This Perspective on multidimensional spectroscopy in the optical and infrared spectral regions focuses on the principles and the scientific and technical challenges facing these new fields. The methods hold great promise for advances in the visualization of time-dependent structural changes in complex systems ranging from liquids to biological assemblies, new materials, and fundamental physical processes. The papers in this special feature on multidimensional spectroscopy in chemistry, physics, and biology are typical of many recent advances.