There is a growing consensus that traditional approaches to submillimeter spectroscopy will continue to be outpaced by the growth of molecular astrophysics and the analytical sciences. We report here a methodology that significantly reduces this challenge by providing three-dimensions of spectroscopic information ( frequency, line strength, and lower-state energy), even for complex, perturbed spectra, without the need for spectral analysis. The method is based on the analysis of complete, intensity-calibrated spectra taken over a range of temperatures. The 3D spectral information significantly reduces the assignment space and leads to much more efficient and accurate spectral assignment and quantum-mechanical modeling. (C) 2010 Published by Elsevier B. V.