Continuously tunable optical multidimensional Fourier-transform spectrometer

A multidimensional optical nonlinear spectrometer (MONSTR) is a robust, ultrastable platform consisting of nested and folded Michelson interferometers that can be actively phase stabilized. The MONSTR provides output pulses for nonlinear excitation of materials and phase-stabilized reference pulses for heterodyne detection of the induced signal. This platform generates a square of identical laser pulses that can be adjusted to have arbitrary time delays between them while maintaining phase stability. This arrangement is ideal for performing coherent optical experiments, such as multidimensional Fourier-transform spectroscopy. The present work reports on overcoming some important limitations on the original design of the MONSTR apparatus. One important advantage of the MONSTR is the fact that it is a closed platform, which provides the high stability. Once the optical alignment is performed, it is desirable to maintain the alignment over long periods of time. The previous design of the MONSTR was limited to a narrow spectral range defined by the optical coating of the beam splitters. In order to achieve tunability over a broad spectral range the internal optics needed to be changed. By using broadband coated and wedged beam splitters and compensator plates, combined with modifications of the beam paths, continuous tunability can be achieved from 520 nm to 1100 nm without changing any optics or performing alignment of the internal components of the MONSTR. Furthermore, in order to achieve continuous tunability in the spectral region between 520 nm and 720 nm, crucially important for studies on numerous biological molecules, a single longitudinal mode laser at 488.5 nm was identified and used as a metrology laser. The shorter wavelength of the metrology laser as compared to the usual HeNe laser has also increased the phase stability of the system. Finally, in order to perform experiments in the reflection geometry, a simple method to achieve active phase stabilization between the signal and the reference beams has been developed.