Electronic carrier dynamics are integral in the design of functional metal transducers. Moreover, the optical properties and dynamics of colloidal metals depend sensitively their structures. Hence, a comprehensive understanding of how structural factors like size, geometry, and composition influence electronic relaxation processes allows for the development of predictive models for judicious selection of nanoscale metals for photonic applications. This dissertation focused on the usage of time-resolved nonlinear spectroscopy techniques, specifically femtosecond transient absorption and two-dimensional electronic spectroscopy (2DES) to probe electronic relaxation dynamics in colloidal metals, including: monolayer-protected clusters (MPCs), plasmonic gold nanorods, metal hybrid nanostructures, and 2-D semiconductors. The ultrafast relaxation mechanisms in all of these systems were understood in relation to structure-specific and state-resolved dynamics. 2DES results resolved excited-state symmetry-dependent relaxation dynamics in 38-atom gold nanoclusters that were influenced by specific metal kernel and inorganic semiring structures. It is shown that Fermi liquid dynamics can be resolved in plasmonic metal ensembles. It is also shown that synthetic modification to size and composition of a single domain in composite metal nanostructures can be used to overcome bulk-like contributions that govern phonon-mediated thermalization. In addition, phonon-mediated renormalization rates across different materials thicknesses (i.e. number layers) in 2-D semiconductors is described. All of these results indicate that specific nanostructures (size, composition, thickness, and geometry) play integral roles in governing ultrafast relaxation dynamics in complex nanoscale metal colloids, which in turn can be leveraged to develop predictive models for optimal design of functional metal transducers.

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.

Multiresonant coherent multidimensional spectroscopy (MR-CMDS) is a fully coherent mixed frequency/time domain technique that selectively characterizes vibrational and electronic energetic structure and dynamics. The work reported here describes technique development with 1-picosecond pulses on model vibrational systems, application of this technique to PbSe quantum dots, and recent adaptation to include use of 50-femtosecond pulses. An overview of the quantum mechanical theory behind experimental design and interpretation, with an emphasis on the perturbative limit, is included. A record of the instrumentation and optical component selection associated with both laser systems is provided, which is particularly important for the development of the femtosecond laser table. Initial experiments on the femtosecond system revealed environmental artifacts that have now been identified and characterized. Picosecond pulses are not a good match for studying PbSe quantum dots with MR-CMDS because the pulses are too long to isolate coherence lifetimes and fully coherent processes. Frequency domain results previously acquired on the picosecond system revealed coherence lifetimes near 50fs, which directed the selection of a more appropriate laser system. Experiments with femtosecond pulses are now confirmed to directly measure coherence lifetimes and selectively emphasize spectral signatures from fully coherent processes that were not visible with longer pulses. These confirmations reveal that the flexibility of MR-CMDS techniques, as developed on the model vibrational systems, is available for quantum-confined semiconductor structures. Future directions include laser system improvements and suggestions of samples that may better inform dye-sensitized solar cell core charge transfer events.

A valuable tool for individuals using correlation spectroscopy and those that want to start using this technique. Noda is known as the founder of this technique, and together with Ozaki, they are the two biggest names in the area First book on 2D vibrational and optical spectroscopy - single source of information, pulling together literature papers and reveiws Growing number of applications of this methodology - book now needed for people thinking of using this technique Limitations and benefits discussed and comparisons made with 2D NMR Discusses 20 optical and vibrational spectroscopy (IR, Raman, UV, Visible)

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 developm

This detailed, accessible introduction to the field of quantum decoherence reviews the basics and then explains the essential consequences of the phenomenon for our understanding of the world. The discussion includes, among other things: How the classical world of our experience can emerge from quantum mechanics; the implications of decoherence for various interpretations of quantum mechanics; recent experiments confirming the puzzling consequences of the quantum superposition principle and making decoherence processes directly observable.