Diffractive Imaging of ${\mathrm{C}}_{60}$ Structural Deformations Induced by Intense Femtosecond Midinfrared Laser Fields

Diffractive Imaging of $C_{60}$ Structural Deformations Induced by Intense Femtosecond Midinfrared Laser Fields

Harald Fuest, Yu Hang Lai, Cosmin I. Blaga, Kazuma Suzuki, Junliang Xu, Philipp Rupp, Hui Li, Pawel Wnuk, Pierre Agostini, Kaoru Yamazaki, Manabu Kanno, Hirohiko Kono, Matthias F. Kling, and Louis F. DiMauro

Phys. Rev. Lett. 122, 053002 – Published 6 February 2019

Abstract

Theoretical studies indicated that $C_{60}$ exposed to linearly polarized intense infrared pulses undergoes periodic cage structural distortions with typical periods around 100 fs ( $1 fs = 10^{- 15} s$ ). Here, we use the laser-driven self-imaging electron diffraction technique, previously developed for atoms and small molecules, to measure laser-induced deformation of $C_{60}$ in an intense $3.6 μ m$ laser field. A prolate molecular elongation along the laser polarization axis is determined to be $(6.1 \pm 1.4) %$ via both angular- and energy-resolved measurements of electrons that are released, driven back, and diffracted from the molecule within the same laser field. The observed deformation is confirmed by density functional theory simulations of nuclear dynamics on time-dependent adiabatic states and indicates a nonadiabatic excitation of the $h_{g} (1)$ prolate-oblate mode. The results demonstrate the applicability of laser-driven electron diffraction methods for studying macromolecular structural dynamics in four dimensions with atomic time and spatial resolutions.

Received 4 December 2017

DOI:https://doi.org/10.1103/PhysRevLett.122.053002

Physics Subject Headings (PhySH)

Atomic & molecular structure

Atomic, Molecular & Optical

Authors & Affiliations

Harald Fuest^1,2, Yu Hang Lai³, Cosmin I. Blaga³, Kazuma Suzuki⁴, Junliang Xu³, Philipp Rupp^1,2, Hui Li^1,5,6, Pawel Wnuk^1,2,7, Pierre Agostini³, Kaoru Yamazaki⁸, Manabu Kanno⁴, Hirohiko Kono⁴, Matthias F. Kling^1,2,5, and Louis F. DiMauro³

¹Physics Department, Ludwig-Maximilians-Universität Munich, D-85748 Garching, Germany
²Max Planck Institute of Quantum Optics, D-85748 Garching, Germany
³Department of Physics, The Ohio State University, Columbus, Ohio 43210, USA
⁴Department of Chemistry, Graduate School of Science, Tohoku University, Sendai 980-8578, Japan
⁵J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, Kansas 66506, USA
⁶State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai 200062, China
⁷Institute of Experimental Physics, Faculty of Physics, University of Warsaw, ul. Pasteura 5, 02-093 Warsaw, Poland
⁸Institute for Material Research, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577, Japan

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Vol. 122, Iss. 5 — 8 February 2019

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Figure 1
The concept of ultrafast molecular imaging. (a) Illustration of the three-step LIED process and graphical illustration of $C_{60}$ cage field-induced elongation during the pulse. (b) 2D photoelectron angular distribution data recorded for $C_{60}$ irradiated with $3.6 μ m$ , 100 fs pulses at $80 TW / {cm}^{2}$ . The solid circles represent the integration area for LIED whereas the dashed line marks the area for FABLES (see text for details).
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Figure 2
Comparison of elastic DCS from experimental LIED data (upper panel) vs IAM calculation (lower panel) at 90 eV. Each line in the lower panel corresponds to a cage elongated along the laser polarization by the value indicated in the legend with respect to the field-free, spherical cage. The minima and maxima indicated in the figure are diffraction extremes, whose angular positions are determined by the size of the cage. The four circles indicate the elongations that best match the corresponding experimental values. From the highest angle to the lowest angle extrema, the elongations are 6%, 5%, 4%, and 7%.
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Figure 3
Results for FABLES. Experimental data extracted from the photoelectron spectrum along the laser polarization (FABLES) are shown as blue symbols with associated statistical errors (shaded area). The unperturbed cage theoretical prediction is shown in red, whereas the best theoretical fit with the cage elongation as fit parameter is shown in green $(8 \pm 2) %$ .
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Figure 4
Density-functional theory results. (a) Temporal profile of the elongation $[d (t) / d_{eq}] − 1$ (DFT- magenta, DFTB—purple) of neutral $C_{60}$ in a midinfrared Gaussian pulse (blue line) at peak intensity $I_{0} = 80 TW / {cm}^{2}$ , 60 fs duration, and $3.6 μ m$ wavelength. Here, $d (t)$ is the length of $C_{60}$ along the polarization direction of the applied field and $d_{eq}$ is its equilibrium value. (b) Elongation as a function of charge species, wavelength, and pulse duration. Simulations to obtain the values of field-induced distortion are carried out by using the time-dependent adiabatic state approach [18] combined with the SCC-DFTB method (mio-1-1 parameter set). The time step $Δ t$ was chosen to be 0.1 fs. Black squares show values at $λ = 3.1 μ m$ for neutral $C_{60}$ and magenta squares at $λ = 3.6 μ m$ . The blue star symbol indicates the value for $C_{60}^{+}$ and the red square symbol indicates the value for $C_{60}^{2 +}$ . The value for $λ = 3.6 μ m$ is also evaluated by B3LYP/6-31G(d) of DFT, indicated by the purple square symbol.
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Physical Review Letters

Diffractive Imaging of C60 Structural Deformations Induced by Intense Femtosecond Midinfrared Laser Fields

Harald Fuest, Yu Hang Lai, Cosmin I. Blaga, Kazuma Suzuki, Junliang Xu, Philipp Rupp, Hui Li, Pawel Wnuk, Pierre Agostini, Kaoru Yamazaki, Manabu Kanno, Hirohiko Kono, Matthias F. Kling, and Louis F. DiMauro

Phys. Rev. Lett. 122, 053002 – Published 6 February 2019

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Diffractive Imaging of $C_{60}$ Structural Deformations Induced by Intense Femtosecond Midinfrared Laser Fields