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The Response of a He-3 Fermi Liquid Droplet to Vibronic Excitation of an Embedded Glyoxal Molecule

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Benedek,  Giorgio
Emeritus Group Molecular Interactions, Max Planck Institute for Dynamics and Self-Organization, Max Planck Society;

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Toennies,  Jan Peter
Emeritus Group Molecular Interactions, Max Planck Institute for Dynamics and Self-Organization, Max Planck Society;

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Citation

Benedek, G., Hizhnyakov, V., & Toennies, J. P. (2014). The Response of a He-3 Fermi Liquid Droplet to Vibronic Excitation of an Embedded Glyoxal Molecule. Journal of Physical Chemistry A, 118(33): 10.1021/jp503184d, pp. 6574-6583. doi:10.1021/jp503184d.


Cite as: https://hdl.handle.net/11858/00-001M-0000-0029-0F11-C
Abstract
The zero-phonon line (ZPL) and the sideband in the vibronic spectrum of a single glyoxal molecule inside a He-3 droplet are analyzed within the framework of the Lax formalism. The new theory takes full account of the coupling of the molecule to the single particle-hole (PH) and collective excitations of the doped Fermionic droplet. The effect on the coupling of the wavevector dependence of the effective He-3 mass and the large local density of the first He-3 shell, resulting from the interaction with the chromophore, are also included in the theory. By fitting of a coupling parameter and the phase factor between the PH and collective response functions, the shape and relative intensity of the observed ZPL and its slowly decreasing multiexcitation sideband are well-reproduced. The new theory is consistent with the previous explanation of the surprisingly sharp phonon line superimposed on the sideband in terms of the dense first He-3 shell, which acts as a Helmholtz resonator for the zero sound of the droplet.