Optical Multidimensional Coherent Spectroscopy

This book provides an introduction to optical multidimensional coherent spectroscopy, a relatively new method of studying materials based on using ultrashort light pulses to perform spectroscopy. The technique has been developed and perfected over the last 25 years, resulting in multiple experimental approaches and applications to a broad array of systems ranging from atoms and molecules to solids and biological systems. Indeed, while this method is most often used by physical chemists, it is also relevant to materials of interest to physicists, which is the primary focus of this book. As well as an introduction to the method, the book also provides tutorials on the interpretation of the rather complex spectra that is broadly applicable across all subfields, and finishes with a survey of several emerging material systems and a discussion of future directions.

This book will fulfill the needs of time-domain spectroscopists who wish to deepen their understanding of both the theoretical and experimental features of this cutting-edge spectroscopy technique. Coherent Multidimensional Spectroscopy (CMDS) is a state-of-the-art technique with applications in a variety of subjects like chemistry, molecular physics, biochemistry, biophysics, and material science. Due to dramatic advancements of ultrafast laser technologies, diverse multidimensional spectroscopic methods utilizing combinations of THz, IR, visible, UV, and X-ray radiation sources have been developed and used to study real time dynamics of small molecules in solutions, proteins and nucleic acids in condensed phases and membranes, single and multiple excitons in functional materials like semiconductors, quantum dots, and solar cells, photo-excited states in light-harvesting complexes, ions in battery electrolytes, electronic and conformational changes in charge or proton transfer systems, and excess electrons and protons in water and biological systems.

Two-Dimensional Optical Spectroscopy discusses the principles and applications of newly emerging two-dimensional vibrational and optical spectroscopy techniques. It provides a detailed account of basic theory required for an understanding of two-dimensional vibrational and electronic spectroscopy. It also bridges the gap between the formal development of nonlinear optical spectroscopy and the application of the theory to explain experimental results. Focusing on time-domain spectroscopy, the book presents detailed discussions on the underlying physics and interpretation methods of a variety of two-dimensional optical spectroscopic methods. It illustrates how novel diagrammatic techniques are useful in graphically describing the associated nonlinear optical transition pathways and involved population or coherence evolutions. The author also explains the basics of quantum dynamics and time-dependent perturbation theories that are required in describing nonlinear optical processes. From the development of the theory to novel applications, this book covers a gamut of topics in this field, including perturbation theory, coherent Raman scattering, pump-probe spectroscopy, photon echo spectroscopy, IR-visible four-wave mixing, and linear and nonlinear optical activity spectroscopy. It shows how to apply the recently developed tools of vibrational and electronic spectroscopy in two dimensions.

Advanced spectroscopic techniques allow the probing of very small systems and very fast phenomena, conditions that can be considered "extreme" at the present status of our experimentation and knowledge. Quantum dots, nanocrystals and single molecules are examples of the former and events on the femtosecond scale examples of the latter. The purpose of this book is to examine the realm of phenomena of such extreme type and the techniques that permit their investigations. Each author has developed a coherent section of the program starting at a somewhat fundamental level and ultimately reaching the frontier of knowledge in the field in a systematic and didactic fashion. The formal lectures are complemented by additional seminars.

This volume contains the lectures and seminars presented at the NATO Advanced Study Institute on "Coherence in Spectroscopy and Modern Physics," the seventh course of the International School of Quantum Electronics, affiliated with the "Ettore Majorana" Centre for Scientific Culture, Erice, Sicily. The Institute was held at Villa LePianore (Lucca), Versilia, Italy, July 17-30, 1977. The International School of Quantum Electronics was started in 1970 with the aim of providing instruction for young researchers and advanced students already engaged in the area of quantum electronics or wishing to switch to this area from a different background. From the outset the School has been under the direction of Prof. F. T. Arecchi, then at the University of Pavia, now at the University of Florence, and Dr. D. Roess of Siemens, Munich. Each year the Directors choose a subject of particular interest, alternating fundamental topics with technological ones, and ask colleagues specifically competent in a given area to take the scientific responsibility for that course.