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Journal Article

Strong Local-Field Enhancement of the Nonlinear Soft-Mode Response in a Molecular Crystal

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Hoja,  Johannes
Theory, Fritz Haber Institute, Max Planck Society;
Physics and Materials Science Research Unit, University of Luxembourg;

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Tkatchenko,  Alexandre
Theory, Fritz Haber Institute, Max Planck Society;
Physics and Materials Science Research Unit, University of Luxembourg;

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PhysRevLett.119.097404.pdf
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Citation

Folpini, G., Reimann, K., Woerner, M., Elsaesser, T., Hoja, J., & Tkatchenko, A. (2017). Strong Local-Field Enhancement of the Nonlinear Soft-Mode Response in a Molecular Crystal. Physical Review Letters, 119(09): 097404. doi:10.1103/PhysRevLett.119.097404.


Cite as: https://hdl.handle.net/11858/00-001M-0000-002D-E775-D
Abstract
The nonlinear response of soft-mode excitations in polycrystalline acetylsalicylic acid (aspirin) is studied with two-dimensional terahertz spectroscopy. We demonstrate that the correlation of CH3 rotational modes with collective oscillations of π electrons drives the system into the nonperturbative regime of light-matter interaction, even for a moderate strength of the THz driving field on the order of 50  kV/cm. Nonlinear absorption around 1.1 THz leads to a blueshifted coherent emission at 1.7 THz, revealing the dynamic breakup of the strong electron-phonon correlations. The observed behavior is reproduced by theoretical calculations including dynamic local-field correlations.