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Electron-phonon coupling (EPC) is foundational in condensed matter physics,determining intriguing phenomena and properties in both conventional andquantum materials. In this manuscript, we propose and demonstrate a novel twodimensional (2D) EPC spectroscopy which allows for direct extraction of EPCmatrix elements. We find that two pronounced phonon modes of methylammoniumlead iodide (MAPI) at room temperature exhibit highly distinctive EPCbehaviors, both in strength, geometry, and temperature dependence across thephase transition. This demonstration indicates the potential of our novel 2Dspectroscopy for studying the evolution of mode-resolved EPC at variousexternal conditions and phonon-mediated light induced ultrafast control ofcondensed materials.

Direct Measurement of Mode-resolved Electron-Phonon Coupling with Two-Dimensional Spectroscopy