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.

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.

Coherent multidimensional spectroscopy (CMDS) encompasses a family of experimental strategies involving the nonlinear interaction between electric fields and a material under investigation. This approach has several unique capabilities: (1) resolving congested states, (2) extracting spectra that would otherwise be selection-rule disallowed, (3) resolving fully coherent dynamics, (4) measuring coupling, and (5) resolving ultrafast dynamics. CMDS can be collected in the frequency or the time domain, and each approach has advantages and disadvantages. Frequency domain ``Multi-resonant'' CMDS (MR-CMDS) requires pulsed ultrafast light sources with tunable output frequencies. These pulses are directed into a material under investigation. The pulses interact with the material, and due to the specific interference between the multiple fields the material is driven to emit a new pulse: the MR-CMDS signal. This signal may have a different frequency and/or direction than the input pulses, depending on the exact experiment being performed. The MR-CMDS experiment involves tracking the intensity of this output signal as a function of different properties of the excitation pulses. These properties include (1) frequency. (2) relative arrival time and separation (delay), (3) fluence, and (4) polarization, among others. Thus MR-CMDS can be thought of as a multidimensional experimental space, where experiments typically involve explorations in one to four of the properties above. Because MR-CMDS is a family of related-but-separate experiments, each of them a multidimensional space, there are special challenges that must be addressed when designing a general-purpose MR-CMDS instrument. These issues require development of software, hardware, and theory. Part I: Background introduces relevant literature which informs on this development work. Part II: Development presents five strategies used to improve MR-CMDS: (1) processing software, (2) acquisition software (3), active artifact correction, (4) automated OPA calibration, and (5) finite pulse accountancy. Finally, Part III: Applications presents four examples where these instruments, with these improvements, have been used to address chemical questions in semiconductor systems.

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.

Advances in Atomic, Molecular, and Optical Physics, Volume 66 provides a comprehensive compilation of recent developments in a field that is in a state of rapid growth. New to this volume are chapters devoted to 2D Coherent Spectroscopy of Electronic Transitions, Nonlinear and Quantum Optical Properties and Applications of Intense Twin-Beams, Non-classical Light Generation from III-V and Group-IV Solid-State Cavity Quantum Systems, Trapping Atoms with Radio Frequency Adiabatic Potentials, Quantum Control of Optomechanical Systems, and Efficient Description of Bose–Einstein Condensates in Time-Dependent Rotating Traps. With timely articles written by distinguished experts that contain relevant review materials and detailed descriptions of important developments in the field, this series is a must have for those interested in the variety of topics covered. Presents the work of international experts in the field Contains comprehensive articles that compile recent developments in a field that is experiencing rapid growth, with new experimental and theoretical techniques emerging Ideal for users interested in optics, excitons, plasmas, and thermodynamics Topics covered include atmospheric science, astrophysics, surface physics, and laser physics, amongst others