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Updated: May 18, 2026

Direct Imaging of Laser-driven Ultrafast Molecular Rotation
Published on: February 4, 2017
Angle determination and scattering suppression in polarization-enhanced two-dimensional infrared spectroscopy in the
1Physikalisch-chemisches Institut, Universitat Zurich, Winterthurerstrasse 190, 8057 Zurich, Switzerland.
Abstract:
The signal to noise in two-dimensional spectra recorded in the pump-probe geometry can be significantly improved with a quasi-crossed polarizer configuration, often employed in linear dichroism measurements. Here we examine this method in detail and demonstrate how to analyse and interpret the amplified signals. The angle between transition dipole moments can be determined with better accuracy than in conventional anisotropy measurements, and the method can be used to selectively suppress individual peaks and to efficiently remove scattering contributions. We present spectra of the coupled CO-stretch modes of a Ruthenium-carbonyl complex in DMSO for experimental illustration.
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