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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Diffraction and microscopy with attosecond electron pulse trains

Nature Physics, Journal Year: 2017, Volume and Issue: 14(3), P. 252 - 256

Published: Nov. 21, 2017

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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Charge migration and charge transfer in molecular systems

Structural Dynamics, Journal Year: 2017, Volume and Issue: 4(6)

Published: Nov. 1, 2017

The transfer of charge at the molecular level plays a fundamental role in many areas chemistry, physics, biology and materials science. Today, more than 60 years after seminal work R. A. Marcus, is still very active field research. An important recent impetus comes from ability to resolve ever faster temporal events, down attosecond time scale. Such high resolution now offers possibility unravel most elementary quantum dynamics both electrons nuclei that participate complex process transfer. This review covers research addresses following questions. Can we reconstruct migration across molecule on atomic length electronic scales? use strong laser fields control migration? temporally understand intramolecular dissociative ionization small molecules, transition-metal complexes conjugated polymers? tailor systems towards specific charge-transfer processes? What are scales steps liquids nanoparticles? Important new insights into each these topics, obtained state-of-the-art ultrafast spectroscopy and/or theoretical methods, summarized this review.

Language: Английский

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High average power and single-cycle pulses from a mid-IR optical parametric chirped pulse amplifier

Optica, Journal Year: 2017, Volume and Issue: 4(9), P. 1024 - 1024

Published: Aug. 24, 2017

In attosecond and strong-field physics, the acquisition of data in an acceptable time demands combination high peak power with average power. We report a 21 W mid-IR optical parametric chirped pulse amplifier (OPCPA) that generates 131 μJ 97 fs (sub-9-cycle) pulses at 160 kHz repetition rate center wavelength 3.25 μm. Pulse-to-pulse stability carrier envelope phase (CEP)-stable output is excellent 0.33% rms over 288 million (30 min) compression close to single cycle was achieved through soliton self-compression inside gas-filled antiresonant-guiding photonic crystal fiber. Without any additional device, stable generation 14.5 fs (1.35-optical-cycle) 9.6 W. The resulting 3.9 GW near-single-cycle duration intrinsic CEP makes our OPCPA key-enabling technology for next extreme photonics, research, coherent x-ray science.

Language: Английский

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Simulating the vibrational quantum dynamics of molecules using photonics

Nature, Journal Year: 2018, Volume and Issue: 557(7707), P. 660 - 667

Published: May 1, 2018

Language: Английский

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Symphony on strong field approximation

Reports on Progress in Physics, Journal Year: 2019, Volume and Issue: 82(11), P. 116001 - 116001

Published: June 21, 2019

This paper has been prepared by the Symphony collaboration (University of Warsaw, Uniwersytet Jagielloński, DESY/CNR and ICFO) on occasion 25th anniversary 'simple man's models' which underlie most phenomena that occur when intense ultrashort laser pulses interact with matter. The in question include high-harmonic generation (HHG), above-threshold ionization (ATI), non-sequential multielectron (NSMI). 'Simple provide both an intuitive basis for understanding numerical solutions time-dependent Schrödinger equation motivation powerful analytic approximations generally known as strong field approximation (SFA). In this we first review SFA form developed us last 25 years. approach is a method to solve TDSE, non-perturbative interactions are described including continuum–continuum systematic perturbation-like theory. focus recent applications HHG, ATI NSMI from multi-electron atoms multi-atom molecules. main novel part presented theory concerns generalizations to: (i) treatment two-electron atoms, allowing studies interplay between electron impact resonant excitation subsequent ionization; (ii) single active 'large' molecules targets themselves undergoing dynamics during HHG or processes. particular, formulate general expressions case arbitrary molecules, combining input quantum chemistry dynamics. We also separable molecular potentials model analytically realistic electronic wave packets fields. dedicate work memory Bertrand Carré, who passed away March 2018 at age 60.

Language: Английский

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Optical Excitations with Electron Beams: Challenges and Opportunities

ACS Photonics, Journal Year: 2021, Volume and Issue: 8(4), P. 945 - 974

Published: March 25, 2021

Free electron beams such as those employed in microscopes have evolved into powerful tools to investigate photonic nanostructures with an unrivaled combination of spatial and spectral precision through the analysis energy losses cathodoluminescence light emission. In ultrafast optics, emerging field microscopy utilizes synchronized femtosecond pulses that are aimed at sampled structures, holding promise bring simultaneous sub-Å-sub-fs-sub-meV space-time-energy resolution study material optical-field dynamics. addition, these advances enable manipulation wave function individual free electrons unprecedented ways, opening sound prospects probe control quantum excitations nanoscale. Here, we provide overview photonics research based on electrons, supplemented by original theoretical insights discussion several stimulating challenges opportunities. particular, show excitation probability a single is independent its function, apart from classical average over transverse beam density profile, whereas for two or more modulated depends their relative arrangement, thus reflecting nature interactions. We derive first-principles analytical expressions embody results general validity arbitrarily shaped any type electron-sample interaction. conclude some perspectives various exciting directions include disruptive approaches noninvasive spectroscopy microscopy, possibility sampling nonlinear optical response nanoscale, matrices associated sample modes, appealing applications modulation beams, all which could potentially revolutionize use photonics.

Language: Английский

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X-ray multiphoton-induced Coulomb explosion images complex single molecules

Nature Physics, Journal Year: 2022, Volume and Issue: 18(4), P. 423 - 428

Published: Feb. 21, 2022

Abstract Following structural dynamics in real time is a fundamental goal towards better understanding of chemical reactions. Recording snapshots individual molecules with ultrashort exposure times key ingredient this goal, as atoms move on femtosecond (10 −15 s) timescales. For condensed-phase samples, ultrafast, atomically resolved structure determination has been demonstrated using X-ray and electron diffraction. Pioneering experiments have also started addressing gaseous samples. However, they face the problem low target densities, scattering cross sections random spatial orientation molecules. Therefore, obtaining images entire, isolated capturing all constituents, including hydrogen atoms, remains challenging. Here we demonstrate that intense pulses from an free-electron laser trigger rapid complete Coulomb explosions 2-iodopyridine 2-iodopyrazine We obtain intriguingly clear momentum depicting ten or eleven hydrogens, thus overcome so-far impregnable barrier for explosion imaging—its limitation consisting three to five atoms. In combination state-of-the-art multi-coincidence techniques elaborate theoretical modelling, allows tracing ultrafast emission information result intramolecular rearrangement. Our work represents important step imaging chemistry via explosion.

Language: Английский

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Attosecond field emission

Nature, Journal Year: 2023, Volume and Issue: 613(7945), P. 662 - 666

Published: Jan. 25, 2023

Field-emission of electrons underlies major advances in science and technology, ranging from imaging the atomic-scale structure matter to signal processing at ever-higher frequencies. The advancement these applications their ultimate limits temporal resolution frequency calls for techniques that can confine probe field emission on sub-femtosecond time scale. We used intense, sub-cycle transients induce optical electron pulses tungsten nanotips a weak replica same transient directly dynamics real-time. Access into profile emerging pulses, including duration $\tau$ = (53 as $\pm$ 5 as) chirp, direct probing nanoscale near-fields, open new prospects research interface attosecond physics nanooptics.

Language: Английский

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