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Measurement of Ultrafast Vibrational Coherences in Polyatomic Radical Cations with Strong-Field Adiabatic Ionization

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High-sensitivity fluorescence-detected multidimensional electronic spectroscopy through continuous pump-probe delay

Amitav Sahu¹, Vivek N Bhat¹, Sanjoy Patra¹

¹Solid State and Structural Chemistry Unit, Indian Institute of Science, Bangalore, Karnataka, 560012, India.

The Journal of Chemical Physics

|January 14, 2023

Summary

This summary is machine-generated.

We developed a highly sensitive fluorescence-detected multidimensional electronic spectroscopy (fMES) method. This technique enables detailed analysis of molecular vibrations at significantly lower sample concentrations than previously possible.

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Area of Science:

Spectroscopy
Quantum Chemistry
Physical Chemistry

Background:

Multidimensional electronic spectroscopy (MES) offers detailed insights into molecular dynamics.
Conventional MES lacks the sensitivity required for analyzing dilute samples.
Integrating fluorescence detection with MES (fMES) aims to enhance sensitivity and spatial resolution.

Purpose of the Study:

To present a visible white light continuum-based fMES spectrometer.
To systematically evaluate the sensitivity enhancement offered by fluorescence detection in fMES.
To demonstrate the capability of fMES for analyzing molecular coherences at low concentrations.

Main Methods:

Development of a visible white light continuum-based fMES spectrometer.
Implementation of biased sampling along optical coherence time axes.
Rapid scanning of pump-probe waiting time (T) with acousto-optic phase modulation and phase-sensitive lock-in detection.
Utilizing non-uniform undersampled grids for faster data acquisition.

Main Results:

Demonstration of room-temperature two-dimensional coherence maps of vibrational quantum coherences.
Successful analysis of a laser dye at optical densities 2-3 orders of magnitude lower than conventional methods.
Detection of vibrational wavepackets at very low optical densities using the developed fMES system.

Conclusions:

Fluorescence-detected multidimensional electronic spectroscopy significantly enhances sensitivity for molecular dynamics studies.
The developed fMES spectrometer enables the study of vibrational quantum coherences in dilute systems.
This approach paves the way for combining high sensitivity with microscopic spatial resolution in spectroscopy.