Simultaneous optical second harmonic and sum frequency intensity image observation of hydrogen deficiency on a H–Si(1 1 1) 1 × 1 surface after IR light pulse irradiation

In this study, we developed a microscope for the simultaneous acquisition of optical sum frequency (SF) and second harmonic (SH) intensity images in UHV conditions, and observed resonant electronic and vibrational images of the H–Si(1 1 1) surface after IR light irradiation of pulse width ∼6 μs. The SH intensity images showed a spatial distribution of resonant electronic states, associated with the dangling bonds formed after hydrogen desorption induced by the IR light pulses. This result indicates that the hydrogen coverage decreased to less than ∼0.6 ML in the irradiated area. The SF intensity images before the IR light pulse irradiation showed signals attributed to Si–H stretching vibration on the H–Si(1 1 1) surface. After the IR light pulse irradiation, non-resonant SF signals appeared in the irradiated area. The non-resonant SF signals may originate from a nonlinear optical transition involving the surface electronic levels in the dangling bonds. We also found an unidentified bonding state on the edges of the irradiated area in some light conditions. Both the resonant and non-resonant signals were very weak in this area.