Quantum Dynamics

remiAt a most fundamental level, electronic motion determines all aspect of technology and life. Electrons determine whether and how a molecule dissociates and how a chemical reaction occurs; electrons sustain the energy flow in human vision or of our nerve system, and they determine whether biological life ends. Our aim is to zoom into the microcosm of electronic motion to observe and possibly control their dynamics. The research therefore deals with a wide range of aspects from the quantum nature of electronic correlation to tracking their dynamics on the attosecond timescale despite velocities thousand times faster than that of the nuclei. We have, e.g. pioneered attosecond angular streaking, which permits attosecond resolution measurements of electron wavepackets without attosecond x-ray pulses. Currently, we use a reaction microscope to investigate the concerted motion of electrons and ions on their attosecond timescale and to realize self-imaging of molecular structure.


OURCONTRIBUTIONS

liedLaser-induced electron diffraction is an evolving tabletop method, which aims to image ultrafast structural changes in gas-phase polyatomic molecules with sub-Ångström spatial and femtosecond temporal resolution. Here, we provide the general foundation for the retrieval of multiple bond lengths from a polyatomic molecule by simultaneously measuring the C-C and C-H bond lengths in aligned acetylene. Our approach takes the method beyond the hitherto achieved imaging of simple diatomic molecules and is based upon the combination of a 160 kHz mid-IR few-cycle laser source with full three-dimensional electron-ion coincidence detection. Our technique provides an accessible and robust route towards imaging ultrafast processes in complex gas phase molecules with atto- to femto-second temporal resolution.

  1. M. Pullen, B. Wolter, A.-T. Le, M. Baudisch, M. Hemmer, A. Senftleben, C. D. Schröter, J. Ullrich, R. Moshammer, C.-D. Lin, J. Biegert, “Imaging aligned polyatomic molecules with laser-induced electron diffraction”, Nature Communications 6, 7262 (2015).
  2. B. Wolter, M. Pullen, M. Baudisch, M. Sclafani, M. Hemmer, A. Senftleben, C.D. Schröter, J. Ullrich, R. Moshammer, J. Biegert, “Strong-field physics with mid-IR fields”, Phys. Rev. X 5, 021034 (2015).
  3. B. Wolter, M. G. Pullen, A.-T. Le, M. Baudisch, K. Doblhoff-Dier, A. Senftleben, M. Hemmer, C. Dieter Schröter, J. Ullrich, T. Pfeifer, R. Moshammer, S. Gräfe, O. Vendrell, C. D. Lin, J Biegert, “Ultrafast electron diffraction imaging of bond breaking in di-ionized acetylene”, Science 354, 308 (2016).

RELATEDPUBLICATIONS

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Liu, X. et al. Imaging an isolated water molecule using a single electron wave packet. J. Chem. Phys. 151, 024306 (2019).
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Shaaran, T. et al. Role of high ponderomotive energy in laser-induced nonequential double ionization. Physical Review A 99, 023421 (2019).
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Amini, K. et al. Symphony on Strong Field Approximation. Rep. Prog. Phys. (2019) doi:doi.org/10.1088/1361-6633/ab2bb1.
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Amini, K. et al. Imaging the Renner–Teller effect using laser-induced electron diffraction. 10, 1817465116 (2019).
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Suarez, N. et al. Above-threshold ionization in multicenter molecules: The role of the initial state. Physical Review A 97, 033415 (2017).
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Pullen, M. et al. Transition from nonsequential to sequential double ionization in many-electron systems. Physical Review A 96, 033401 (2017).
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Suárez, N. et al. High-order-harmonic generation in atomic and molecular systems. Physical Review A 95, 033415 (2017).
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Suárez, N. et al. Above-threshold ionization and laser-induced electron diffraction in diatomic molecules. Physical Review A 94, 043423 (2016).
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Wolter, B. et al. Ultrafast electron diffraction imaging of bond breaking in di-ionized acetylene. Science (New York, N.Y.) 354, 308–312 (2016).
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Baudisch, M., Wolter, B., Pullen, M., Hemmer, M. & Biegert, J. High power optical parametric synthesizer for femtosecond, deep-UV to mid-IR pump-probe experiments. Opt. Lett. 15, 3583 (2016).