Powders Analysis by Second Harmonic Generation Microscopy

Abstract

A microscopy approach is developed for quantifying second harmonic generation (SHG) activity of powders that largely decouples linear and nonlinear optical interactions. Decoupling the linear and nonlinear optical effects provides a means to independently evaluate and optimize the role of each in crystal engineering efforts and facilitates direct comparisons between experimental and computational predictions of lattice hyperpolarizabilities. In this respect, the microscopy-based approach nicely complements well-established Kurtz-Perry ( J. Appl. Phys. 1968 , 39 , 3798 ) and related methods, in which collimated sources are used for powders analysis. Using a focused fundamental beam places a controllable upper bound on the interaction length, given by the depth of field. Because measurements are performed on a per-particle basis, crystal size-dependent trends can be recovered from a single powdered sample. An analytical model that includes scattering losses of a focused Gaussian beam reliably predicted several experimental observations. Specifically, the measured scattering length for SHG was in excellent agreement with the value predicted based on the particle size distribution. Additionally, histograms of the SHG intensities as functions of particle size and orientation agreed nicely with predictions from the model.