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Published June 29, 2023 | Supplemental Material
Journal Article Open

Entangled Photon Correlations Allow a Continuous-Wave Laser Diode to Measure Single-Photon, Time-Resolved Fluorescence

Abstract

Fluorescence lifetime experiments are a standard approach for measuring excited-state dynamics and local environmental effects. Here, we show that entangled photon pairs produced from a continuous-wave (CW) laser diode can replicate pulsed laser experiments without phase modulation. As a proof of principle, picosecond fluorescence lifetimes of indocyanine green are measured in multiple environments. The use of entangled photons has three unique advantages. First, low-power CW laser diodes and entangled photon source design lead to straightforward on-chip integration for a direct path to distributable fluorescence lifetime measurements. Second, the entangled pair's wavelength is easily tuned by adjusting the temperature or electric field, allowing a single source to cover octave bandwidths. Third, femtosecond temporal resolutions can be reached without requiring major advances in source technology or external phase modulation. Entangled photons could therefore provide increased accessibility to time-resolved fluorescence while also opening new scientific avenues in photosensitive and inherently quantum systems.

Additional Information

© 2023 American Chemical Society. Verification of the lifetimes of the ICG dyes in this study with classical TCSPC was performed at the Caltech Biological Imaging Facility with the help of Giada Spigolon. Verification of the absorption spectra of the dye solutions was performed with the help of Helena Awad. This work was funded by the U.S. Department of Energy (DE-SC0020151). N.H. was supported by the Department of Defense through the National Defense Science and Engineering Graduate Fellowship Program. B.P.H. was supported by an NSF Graduate Research Fellowship (DGE-1745301). Author Contributions: N.H. and B.P.H. contributed equally to this work. Any opinion, findings, and conclusions or recommendations expressed in this material are those of the authors(s) and do not necessarily reflect the views of the National Science Foundation. The authors declare no competing financial interest.

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Created:
August 22, 2023
Modified:
October 20, 2023