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Direct Imaging of Laser-driven Ultrafast Molecular Rotation

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Published on: February 4, 2017

Tracking autoionizing-wave-packet dynamics at the 1-fs temporal scale.

E Skantzakis¹, P Tzallas, J E Kruse

¹Foundation for Research and Technology-Hellas, Institute of Electronic Structure and Laser, P.O. Box 1527, GR-711 10 Heraklion, Crete, Greece.

Physical Review Letters

|September 28, 2010

Summary

We used extreme-ultraviolet (XUV) light to study ultrafast electron dynamics in atoms and molecules. This new spectroscopic method allows detailed observation of electron behavior following excitation.

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Area of Science:

Atomic and Molecular Physics
Ultrafast Spectroscopy
Quantum Dynamics

Background:

Inner-shell excitation leads to complex electron dynamics like Auger decay.
Doubly excited autoionizing states are crucial for understanding electron correlation.
Previous methods lacked the bandwidth to probe multiple states simultaneously.

Purpose of the Study:

To develop and demonstrate a novel time-resolved spectroscopic technique.
To simultaneously excite and probe a series of electronic states.
To investigate ultrafast dynamics of Auger decay and autoionization.

Main Methods:

Utilizing coherent extreme-ultraviolet (XUV) radiation continua for excitation.
Employing time-resolved pump-probe spectroscopy with XUV pulses.
Applying Fourier transform spectroscopy to analyze wave packet evolution.

Main Results:

Simultaneous excitation of multiple states spanning ~4 eV achieved.
Oscillatory and decaying wave packet evolution was tracked in real-time.
Fourier transform of time-resolved data successfully reproduced the excitation spectrum.

Conclusions:

The developed technique enables ultrabroadband XUV spectroscopy.
This method opens new avenues for studying ultrafast dynamics across all matter states.
Provides unprecedented insight into electron correlation and decay processes.