Ultrashort Extreme Ultraviolet Pulses Research Articles

FEL Pulse Duration Evolution along Undulators at FLASH

Self-amplified spontaneous-emission (SASE) free-electron lasers (FELs) deliver ultrashort pulses with femtosecond durations. Due to the fluctuating nature of the radiation properties of SASE FELs, characterizing FEL pulses on a single-shot basis is necessary. Therefore, we use terahertz streaking to characterize the temporal properties of ultrashort extreme ultraviolet pulses from the free-electron laser in Hamburg (FLASH). In this study, pulse duration as well as pulse energy are measured in a wavelength range from 8 to 34 nm as functions of undulators contributing to the lasing process. The results are compared to one-dimensional and three-dimensional, time-dependent FEL simulations.

Optimization of pulse self-compression in hollow capillary fibers using decreasing pressure gradients.

The improvement of techniques for the generation of near-infrared (NIR) few-cycle pulses is paving the way for new scenarios in time-resolved spectroscopy and the generation of ultrashort extreme-ultraviolet pulses through high-harmonic generation. In this work, we numerically study how to optimize the self-compression of NIR pulses using decreasing pressure gradients in hollow capillary fibers (HCFs). We identify a moderate nonlinear regime in which sub-cycle pulses are obtained with very good temporal quality from an input 30 fs pulse centered at a 800 nm wavelength and coupled as the fundamental mode of an argon-filled HCF fully evacuated at the output end. Surprisingly, we observe that there is a relatively broad region of parameters for which the optimum self-compression takes place, defined by a simple relation between the input pulse energy and the initial gas pressure.

Real-Time Probing of an Atmospheric Photochemical Reaction by Ultrashort Extreme Ultraviolet Pulses: Nitrous Acid Release from o-Nitrophenol.

Photolysis of o-nitrophenol, contained in brown carbon, is considered to be a major process for the generation of nitrous acid (HONO) in the atmosphere. In this Letter, we used time-resolved photoelectron spectroscopy with 29.5 eV probe pulses and ab initio calculations to disentangle all reaction steps from the excitation to the dissociation of HONO. After excitation, intersystem crossing to the triplet manifold follows ultrafast excited-state intramolecular hydrogen transfer, where the molecules deplanarizes and finally splits off HONO after 0.5-1 ps.

A solid look at molecules

When molecular model systems, such as polycyclic aromatic hydrocarbons, are ionized by ultrashort extreme ultraviolet pulses, their relaxation path proceeds via electron–phonon scattering, linking molecules to typical solid-state matter behaviour.

Single-shot temporal characterization of XUV pulses with duration from ∼10 fs to ∼350 fs at FLASH

Ultra-short extreme ultraviolet pulses from the free-electron laser FLASH are characterized using terahertz-field driven streaking. Measurements at different ultra-short extreme ultraviolet wavelengths and pulse durations as well as numerical simulations were performed to explore the application range and accuracy of the method. For the simulation of streaking, a standard classical approach is used which is compared to quantum mechanical theory, based on strong field approximation. Various factors limiting the temporal resolution of the presented terahertz streaking setup are investigated and discussed. Special attention is paid to the cases of very short (∼10 fs) and long (up to ∼350 fs) pulses.

Delayed Relaxation of Highly Excited Cationic States in Naphthalene.

Rapid energy transfer from electronic to nuclear degrees of freedom underlies many biological processes and astrophysical observations. The efficiency of this energy transfer depends strongly on the complex interplay between electronic and nuclear motions. In this study, we report two-color pump-probe experiments that probe the relaxation dynamics of highly excited cationic states of naphthalene, a prototypical polycyclic aromatic hydrocarbon molecule, which are produced using wavelength-selected, ultrashort extreme ultraviolet pulses. Surprisingly, the relaxation lifetimes increase with the cationic excitation energy. We postulate that the observed effect is the result of a population trapping that leads to delayed relaxation.

Electron correlation\xa0driven non-adiabatic relaxation in molecules excited by an ultrashort extreme ultraviolet pulse

The many-body quantum nature of molecules determines their static and dynamic properties, but remains the main obstacle in their accurate description. Ultrashort extreme ultraviolet pulses offer a means to reveal molecular dynamics at ultrashort timescales. Here, we report the use of time-resolved electron-momentum imaging combined with extreme ultraviolet attosecond pulses to study highly excited organic molecules. We measure relaxation timescales that increase with the state energy. High-level quantum calculations show these dynamics are intrinsic to the time-dependent many-body molecular wavefunction, in which multi-electronic and non-Born−Oppenheimer effects are fully entangled. Hints of coherent vibronic dynamics, which persist despite the molecular complexity and high-energy excitation, are also observed. These results offer opportunities to understand the molecular dynamics of highly excited species involved in radiation damage and astrochemistry, and the role of quantum mechanical effects in these contexts.

A Special Section on X-ray and Extreme Ultraviolet Multilayer Coatings.

Soft X-ray and Extreme Ultraviolet (EUV) radiation (defined as light with wavelength in the 1 to 100 nm range) has been playing a growing role in major scientific and industrial applications over the last 20 years: astrophysics and solar physics, materials sciences, biology, semiconductor industry, plasma diagnostics. Especially the emergence of novel EUV/X-ray sources with unprecedented brightness and coherence (4th generation synchrotrons, free-electron lasers, tabletop lasers, high-harmonic generation and attosecond sources) has ushered a new era in the fields of materials science, chemistry, plasma physics, biology and life sciences. Several scientific and technological breakthroughs have been achieved recently. X-ray radiation from the SPRING-8 synchrotron light source in Japan has been focused on a spot with diameter smaller than 10 nm; this constitutes the smallest spot of light ever produced and could enable studies with the most exquisite spatial resolution. The generation of ultrashort EUV pulses with a duration less than 0.1 femtosecond (= 100 attosec-onds) made it possible for the first time to observe electron orbitals in molecules. Photolithography scanners based on EUV light have entered the world of semiconductor manufacturing in order to produce the next generation of computer chips. In 2007, the EUV telescopes aboard NASA's Solar Terrestrial Relations Observatory (STEREO) mission provided the first 3D images of the solar corona with its protuberances. Furthermore, since 2010, the Solar Dynamics Observatory (SDO), NASA's most advanced solar mission , has been continuously transmitting full-disk images of the solar corona every 10 seconds, simultaneously at 7 EUV wavelengths with 1 arcsec resolution. Observing the Sun with such unprecedented temporal and spatial resolution has led to groundbreaking discoveries related to the Sun's extremely complex magnetic field and has led to better understanding of extreme events such as solar flares and coronal mass ejections, which can seriously affect earth and space environments. These breakthroughs have been enabled by the development of new optical components dedicated to the EUV/ X-ray spectral range. The main challenges in fabricating EUV/X-ray optics come from the properties of materials in this spectral range. With the refractive index of any material being very close to 1, the refractive phenomena at any interface are weak and the reflectivity of any single material at non-grazing incidence angles is near zero. Moreover, all materials strongly absorb X-rays, so the transmission of any component is almost zero. Multi-layer interference mirrors are enabling optical components in most EUV/X-ray optical systems. Demonstrated experimentally for the first time in the 1970s by E. Spiller, these mirrors consist of periodic or aperiodic structures of alternating thin film layers of 2 or more materials with nanometer-scale thickness, deposited on an optical sub-strate. The constructive interference between the layers results in efficient reflectance at EUV/X-ray wavelengths even at near-normal incidence angles thus enabling the operation of a wide range of optical components including imaging and illumination systems, reflective filters, grating spectrometers and polarizers. However, the fabrication of high-performance multi-layer coatings poses serious technical challenges. Multi-layer coatings need to obey several stringent (and often conflicting) requirements, including: (i) contain materials with good optical contrast in the wavelength region of operation (ii) contain tens or hundreds of layers with nanometer-scale thickness, where each layer is deposited with picometer-scale precision (iii) form stable layer interfaces with minimal interdiffusion and with smoothness on the order of the atomic dimension, (iv) have low thin film stress, (v) have stable reflective performance for periods up to 10 years, or even longer. This special section aims to provide a survey of current topics and major development lines in the very active research area of X-ray and EUV multilayer coating development. It gathers studies of the properties of these nanoscale structures (microstructure, mechanical stress, lifetime stability) with a focus on new promising material combinations and on short-period multilay-ers, with individual layer thicknesses around (or less than) 1 nm. Technological developments, new characterization 516

Observation of autoionization dynamics and sub-cycle quantum beating in electronic molecular wave packets

The coherent interaction with ultrashort light pulses is a powerful strategy for monitoring and controlling the dynamics of wave packets in all states of matter. As light presents an oscillation period of a few femtoseconds (T = 2.6 fs in the near infrared spectral range), an external optical field can induce changes in a medium on the sub-cycle timescale, i.e. in a few hundred attoseconds. In this work, we resolve the dynamics of autoionizing states on the femtosecond timescale and observe the sub-cycle evolution of a coherent electronic wave packet in a diatomic molecule, exploiting a tunable ultrashort extreme ultraviolet pulse and a synchronized infrared field. The experimental observations are based on measuring the variations of the extreme ultraviolet radiation transmitted through the molecular gas. The different mechanisms contributing to the wave packet dynamics are investigated through theoretical simulations and a simple three level model. The method is general and can be extended to the investigation of more complex systems.

Criterion for Distinguishing Sequential from Nonsequential Contributions to the Double Ionization of Helium in Ultrashort Extreme-Ultraviolet Pulses.

We quantify sequential and nonsequential contributions in two-photon double ionization of helium atoms by intense ultrashort extreme-ultraviolet pulses with central photon energies ℏω_{ctr} near the sequential double-ionization threshold. If the spectrum of such pulses overlaps both the sequential (ℏω>54.4 eV) and nonsequential (ℏω<54.4 eV) double-ionization regimes, the sequential and nonsequential double-ionization mechanisms are difficult to distinguish. By tracking the double-ionization asymmetry in joint photoelectron angular distributions, we introduce the two-electron forward-backward-emission asymmetry as a measure that allows the distinction of sequential and nonsequential contributions. Specifically, for ℏω_{ctr}=50 eV pulses with a sine-squared temporal profile, we find that the sequential double-ionization contribution is the largest at a pulse length of 650 as, due to competing temporal and spectral constraints. In addition, we validate a simple heuristic expression for the sequential double-ionization contribution in comparison with ab initio calculations.

Ultrafast near-field enhancement dynamics in a resonance-mismatched nanorod excited by temporally shaped femtosecond laser double pulses

The spatial–temporal dynamics of the near e-field enhancement in a resonance-mismatched nanorod irradiated by the femtosecond laser double pulses is theoretically investigated. A model combining the non-equilibrium electron excitation dynamics and the near field scattering was built for well exploring ultrafast dynamics of the e-field enhancement around the nanorod. It is revealed that the average enhancement factor can be evidently improved with increasing the double pulses separation. The energy ratio of the temporally shaped double pulses with respect to the highest enhancement factor shows an evident decrease with the increasing the total laser fluence. In addition, the most evident promotion of average enhancement factor from 51.2 to 78.8 can be acquired under laser fluence of 0.7Fth, which could be attributed to the temperature modulation of electron states excited by the temporally shaped double pulses. The study provides the base for understanding ultrafast plasmon dynamics for advancing the applications such as fs super-resolution fabrication, fs near field imaging and the generation of ultrashort extreme-ultraviolet pulses.

Quantum-mechanical simulation of attosecond streaked photoemission from Mg-covered W(110) surfaces

SynopsisWe apply a quantum-mechanical model to simulate infrared-streaked photoelectron emission by an ultrashort extreme ultraviolet pulse from adsorbate-covered metal surfaces. Incorporating effects of energy- dependent electron mean-free paths, the properties of initial states, photoelectron energy dispersion, and the screening of the streaking field, this model is able to reproduce recently measured photoelectron spectrograms and adsorbate-thickness-dependent photoemission time delays.

Generation of ultrashort extreme-ultraviolet pulses by enhanced plasmonic near-fields in metallic nanoparticles

We investigate high-order harmonic generation in a metallic-nanoparticle–quantum-dot hybrid system. Driven by a moderate electric field intensity Guassian-shape few-cycle pulse which is chirped by a hyperbolic-tangent-form carrier envelope phase, the hybrid system can generate extreme-ultraviolet super-continuum harmonics (13.3 eV maximal photon energy) and isolated ultrashort pulses ( FWHM). Numerical simulation results reveal that the plasmonic field enhancement could extend the cutoff order and continuum region in harmonic spectra. The extension effect by plasmonic enhancement could be well understood theoretically by the semi-classical two-level atom model.

Compression of Extreme-Ultraviolet Ultrashort Pulses by Grating Configurations

The design and realization of grating instruments to condition the spectral phase of ultrashort extreme-ultraviolet pulses are discussed. The main application of such configurations is the temporal compression of pulses by compensating the phase chirp and getting close to the Fourier limit. We discuss the two configurations useful for the realization of ultrafast grating compressors, namely, the classical diffraction mount and the off-plane one. The configuration may be applied to free-electron lasers and high-order laser harmonics.

Development of experimental techniques for the characterization of ultrashort photon pulses of extreme ultraviolet free-electron lasers

One of the most challenging tasks for extreme ultraviolet, soft and hard x-ray free-electron laser photon diagnostics is the precise determination of the photon pulse duration, which is typically in the sub 100 fs range. Nine different methods, able to determine such ultrashort photon pulse durations, were compared experimentally at FLASH, the self-amplified spontaneous emission free-electron laser at DESY in Hamburg, in order to identify advantages and disadvantages of different methods. Radiation pulses at a wavelength of 13.5 and 24.0 nm together with the corresponding electron bunch duration were measured by indirect methods like analyzing spectral correlations, statistical fluctuations, and energy modulations of the electron bunch and also by direct methods like autocorrelation techniques, terahertz streaking, or reflectivity changes of solid state samples. In this paper, we present a comprehensive overview of the various techniques and a comparison of the individual experimental results. The information gained is of utmost importance for the future development of reliable pulse duration monitors indispensable for successful experiments with ultrashort extreme ultraviolet pulses.9 MoreReceived 16 July 2014DOI:https://doi.org/10.1103/PhysRevSTAB.17.120702This article is available under the terms of the Creative Commons Attribution 3.0 License. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.Published by the American Physical Society

Resolving the enhanced nonlinear double excitation of helium in intense ultra-short extreme-ultraviolet pulses

We present a theoretical study for multiphoton double excitation of He atoms exposed to an intense ul-trashort extreme-ultraviolet (EUV) pulse, where the photon energy coincides with the transition energy from the ground state to a Rydberg state. We identify the mechanism of the enhanced three-photon absorption probability as observed in the experiment.

Resonance-enhanced three-photon single ionization of Ne by ultrashort extreme-ultraviolet pulses

Time-resolved extreme-ultraviolet (EUV) fluorescence spectroscopy has been applied to study the multi-photon, single ionization of Ne irradiated by intense EUV-free-electron laser (FEL) pulses at a wavelength of 51 nm. A broad, intense peak at a wavelength of around 46 nm is observed, which is shorter than the incident FEL wavelength. The time dependence of the fluorescence reveals that the peak has two unresolved components, which we attribute to the decay of the excited ion states Ne+ 2s−1(2S) and 2p−2(3Pe)3s(2Pe) at 46.0 and 44.6 nm. From the observed intensity ratios and fluorescence lifetimes we conclude that the Ne+ 2p−2(3Pe)3s(2Pe) state is populated by two-photon resonance enhancement, via a 2p43p2 doubly excited state of Ne.

Two-electron dynamics in nonlinear double excitation of helium by intense ultrashort extreme-ultraviolet pulses

We present a theoretical study for multiphoton double excitation of He atoms exposed to an intense ultrashort extreme-ultraviolet (EUV) pulse, where the photon energy coincides with the transition energy from the ground state to a Rydberg state, by solving the time-dependent Schr\odinger equation in the hyperspherical coordinates. Photoelectron spectra under the conditions comparable with a recent experiment [Hishikawa et al., Phys. Rev. Lett. 107, 243003 (2011)] are calculated and analyzed. We identify the mechanism of the enhanced three-photon absorption probability which is more than one order of magnitude larger than that for the two-photon process in accordance with the experiment. The enhancement is attributed to a propensity rule for double excitation in a two-step mechanism, in which a one-photon absorption by one electron to a Rydberg state is followed by a two-photon absorption by the other electron to an excited orbital, while the first electron remains at nearly the same principle quantum number. Based on the time-dependent perturbation theory, the three-photon absorption probability exhibits peculiar cubic dependence on the pulse duration due to the propensity rule, in contrast to the linear dependence of the two-photon absorption probability. Thus a crossover between the two- and three-photon absorption probabilities takes place for sufficiently intense and long pulses. We also study the time evolution of a doubly excited two-electron wave packet created by an intense ultrashort EUV pulse efficiently using the same enhancement scheme, opening up the possibility of visualizing the correlated motion of two electrons in the time domain.

Imaging molecular structures with high-energy photoelectrons produced by extreme ultraviolet pulses

We have investigated the diffraction spectra of photoelectrons from one-photon single ionization of diatomic molecules by ultrashort extreme ultraviolet pulses. The result shows that the diffraction patterns strongly depend on the internuclear distances of molecules. With these diffraction patterns, we succeed in measuring the transient internuclear distances of small-distance molecules with a high precision. This provides a simple and efficient method for imaging molecular transient structures, avoiding the complicated recovering process of the diffraction pattern in the imaging with rescattered electrons.

Competition of Resonant and Nonresonant Paths in Resonance-Enhanced Two-Photon Single Ionization of He by an Ultrashort Extreme-Ultraviolet Pulse

We theoretically study the pulse-width dependence of the photoelectron angular distribution (PAD) from the resonance-enhanced two-photon single ionization of He by femtosecond (≲20 fs) extreme-ultraviolet pulses, based on the time-dependent perturbation theory and simulations with the full time-dependent Schrödinger equation. In particular, we focus on the competition between resonant and nonresonant ionization paths, which leads to the relative phase δ between the S and D wave packets distinct from the corresponding scattering phase shift difference. When the spectrally broadened pulse is resonant with an excited level, the competition varies with pulse width, and, therefore, δ and the PAD also change with it. On the other hand, when the Rydberg manifold is excited, δ and the PAD do not much vary with the pulse width, except for the very short-pulse regime.