Studies of interfacial regions by sum-frequency generation with a free-electron laser

The use of a Free-Electron Laser (FEL) allows the study of (non)linear optical properties of materials over unsurpassed large spectral intervals. As an example, we report on the use of a FEL as the infrared source in spectroscopic infrared-visible Sum-Frequency Generation (SFG). Employing the extremely wide tunability of the Free-Electron Laser for Infrared eXperiments (FELIX) at Rijnhuizen, we have studied the frequency dependence of the nonlinear susceptibility for sumfrequency generation in gallium phosphide between 20 and 32 μm in great detail. We have developed a shortpulse visible laser system that is highly synchronous with FELIX thereby creating a two-color setup that can be broadly applied. Resonantly enhanced SFG in alphaquartz has been used to study the relative timing stability of FELIX and the synchronized picosecond-laser system.