Nonlinear Laser Chemistry

Prefaces are usually written when a manuscript is finished. Having finished this book I can clearly see many shortcomings in it. But if I began to eliminate them I would probably write quite a different book in another two years; indeed, this has already happened once. In 1979, when I finished the first version of this book, it was much broader in scope and was to be titled "Laser Photochemistry." Corrections and additions to that unpublished manuscript gave rise to the present book with its revised title and more specific subject matter. I resolved to have it published in exactly this form, despite the fact that it concerns a dynamically developing field of research and will soon make way for other works. This book contains the basic ideas and results I have been developing with my colleagues, friends and students at the Institute of Spectroscopy, USSR Academy of Sciences, in the town of Troitsk since 1970. It deals with the interaction of light with atoms and molecules via multiple-phonon inter action. Nonlinear processes in the resonant interaction are used to illustrate the physical mechanisms involved and to indicate how these processes have led to modern applications such as isotope separation, detection of single atoms and molecules, and chemical and biochemical synthesis.

Contenu

1. Introduction.- 1.1 General Concepts of Selective Photophysics and Photochemistry.- 1.2 Classification of Selective Molecular Photoprocesses Induced by Laser Radiation.- 1.3 Selectivity and Yields of Photochemical Processes.- 1.4 Applications of Selective Laser Photochemistry.- 2. Selective Photoexcitation of Atoms and Molecules.- 2.1 Isotopic Selectivity in Linear Photoexcitation of Atoms and Molecules.- 2.2 Limitations of Linear Selectivity of Photoexcitation and Methods for Its Enhancement.- 2.3 Methods for the Enhancement of Selectivity with Nonlinear Photoexcitation.- 2.4 Overall Selectivity of Photochemical Processes.- 3. Multi-Step Selective Photoionization of Atoms.- 3.1 Introduction.- 3.2 Characteristics of Multi-Step Photoionization.- 3.3 Photoionization from Excited States to the Continuum and Autoionization States.- 3.4 Ionization of Highly Excited (Rydberg) Atomic States.- 3.5 Collision Processes in the Multi-Step Ionization of Atoms.- 4. Selective Monomolecular Photoprocesses with Nonlinear Excitation of Electronic States.- 4.1 Methods Used in the Multi-Step Excitation of Molecular Electronic States.- 4.2 Photodissociation of Molecules by Two-Step Excitation Through Vibrational States.- 4.3 Monomolecular Photoprocesses with Multi-Photon Vibrational and Subsequent Electronic Excitation.- 4.4 Photoionization of Molecules Through Nonlinear Excitation of Electronic States.- 5. Multi-Photon Monomolecular Photoprocesses in the Ground Electronic State.- 5.1 Introduction to IR Multi-Photon Laser Chemistry.- 5.2 Multi-Photon (MP) Absorption of IR Radiation and Excitation of Molecules Through Lower Vibrational Levels.- 5.3 Multi-Photon Excitation of Molecules in the Vibrational Quasi-Continuum and Distribution of Vibrational Energy.- 5.4 Dissociation of Highly Excited Molecules.- 5.5 Molecular Isomerization under MP Excitation.- 5.6 Isotopic Selectivity of the MP Dissociation.- 6. Laser Photoseparation on an Atomic and a Molecular Level.- 6.1 Introduction to Methods of Laser Photoseparation.- 6.2 Separation of Atoms Through Photoionization.- 6.3 Separation of Molecules Through Photodissociation.- 7. Selective Laser Detection of Atoms and Molecules.- 7.1 Detection of Single Atoms by Selective Multi-Step Photoionization.- 7.2 Detection of Molecules by Selective Photoionization and Mass Spectrometry.- 7.3 Laser Photoionization Visualization of Molecules and Spatial Localization of Molecular Bonds.- 8. Laser Photochemistry and Photobiochemistry.- 8.1 IR Multi-Photon Photochemistry.- 8.2 Nonlinear Photochemistry of Biomolecules in Solution.- Main Notations.- References.- Additional Reading.