Coherent Control of Vibrational State Population in a Nonpolar Molecule

A coherent control scheme for the population distribution in the vibrational states of nonpolar molecules is proposed. Our theoretical analysis and results of numerical simulations for the interaction of the hydrogen molecular ion in its electronic ground state with an infrared laser pulse reveal a selective two-photon transition between the vibrational states via a coupling with the first excited dissociative state. We demonstrate that for a given temporal intensity profile the population transfer between vibrational states, or a superposition of vibrational states, can be made complete for a single chirped pulse or a train of chirped pulses, which accounts for the accumulated phase difference due to the AC Stark effect. Effects of a spatial intensity (or, focal) averaging are discussed

Attosecond x-ray transient absorption in condensed-matter: a core-state-resolved Bloch model

Attosecond transient absorption is an ultrafast technique that has opened the possibility to study electron dynamics in condensed matter systems at its natural timescale. The extension to the x-ray regime permits one to use this powerful technique in combination with the characteristic element specificity of x-ray spectroscopy. At these timescales, the coherent effects of the electron transport are essential and have a relevant signature on the absorption spectrum. Typically, the complex light-driven dynamics requires a theoretical modeling for shedding light on the time-dependent changes in the spectrum. Here we construct a semiconductor Bloch equation model for resolving the light-induced and core-electron dynamics simultaneously, which enables to easily disentangle the interband and intraband contributions. By using the Bloch model, we demonstrate a universal feature on attosecond x-ray transient absorption spectra that emerges from the light-induced coherent intraband dynamics. This feature is linked to previous studies of light-induced Fano resonances in atomic systemsThis project has received funding from the European Union's Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie Grant Agreement No. 702565 as well as from Comunidad de Madrid through the TALENTO program with ref. 2017-T1/IND-5432. LP acknowledges support from Junta de Castilla y León (Project SA046U16) and MINECO (FIS2016-75652-P). JB acknowledges financial support from the Spanish Ministry of Economy and Competitiveness (MINECO), through the Severo Ochoa Programme for Centres of Excellence in R&D (SEV- 2015-0522) Fundació Cellex Barcelona and the CERCA Programme / Generalitat de Catalunya, the European Research Council for ERC Advanced Grant TRANSFORMER (788218), MINECO for Plan Nacional FIS2017-89536-P; AGAUR for 2017 SGR 1639 and Laserlab-Europe (EU-H2020 654148

Evolution of outer membrane beta-barrels from an ancestral beta beta hairpin.

Outer membrane β-barrels (OMBBs) are the major class of outer membrane proteins from Gram-negative bacteria, mitochondria, and plastids. Their transmembrane domains consist of 8–24 β-strands forming a closed, barrel-shaped β-sheet around a central pore. Despite their obvious structural regularity, evidence for an origin by duplication or for a common ancestry has not been found. We use three complementary approaches to show that all OMBBs from Gram-negative bacteria evolved from a single, ancestral ββ hairpin. First, we link almost all families of known single-chain bacterial OMBBs with each other through transitive profile searches. Second, we identify a clear repeat signature in the sequences of many OMBBs in which the repeating sequence unit coincides with the structural ββ hairpin repeat. Third, we show that the observed sequence similarity between OMBB hairpins cannot be explained by structural or membrane constraints on their sequences. The third approach addresses a longstanding problem in protein evolution: how to distinguish between a very remotely homologous relationship and the opposing scenario of “sequence convergence.” The origin of a diverse group of proteins from a single hairpin module supports the hypothesis that, around the time of transition from the RNA to the protein world, proteins arose by amplification and recombination of short peptide modules that had previously evolved as cofactors of RNAs

Above threshold ionization by few-cycle spatially inhomogeneous fields

We present theoretical studies of above threshold ionization (ATI) produced by spatially inhomogeneous fields. This kind of field appears as a result of the illumination of plasmonic nanostructures and metal nanoparticles with a short laser pulse. We use the time-dependent Schr\"odinger equation (TDSE) in reduced dimensions to understand and characterize the ATI features in these fields. It is demonstrated that the inhomogeneity of the laser electric field plays an important role in the ATI process and it produces appreciable modifications to the energy-resolved photoelectron spectra. In fact, our numerical simulations reveal that high energy electrons can be generated. Specifically, using a linear approximation for the spatial dependence of the enhanced plasmonic field and with a near infrared laser with intensities in the mid- 10^{14} W/cm^{2} range, we show it is possible to drive electrons with energies in the near-keV regime. Furthermore, we study how the carrier envelope phase influences the emission of ATI photoelectrons for few-cycle pulses. Our quantum mechanical calculations are supported by their classical counterparts

Three-wave mixing mediated femtosecond pulse compression in BBO

Nonlinear pulse compression mediated by three-wave mixing is demonstrated for ultrashort Ti:sapphire pulses in a type II phase-matched �β-barium borate (BBO) crystal using noncollinear geometry. 170 μJ pulses at 800 nm with a pulse duration of 74 fs are compressed at their sum frequency to 32 fs with 55 μJ of pulse energy. Experiments and computer simulations demonstrate the potential of sum-frequency pulse compression to match the group velocities of the interacting waves to crystals that were initially not considered in the context of nonlinear pulse compression.Peer ReviewedPostprint (author's final draft

Attosecond Streaking in the Water Window: A New Regime of Attosecond Pulse Characterization

We report on the first streaking measurement of water-window attosecond pulses generated via high harmonic generation, driven by sub-2-cycle, CEP-stable, 1850 nm laser pulses. Both the central photon energy and the energy bandwidth far exceed what has been demonstrated thus far, warranting the investigation of the attosecond streaking technique for the soft X-ray regime and the limits of the FROGCRAB retrieval algorithm under such conditions. We also discuss the problem of attochirp compensation and issues regarding much lower photo-ionization cross sections compared with the XUV in addition to the fact that several shells of target gases are accessed simultaneously. Based on our investigation, we caution that the vastly different conditions in the soft X-ray regime warrant a diligent examination of the fidelity of the measurement and the retrieval procedure.Comment: 14 Pages, 12 figure

Generation of intense, carrier-envelope phase-locked few-cycle laser pulses through filamentation

Intense, well-controlled light pulses with only a few optical cycles start to play a crucial role in many fields of physics, such as attosecond science. We present an extremely simple and robust technique to generate such carrier-envelope offset (CEO) phase locked few-cycle pulses, relying on self-guiding of intense 43-fs, 0.84mJ optical pulses during propagation in a transparent noble gas. We have demonstrated 5.7-fs, 0.38mJ pulses with an excellent spatial beam profile and discuss the potential for much shorter pulses. Numerical simulations confirm that filamentation is the mechanism responsible for pulse shortening. The method is widely applicable and much less sensitive to experimental conditions such as beam alignment, input pulse duration or gas pressure as compared to gas-filled hollow fiber

Single-shot dynamics of pulses from a gas-filled hollow fiber

We present measurements of the performance characteristics of few-cycle laser pulses generated by propagation through a gas-filled hollow fiber. The pulses going into the fiber and the compressed pulses after the fiber were simultaneously fully characterized shot-by-shot by using two kHz SPIDER setups and kHz pulse energy measurements. Output-pulse properties were found to be exceptionally stable and pulse characteristics relevant for non-linear applications like high-harmonic generation are discusse