Streaking of 43-attosecond soft-X-ray pulses generated by a passively CEP-stable mid-infrared driver

Optics Express, Journal Year: 2017, Volume and Issue: 25(22), P. 27506 - 27506

Published: Oct. 24, 2017

Attosecond metrology has so far largely remained limited to titanium:sapphire lasers combined with an active stabilization of the carrier-envelope phase (CEP).These sources limit achievable photon energy ∼100 eV which is too low access X-ray absorption edges most second-and third-row elements are central chemistry, biology and material science.Therefore, intense efforts underway extend attosecond soft-X-ray (SXR) domain using mid-infrared (mid-IR) drivers.Here, we introduce experimentally demonstrate a method that solves long-standing problem complete temporal characterization ultrabroadband ( 10 eV) pulses.We generalize recently proposed Volkov-transform generalized projection algorithm (VTGPA) case multiple overlapping photoelectron spectra its application isolated pulses.This new approach overcomes all key limitations previous attosecond-pulse reconstruction methods, in particular central-momentum approximation (CMA), it incorporates physical, complex-valued energy-dependent photoionization matrix elements.These properties make our general particularly suitable for supercontinua arbitrary bandwidth.We apply this SXR pulses generated from two-cycle mid-IR driver, covering bandwidth reaching energies up 180 eV.We extract pulse duration (43±1) as streaking measurements, defining world record.Our results prove popular broadly available scheme post-compressing output white-lightseeded optical parametric amplifiers adequate produce high-contrast L-edges silicon, phosphorous sulfur.Our experimental open path production lasting less than one atomic unit time (24 as) light elements.

Language: Английский

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Attosecond Electron Dynamics in Molecules

Chemical Reviews, Journal Year: 2017, Volume and Issue: 117(16), P. 10760 - 10825

Published: May 10, 2017

Advances in attosecond science have led to a wealth of important discoveries atomic, molecular, and solid-state physics are progressively directing their footsteps toward problems chemical interest. Relevant technical achievements the generation application extreme-ultraviolet subfemtosecond pulses, introduction experimental techniques able follow time electron dynamics quantum systems, development sophisticated theoretical methods for interpretation outcomes such experiments raised continuous growing interest phenomena, as demonstrated by vast literature on subject. In this review, after introducing physical mechanisms at basis pulse technology describing tools that complement research field, we will concentrate investigation ultrafast processes molecules, with emphasis molecules biological The measurement control electronic motion complex molecular structures is formidable challenge, both theory experiment, but indubitably tremendous impact chemistry years come.

Language: Английский

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Advances in attosecond science

Journal of Physics B Atomic Molecular and Optical Physics, Journal Year: 2016, Volume and Issue: 49(6), P. 062001 - 062001

Published: Feb. 22, 2016

Attosecond science offers formidable tools for the investigation of electronic processes at heart important physical in atomic, molecular and solid-state physics. In last 15 years impressive advances have been obtained from both experimental theoretical points view. pulses, form isolated pulses or trains are now routinely available various laboratories. this review recent attosecond reported applications discussed. After a brief presentation techniques that can be employed generation diagnosis sub-femtosecond condensed-matter

Language: Английский

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Roadmap of ultrafast x-ray atomic and molecular physics

Journal of Physics B Atomic Molecular and Optical Physics, Journal Year: 2018, Volume and Issue: 51(3), P. 032003 - 032003

Published: Jan. 9, 2018

X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field ultrafast x-ray atomic molecular physics, largely due to an explosive growth in capabilities past decade. XFELs now provide unprecedented intensity (1020 W cm−2) at wavelengths down ∼1 Ångstrom, HHG provides time resolution (∼50 attoseconds) a correspondingly large coherent bandwidth longer wavelengths. For context, timescales can be referenced Bohr orbital period hydrogen atom 150 attoseconds hydrogen-molecule vibrational 8 femtoseconds; wavelength scales chemically significant carbon K-edge photon energy ∼280 eV (44 Ångstroms) bond length methane Ångstrom. With these modern one has ability focus on individual atoms, even when embedded complex molecule, view electronic nuclear motion their intrinsic (attoseconds Ångstroms). These enabled diffractive imaging, where image non-crystalline objects three dimensions timescales, potentially with resolution. The available opened new fields multiphoton nonlinear physics behavior matter under extreme conditions explored. pulse synchronization provided by kindled fundamental investigations delays photoionization, charge migration molecules, dynamics near conical intersections that are foundational AMO chemistry. This roadmap coincides year XFEL facilities, operating Ångstrom wavelengths, for users (European XFEL, Swiss-FEL PAL-FEL Korea) almost doubling present worldwide number XFELs, documents remarkable progress since its discovery roughly 30 years ago, showcasing experiments other applications. Here we capture perspectives 17 leading groups organize contributions into four categories: dynamics, multidimensional spectroscopies; high-intensity phenomena; attosecond science.

Language: Английский

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The ultrafast X-ray spectroscopic revolution in chemical dynamics

Nature Reviews Chemistry, Journal Year: 2018, Volume and Issue: 2(6), P. 82 - 94

Published: May 29, 2018

Language: Английский

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Quantum control of molecular rotation

Reviews of Modern Physics, Journal Year: 2019, Volume and Issue: 91(3)

Published: Sept. 18, 2019

Rotation is a fundamental degree of freedom isolated molecules and property that affects their interaction with other physical systems. This article reviews theory multitude experimental methods aiming to control molecular rotation. Applications include studies variety single particle quantum phenomena, controlled collisions, rotational dynamics in solvents, as well the perspective use long distance dipolar interactions simulate many-body Hamiltonians.

Language: Английский

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Ultrafast electron diffraction imaging of bond breaking in di-ionized acetylene

Science, Journal Year: 2016, Volume and Issue: 354(6310), P. 308 - 312

Published: Oct. 20, 2016

Acetylene's scission visualized by selfie Can molecules take pictures of themselves? That is more or less the principle underlying laser-induced electron diffraction (LIED): A laser field strips an from a molecule and then sends it back to report on structure remaining ion. Wolter et al. applied this technique acetylene track cleavage its C–H bond after double ionization (see Perspective Ruan). They imaged full also distinguished rapid dissociative dynamics when was oriented parallel rather than perpendicular LIED field. Science , issue p. 308 ; see 283

Language: Английский

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The density matrix renormalization group in chemistry and molecular physics: Recent developments and new challenges

The Journal of Chemical Physics, Journal Year: 2020, Volume and Issue: 152(4)

Published: Jan. 23, 2020

In the past two decades, density matrix renormalization group (DMRG) has emerged as an innovative new method in quantum chemistry relying on a theoretical framework very different from that of traditional electronic structure approaches. The development chemical DMRG been remarkably fast: it already become one reference approaches for large-scale multiconfigurational calculations. This perspective discusses major features DMRG, highlighting its strengths and weaknesses also comparison with other novel is presented following historical development, starting original formulation up to most recent applications. Possible routes recover dynamical correlation are discussed detail. Emerging fields applications explored, such time-dependent application vibrational spectroscopy.

Language: Английский

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Attosecond science based on high harmonic generation from gases and solids

Nature Communications, Journal Year: 2020, Volume and Issue: 11(1)

Published: June 2, 2020

Abstract Recent progress in high power ultrafast short-wave and mid-wave infrared lasers has enabled gas-phase harmonic generation (HHG) the water window beyond, as well demonstration of HHG condensed matter. In this Perspective, we discuss recent advancements future trends generating characterizing soft X-ray pulses from extreme ultraviolet (XUV) solid-state HHG. Then, their current potential usage time-resolved study electron nuclear dynamics atomic, molecular matters.

Language: Английский

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Attosecond Delays in Molecular Photoionization

Physical Review Letters, Journal Year: 2016, Volume and Issue: 117(9)

Published: Aug. 22, 2016

We report measurements of energy-dependent photoionization delays between the two outermost valence shells N_{2}O and H_{2}O. The combination single-shot signal referencing with use different metal foils to filter attosecond pulse train enables us extract from congested spectra. Remarkably large up 160 as are observed in N_{2}O, whereas H_{2}O all smaller than 50 photon-energy range 20-40 eV. These results interpreted by developing a theory molecular delays. long measured shown reflect population shape resonances that trap photoelectron for duration ∼110 as. unstructured continua result much at same photon energies. Our experimental theoretical methods make study dynamics accessible.

Language: Английский

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