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Abstract Pathway selectivity in quantum spectroscopy with entangled photons is a powerful spectroscopic tool. Phase‐matched signals involving classical light contain contributions from multiple material pathways, whereas quantum spectroscopy may allow the selection of individual pathways. 2D electronic‐vibrational spectroscopy (2DEVS) is a four‐wave mixing technique which employs visible and infrared entangled photons. It is showed how the three contributing pathways—ground state bleach, excited state absorption, and excited state emission—can be separated by photon‐number‐resolved coincidence measurements. Entangled photons thus reveal spectral features not visible in the classical signal, with an enhanced spectral resolution.
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Enhanced Photochemical Reaction Rates with Entangled Photons
Photochemistry is a powerful tool for synthesizing important molecules which are challenging to create without light. We report compelling results which indicate that photochemical reaction rates (oxygenation and cycloaddition) can be notably enhanced by utilizing a very small number of entangled photons. Measurements with the same small number of classical photons show the rate of product formation is considerably lower. This suggests that the reaction rate with entangled photons is enhanced by many orders of magnitude. Theoretical calculations show that classical photons and entangled photons excite the photocatalyst to different final excited states. This chemical synthesis approach with entangled photons could have a large impact on our understanding of chemical reactivity and provide new insights into photochemical processes.
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- Award ID(s):
- 2347622
- PAR ID:
- 10652681
- Publisher / Repository:
- J. Phys. Chem. Lett; American Chemical Society
- Date Published:
- Journal Name:
- The Journal of Physical Chemistry Letters
- Volume:
- 16
- Issue:
- 18
- ISSN:
- 1948-7185
- Page Range / eLocation ID:
- 4372 to 4381
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript
- Journal Article:
- https://doi.org/10.1021/acs.jpclett.5c00836
