Multidimensional signals are generated by subjecting molecules to sequences of short optical pulses and recording correlation plots related to the various controlled delay periods. These techniques which span all the way from the THz to the x-ray regimes provide qualitatively new structural and dynamical molecular information not available from conventional one-dimensional techniques. This issue surveys the recent experimental and theoretical progresses in this rapidly developing 20 year old field which illustrates the novel insights provided by multidimensional techniques into electronic and nuclear motions. It should serve as a valuable source for experts in the field and help introduce newcomers to this exciting and challenging branch of nonlinear spectroscopy.

J. Chem. Phys.
Ultrafast Spectroscopy

Mukamel, S, & Bakker, H.J. (2015). Preface: Special Topic on Multidimensional Spectroscopy. J. Chem. Phys., 142(21, Article number: 212101), 1–2. doi:10.1063/1.4921015