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Updated: Jun 23, 2026

A Multimodal Wide-Field Fourier-Transform Raman Microscope

A Multimodal Wide-Field Fourier-Transform Raman Microscope

Published on: December 30, 2025

Mixed frequency-/time-domain coherent multidimensional spectroscopy: research tool or potential analytical method?

Andrei V Pakoulev¹, Mark A Rickard, Kathryn M Kornau

¹Department of Chemistry, University of Wisconsin, Madison, Wisconsin 53706, USA.

Accounts of Chemical Research

|May 19, 2009

Summary

Coherent multidimensional spectroscopy (CMDS) advances by enabling multiple quantum coherences, similar to nuclear magnetic resonance (NMR). This allows detailed study of molecular energy states and dynamics using frequency-domain techniques.

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Last Updated: Jun 23, 2026

A Multimodal Wide-Field Fourier-Transform Raman Microscope

A Multimodal Wide-Field Fourier-Transform Raman Microscope

Published on: December 30, 2025

Area of Science:

Physical Chemistry
Spectroscopy
Quantum Mechanics

Background:

Coherent multidimensional spectroscopy (CMDS) is the optical analog of nuclear magnetic resonance (NMR).
Widespread application of CMDS requires excitation of multiple quantum coherences across diverse quantum state energies.
Existing CMDS methods need enhancement to match NMR's capability in generating multiple quantum coherences.

Purpose of the Study:

To focus on frequency-domain CMDS methods for exciting multiple quantum coherences.
To explore the formation of multiple quantum coherences between states with significantly different energies.
To utilize nickel and rhodium chelates as model systems for understanding mixed frequency-/time-domain CMDS.

Main Methods:

Employing frequency-domain CMDS to tune excitation frequencies to quantum state resonances.
Utilizing multiple excitation pulses to generate multiple quantum states within their dephasing time.
Analyzing two-dimensional contour plots to visualize state energies and dynamics, and scanning time delays in mixed-domain methods.

Main Results:

Frequency-domain CMDS successfully forms multiple quantum coherences between states with large energy differences.
Mixed frequency-/time-domain methods reveal dynamics by scanning time delays, showing changes in spectral features based on coherence order.
Coherence transfer and higher-order coherences (e.g., double quantum) are observed, leading to new spectral features and dynamic Stark splittings.

Conclusions:

Frequency-domain CMDS provides a powerful approach for generating and studying multiple quantum coherences.
Mixed-domain methods offer insights into coherence and population dynamics, visualizing temporal changes in spectral features.
The observed phenomena pave the way for advanced higher-order multiple quantum coherence methods and probing molecular potential energy surfaces.