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CPP: Fachverband Chemische Physik und Polymerphysik
CPP 30: Emerging Topics in Chemical and Polymer Physics, New Instruments and Methods I
CPP 30.6: Talk
Wednesday, March 19, 2025, 17:45–18:00, H34
Phase-cycling and double-quantum two-dimensional electronic spectroscopy using a common-path birefringent interferometer — Daniel Timmer1, •Daniel C. Lünemann1, Moritz Gittinger1, Antonietta De Sio1, Cristian Manzoni2, Giulio Cerullo2, and Christoph Lienau1 — 1Carl von Ossietzky Universität Oldenburg, Germany — 2Politecnico di Milano, Italy
Ultrafast coherent spectroscopy techniques provide unique insights into the coherent dynamics of atomic, molecular and solid state quantum systems. For this, an experimentally challenging but all the more powerful technique is two-dimensional electronic spectroscopy (2DES), which allows to selectively probe coherent and incoherent couplings and to isolate individual excitation pathways by controlling the absolute phases of the ultrashort optical pulses that interact with the system (phase-cycling, PC). Its experimental implementation can be greatly simplified by employing birefringent in-line interferometers (TWINS) which are inherently phase stable. However, TWINS is so far considered to be incapable of this phase control. Here, we demonstrate PC capabilities for 2DES using an adapted TWINS interferometer by recording rephasing, non-rephasing, zero-quantum and double-quantum 2DES on a molecular J-aggregate. This extension is easy to implement and enables new experimental capabilities for TWINS-based 2DES in multidimensional all-optical and photoemission spectroscopy and microscopy.
[1]: D Timmer, DC Lünemann, et al., Optica (accepted, DOI: 10.1364/OPTICA.543007)
Keywords: 2DES; phase-cycling; double-quantum; ultrafast spectroscopy; molecular aggregates