This unique volume presents a comprehensive but accessible introduction to the field of ultrafast two-dimension infrared (2D IR) vibrational echo spectroscopy based on the pioneering work of Professor Michael D Fayer, Department of Chemistry, Stanford University, USA. It contains in one place a qualitative introduction to the field of 2D IR spectroscopy and a comprehensive set of scientific papers that underlie the qualitative discussion. The introductory material contains several detailed illustrations, and is based on the Centenary Lecture at the Indian Institute of Science given by Professor Fayer July 16, 2008 as part of the celebration of the 100th anniversary of the founding of IIS in Bangalore, India. The second part of the volume contains reprints of Fayer's relevant papers. The compilation will be very useful because it presents the historical background, motivation, methodology, and experimental results at a level that is accessible to the non-expert. The reprints of the scientific papers, from review articles to detailed theoretical papers, provide rigorous supporting material so that the reader can delve as deeply as desired into the subject.

The advent of laser-based sources of ultrafast infrared pulses has extended the study of very fast molecular dynamics to the observation of processes manifested through their effects on the vibrations of molecules. In addition, non-linear infrared spectroscopic techniques make it possible to examine intra- and intermolecular interactions and how such interactions evolve on very fast time scales, but also in some instances on very slow time scales. Ultrafast Infrared Vibrational Spectroscopy is an advanced overview of the field of ultrafast infrared vibrational spectroscopy based on the scientific research of the leading figures in the field. The book discusses experimental and theoretical topics reflecting the latest accomplishments and understanding of ultrafast infrared vibrational spectroscopy. Each chapter provides background, details of methods, and explication of a topic of current research interest. Experimental and theoretical studies cover topics as diverse as the dynamics of water and the dynamics and structure of biological molecules. Methods covered include vibrational echo chemical exchange spectroscopy, IR-Raman spectroscopy, time resolved sum frequency generation, and 2D IR spectroscopy. Edited by a recognized leader in the field and with contributions from top researchers, including experimentalists and theoreticians, this book presents the latest research methods and results. It will serve as an excellent resource for those new to the field, experts in the field, and individuals who want to gain an understanding of particular methods and research topics.

Vibrational spectroscopy is one of the most powerful techniques in chemistry due to its ability to report direct information on the geometries and nuclear motions of complex molecules. At thermal equilibrium, rearrangements between different, or equivalent, molecular structures help to define the reactivity of the system. On the ultrafast timescale, these chemical exchange reactions may cause features in the vibrational spectrum to become averaged. The Bloch equations have been used previously to quantitatively predict the rates of such reactions. This approach has been quite successful in NMR spectroscopy where exchange on the microsecond timescale is often sufficient to cause peak coalescence. The application of the Bloch equations to IR spectroscopy has been debated due to the presence of other contributions to the vibrational lineshape that may prevent an accurate description of the relevant dynamics. Two dimensional infrared spectroscopy (2D-IR) is a time resolved ultrafast technique that is capable of directly measuring the kinetics of chemical exchange at thermal equilibrium where there is no net change in the populations of reactants and products. This work examines two model systems that display dynamic IR peak coalescence. A group of mixed valence dimers of trinuclear ruthenium clusters have exhibited a wide range of IR coalescence that is sensitive to solvent, temperature, and ligand substitution. No electron exchange was observed by 2D-IR during the timescale required for peak coalescence. The two isomers of a square pyramidal ruthenium dithiolene compound also result in highly coalesced spectra. The equilibrium populations, as well as the extent of peak coalescence, are strongly dependent on temperature and solvent. The experimental results of this second project were largely inconconclusive; however, future work with density functional theory calculations looks promising for revealing more information on these dynamics. Ultimately, the application of the Bloch equations to IR spectra is not generally reliable. While this type of analysis may still yield accurate results in some special cases, it is very difficult to distinguish legitimate exchange induced coalescence from similar broadened lineshape features, and this approach should be avoided.

This book summarizes several years of research carried out by a collaboration of many groups on ultrafast photochemical reactions. It emphasizes the analysis and characterization of the nuclear dynamics within molecular systems in various environments induced by optical excitations and the study of the resulting molecular dynamics by further interaction with an optical field.

This volume is a collection of papers presented at the Fifteenth International Conference on Ultrafast Phenomena held at the Asilomar Conference Grounds, Pacifc Grove, CA, USA, from July 31 – August 4, 2006. The Ultrafast P- nomena conferences are held every two years and provide a forum for disc- sion of the latest results in ultrafast optics and their applications in science and engineering. These meetings bring together researchers spanning several felds of science and engineering to discuss and debate the latest advances in ult- fast science. This unique forum provides a conduit for the greater dissemi- tion of the latest advances using ultrashort coherent pulses of light. More than 280 papers were presented. Signifcant progress in creating ever shorter pulses of light was reported in the attosecond range, with new applications in high harmonic generation and frequency comb metrology. Multidimensional sp- troscopy is rapidly evolving to provide new insights into quantum coherence and interactions in complex systems. Improvements in time resolved electron and x-ray diffraction provide better atomic scale perspectives on structural dynamics. These examples are but a small subset of the collected works ga- ered in this volume, which provides a valuable synopsis of the recent advances and impact of ultrafast technology in illuminating fundamental processes in physics, chemistry, and biology. There were 323 attendees at the meeting, more than one third of which were graduate and postdoctoral students. Increased s- dent attendance energized the proceedings.