Toward a quantitative theoretical method for infrared and Raman spectroscopic studies on single-crystal electrode/liquid interfaces

摘要: In situ electrochemical infrared spectroscopy and Raman are powerful tools for probing potential-dependent adstructures at solid/liquid interfaces. However, it is very difficult to quantitatively interpret the observed spectral features including vibrational frequency intensity, even from model systems such as single-crystal electrode/liquid The clear understanding of spectra has remained a fundamental issue four decades. Here, we have developed method combine computational with interfacial models accurately calculate spectra. We found that solvation high precision level in self-consistent-field convergence critical elements realize quantitative predictions. This method's predictive power verified by analysis classic spectroelectrochemical system, saturated CO molecules electro-adsorbed on Pt(111) electrode. expect this will pave way precisely reveal physicochemical mechanism some processes electrocatalytic reactions.