Introduction to State-of-the-Art Multidimensional Time-Resolved Spectroscopy Methods.

The field of multidimensional laser spectroscopy comprises a variety of highly developed state-of-the-art methods, which exhibit broad prospects for applications in several areas of natural, material, and even medical sciences. This collection summarizes the main achievements from this area and gives basic introductory insight into what is currently possible with such methods. In the present introductory contribution, we briefly outline the general concept behind multidimensional laser spectroscopy, for instance by highlighting the often-employed analogy between multidimensional laser spectroscopy and NMR methods. Our initial introduction is followed by an overview of the most important and widely used multidimensional spectroscopies' classification. Special emphasis is placed on how the contributing spectral region defines a natural way of grouping the techniques in terms of their information content. On this basis, we introduce the most important graphical ways in which multidimensional data is generally visualized. This is done by comparing specifically temporal and spectra axes that make up each single multidimensional data plot. Several central experimental methods that are common to the various techniques reviewed in this collection are addressed in the perspective of recent developments and their impact on the field. These methods include, for example, heterodyne/homodyne detection, fast scanning, spatial light modulation, and sparse sampling methods. Importantly, we address the central and fundamental questions where multidimensional ultrafast spectroscopy can be used to help understanding chemical dynamics and intermolecular interactions. Finally, we briefly pinpoint what we believe are the main open questions and what will be the future directions for technical developments and promotion of scientific understanding that multidimensional spectroscopy can provide for chemistry, physics, and life sciences.