An Introduction to Coherent Multidimensional Spectroscopy

Abstract

Coherent multidimensional spectroscopy is a field that has drawn much attention as an optical analogue to multidimensional nuclear magnetic resonance imaging. Coherent multidimensional spectroscopic techniques produce spectra that show the magnitude of an optical signal as a function of two or more pulsed laser frequencies. Spectra can be collected in either the frequency or the time domain. In addition to improving resolution and overcoming spectral congestion, coherent multidimensional spectroscopy provides the ability to investigate and conduct studies based upon the relationship between different peaks. The purpose of this paper is to provide a general introduction to the area of coherent multidimensional spectroscopy, to provide a brief overview of current experimental approaches, and to discuss some emerging developments in this relatively young field.

Proof and Use of the Method of Combination Differences for Analyzing High-Resolution Coherent Multidimensional Spectra

“…Since E 1 (J) and E 2 (J) are 2nth degree polynomials, it follows E 1 (J) − E 2 (J − J 1 + J 2 ) is polynomial of degree at most 2n. However, the above computation (recalling the definition of L) shows E 1…”

“…During the past two decades, coherent multidimensional spectroscopy (CMDS) has emerged as a powerful tool that can overcome the limitations of traditional one-dimensional techniques [1][2][3][4][5]. High-resolution coherent multidimensional spectroscopy (HRCMDS) is a form of CMDS that is designed to overcome congestion problems commonly found in the high-resolution spectra of gas-phase molecules [6].…”

Worthwhile Relevance of Infrared Spectroscopy in Characterization of Samples and Concept of Infrared Spectroscopy-Based Synchrotron Radiation

“…e cross peaks in the first are relevant to the scalar coupling, whereas, in the later, they are relevant to the spin transfer between diverse nuclei [81,82]. e 2DNMR techniques analogs are imitated in nonlinear two-dimensional IR spectroscopy, where the nonlinear two-dimensional IR spectroscopy with zero delay time corresponds to COSY [83]. In addition, nonlinear two-dimensional IR spectroscopy with fixed delay time permitting vibrational population transfer which corresponds to NOESY [84].…”

iSPECTRON: A simulation interface for linear and nonlinear spectra with ab‐initio quantum chemistry software

“…The past few decades have witnessed the birth of multi-dimensional multi-pulse techniques, which allow one to study elementary molecular events such as energy and charge transfer processes, formation and evolution of vibrational and electronic coherences, conformational and solvent dynamics and even to study the evolution of a system simultaneously in time and space (4D spectroscopy). [1][2][3][4][5][6][7][8] In combination with ultra-short laser pulses with high phase stability, these novel techniques have equipped researchers with the necessary tools to unravel gas-and condensed-phase dynamics in the sub-femtosecond (fs, 10 −15 s) and even in the attosecond (as, i.e., 10 −18 s) 9,10 regimes with an unprecedented level of detail. Nonetheless, connecting the optical response of the system to the underlying quantum-chemical structure and vibronic…”