X-ray diffractive imaging of controlled gas-phase molecules: Toward imaging of dynamics in the molecular frame

Kierspel, Thomas; Morgan, Andrew J.; Wiese, Joss; Mullins, Terry; Aquila, Andrew; Barty, Anton; Bean, Richard; Boll, Rebecca; Boutet, Sébastien; Bucksbaum, P. H.; Chapman, Henry N.; Christensen, Lars Rune; Fry, Alan; Hunter, Mark S.; Koglin, Jason E.; Liang, Mao; Mariani, Valerio; Natan, Adi; Robinson, Joseph S.; Rolles, Daniel; Rudenko, Artem; Schnorr, Kirsten; Stapelfeldt, Henrik; Stern, Stephan; Thøgersen, Jan; Yoon, Chun Hong; Wang, Fenglin; Küpper, Jochen

doi:10.1063/1.5133963

Cited by 31 publications

(22 citation statements)

References 40 publications

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“…Although the first interference maximum is not recorded due to relative long wavelength, the distance of two iodine atoms can be derived from measured diffraction intensity by χ 2 analysis with simulation results. A more precise result showing the first three maxima of iodine-iodine interference is obtained by increasing the photon energy to 9.5 keV [78].…”

Section: Ultrafast X-ray Diffraction Imagingmentioning

confidence: 99%

Perspective: Ultrafast Imaging of Molecular Dynamics Using Ultrafast Low-Frequency Lasers, X-ray Free Electron Laser and Electron Pulses

Zhang¹,

Guo²,

Mi³

et al. 2022

Preprint

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The requirement of high space-time resolution and brightness is a great challenge for imaging atomic motion and making molecular movies. Important breakthroughs in ultrabright tabletop laser, x-ray and electron sources have enabled the direct imaging of evolving molecular structures in chemical processes.And recent experimental advances in preparing ultrafast laser and electron pulses equipped molecular imaging with femtosecond time resolution. This Perspectives present an overview of versatile imaging methods of molecular dynamics. High-order harmonic generation imaging maps the harmonic order of photons to the time delay for nuclear motion and can reach attosecond time resolution. Coulomb explosion imaging retrieves molecular structural information by detecting the momentum vectors of fragmented ions. Diffraction imaging encodes molecular structural and electronic information in reciprocal space, achieving high spatial resolution by using x-ray or electrons with short wavelengths. The enhancement of x-ray and electron source brightness pushes diffraction into single molecular limit without the restriction of crystalline materials. Laser-induced electron diffraction is a self-imaging method based on coherent electron scattering. We also present various applications of these ultrafast imaging methods in resolving laser-induced nuclear and electronic dynamics, as well as dynamic symmetry evolution of molecules.

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Section: Ultrafast X-ray Diffraction Imagingmentioning

confidence: 99%

Perspective: Ultrafast Imaging of Molecular Dynamics Using Ultrafast Low-Frequency Lasers, X-ray Free Electron Laser and Electron Pulses

Zhang¹,

Guo²,

Mi³

et al. 2022

Preprint

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“…Impulsive alignment has also been detected using ultrafast electron diffraction on trifluoroiodomethane (CF 3 I) [15] and carbon disulfide (CS 2 ) [16] and fully time-resolved detection of the rotational dynamics has been achieved in nitrogen molecules [17]. Moreover, static adiabatic alignment induced by pulses with longer duration has been demonstrated with x-ray scattering [18,19]. The benefits of alignment for a complete retrieval of three-dimensional structure of molecules in the gas phase are significant [20].…”

Section: Introductionmentioning

confidence: 99%

Time-resolved x-ray scattering from impulsively aligned or oriented molecules

2020

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Impulsive laser excitation of molecules can create rotational wave packets that lead to transient alignment or orientation. We present a theoretical analysis of the signatures of post-pulse field-free time-dependent alignment and orientation of diatomic molecules in time-resolved nonresonant x-ray scattering. This shows that alignment and its time dependence due to the interference terms of the rotational wave packet are visible in the x-ray scattering signal whereas signatures of orientation and its time dependence are absent. To that end, we discuss the time dependence of the coherent rotational motion associated with electronically resonant one-photon excitations. We illustrate our findings with calculated two-dimensional scattering signals for the sodium fluoride molecule (NaF) in the gas phase.

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“…Ultrafast x-ray scattering using advanced light sources is an emerging tool to probe the motion of photo-excited molecular systems at the angstrom and femtosecond scales. In recent years this method was successfully used to trace coherent motions and dynamics in molecules in the gas phase [1][2][3][4][5][6][7] , as well as structural changes in molecules in solution after the electronic excitation [8][9][10][11][12][13][14][15]. Inversion of the scattering signal to obtain the real-space pair distribution function for these studies was limited by the available range of the scattering vector for the photon energies used.…”

mentioning

confidence: 99%

Real-Space Inversion and Super-Resolution of Ultrafast Scattering

Natan¹

2021

Preprint

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Directly resolving in real-space multiple atomic motions using ultrafast x-ray scattering is generally limited by the finite detector range. As a result, signal interpretation mostly relies on modeling and simulations of specific excitation pathways. Here, we demonstrate an approach to resolve ultrafast diffuse x-ray scattering signals in real space and recover multiple atomic motions de-novo. We introduce a scattering basis representation that is composed of the measurement parameters and constraints, and the subsequent inversion analysis. We then leverage signal priors, such as smoothness and sparsity to deconvolve and super-resolve the spatially transformed signals using convex optimization. We validate the approach on simulated data with detection limits similar to X-ray free-electron laser experiments and discuss the resolution limits and noise dependence on the accuracy of the recovery.

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X-ray diffractive imaging of controlled gas-phase molecules: Toward imaging of dynamics in the molecular frame

Cited by 31 publications

References 40 publications

Perspective: Ultrafast Imaging of Molecular Dynamics Using Ultrafast Low-Frequency Lasers, X-ray Free Electron Laser and Electron Pulses

Perspective: Ultrafast Imaging of Molecular Dynamics Using Ultrafast Low-Frequency Lasers, X-ray Free Electron Laser and Electron Pulses

Time-resolved x-ray scattering from impulsively aligned or oriented molecules

Real-Space Inversion and Super-Resolution of Ultrafast Scattering

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