Spectral Phase Measurements of Heterodyne Detection in Interfacial Broadband Electronic Spectroscopy

A spectral phase is vital to retrieve both the real and imaginary parts of both second-order vibrational and electronic sum frequency generation spectra. Despite recent efforts, phase measurements in electronic spectra at interfaces are lacking. In particular, references are not well established for frequency-dependent spectral phases in interfacial electronic spectroscopy. In this work, we present broadband heterodyne detection (HD) of interfacial electronic spectroscopy for spectral phases of references. Such a broadband HD method was based upon a broadband short-wave IR laser source from 1100 to 2200 nm. A collinear geometry method was adopted for passive phase stability. We further compared often-used reference samples, including gold (Au) thin films, silver (Ag) thin films, p-type GaP (100), p-type GaAs (100), as well as left-handed and right-handed z-cut alpha-quartz crystals. The phases of the second-order susceptibilities for Ag thin films, the GaP crystal, the GaAs crystal, and the quartz crystals are independent of frequency from 630 to 730 nm. More importantly, it was found that the often-used Au thin film in the literature is not a good phase reference for frequency-dependent phases.