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## Geração de harmônicos de pulsos laser de femtossegundo pela técnica de conversão de frequência em capilares preenchidos com gases nobres; Harmonics generation of femtosecond laser pulses by the technique of frequency conversion in noble gas filled capillaries

Siqueira, Jonathas de Paula
Fonte: Biblioteca Digitais de Teses e Dissertações da USP Publicador: Biblioteca Digitais de Teses e Dissertações da USP
Tipo: Tese de Doutorado Formato: application/pdf
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O propósito principal desta tese foi a implementação e estudo da geração de pulsos laser de femtossegundos em comprimentos de onda curtos (ultravioleta profundo, ultravioleta de vácuo e ultravioleta extremo) pela técnica de conversão de frequência em capilar preenchido com gás nobre. Esta técnica de conversão de frequência tem feito diversas contribuições nas últimas décadas para o avanço da geração de pulsos laser ultracurtos nesta região espectral. O desenvolvimento de tais fontes de luz coerente possui importantes implicações nos estudos de espectroscopia resolvida no tempo em átomos, moléculas e materiais. Através da implementação da técnica de conversão de frequência com casamento de fase em capilar preenchido com gás argônio, foi possível a obtenção de pulsos de femtossegundos centrados em 260 nm e 195 nm utilizando um sistema laser amplificado Ti: safira (780 nm, 1.5 mJ, 43 fs, 1 KHz). Estes comprimentos de onda correspondem, respectivamente, aos terceiro e quarto harmônicos da frequência fundamental do laser utilizado. Pulsos centrados em 260 nm com excelente perfil espacial, energias da ordem de microjoules e durações temporais tão curtas quanto 18 fs, possibilitadas pela recompressão por um par de prismas...

## Monitoring molecular dynamics using coherent electrons from high harmonic generation

Wagner, Nicholas L.; Wüest, Andrea; Christov, Ivan P.; Popmintchev, Tenio; Zhou, Xibin; Murnane, Margaret M.; Kapteyn, Henry C.
Tipo: Artigo de Revista Científica
EN
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We report a previously undescribed spectroscopic probe that makes use of electrons rescattered during the process of high-order harmonic generation. We excite coherent vibrations in SF6 using impulsive stimulated Raman scattering with a short laser pulse. A second, more intense laser pulse generates high-order harmonics of the fundamental laser, at wavelengths of ≈20–50 nm. The high-order harmonic yield is observed to oscillate, at frequencies corresponding to all of the Raman-active modes of SF6, with an asymmetric mode most visible. The data also show evidence of relaxation dynamics after impulsive excitation of the molecule. Theoretical modeling indicates that the high harmonic yield should be modulated by both Raman and infrared-active vibrational modes. Our results indicate that high harmonic generation is a very sensitive probe of vibrational dynamics and may yield more information simultaneously than conventional ultrafast spectroscopic techniques. Because the de Broglie wavelength of the recolliding electron is on the order of interatomic distances, i.e., ≈1.5 Å, small changes in the shape of the molecule lead to large changes in the high harmonic yield. This work therefore demonstrates a previously undescribed spectroscopic technique for probing ultrafast internal dynamics in molecules and...

## Oriented rotational wave-packet dynamics studies via high harmonic generation

Frumker, E.; Hebeisen, C. T.; Kajumba, N.; Bertrand, J. B.; Worner, H. J.; Spanner, M.; Villeneuve, D. M.; Naumov, A.; Corkum, P. B.
Tipo: Artigo de Revista Científica
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We produce oriented rotational wave packets in CO and measure their characteristics via high harmonic generation. The wavepacket is created using an intense, femtosecond laser pulse and its second harmonic. A delayed 800 nm pulse probes the wave packet, generating even-order high harmonics that arise from the broken symmetry induced by the orientation dynamics. The even-order harmonic radiation that we measure appears on a zero background, enabling us to accurately follow the temporal evolution of the wave packet. Our measurements reveal that, for the conditions optimum for harmonic generation, the orientation is produced by preferential ionization which depletes the sample of molecules of one orientation.

## A theory of intense-field dynamic alignment and high harmonic generation from coherently rotating molecules and interpretation of intense-field ultrafast pump-probe experiments

Abdurrouf, A.; Faisal, F. H. M.
Tipo: Artigo de Revista Científica
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A theory of ultra-fast pump-probe experiments proposed by us earlier [F.H.M. Faisal et al., Phys. Rev. Lett. 98, 143001 (2007) and F.H.M. Faisal and A. Abdurrouf, Phys. Rev. Lett. 100, 123005 (2008)] is developed here fully and applied to investigate the phenomena of dynamic alignment and high harmonic generation (HHG) from coherently rotating linear molecules. The theory provides essentially analytical results for the signals that allow us to investigate the simultaneous dependence of the HHG signals on the two externally available control parameters, namely, the relative angle between the polarizations, and the delay-time between the two pulses. It is applied to investigate the characteristics of high harmonic emission from nitrogen and oxygen molecules that have been observed experimentally in a number of laboratories. The results obtained both in the time-domain and in the frequency-domain are compared with the observed characteristics as well as directly with the data and are found to agree remarkably well. In addition we have predicted the existence of a "magic" polarization angle at which all modulations of the harmonic emission from nitrogen molecule changes to a steady emission at the harmonic frequency. Among other things we have also shown a correlation between the existence of the "magic" or critical polarization angles and the symmetry of the active molecular orbitals...

## Efficient output coupling of intracavity high harmonic generation

Yost, D. C.; Schibli, T. R.; Ye, Jun
Tipo: Artigo de Revista Científica
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We demonstrate a novel technique for coupling XUV harmonic radiation out of a femtosecond enhancement cavity. We use a small-period diffraction grating etched directly into the surface of a dielectric mirror. For the fundamental light, this element acts as a high reflector. For harmonic wavelengths, it acts as a diffraction grating, coupling XUV radiation out of the cavity. Using this method, we observed the 3rd through 21st odd harmonics with a dramatic increase in usable power over previous results of high harmonic generation at high repetition rates.; Comment: 3 pages, 2 figures

## High-harmonic generation and periodic level crossings: time profile and control

Faria, C. Figueira de Morisson; Rotter, I
Tipo: Artigo de Revista Científica
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We investigate high-harmonic generation in closed systems, using the two-level atom as a simplified model. By means of a windowed Fourier transform of the time-dependent dipole acceleration, we extract the main contributions to this process within a cycle of the driving field. We show that the patterns obtained can be understood by establishing a parallel between the two-level atom and the three-step model. In both models, high-harmonic generation is a consequence of a three-step process, which involves either the continuum and the ground state, or the adiabatic states of the two-level Hamiltonian. The knowledge of this physical mechanism allows us to manipulate the adiabatic states, and consequently the harmonic spectra, by means of a bichromatic driving field. Furthermore, using scaling laws, we establish sharp criteria for the invariance of the physical quantities involved. Consequently, our results can be extended to a broader parameter range, as for instance those characteristic of solid-state systems in strong fields.; Comment: 17 pages revtex, 15 figures (ps and eps files); figs. 1, 4, 6, 7, 10, 12 and 14 have been compressed due to memory problems

## Theory of plasmon-enhanced high-harmonic generation in the vicinity of metal nanostructures in noble gases

Husakou, A.; Im, S. -J.; Herrmann, J.
Tipo: Artigo de Revista Científica
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We present a semiclassical model for plasmon-enhanced high-harmonic generation (HHG) in the vicinity of metal nanostructures. We show that both the inhomogeneity of the enhanced local fields and electron absorption by the metal surface play an important role in the HHG process and lead to the generation of even harmonics and to a significantly increased cutoff. For the examples of silver-coated nanocones and bowtie antennas we predict that the required intensity reduces by up to three orders of magnitudes and the HHG cutoff increases by more than a factor of two. The study of the enhanced high-harmonic generation is connected with a finite-element simulation of the electric field enhancement due to the excitation of the plasmonic modes.; Comment: 4 figures

## Effective ATI Channels in High Harmonic Generation

Kuchiev, M. Yu.; Ostrovsky, V. N.
Tipo: Artigo de Revista Científica
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Harmonic generation by an atom in a laser field is described by the three-step mechanism as proceeding via above-threshold ionization (ATI) followed by the electron propagation in the laser-dressed continuum and the subsequent laser assisted recombination (LAR). An amplitude of harmonic production is given by the coherent sum of contributions from different intermediate ATI channels labeled by the number m of absorbed laser photons. The range of m-values that gives substantial contribution is explored and found to be rather broad for high harmonic generation. The coherence effects are of crucial importance being responsible for the characteristic pattern of harmonic intensities with a plateau domain followed by a cutoff region. Due to multiphoton nature of the process, an efficient summation of m-contributions can be carried out in the framework of the saddle point method. The saddle points correspond to some complex-valued labels m=m_c associated with the intermediate effective ATI channels in the three-step harmonic generation process. The advantage of this approach stems from the fact that summation over large number of conventional ATI m-channels is replaced by summation over small number of effective m_c-channels. The equation governing m_c has a transparent physical meaning: the electron ejected from the atom on the first (ATI) stage should return to the core to make LAR possible. The calculated rates are in good agreement with the results obtained by other approaches.; Comment: 26 pages...

## Theoretical studies of high-harmonic generation: Effects of symmetry, degeneracy and orientation

Tipo: Artigo de Revista Científica
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Using a quantum mechanical three-step model we present numerical calculations on the high-harmonic generation from four polyatomic molecules. Ethylene (C$_2$H$_4$) serves as an example where orbital symmetry directly affects the harmonic yield. We treat the case of methane (CH$_4$) to address the high-harmonic generation resulting from a molecule with degenerate orbitals. To this end we illustrate how the single orbital contributions show up in the total high-harmonic signal. This example illustrates the importance of adding coherently amplitude contributions from the individual degenerate orbitals. Finally, we study the high-harmonic generation from propane (C$_3$H$_8$) and butane (C$_4$H$_{10}$). These two molecules, being extended and far from spherical in structure, produce harmonics with non-trivial orientational dependencies. In particular, propane can be oriented so that very high-frequency harmonics are favorized, and thus the molecule contains prospects for the generation of UV attosecond pulses.; Comment: 9 pages, 6 figures, 1 table

## Optimal control of high-harmonic generation by intense few-cycle pulses

Solanpää, J.; Budagosky, J. A.; Shvetsov-Shilovski, N. I.; Castro, A.; Rubio, A.; Räsänen, E.
Tipo: Artigo de Revista Científica
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At the core of attosecond science lies the ability to generate laser pulses of sub-femtosecond duration. In tabletop devices the process relies on high-harmonic generation, where a major challenge is to obtain high yields and high cutoff energies required for the generation of attosecond pulses. We develop a computational method that can simultaneously resolve these issues by optimizing the driving pulses using quantum optimal control theory. Our target functional, an integral over the harmonic yield over a desired energy range, leads to a remarkable cutoff extension and yield enhancement for a one-dimensional model H-atom. The physical enhancement process is shown to be twofold: the cutoff extension is of classical origin, whereas the yield enhancement arises from increased tunneling probability. The scheme is directly applicable to more realistic models and, within straightforward refinements, also to experimental verification.

## Single-shot fluctuations in waveguided high-harmonic generation

Goh, S. J.; Tao, Y.; van der Slot, P. J. M.; Bastiaens, H. J. M.; Herek, J.; Biedron, S. G.; Danailov, M. B.; Milton, S. V.; Boller, K. -J.
Tipo: Artigo de Revista Científica
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For exploring the application potential of coherent soft x-ray (SXR) and extreme ultraviolet radiation (XUV) provided by high-harmonic generation, it is important to characterize the central output parameters. Of specific importance are pulse-to-pulse (shot-to-shot) fluctuations of the high-harmonic output energy, fluctuations of the direction of the emission (pointing instabilities), and fluctuations of the beam divergence and shape that reduce the spatial coherence. We present the first single-shot measurements of waveguided high-harmonic generation in a waveguided (capillary-based) geometry. Using a capillary waveguide filled with Argon gas as the nonlinear medium, we provide the first characterization of shot-to-shot fluctuations of the pulse energy, of the divergence and of the beam pointing. We record the strength of these fluctuations vs. two basic input parameters, which are the drive laser pulse energy and the gas pressure in the capillary waveguide. In correlation measurements between single-shot drive laser beam profiles and single-shot high-harmonic beam profiles we prove the absence of drive laser beam-pointing-induced fluctuations in the high-harmonic output. We attribute the main source of high-harmonic fluctuations to ionization-induced nonlinear mode mixing during propagation of the drive laser pulse inside the capillary waveguide.

## Near infrared few-cycle pulses for high harmonic generation

Driever, Steffen; Holzner, Konstantin B.; Delagnes, Jean-Christophe; Fedorov, Nikita; Arnold, Martin; Bigourd, Damien; Cormier, Eric; Guichard, Roland; Constant, Eric; Zair, Amelle
Tipo: Artigo de Revista Científica
Relevância na Pesquisa
67.86622%
We report on the development of tunable few-cycle pulses with central wavelengths from 1.6 um to 2 um. Theses pulses were used as a proof of principle for high harmonic generation in atomic and molecular targets. In order to generate such pulses we produced a filament in a 4 bar krypton cell. Spectral broadening by a factor of 2 to 3 of a 40 fs near infrared input pulse was achieved. The spectrally broadened output pulses were then compressed by fused silica plates down to the few-cycle regime close to the Fourier limit. The auto-correlation of these pulses revealed durations of about 3 cycles for all investigated central wavelengths. Pulses with a central wavelength of 1.7 um and up to 430 uJ energy per pulse were employed to generate high order harmonics in Xe, Ar and N2. Moving to near infrared few-cycle pulses opens the possibility to operate deeply in the non-perturbative regime with a Keldysh parameter smaller than 1. Hence, this source is suitable for the study of the non-adiabatic tunneling regime in most generating systems used for high order harmonic generation and attoscience.; Comment: 12 pages, 4 figures

## Quantum theory of a high harmonic generation as a three-step process

Kuchiev, M. Yu.; Ostrovsky, V. N.
Tipo: Artigo de Revista Científica
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Fully quantum treatment explicitly presents the high harmonic generation as a three-step process: (i) above threshold ionization (ATI) is followed by (ii) electron propagation in a laser-dressed continuum. Subsequently (iii) stimulated (or laser assisted) recombination brings the electron back into the initial state with emission of a high-energy photon. Contributions of all ATI channels add up coherently. All three stages of the process are described by simple, mostly analytical expressions that allow a detailed physical interpretation. A very good quantitative agreement with the previous calculations on the harmonic generation by H-minus ion is demonstrated, thus supplementing the conceptual significance of the theory with its practical efficiency. The virtue of the present scheme is further supported by a good accord between the calculations in length and velocity gauges for the high-energy photon.; Comment: Revtex 23 pages, 4 figures. Accepted for publication in Phys.Rev.A (1999)

## Multielectron High Harmonic Generation: simple man on a complex plane

Smirnova, Olga; Ivanov, Misha
Tipo: Artigo de Revista Científica
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From the famous classical "simple man" model to the recent multichannel model for polyatomic molecules, this tutorial will guide you through the several landmarks in our understanding of high harmonic generation and high harmonic spectroscopy. Our goal was to provide recipes and insights for modelling the harmonic response in various regimes, from the single active electron regime typical for noble gas atoms to the laser-driven attosecond hole dynamics in polyatomics. We have tried to pay particular attention to both simple recipes and their limitations, including the connection of real-valued classical and complex-valued quantum times and velocities. In addition to physical pictures, general approaches and their practical realizations, we have also tried to discuss some of the sticky technical issues, such as the possibility to factorize high harmonic response into the three steps of ionization, propagation and recombination and practical ways to treat strong field ionization, search for the saddle points of multi-dimensional integrals, deal with poles arising in the quantum-mechanical integrands, remove divergences appearing in approximate saddle point expressions, etc.; Comment: 55 pages, 16 figures, Book Chapter

## Does high harmonic generation conserve angular momentum?

Fleischer, Avner; Kfir, Ofer; Diskin, Tzvi; Sidorenko, Pavel; Cohen, Oren
Tipo: Artigo de Revista Científica
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High harmonic generation (HHG) is a unique and useful process in which infrared or visible radiation is frequency up converted into the extreme ultraviolet and x ray spectral regions. As a parametric process, high harmonic generation should conserve the radiation energy, momentum and angular momentum. Indeed, conservation of energy and momentum have been demonstrated. Angular momentum of optical beams can be divided into two components: orbital and spin (polarization). Orbital angular momentum is assumed to be conserved and recently observed deviations were attributed to propagation effects. On the other hand, conservation of spin angular momentum has thus far never been studied, neither experimentally nor theoretically. Here, we present the first study on the role of spin angular momentum in extreme nonlinear optics by experimentally generating high harmonics of bi chromatic elliptically polarized pump beams that interact with isotropic media. While observing that the selection rules qualitatively correspond to spin conservation, we unequivocally find that the process of converting pump photons into a single high-energy photon does not conserve angular momentum, i.e. this process is not self contained. In one regime, we numerically find that this major fundamental discrepancy can be explained if the harmonic photons are emitted in pairs. Yet in another regime...

## Theory of high harmonic generation in relativistic laser interaction with overdense plasma

Baeva, T.; Gordienko, S.; Pukhov, A.
Tipo: Artigo de Revista Científica
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High harmonic generation due to the interaction of a short ultra relativistic laser pulse with overdense plasma is studied analytically and numerically. On the basis of the ultra relativistic similarity theory we show that the high harmonic spectrum is universal, i.e. it does not depend on the interaction details. The spectrum includes the power law part $I_n\propto n^{-8/3}$ for $n<\sqrt{8\alpha}\gamma_{\max}^3$, followed by exponential decay. Here $\gamma_{\max}$ is the largest relativistic $\gamma$-factor of the plasma surface and $\alpha$ is the second derivative of the surface velocity at this moment. The high harmonic cutoff at $\propto \gamma_{\max}^3$ is parametrically larger than the $4 \gamma_{\max}^2$ predicted by the oscillating mirror'' model based on the Doppler effect. The cornerstone of our theory is the new physical phenomenon: spikes in the relativistic $\gamma$-factor of the plasma surface. These spikes define the high harmonic spectrum and lead to attosecond pulses in the reflected radiation.; Comment: 12 pages, 9 figures

## Exact solution for high harmonic generation and the response to an ac driving field for a charge density wave insulator

Shen, W. S.; Devereaux, T. P.; Freericks, J. K.
Tipo: Artigo de Revista Científica
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We develop and exactly solve a model for electrons driven by pulsed or continuous ac fields. The theory includes both the photoexcitation process as well as the subsequent acceleration of the electrons. In the case of an ac response, we examine both the nonequilibrium density of states and the current. In the case of pulsed light for high harmonic generation, we find the radiated light assumes a nearly universal behavior, with only limited dependence on the parameters of the system, except for the amplitude of the driving field, which determines the range of high harmonics generated and a tendency toward a narrowing of the peaks in a charge density wave versus a metal. This type of high harmonic generation can potentially be used for the creation of solid-state-based ultrafast light sources.; Comment: (11 pages, 11 figures, ReVTeX)

## Vacuum high harmonic generation in the shock regime

Böhl, P.; King, B.; Ruhl, H.
Tipo: Artigo de Revista Científica
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Electrodynamics becomes nonlinear and permits the self-interaction of fields when the quantised nature of vacuum states is taken into account. The effect on a plane probe pulse propagating through a stronger constant crossed background is calculated using numerical simulation and by analytically solving the corresponding wave equation. The electromagnetic shock resulting from vacuum high harmonic generation is investigated and a nonlinear shock parameter identified.; Comment: 19 pages, 16 figures

## A Novel-type Tunable and Narrowband Extreme Ultraviolet Radiation Source Based on High-harmonic Conversion of Picosecond Laser Pulses

Barkauskas, M; Brandi, F; Giammanco, F; Neshev, Dragomir; Pirri, A; Ubachs, Wim
Tipo: Artigo de Revista Científica
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At the Laser Centre Vrije Universiteit a table-top size, tunable and narrowband laser-based source of extreme ultraviolet radiation was developed using high-harmonic generation of powerful laser pulses of 300 ps duration and Fourier-transform limited bandwidth. The generated radiation has unprecedented spectral purity of λ/Δλ>2.5×105 at wavelengths covering the entire tunability range of 40-100 nm. The process of high-order harmonic generation was investigated in different gases (Ar, Kr, Xe, N 2) uncovering resonance phenomena for the conversion efficiency of specific harmonic orders.

## Density structure in low-order harmonic emission from laser-plasma interactions

Boyd,T.J.M.; Ondarza-Rovira,R.