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.
Author(s): Hebin Li, Bachana Lomsadze, Galan Moody, Christopher Smallwood, Steven Cundiff
Publisher: Oxford University Press
Year: 2023
Language: English
Pages: 298
City: Oxford
cover
titlepage
copyright
dedication
preface
Acknowledgements
Table of symbols
Table of
acronyms
contents
Basics of ultrafast spectroscopy
Basics of spectroscopy: linear versus nonlinear
Ultrashort pulses
Ultrafast nonlinear/coherent spectroscopy
The density matrix
Bloch sphere representation of quantum states
Introduction to multidimensional coherent spectroscopy
Concepts of multidimensional coherent spectroscopy
Coherent spectroscopy
Multidimensional coherent spectroscopy
Spectrum classification
Density matrix formalism and double-sided Feynman diagrams
Interpreting MDCS in the perturbative limit
Double-sided Feynman diagrams
Measured observables
Putting it all together
Case study: Two-level system
Phase matching
Two-dimensional infrared (2D IR) spectroscopy
Interpretation of multidimensional coherent spectra
Isolated two-level system
Inhomogeneously broadened ensemble of two-level systems
Gaussian inhomogeneity, constant homogeneous linewidth
Large inhomogeneity
Coherent coupling signatures
Incoherent coupling signatures
Doubly excited states and many-body interactions
Double-quantum spectra
Zero-quantum spectra
Three-dimensional coherent spectroscopy
Nonrephasing pathways and purely absorptive spectra
Finite-pulse effects
Mathematical formulations
Example spectra
Further applications
Experimental implementations
Experimental requirements and considerations
Precision and stability of time delays
Isolation of the signal
Detection of the signal
Overview of experimental approaches
Actively stabilized box geometry
Phase modulated collinear geometry
Comparison of different approaches
Data analysis
Multidimensional coherent spectroscopy of atomic ensembles
Single- and zero-quantum 2D spectra of atomic vapors
MDCS in optically thick samples
Probing many-body interactions with double-quantum 2D spectroscopy
Probing many-body correlations with multi-quantum 2D spectroscopy
Frequency comb-based multidimensional coherent spectroscopy
Introduction to frequency combs and dual-comb spectroscopy
Frequency comb-based four-wave-mixing spectroscopy
Frequency comb-based single-quantum 2D spectroscopy
Frequency comb-based double-quantum 2D spectroscopy
Tri-comb spectroscopy
Two-dimensional spectroscopy of semiconductor quantum wells
Introduction to semiconductor optics
Many-body signatures in one-quantum 2D spectra
Many-body signatures in double- and multi-quantum 2D spectra
Two-dimensional spectroscopy of coupled quantum wells
Quantum well exciton-polaritons in microcavities
Three-dimensional coherent spectroscopy
Fifth-order 3D infrared spectroscopy
Fifth-order 3D electronic spectroscopy
Third-order 3D electronic spectroscopy
Three-dimensional spectra of atomic vapors
Three-dimensional spectroscopy of semiconductor quantum wells
3D coherent spectroscopy of light-harvesting centers
3D coherent frequency domain spectroscopy
Two-dimensional spectroscopy of semiconductor quantum dots
Optical and electronic properties of quantum dots
2D coherent spectroscopy of GaAs quantum dots
2D spectroscopy of self-assembled In(Ga)As quantum dots
Coherent control of quantum dots
Coherent control within an ensemble of quantum dots
Coherent control of interactions between individual quantum dots
Two-dimensional spectroscopy of colloidal quantum dots
Two-dimensional spectroscopy of atomically thin 2D materials
Introduction to 2D materials
Homogeneous linewidth in 2D materials
Valley coherence and coupling in 2D materials
Other applications of multi-dimensional coherent spectroscopy in Physics
Semiconducting carbon nanotubes
Color centers in diamond
Perovskite materials
New trends in multidimensional coherent spectroscopy
Broadening the spectral range: from terahertz to x-rays
THz MDCS
Improving the spatial resolution
Multidimensional spectroscopy with quantum light
Photoemission-detected MDCS
Figure Credits
References
Index
Blank Page
Blank Page
Blank Page
Blank Page
Blank Page
Blank Page
