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The allure of high-resolution spectroscopy arises from the fact that the resulting spectra can be theoretically analyzed with a high degree of accuracy. Deduced parameters such as bond lengths, dipole moments, rotational constants, and quadrupole and centrifugal distortion parameters can be very well determined, both numerically and also in terms of their physical description. This “knowing a lot about very little things” is a rarity in science [Frontiers of Molecular Spectroscopy; J. Laane, Ed.; Elsevier, 2009]. However, the assignment of rotationally resolved spectra measured on samples at room temperature can be extremely difficult or even impossible for large molecular systems due to the high density of states. Thus, HR spectroscopy combined with jet-cooling techniques has proved essential for the study of such systems.

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