Optimized interferometric setup for chiral and achiral ultrafast IR spectroscopy

We report an actively stabilized interferometer-based set-up for the detection of vibrational circular dichroism (VCD) and optical rotatory dispersion (VORD) with femtosecond laser pulses. Our approach combines and improves elements of several previous measurement strategies, including signal amplification in a crossed polarizer configuration, precise control and modulation of polarization, phase stability, tight focusing, broad-band detection and spectral interferometry. Their importance for static and transient measurements is motivated by a signal analysis based on Jones matrices and response theory. Only depending on the pump-beam polarization, the set-up can selectively detect transient VCD and VORD or transient linear birefringence (LB) and linear dichroism (LD), which usually constitute the dominant artifacts in the chiral measurements. For illustration we present transient LB and LD data of an achiral Rhenium carbonyl complex, detected simultaneously by spectral interferometry, and we analyze residual background signals in the experimental configuration for transient chiral spectroscopy.