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Fluorescence-detected two-dimensional electronic coherence spectroscopy by acousto-optic phase modulation.

Patrick F Tekavec¹, Geoffrey A Lott, Andrew H Marcus

¹Department of Physics, University of Oregon, Eugene, Oregon 97403, USA.

The Journal of Chemical Physics

|December 11, 2007

Summary

This summary is machine-generated.

We developed a new phase-selective method for two-dimensional electronic coherence spectroscopy (ECS) using acousto-optic modulation. This robust technique simplifies measurements of optical mode coupling in photoluminescent systems.

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Area of Science:

Nonlinear optics
Quantum spectroscopy
Materials science

Background:

Two-dimensional electronic coherence spectroscopy (ECS) probes coupling between optical modes using ultrashort laser pulses.
Conventional ECS requires precise control over pulse delays, complicating experiments.
Understanding resonant nonlinear optical responses is crucial for materials development.

Purpose of the Study:

Introduce a novel, robust experimental scheme for phase-selective nonlinear ECS.
Overcome limitations of conventional methods in controlling pulse temporal phases.
Accurately determine the complex-valued third-order susceptibility of photoluminescent systems.

Main Methods:

Combined acousto-optic phase modulation with ultrashort laser excitation.
Generated intensity-modulated nonlinear fluorescence signals.
Utilized synchronous detection with tailored references to isolate specific nonlinear contributions.
Decoupled relative temporal phases from pulse envelopes in a collinear four-pulse sequence.

Main Results:

Achieved a robust, high signal-to-noise phase-selective ECS scheme.
Demonstrated the method's validity using atomic Rubidium vapor as a model quantum three-level system.
Successfully determined the resonant complex-valued third-order susceptibility.

Conclusions:

The developed method offers a simplified and reliable approach to phase-selective ECS.
This technique enhances the study of optical mode coupling and nonlinear optical responses.
Provides a powerful tool for characterizing photoluminescent materials.