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The JILA multidimensional optical nonlinear spectrometer (JILA-MONSTR) is a robust, ultrastable platform consisting of 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. Also shown is a spectrum that accesses two-quantum coherences, where all excitation pulses require phase locking for detection of the signal.

We present the experimental and simulation results of two-dimensional optical coherent correlation spectroscopy signals along the phase-matching direction k(I) = -k(1) + k(2) + k(3) projected on the two-dimensional (2D) (Omega(3),Omega(2)) plane corresponding to the second and third delay periods. Overlapping Raman coherences in the conventional (Omega(3),Omega(1)) 2D projection may now be clearly resolved. The linewidths of the heavy-hole (HH) and light-hole (LH) excitonic Raman coherence peaks are obtained. Further insights on the higher-order (beyond time-dependent Hartree-Fock) correlation effects among mixed (HH and LH) two excitons can be gained by using a cocircular pulse polarization configuration.