Phase-cycling and double-quantum two-dimensional electronic spectroscopy using a common-path birefringent interferometer

Ultrafast spectroscopy provides unique access to the coherent dynamics of atomic, molecular, and solid state quantum systems. A most powerful, yet experimentally challenging tool for this is two-dimensional electronic spectroscopy (2DES), allowing to isolate excitation pathways and to selectively probe coherent and incoherent couplings by controlling the phase of the ultrashort pulses that interact with the system. Its experimental implementation can in principle greatly be simplified by employing inherently phase stable birefringent in-line interferometers (TWINS), which, however, are thought to lack sufficient phase control. Here, we demonstrate an adaptation of TWINS providing full phase-cycling capabilities for 2DES. This is demonstrated by recording rephasing, non-rephasing, zero-quantum, and double-quantum 2DES on a molecular J-aggregate. This easy-to-implement extension opens up new experimental possibilities for TWINS-based 2DES in multidimensional all-optical and photoemission spectroscopy and microscopy. © 2024 Optica Publishing Group.