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Two-dimensional fluorescence spectroscopy with quantum entangled photons: Idler-referenced timing without pump
Yuta Fujihashi1, Akihito Ishizaki1
1Department of Chemistry, The University of Tokyo, Tokyo 113-0033, Japan.
The Journal of Chemical Physics
|June 9, 2026
Summary
This study introduces an idler-referenced timing scheme for entangled photon spectroscopy, simplifying experiments. This method enhances time-resolved fluorescence spectroscopy by removing cumbersome pump-timing requirements.
Area of Science:
- Quantum Optics
- Spectroscopy
- Nonlinear Optics
Background:
- Entangled photons are increasingly used for time-resolved spectroscopy.
- Previous methods required cumbersome pump-timing synchronization.
- Non-classical correlations offer unique spectroscopic capabilities.
Purpose of the Study:
- To theoretically examine an alternative protocol for time-resolved spectroscopy using entangled photons.
- To simplify experimental setups by eliminating the need for pump-timing.
- To enable easier realization of time-resolved two-dimensional fluorescence spectroscopy.
Main Methods:
- Theoretical examination of an idler-photon-referenced timing protocol.
- Analysis of entangled photons with negative or negligible frequency correlations.
- Evaluation of frequency-time degrees of freedom over the measurement timescale.
Main Results:
- The idler-referenced scheme effectively defines the time origin.
- Eliminating the pump-timing channel simplifies the optical layout.
- The scheme is effective for entangled photons with specific frequency correlation properties.
Conclusions:
- An idler-referenced timing protocol simplifies entangled photon spectroscopy.
- This simplification lowers the experimental barrier for time-resolved fluorescence spectroscopy.
- Careful matching of photon temporal characteristics to the experimental timescale is crucial for exploiting non-classical correlations.

