We explore various aspects of electrochemistry and photoelectrochemistry using in situ spectroscopy of electrode (metal) and photoelectrode (semiconductor) interfaces in situ under electrochemical working conditions. These spectroscopies include sum frequency generation (SFG), transient reflectance/absorption spectroscopy (TAS/TRS), and surface enhanced Raman spectroscopy (SERS). Using sum frequency generation (SFG) spectroscopy, we measure the voltage dependence of the orientation of D2O molecules at a graphene electrode surface, which related back to the “stiffness of the ensemble”.1 In particular, we look at the “free OD” feature in the spectra, which corresponds to the topmost water molecule that is rotated up out of the bulk water solution and is, therefore, not hydrogen bonded. Using transient absorption spectroscopy (TAS), we measure the lifetime of hot electrons photoexcited in plasmon resonant nanostructures.5 Using transient reflectance spectroscopy (TRS), we measure the photoexcited carrier dynamics in a GaP/TiO2 photoelectrode, as well as the electrostatic field dynamics at this semiconductor-liquid interfaces in situ under various electrochemical potentials.2 Here, the electrostatic fields at the surface of the semiconductor are measured via Franz−Keldysh oscillations (FKO). These spectra reveal that the nanoscale TiO2 protection layer enhances the built-in field and charge separation performance of GaP photoelectrodes. Using surface enhanced Raman scattering (SERS) spectroscopy, we monitor local electric fields using Stark-shifts of nitrile-functionalized silicon photoelectrodes.6 Using Graphene-enhanced Raman spectroscopy (GERS)-based Stark-shifts, we measure local electric fields and local charge densities at monolayer graphene electrode surfaces.3 Lastly, we measured the stacking dependence and Resonant interlayer excitation of monolayer WSe2/MoSe2 heterostructures for photocatalytic energy conversion.4

In situ spectroscopy of photocatalytic and electrocatalytic interfaces

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