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Entangled photon pairs are predicted to linearize and increase the efficiency of two-photon absorption, allowing continuous wave laser diodes to drive ultrafast time-resolved spectroscopy and nonlinear processes. Despite a range of…

Quantum Physics · Physics 2022-05-31 Bryce P. Hickam , Manni He , Nathan Harper , Szilard Szoke , Scott Cushing

Excitation with entangled photon pairs may lead to an increase in the efficiency of two-photon absorption at low photon flux. The corresponding process, entangled two-photon absorption (E2PA), has been investigated in numerous theoretical…

We experimentally study entangled two-photon absorption in Rhodamine 6G as a function of the spatial properties of a high flux of broadband entangled photon pairs. We first demonstrate a key signature dependence of the entangled two-photon…

Quantum Physics · Physics 2022-06-10 D. Tabakaev , A. Djorovic , L. La Volpe , G. Gaulier , S. Ghosh , L. Bonacina , J. -P. Wolf , H. Zbinden , R. T. Thew

We closely replicated and extended a recent experiment ("Spatial properties of entangled two-photon absorption," Phys. Rev. Lett. 129, 183601, 2022) that reportedly observed enhancement of two-photon absorption rates in molecular samples by…

Quantum Physics · Physics 2024-04-26 Tiemo Landes , Brian J. Smith , Michael G. Raymer

It has been proposed that entangled two-photon absorption (E2PA) can be observed with up to 10 orders of magnitude lower photon flux than its classical counterpart. However, there is a significant controversy regarding the magnitude of this…

When a low flux of time-frequency-entangled photon pairs (EPP) illuminates a two-photon transition, the rate of two-photon absorption (TPA) can be enhanced considerably by the quantum nature of photon number correlations and frequency…

We calculate the rate of two-photon absorption for frequency entangled photons in a tapered optical fiber whose diameter is comparable to the wavelength of the light. The confinement of the electric field in the transverse direction…

Quantum Physics · Physics 2010-04-12 Hao You , S. M. Hendrickson , J. D. Franson

Nonlinear spectroscopy and microscopy techniques are ubiquitous in a wide range of applications across physics and biology. However, these usually rely on high-powered pulsed laser systems. A promising alternative is to exploit entangled…

In virtual-state spectroscopy, information about the energy-level structure of an arbitrary sample is retrieved by Fourier transforming sets of measured two-photon absorption probabilities of entangled photon pairs where the degree of…

Quantum Physics · Physics 2021-08-04 Lutz Mertenskötter , Kurt Busch , Roberto de J. León-Montiel

We investigate how entanglement can enhance two-photon absorption in a three-level system. First, we employ the Schmidt decomposition to determine the entanglement properties of the optimal two-photon state to drive such a transition, and…

Quantum Physics · Physics 2021-10-29 Edoardo G Carnio , Andreas Buchleitner , Frank Schlawin

Entangled two-photon spectroscopy is expected to provide advantages compared with classical protocols. It is achieved by coherently controlling the spectral properties of energy-entangled photons. We present here an experimental setup that…

Quantum Physics · Physics 2021-08-25 Stefan Lerch , André Stefanov

Two-photon processes are crucial in applications like microscopy and microfabrication, but their low cross-section requires intense illumination and limits, e.g., the penetration depth in nonlinear microscopy. Entangled states have been…

For dissipation-free photon-photon interaction at the single photon level, we analyze one-photon transition and two-photon transition induced by photon pairs in three-level atoms using two-photon wavefunctions. We show that the two-photon…

Quantum Physics · Physics 2011-06-16 Toshihiro Nakanishi , Hirokazu Kobayashi , Kazuhiko Sugiyama , Masao Kitano

Quantum entanglement offers an incredible resource for enhancing the sensing and spectroscopic probes. Here we develop a microscopic theory for the stimulated Raman scattering (SRS) using entangled photons. We demonstrate that the…

Quantum Physics · Physics 2026-01-21 Mingran Zhang , Jiahao Joel Fan , Frank Schlawin , Zhedong Zhang

Two-photon absorption (TPA) and other nonlinear interactions of molecules with time-frequency-entangled photon pairs (EPP) has been predicted to display a variety of fascinating effects. Therefore, their potential use in practical…

Quantum Physics · Physics 2021-09-15 Michael G. Raymer , Tiemo Landes , Andrew H. Marcus

While two-photon absorption (TPA) and other forms of nonlinear interactions of molecules with isolated time-frequency-entangled photon pairs (EPP) have been predicted to display a variety of fascinating effects, their potential use in…

Quantum spectroscopy seeks to probe chemical systems using nonclassical light, which has properties that are qualitatively and quantitatively different than conventional light sources. One promising technique uses intensity-correlated twin…

We present a theoretical analysis of two-photon absorption of classical and squeezed light valid when one-photon absorption to an intermediate state is either resonant or far-detuned from resonance, and in both the low and high intensity…

Quantum Physics · Physics 2022-09-14 Christian Drago , John Sipe

Quantum light spectroscopy, providing novel molecular information non-accessible by classical light, necessitates new computational tools when applied for complex molecular systems. We introduce two computational protocols for the molecular…

Chemical Physics · Physics 2021-09-14 Bing Gu , Daniel Keefer , Shaul Mukamel

Recent theoretical studies in quantum spectroscopy have emphasized the potential of non-classical correlations in entangled photon pairs for selectively targeting specific nonlinear optical processes in nonlinear optical responses. However,…

Chemical Physics · Physics 2026-04-21 Yuta Fujihashi , Ozora Iso , Ryosuke Shimizu , Akihito Ishizaki
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