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In molecular aggregates, multiple delocalized exciton states interact with phonons, making the state-resolved spectroscopic monitoring of dynamics challenging. We propose a protocol that combines photon-entanglement-enhanced narrowband…

Quantum Physics · Physics 2026-04-24 Arunangshu Debnath , Shaul Mukamel

Entangled photon pairs have been promised to deliver a substantial quantum advantage for two-photon absorption spectroscopy. However, recent work has challenged the previously reported magnitude of quantum enhancement in two-photon…

We use a non-perturbative theoretical approach to the parametric down-conversion (PDC) process, which generates entangled-photon field for an arbitrarily strong pump-pulse. This approach can be used to evaluate multi-point field correlation…

Chemical Physics · Physics 2025-10-22 Deependra Jadoun , Upendra Harbola , Vladimir Y. Chernyak , Shaul Mukamel

Nonlinear spectroscopic techniques using entangled photon pairs can provide an opportunity to exploit non-classical correlations encoded in two-photon wavefunctions to manipulate two-exciton wavefunctions. We propose an entangled photon…

Quantum Physics · Physics 2026-04-10 Arunangshu Debnath , Shaul Mukamel

Spectroscopy is an important tool for probing the properties of materials, chemicals and biological samples. We design a practical transmitter-receiver system that exploits entanglement to achieve a provable quantum advantage over all…

Quantum Physics · Physics 2020-11-03 Haowei Shi , Zheshen Zhang , Stefano Pirandola , Quntao Zhuang

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

Two-photon excitation spectroscopy is a nonlinear technique that has gained rapidly in interest and significance for studying the complex energy-level structure and transition probabilities of materials. While the conventional spectroscopy…

Quantum Physics · Physics 2022-11-23 Yuanyuan Chen , Roberto de J. León-Montiel , Lixiang Chen

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…

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

Classical time-resolved optical spectroscopy experiments are performed using sequences of ultrashort light pulses, with photon fluxes incident on the sample which are many orders of magnitude higher than real-world conditions corresponding…

Entangled two-photon absorption (ETPA) could form the basis of nonlinear quantum spectroscopy at very low photon fluxes, since, at sufficiently low photon fluxes, ETPA scales linearly with the photon flux. When different pairs start to…

Quantum Physics · Physics 2023-12-04 Frank Schlawin

It is well known that energy-time entanglement can enhance two photon absorption (TPA) by simultaneously optimizing the two photon resonance and the coincidence rate of photons at the absorber. However, the precise relation between…

Quantum Physics · Physics 2021-08-31 Baihong Li , Holger F. Hofmann

Entangled two-photon absorption can enable a linear scaling of fluorescence emission with the excitation power. In comparison to classical two-photon absorption with a quadratic scaling, this can allow fluorescence imaging or…

Invariant entangled states remain unchanged under simultaneous identical unitary transformations of all their subsystems. We experimentally generate and characterize such invariant two-, four-, and six-photon polarization entangled states.…

Quantum Physics · Physics 2015-05-13 Magnus Radmark , Marcin Wiesniak , Marek Zukowski , Mohamed Bourennane

Quantum entanglement among multiple spatially separated particles is of fundamental interest, and can serve as central resources for studies in quantum nonlocality, quantum-to-classical transition, quantum error correction, and quantum…

A pulsed source of energy-time entangled photon pairs pumped by a standard laser diode is proposed and demonstrated. The basic states can be distinguished by their time of arrival. This greatly simplifies the realization of 2-photon quantum…

Quantum Physics · Physics 2016-09-08 J. Brendel , N. Gisin , W. Tittel , H. Zbinden

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

We describe two-photon absorption processes excited by entangled pairs, but not by non-entangled pairs of the same energy and polarization. Photon states are selected for destructive interference in the non-entangled process between…

Quantum Physics · Physics 2010-12-21 Keith Kastella , Ralph S. Conti

Entangled photons, generated by spontaneous parametric down-conversion from a second-order nonlinear crystal, present a rich potential for imaging and image-processing applications. Since this source is an example of a three-wave mixing…

Quantum Physics · Physics 2015-06-26 Ayman F. Abouraddy , Bahaa E. A. Saleh , Alexander V. Sergienko , Malvin C. Teich

Entangled photons exhibit non-classical light-matter interactions that create new opportunities in materials and molecular science. For example, in entangled two-photon absorption, the intensity-dependence scales linearly as if only one…

Optics · Physics 2020-05-15 Szilard Szoke , Hanzhe Liu , Bryce P. Hickam , Manni He , Scott K. Cushing