Volume averaging effect in nonlinear processes of focused laser fields

We report theoretical derivations and experimental results on the volume averaging effect of nonlinear processes in focused laser fields. This effect is considered detrimental in revealing the intensity dependence of a nonlinear process, caused by the intensity variation across the sampled volume of a focused laser. Following the treatment in the literature, we prove that if the signal dependence can be expressed as a simple power function of the laser intensity and if the detection region encompasses effectively the whole volume, volume average does not affect the final conclusion on the derived exponent. However, to reveal the detailed saturation effect of a multi-photon process, intensity selective scans involving spatial filters and displacement of the laser focus (z-scan) are required. Moreover, to fully capture the dependence of the signal on the variation of the laser intensity, the degree of spatial discrimination and the corresponding range of the z-scan need to be modeled carefully. Limitations in the dynamic range of the detector or the laser power, however, can thwart the desired scan range, resulting in erroneous fitting exponents. Using our nanosecond laser with a non-ideal Gaussian beam profile based on multiphoton ionization of argon atoms from a collimated molecular beam and from ambient argon gas, we report experimental measurements of the beam waist and Rayleigh range and compare the experimental intensity dependence of Ar⁺ with theoretical values. Agreements between theory and experiment are remarkable.