A Versatile Ultra-Stable Platform for Optical Multidimensional Fourier-Transform Spectroscopy

Abstract

The JILA Multidimensional Optical Nonlinear SpecTRometer (JILA-MONSTR) is a robust, ultra-stable platform consisting nested and folded Michelson interferometers that can be actively phase stabilized. This platform generates a square of identical laser pulses that can be adjusted to have arbitrary time delay between them, while maintaining phase stability. The JILA-MONSTR provides output pulses for nonlinear excitation of materials and phase-stabilized reference pulses for heterodyne detection of the induced signal. This arrangement is ideal for performing coherent optical experiments, such as multidimensional Fourier-transform spectroscopy, which records the phase of the nonlinear signal as a function of the time delay between several of the excitation pulses. The resulting multidimensional spectrum is obtained from a Fourier transform. This spectrum can resolve, separate and isolate coherent contributions to the light-matter interactions associated with electronic excitation at optical frequencies. To show the versatility of the JILA-MONSTR, several demonstrations of two-dimensional Fourier-transform spectroscopy are presented, including an example of a phase-cycling scheme that reduces noise.