Mainz 2017 – wissenschaftliches Programm
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MO: Fachverband Molekülphysik
MO 17: Experimental Techniques
MO 17.3: Vortrag
Freitag, 10. März 2017, 11:45–12:00, N 6
Broadband 7-fs 2D electronic spectroscopy by hollow-core fiber compression — •Xiaonan Ma, Jakub Dostál, and Tobias Brixner — Institut für Physikalische und Theoretische Chemie, Universität Würzburg, Am Hubland, 97074 Würzburg, Germany
Coherent two-dimensional electronic spectroscopy (2DES) is a powerful technique for resolving excited-state dynamics within coupled systems. To date, 2DES is mainly limited by laser bandwidth and peak-shape distortion (e.g. directional filtering) [1]. In this work, we combine a sub-7-fs supercontinuum generated in Ar-filled hollow-core fiber (HCF) with a diffractive-optic-based 2DES spectrometer for broadband 2DES measurement (500-700 nm) and reducing peak-shape distortion to a minimum [2].
We demonstrated the technique with cresyl-violet in ethanol. Measuring transient absorption in the same setup allow us to phase the 2DES data. The resulting peak-shape and quantum beating behaviour (585 and 2820 cm−1) agree with a previous report [3]. We note that with sub-7-fs temporal resolution, our setup has the potential to observe extremely fast quantum beating (up to 3500 cm−1), which is especially suited to investigate multi-chromophore systems with strong excitonic coupling. Meanwhile, this technique can be extended to even broader wavelength range (i.e. > 1 octave) or other regimes (i.e. UV and NIR).
[1] M. K. Yetzbacher et al., J. Chem. Phys. 126, 044511 (2007).
[2] X. Ma et al., Opt. Express 24, 20781 (2016).
[3] L. A. Bizimana et al., J. Chem. Phys. 143, 164203 (2015).