Efficient time-resolved interface-specific four-order electronic spectroscopy is crucial for understandings of structural and dynamics of surfaces and interfaces for energy conversion, catalysis, and photosynthesis.Here we developed two novel interface-specific two-dimensional electronic spectroscopies. (1) We first demonstrate one novel fourth-order interface-specific two-dimensional electronic sum frequency generation (2D-ESFG) for structures and dynamics at interfaces/surfaces. As a proof-of-principle experiment, the fourth-order 2D-ESFG spectroscopy was used to demonstrate couplings of surface states for GaAs surfaces. (2) We further introduce another novel fourth-order interface-specific two-dimensional electronic-vibrational sum frequency generation (2D-EVSFG) for electron-vibration coupling of molecules at interfaces/surfaces. The 2D-EVSFG technique was used to examine charge transfer of molecules at the air/water interface.  To our best knowledge, these are first demonstrations of interface-specific two-dimensional electronic spectroscopy. All the methodologies developed hereare readily applied to not only classical inorganic semiconductors surfaces and their interfaces with other materials, but also organic semiconductor surfaces, buried interfaces, and hybrid interfaces.<br/>

Development of interface-specific two-dimensional electronic spectroscopy

ACS Fall 2020 Virtual Meeting

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