Nonresonant two-photon electronic spectroscopy of polyatomic molecules
is reviewed for the period since 1979. Emphasis is placed on studies
that expose patterns in the two-photon fluorescence (also ionization,
optoacoustic) excitation spectra of aromatic hydrocarbons and the effe
ct of vibrations and substitution, particularly within the framework o
f pseudoparity rules. A section is devoted to biological molecules and
the emerging use of two-photon-induced fluorescence anisotropy. Relev
ant theoretical results are discussed, with emphasis on quantum chemic
al predictions of vibronic coupling and substituent effects on two-pho
ton absorptivity and tensor properties of individual molecules. This c
hapter includes higher-order spectroscopy, and a limited number of thr
ee- and four-photon studies are discussed.