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In 1961, Peter Alden Franken, Alan Hill, C. Wilbur Peters and Gabriel Weinreich focused a pulsed ruby laser through a red optical filter into quartz. The filter suppressed xenon-flash background. A quartz-prism spectrograph used red-insensitive Eastman Type 103 plates. A single shot recorded a feature near $347.2\mathrm{nm}$ from $694.3\mathrm{nm}$ input. Removing the quartz or substituting glass removed the feature; changing polarization of waves and orientation followed their predicted pattern. These controls supported second-harmonic generation; photographic density gave an estimated yield.^[ref]

A spectrograph turns output frequency into a recording position. Its spectral separation makes a faint new component distinguishable from bright input light. The reported rounded wavelengths do not constitute an independent precision measurement of the ratio two. Nor do these observations demonstrate perfect phase matching or complete conversion. The experiment and Nicolaas S later theoretical account are distinct contributions to nonlinear optics.

Nicolaas Bloembergen and Arthur Leonard Schawlow received one quarter each for developing laser spectroscopy. Kai Manne Börje Siegbahn received one half for developing high-resolution electron spectroscopy.^[ref]

Nonlinear optics studies the response of matter to light when the induced electric polarization is not proportional to the driving electric field. An intense laser can make these additional terms observable. The striking consequence is that a material can emit light at a frequency absent from the incident beam: second-harmonic generation doubles it. This extends a s usable optical spectrum without requiring a second lasing transition.

Franken and colleagues frequency-doubling experiment established an optical harmonic in 1961. Nicolaas S theoretical work developed the description of interacting light waves in nonlinear matter. His 1981 lecture connects a nonlinear constitutive relation with Maxwell's equations and explains compensation of optical dispersion by birefringence.^[ref]