The main topic in this book is the low temperature selective spectroscopy of impurity centers. It deals not only with the well developed methods of selective spectroscopy of molecular ensembles such as spectral hole-burning, fluorescence line-narrowing and femtosecond photon echoes, but also new methods of nanospectroscopy such as single-molecule spectroscopy. Both the ory and experimental data are discussed. Theory united with experimental data enables one to organize the experimental facts. This organization is of great importance, especially for young researchers and students, because it can provide better insight into the nature of the rather complicated dynamics of guest molecules in polymers and glasses, where our understanding is still somewhat lacking. The book mainly addresses young researchers and graduate students studying modern methods of spectroscopy of solid solutions. For this rea son, all formulas commonly used in practice are derived in this book. The reader will also find new approaches and formulas which have been used by the author, but are not well known to the majority researchers. When the derivation of a formula seems rather complicated, it is included in appendix. The reader is then free to look the derivation up if he or she is interested. Oth erwise, the book can be read without reference to these sections. The book includes many examples where theory helps us to interpret experimental data of various types, for instance, the data on line- and hole-broadening.
First book to present a detailed theoretical basis for single molecule spectroscopy
It also describes numerous experimental applications of the theory
This book is a comprehensive guide to the theory of optical band shape of guest-molecule-doped crystals, polymers and glasses. The dynamics of a single molecule, measured with the help of a train of photons emitted at random time moments, is a main subject of the book. The dynamics is calculated with the help of quantum-mechanical methods and equations for the density matrix of the system consisting of a single chromophore interacting with light, phonons and non-equilibrium tunneling systems of polymers and glasses. A dynamical theory for one- and two-photon counting methods used in single molecule spectroscopy is presented. Photon bunching and antibunching, jumps of optical lines, and quantum trajectories of various types are further topics addressed. This is the first book to present a detailed theoretical basis for single molecule spectroscopy. It also describes numerous experimental applications of the theory.
I. Single Atom in Transverse Electromagnetic Field.- 1. Quantum Principles of Two-Level Atomic Spectroscopy.- 2. Two-Photon Start—Stop Correlator.- 3. Full Two-Photon Correlator.- II. Phonons and Tunneling Excitations.- 4. Adiabatic Interaction.- 5. Natural Vibrations of Solids.- 6. Tunneling Systems in Solids.- III. Spectroscopy of a Single Impurity Center.- 7. Density Matrix for an Impurity Center.- 8. One- and Two-Photon Counting Methods in the Spectroscopy of a Single Impurity Center.- IV. Optical Band Shape Theory for Impurity Centers.- 9. Stochastic Theories of Line Broadening.- 10. Dynamical Theory of Electron—Phonon Bands.- 11. Vibronic Spectra of Complex Molecules.- 12. Dynamical Theory of Line Broadening.- V. Methods of Selective Spectroscopy.- 13. Fluorescence Line Narrowing.- 14. Spectral Hole Burning in Inhomogeneous Optical Bands.- VI. Transient Coherent Phenomena in Solids.- 15. Coherent Radiation of Molecular Ensembles.- 16. Photon Echo.- 17. Nonexponential Photon Echo.- VII. Low Temperature Spectral Diffusion in Polymers and Glasses.- 18. Theory of Electron—Tunnelon Optical Band.- 19. Chromophore Interacting with Phonons and TLSs Which Are not in Thermal Equilibrium.- 20. Dynamical Theory of Spectral Diffusion.- 21. Theory of Tunneling Transitions in TLSs.- 22. Investigating TLS Relaxation by Single-Molecule Spectroscopy.- Appendices.- B. Probability of Spontaneous Photon Emission.- C. Unitarity of Amplitudes.- D. Derivation of (3.8).- E. Derivation of (3.24).- F. Proof of the Approximation (7.16).- G. The Wick—Bloch—Dominicis Theorem for Bosons.- H. Influence of FC and HT Interactions on the Optical Band Shape Function.- I. Cumulant Expansion.- J. Relation Between Phonon Green Functions.- L. Derivation of (17.65).- M. The Wick—Bloch—Dominicis Theorem for Fermions.- N. Derivation of (18.37) and (18.38).- O. Derivation of (18.53).- P. Derivation of (18.60).- Q. Stochastic Approach to Spectral Diffusion.