser beam, in the proposed approach the depth of focus is localized due to the inherent physical nature of strong-field interaction and discuss implications of these findings. We explore key aspects of the proposed method and compare it with commonly used single- and multi-photon imaging mechanisms. The proposed method will be particularly useful for strong field and attosecond science experiments.

Multidimensional high harmonic spectroscopy of polyatomic molecules: detecting sub-cycle laser-driven hole dynamics upon ionization in strong mid-IR laser fields.

High harmonic generation (HHG) spectroscopy has opened up a new frontier in ultrafast science, where electronic dynamics can be measured on an attosecond time scale. The strong laser field that triggers the high harmonic response also opens multiple quantum pathways for multielectron dynamics in molecules, resulting in a complex process of multielectron rearrangement during ionization. Using combined experimental and theoretical approaches, we show how multi-dimensional HHG spectroscopy can be used to detect and follow electronic dynamics of core rearrangement on sub-laser cycle time scales. We detect the signatures of laser-driven hole dynamics upon ionization and reconstruct the relative phases and amplitudes for relevant ionization channels in a CO2 molecule on a sub-cycle time scale. Reconstruction of channel-resolved complex ionization amplitudes on attosecond time scales has been a long-standing goal of high harmonic spectroscopy. Our study brings us one step closer to fulfilling this initial promise and developing robust schemes for sub-femtosecond imaging of multielectron rearrangement in complex molecular systems.

Active-grating monochromator for the spectral selection of ultrashort pulses.

Active gratings have been used to realize a grazing-incidence double-grating monochromator for the spectral selection of ultrashort pulses while preserving the temporal duration by compensating for the pulse-front tilt. The active grating consists of a bimorph deformable mirror on the top of which a diffraction grating with laminar profile is realized by UV lithography. The time-delay compensated configuration has been tested with ultrashort pulses at 800 nm. The feasibility of this configuration for the extreme-ultraviolet spectral region has been demonstrated by ray tracing studies.

Interplay between group-delay-dispersion-induced polarization gating and ionization to generate isolated attosecond pulses from multicycle lasers.

We implemented a new experimental scheme for the generation of single-shot extreme-UV continua that exploits a combination of transform-limited 15 fs, 800 nm pulses and chirped 35 fs, 800 nm pulses with orthogonal polarizations. Continua are interpreted as the formation of a single attosecond pulse and attributed to the interplay between polarization, ionization gating, and trajectory selection operated by suitable phase-matching conditions.

Intense femtosecond extreme ultraviolet pulses by using a time-delay-compensated monochromator.

Extreme-ultraviolet pulses, produced by high-order harmonic generation, have been spectrally selected by a time-delay-compensated grating monochromator. Temporal characterization of the harmonic pulses has been obtained using cross-correlation method: pulses as short as 8 fs, with high photon flux, have been measured at the output of the monochromator.

Frequency chirp of long electron quantum paths in high-order harmonic generation.

We report on the first experimental measurement of the spectral broadening of the harmonic emission associated with only the long electron quantum paths as a function of the driving pulse intensity. For such measurements we have estimated the chirp coefficient associated with the long quantum paths, within the strong-field approximation. This coefficient describes how the harmonic phase depends on the intensity of the driving laser field. The dependence of the chirp coefficient on the driving pulse intensity and on the harmonic order, which strongly influence the characteristics of the harmonic radiation, has been experimentally investigated. The experimental values turn out to be in excellent agreement with the results of numerical simulations based on the use of the nonadiabatic saddle-point method.

Optimization of high-order harmonic generation by adaptive control of a sub-10-fs pulse wave front.

We present a method for the optimization of high-order harmonic generation based on wave-front correction of the driving laser beam. The technique exploits wave-front adaptive control by means of a deformable mirror, governed by an optimization procedure.