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We show via numerical simulations that the regime of enhanced frequency chirp can be achieved in gas-filled multipass cells. Our results demonstrate that there exists a region of pulse and cell parameters for which a broad and flat spectrum with a smooth parabolic-like phase can be generated. This spectrum is compatible with clean ultrashort pulses, whose secondary structures are always below the 0.5% of its peak intensity such that the energy ratio (the energy contained within the main peak of the pulse) is above 98%. This regime makes multipass cell post-compression one of the most versatile schemes to sculpt a clean intense ultrashort optical pulse.
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We numerically investigate the regime of nonlinear pulse compression at mid-IR wavelengths in a multi-pass cell (MPC) containing a dielectric plate. This post-compression setup allows for ionization-free spectral broadening and self-compression while mitigating self-focusing effects. We find that self-compression occurs for a wide range of MPC and pulse parameters and derive scaling rules that enable its optimization. We also reveal the solitonic dynamics of the pulse propagation in the MPC and its limitations and show that spatiotemporal/spectral couplings can be mitigated for appropriately chosen parameters. In addition, we reveal the formation of spectral features akin to quasi-phase matched degenerate four-wave mixing. Finally, we present two case studies of self-compression at 3-µm and 6-µm wavelengths using pulse parameters compatible with driving high-field physics experiments. The simulations presented in this paper set a framework for future experimental work using few-cycle pulses at mid-IR wavelengths.
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The vision of using light to manipulate electronic and spin excitations in materials on their fundamental time and length scales requires new approaches in experiment and theory to observe and understand these excitations. The ultimate speed limit for all-optical manipulation requires control schemes for which the electronic or magnetic subsystems of the materials are coherently manipulated on the time scale of the laser excitation pulse. In our work, we provide experimental evidence of such a direct, ultrafast, and coherent spin transfer between two magnetic subsystems of an alloy of Fe and Ni. Our experimental findings are fully supported by time-dependent density functional theory simulations and, hence, suggest the possibility of coherently controlling spin dynamics on subfemtosecond time scales, i.e., the birth of the research area of attomagnetism.
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We present a theoretical analysis of the time-gated phase matching (ionization gating) mechanism in high-order harmonic generation for the isolation of attosecond pulses at near-infrared and mid-infrared driver wavelengths, for both few-cycle and multi-cycle driving laser pulses. Results of our high harmonic generation and three-dimensional propagation simulations show that broadband isolated pulses spanning from the extreme-ultraviolet well into the soft X-ray region of the spectrum can be generated for both few-cycle and multi-cycle laser pulses. We demonstrate the key role of absorption and group velocity matching for generating bright, isolated, attosecond pulses using long wavelength multi-cycle pulses. Finally, we show that this technique is robust against carrier-envelope phase and peak intensity variations.
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Capturing the dynamic electronic band structure of a correlated material presents a powerful capability for uncovering the complex couplings between the electronic and structural degrees of freedom. When combined with ultrafast laser excitation, new phases of matter can result, since far-from-equilibrium excited states are instantaneously populated. Here, we elucidate a general relation between ultrafast non-equilibrium electron dynamics and the size of the characteristic energy gap in a correlated electron material. We show that carrier multiplication via impact ionization can be one of the most important processes in a gapped material, and that the speed of carrier multiplication critically depends on the size of the energy gap. In the case of the charge-density wave material 1T-TiSe2, our data indicate that carrier multiplication and gap dynamics mutually amplify each other, which explains-on a microscopic level-the extremely fast response of this material to ultrafast optical excitation.
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Ultrafast high harmonic beams provide new opportunities for coherently controlling excitation and ionization processes in atoms, molecules, and materials on attosecond time scales by employing multiphoton two-pathway electron-wave-packet quantum interferences. Here we use spectrally tailored and frequency tuned vacuum and extreme ultraviolet harmonic combs, together with two phase-locked infrared laser fields, to show how the total single and double photoionization yields of argon can be coherently modulated by controlling the relative phases of both optical and electronic-wave-packet quantum interferences. This Letter is the first to apply quantum control techniques to double photoionization, which is a fundamental process where a single, high-energy photon ionizes two electrons simultaneously from an atom.
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We demonstrate theoretically that the temporal structure of high harmonic x-ray pulses generated with midinfrared lasers differs substantially from those generated with near-infrared pulses, especially at high photon energies. In particular, we show that, although the total width of the x-ray bursts spans femtosecond time scales, the pulse exhibits a zeptosecond structure due to the interference of high harmonic emission from multiple reencounters of the electron wave packet with the ion. Properly filtered and without any compensation of the chirp, regular subattosecond keV waveforms can be produced.
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Distinguishing insulators by the dominant type of interaction is a central problem in condensed matter physics. Basic models include the Bloch-Wilson and the Peierls insulator due to electron-lattice interactions, the Mott and the excitonic insulator caused by electron-electron interactions, and the Anderson insulator arising from electron-impurity interactions. In real materials, however, all the interactions are simultaneously present so that classification is often not straightforward. Here, we show that time- and angle-resolved photoemission spectroscopy can directly measure the melting times of electronic order parameters and thus identify-via systematic temporal discrimination of elementary electronic and structural processes-the dominant interaction. Specifically, we resolve the debates about the nature of two peculiar charge-density-wave states in the family of transition-metal dichalcogenides, and show that Rb intercalated 1T-TaS(2) is a Peierls insulator and that the ultrafast response of 1T-TiSe(2) is highly suggestive of an excitonic insulator.
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We show that high harmonic generation is the most sensitive probe of rotational wave packet revivals, revealing very high-order rotational revivals for the first time using any probe. By fitting high-quality experimental data to an exact theory of high harmonic generation from aligned molecules, we can extract the underlying electronic dipole elements for high harmonic emission and uncover that the electron gains angular momentum from the photon field.
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Atoms irradiated with combined femtosecond laser and extreme ultraviolet (XUV) fields ionize through multiphoton processes, even when the energy of the XUV photon is below the ionization potential. However, in the presence of two different XUV photons and an intense laser field, it is possible to induce full electromagnetic transparency. Taking helium as an example, the laser field modifies its electronic structure, while the presence of two different XUV photons and the laser field leads to two distinct ionization pathways that can interfere destructively. This work demonstrates a new approach for coherent control in a regime of highly excited states and strong optical fields.
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In rare-gas atoms, Auger decay in which an inner-valence shell ns hole is filled is not energetically allowed. However, in the presence of a strong laser field, a new laser-enabled Auger decay channel can open up to increase the double-ionization yield. This process is efficient at high laser intensities, where an ns hole can be filled within a few femtoseconds of its creation. This novel laser-enabled Auger decay process is of fundamental importance for controlling electron dynamics in atoms, molecules, and materials.
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We demonstrate an experimental control of electron localization in deuterium molecular ions created and dissociated by the combined action of an attosecond pulse train and a many-cycle infrared (IR) pulse. The attosecond pulse train is synthesized using both even and odd high order harmonics of the driving IR frequency so that it can strobe the IR field once per IR cycle. An asymmetric ejection of the deuterium ions oscillates with the full IR period when the APT-IR time-delay is scanned. The observed control is due to the creation of a coherent superposition of 1s sigma{g} and 2p sigma{u} states via interference between one-photon and two-photon dissociation channels.
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We demonstrate fully phase-matched high harmonic emission spanning the water window spectral region important for nano- and bioimaging and a breadth of materials and molecular dynamics studies. We also generate the broadest bright coherent bandwidth (≈300 eV) to date from any light source, small or large, that is consistent with a single subfemtosecond burst. The harmonic photon flux at 0.5 keV is 10³ higher than demonstrated previously. This work extends bright, spatially coherent, attosecond pulses into the soft x-ray region for the first time.
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By combining laser pulse self-compression and high harmonic generation within a single waveguide, we demonstrate high harmonic emission from multiply charged ions for the first time. This approach enhances the laser intensity and counteracts ionization-induced defocusing, extending the cutoff photon energy in argon above 500 eV for the first time, with higher spectral intensity and cutoff energy than He for the same input laser parameters. This Letter demonstrates a pathway for extending high harmonic emission to very high photon energies using large, multiply charged, ions with high ionization potentials.
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By focusing a high repetition rate (50 kHz), compact, femtosecond laser system with low pulse energy (25 muJ) using a tight-focusing geometry, we demonstrate fully phase matched high-order harmonic generation for the first time at very high repetition rates, resulting in EUV light with full spatial coherence. The result is a practical, single-box, coherent source useful for applications in metrology, ultrafast spectroscopy, imaging and microscopy. The soft x-ray flux can be improved further by increasing the laser pulse energy and/or repetition rate.
Assuntos
Lasers , Desenho Assistido por Computador , Desenho de Equipamento , Análise de Falha de Equipamento , Reprodutibilidade dos Testes , Sensibilidade e EspecificidadeRESUMO
We present what we believe to be the first implementation of Fourier transform (FT) holography using a tabletop coherent x-ray source. By applying curvature correction to compensate for the large angles inherent in high-NA coherent imaging, we achieve image resolution of 89 nm using high-harmonic beams at a wavelength of 29 nm. Moreover, by combining holography with iterative phase retrieval, we improve the image resolution to <53 nm. We also demonstrate that FT holography can be used effectively with short exposure times of 30 s. This technique will enable biological and materials microscopy with simultaneously high spatial and temporal resolution on a tabletop soft-x-ray source.
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The generation of attosecond-duration light pulses using the high-order harmonic generation process is a rapidly evolving area of research. In this work, we combine experimental measurements with careful numerical analysis, to demonstrate that even relatively long-duration, 15 fs, carrier-envelope-phase (CEP) unstabilized near-infrared (NIR) pulses can generate isolated attosecond extreme-ultraviolet (EUV) pulses by the dynamically-changing phase matching conditions in a hollow-core waveguide geometry. The measurements are made using the laser-assisted photoelectric effect to cross-correlate the EUV pulse with the NIR pulse. A FROG CRAB analysis of the resulting traces (photoelectron signal versus photoelectron energy and EUV-NIR delay) is performed using a generalized projections (GP) algorithm, adapted for a wide-angle photoelectron detection geometry and non-CEP stabilized driving laser pulses. In addition, we performed direct FROG CRAB simulations under the same conditions. Such direct simulations allow more freedom to explore the effect of specific pulse parameters on FROG CRAB traces than is possible using the automated GP retrieval algorithm. Our analysis shows that an isolated pulse with duration of approximately 200 attoseconds can result from CEP unstabilized, high intensity approximately 15 fs multi-cycle driving pulses coupled into a hollow-core waveguide filled with low-pressure Argon gas. These are significantly longer driving pulses than used in other experimental implementations of isolated attosecond pulses.
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The coupling between electronic states in a surface-adsorbate system is fundamental to the understanding of many surface interactions. In this Letter, we present the first direct time-resolved observations of the lifetime of core-excited states of an atom adsorbed onto a surface. By comparing laser-assisted photoemission from a substrate with a delayed Auger decay process from an adsorbate, we measure the lifetime of the 4d(-1) core level of xenon on Pt(111) to be 7.1+/-1.1 fs. This result opens up time-domain measurements of surface dynamics where energy-resolved measurements may provide incomplete information.
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We extend all-optical quasi-phase matching of high-order harmonic generation into spectral regions where conventional phase matching is not possible. The high laser intensities required to generate harmonics at energy >130 eV, coupled with the resulting high level of ionization, preclude conventional phase matching in all nonlinear media. Selective enhancement factors between 40 and 150 in the flux of harmonics at photon energies around 140 eV are demonstrated using a train of two counterpropagating pulses.
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An experimental setup for time- and angle-resolved photoemission spectroscopy using a femtosecond 1 kHz high harmonic light source and a two-dimensional electron analyzer for parallel energy and momentum detection is presented. A selection of the 27th harmonic (41.85 eV) from the harmonic spectrum of the light source is achieved with a multilayer MoSi double mirror monochromator. The extinction efficiency of the monochromator in selecting this harmonic is shown to be better than 7:1, while the transmitted bandwidth of the selected harmonic is capable of supporting temporal pulse widths as short as 3 fs. The recorded E(k) photoelectron spectrum from a Cu(111) surface demonstrates an angular resolution of better than 0.6 degrees (=0.03 A(-1) at E(kin,e)=36 eV). Used in a pump-probe configuration, the described experimental setup represents a powerful experimental tool for studying the femtosecond dynamics of ultrafast surface processes in real time.