For nearly half a century, scientists have celebrated the happy marriage of laser technology and the science of spectroscopy, the study of atoms, molecules, and solids by their emission and absorption of light. The union of the two fields has led to rich and remarkable fundamental discoveries and experimental techniques for investigating matter and its interaction with light.

The first demonstrations of laser emission in 1960 and 1961 prompted an immediate interest in spectroscopy. 1 That’s no surprise because the laser’s originators and early developers were spectroscopists, eager to exploit the laser’s spectral purity, coherence, and optical power density that were orders of magnitude higher than those of conventional light sources. The laser also provided extremely short pulse lengths over a range of discrete wavelengths that would eventually be tunable and stretch from the IR through the visible and into the vacuum UV. Because the polarizabilities and dielectric susceptibilities...

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