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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

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

We consider the quantum entanglement of the electronic and vibrational degrees of freedom in molecules with a tendency towards double welled potentials using model coupled harmonic diabatic potential-energy surfaces. The von Neumann entropy…

Quantum Physics · Physics 2012-02-24 Laura K. McKemmish , Ross H. McKenzie , Noel S. Hush , Jeffrey R. Reimers

A previously proposed non-canonical coupled-perturbed Kohn-Sham density functional theory (KS-DFT)/Hartree-Fock (HF) treatment for spin-orbit coupling is here generalized to infinite periodic systems. The scalar-relativistic periodic…

Ultrafast optical spectroscopy is a powerful technique for studying the dynamic processes of molecular systems in condensed phases. However, in molecular systems containing many dye molecules, the spectra can become crowded and difficult to…

Chemical Physics · Physics 2025-02-05 Yuta Fujihashi , Akihito Ishizaki , Ryosuke Shimizu

We develop convergent variational perturbation theory for quantum statistical density matrices. The theory is applicable to polynomial as well as nonpolynomial interactions. Illustrating the power of the theory, we calculate the…

Quantum Physics · Physics 2009-10-31 M. Bachmann , H. Kleinert , A. Pelster

We present a theoretical framework for electromagnetic scattering by particles with a permittivity that is periodically varying in time, based on a perturbative approach. Within this framework, we derive explicit expressions for the…

The use of quantum light to probe exciton properties in semiconductor and molecular nanostructures typically occurs in the low-intensity regime. A substantial enhancement of exciton-photon coupling can be achieved with photonic cavities,…

Quantum light is increasingly recognized as a promising resource for developing optical measurement techniques. Particular attention has been paid to enhancing the precision of the measurements beyond classical techniques by using…

Chemical Physics · Physics 2023-10-03 Yuta Fujihashi , Kuniyuki Miwa , Masahiro Higashi , Akihito Ishizaki

Inspired by recent visible pump - infrared probe spectra reported for molecular catalysts adsorbed to quantum dots, we introduce a theory of non-equilibrium vibronic Fano resonances arising from the interference of quantum dot excited-state…

Chemical Physics · Physics 2024-10-16 Luis Martinez-Gomez , Sara T. Gebre , Tianquan Lian , Raphael F. Ribeiro

Prior to recombination photons, electrons, and atomic nuclei rapidly scattered and behaved, almost, like a single tightly-coupled photon-baryon plasma. We investigate here the accuracy of the tight-coupling approximation commonly used to…

Cosmology and Nongalactic Astrophysics · Physics 2015-03-17 Francis-Yan Cyr-Racine , Kris Sigurdson

The perturbation method is an approximation scheme with a solvable leading order. The standard way is to choose a non-interacting sector for the leading order. The adaptive perturbation method improves the solvable part by using all…

High Energy Physics - Theory · Physics 2022-10-17 Chen-Te Ma

Vibrational overtones in deeply bound molecules are sensitive probes for variation of the proton-to-electron mass ratio $\mu$. In nonpolar molecules, these overtones may be driven as two-photon transitions. Here, we present procedures for…

Atomic Physics · Physics 2019-01-03 Ryan Carollo , Alexander Frenett , David Hanneke

Interferometers with single particles are susceptible for dephasing perturbations from the environment, such as electromagnetic oscillations or mechanical vibrations. On the one hand, this limits sensitive quantum phase measurements as it…

Quantum entangled photons provide a sensitive probe of many-body interactions and offer an unique experimental portal for quantifying many-body correlations in a material system. In this paper, we present a theoretical demonstration of how…

Quantum Physics · Physics 2020-03-18 Eric R. Bittner , Hao Li , Andrei Piryatinski , Ajay Ram Srimath Kandada , Carlos Silva

Vibronic coupling has a dramatic influence over a large number of molecular processes, ranging from photo-chemistry, to spin relaxation and electronic transport. The simulation of vibronic coupling with multi-reference wavefunction methods…

Chemical Physics · Physics 2023-10-17 Lorenzo A. Mariano , Sourav Mondal , Alessandro Lunghi

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

This work discusses the problem of optimal excitation of a three-level atom of ladder-configuration by light in the two-photon state and coherent light carrying an average of two photons. The applied atom-light interaction model is based on…

Quantum Physics · Physics 2025-03-25 Masood Valipour , Gniewomir Sarbicki , Karolina Słowik , Anita Dąbrowska

A new general approach is introduced for definining an optimum zero-order Hamiltonian for Rayleigh-Schr\"odinger perturbation theory. Instead of taking the operator directly from a model problem, it is constructed to be a best fit to the…

Quantum Physics · Physics 2021-12-09 Peter J. Knowles

Singlet fission, the molecular process through which photons are effectively converted into pairs of lower energy triplet excitons, holds promise as a means of boosting photovoltaic device efficiencies. In the preceding article of this…

Materials Science · Physics 2017-05-12 Roel Tempelaar , David R. Reichman