Advantages of polarized two-beam second-harmonic generation in precise characterization of thin films

Polarized second-harmonic generation using two fundamental beams, instead of one, offers significant advantages for characterizing nonlinear optical thin films. The technique is more precise and allows the internal consistency of the results to be verified. The superiority of the two-beam arrangement over the traditional single-beam arrangement is demonstrated by determining the susceptibility tensors of Langmuir-Blodgett films. We show that, for a well-understood reference sample, the results obtained using two fundamental beams agree qualitatively with those obtained with a single fundamental beam, but are more precise. In a more complicated situation, however, the single-beam technique appears to work well but yields results that are, in fact, incorrect. The two-beam technique, instead, yields clearly inconsistent results, thereby highlighting systematic errors in the experimental arrangement or in the theoretical model used to interpret the results.