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Developing effective methods to measure the enantiomeric excess of the chiralmixture is one of the major topics in chiral molecular researches, yet remainschallenging. Enantiodetection method via two-dimensional (2D) spectroscopybased on a four level model, containing a cyclic three-level system (CTLS), ofchiral molecules was recently proposed and demonstrated, yet with a strictcondition of the one-photon resonance (where three driving fields are exactlyresonantly coupled to the three electric-dipole transitions, respectively) inthe CTLS and narrowband probe pulse assumption. Here, we extend the 2Dspectroscopy method to more general experimental conditions, with three-photonresonance (where the sum of the two smaller frequencies among the three drivingfields equals to the third one) and broadband probe pulse. Our method remainseffective on enantiodetection with the help of experimental techniques, such asthe chop detection method, which is used to eliminate the influence of theother redundant levels existing in the real system of chiral molecules. Underthese more general conditions, the enantiomeric excess of the chiral mixture isestimated by taking an easily available standard sample (usually the racemicmixture) as the reference.

Enantiodetection via the 2D spectroscopy: extending the methodology to general experimental conditions