Stuttgart 2012 – scientific programme

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A: Fachverband Atomphysik

A 18: Attosecond physics I

A 18.3: Talk

Tuesday, March 13, 2012, 15:00–15:15, V47.03

Two-dimensional spectroscopy methods to explore attosecond electron dynamics — Christian Ott, Philipp Raith, Andreas Kaldun, Kristina Meyer, Martin Laux, Yizhu Zhang, and •Thomas Pfeifer — Max-Planck Institut für Kernphysik, Heidelberg

Traditional two-dimensional (2D) spectroscopy methods are based on time-delayed mutually-coherent pulse sequences, allowing to map out correlations among different vibrational or electronic transition frequencies. This allows the measurement of population and (de-) coherence information of a system’s density matrix and the coupling of quantum states, recently leading to the observation of coherent energy flow in macromolecular photosynthetic light-harvesting complexes, even at room temperature [1]. However, these powerful 2D-spectroscopy methods have thus far been limited to the femtosecond time scale.

Here, we present experimental results demonstrating novel concepts of 2D spectroscopy that are applicable to the attosecond strong-field domain and the exploration of one- and two-electron dynamics. The carrier-envelope phase (CEP) is used as a dynamical parameter, opening a second dimension to gain access to electron dynamics and to separately identify spectrally overlapping quantum paths within one and the same few-cycle strong-field laser pulse. We also used laser-dressed soft-x-ray transient-absorption spectroscopy to create experimental 2D spectrograms, from which we read the quantum-interference pathways of two-electron excited states and their dynamics embedded in an ionization continuum.

[1] Panitchayangkoon et al. PNAS 107, 12766 (2010)