Multi-Dimensional Spectroscopy with Intense Entangled Beams : Entanglement-Enabled Phase Matching in a Collinear Beam Geometry
(2025) In Journal of Physical Chemistry Letters 16. p.12124-12129- Abstract
The experimental realization of quantum molecular spectroscopy with entangled photons remains challenging owing to the low signal-to-noise ratio resulting from the use of low-flux entangled photons. High-flux entangled photons via intense entangled beams can be used to improve the signal-to-noise ratio, but the presence of unentangled photons contaminates the quantum signal stemming from entangled photons. Here, we demonstrate how intense entangled beams can be used in multi-dimensional spectroscopy while retaining the advantage of photon entanglement. Our approach is broadly applicable to odd-ordered nonlinear spectroscopies, and it generates purely quantum spectroscopic signals. The proposed approach allows the recording of desired... (More)
The experimental realization of quantum molecular spectroscopy with entangled photons remains challenging owing to the low signal-to-noise ratio resulting from the use of low-flux entangled photons. High-flux entangled photons via intense entangled beams can be used to improve the signal-to-noise ratio, but the presence of unentangled photons contaminates the quantum signal stemming from entangled photons. Here, we demonstrate how intense entangled beams can be used in multi-dimensional spectroscopy while retaining the advantage of photon entanglement. Our approach is broadly applicable to odd-ordered nonlinear spectroscopies, and it generates purely quantum spectroscopic signals. The proposed approach allows the recording of desired phase-matched signals even in a collinear beam geometry, which lifts the requirement of complicated beam geometry setups for phase matching in multi-dimensional spectroscopies.
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- author
- Jadoun, Deependra LU ; Harbola, Upendra ; Chernyak, Vladimir Y. and Mukamel, Shaul
- organization
- publishing date
- 2025
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Journal of Physical Chemistry Letters
- volume
- 16
- pages
- 6 pages
- publisher
- The American Chemical Society (ACS)
- external identifiers
-
- pmid:41230925
- scopus:105022078675
- ISSN
- 1948-7185
- DOI
- 10.1021/acs.jpclett.5c02496
- language
- English
- LU publication?
- yes
- id
- e818598c-b542-4797-8e9a-54ec4c131dcc
- date added to LUP
- 2026-02-10 11:45:30
- date last changed
- 2026-02-24 13:01:31
@article{e818598c-b542-4797-8e9a-54ec4c131dcc,
abstract = {{<p>The experimental realization of quantum molecular spectroscopy with entangled photons remains challenging owing to the low signal-to-noise ratio resulting from the use of low-flux entangled photons. High-flux entangled photons via intense entangled beams can be used to improve the signal-to-noise ratio, but the presence of unentangled photons contaminates the quantum signal stemming from entangled photons. Here, we demonstrate how intense entangled beams can be used in multi-dimensional spectroscopy while retaining the advantage of photon entanglement. Our approach is broadly applicable to odd-ordered nonlinear spectroscopies, and it generates purely quantum spectroscopic signals. The proposed approach allows the recording of desired phase-matched signals even in a collinear beam geometry, which lifts the requirement of complicated beam geometry setups for phase matching in multi-dimensional spectroscopies.</p>}},
author = {{Jadoun, Deependra and Harbola, Upendra and Chernyak, Vladimir Y. and Mukamel, Shaul}},
issn = {{1948-7185}},
language = {{eng}},
pages = {{12124--12129}},
publisher = {{The American Chemical Society (ACS)}},
series = {{Journal of Physical Chemistry Letters}},
title = {{Multi-Dimensional Spectroscopy with Intense Entangled Beams : Entanglement-Enabled Phase Matching in a Collinear Beam Geometry}},
url = {{http://dx.doi.org/10.1021/acs.jpclett.5c02496}},
doi = {{10.1021/acs.jpclett.5c02496}},
volume = {{16}},
year = {{2025}},
}