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We introduce a theoretical framework that allows for the systematic and efficient description of the ultrafast nonlinear response of molecular polaritons, i.e., hybrid light-matter states, in the collective regime of large numbers of…

Quantum Physics · Physics 2025-05-22 Michael Reitz , Arghadip Koner , Joel Yuen-Zhou

The fast dynamics of molecular polaritonics is scrutinized theoretically through the implementation of two-dimensional spectroscopy protocols. We derive conceptually simple and computationally efficient formulas to calculate two-dimensional…

Quantum Physics · Physics 2024-03-08 Daniela Gallego-Valencia , Lars Mewes , Johannes Feist , José Luis Sanz-Vicario

We present a microscopic theory for nonlinear optical spectroscopy of N molecules in an optical cavity. A quantum Langevin analytical expression is derived for the time- and frequency-resolved signals accounting for arbitrary numbers of…

Quantum Physics · Physics 2023-03-29 Zhedong Zhang , Xiaoyu Nie , Dangyuan Lei , Shaul Mukame

Vibrational polaritons are formed by strong coupling of molecular vibrations and photon modes in an optical cavity. Experiments have demonstrated that vibrational strong coupling can change molecular properties and even affect chemical…

Quantum Physics · Physics 2025-01-14 Thomas Schnappinger , Cyril Falvo , Markus Kowalewski

Molecular polaritons have gained considerable attention due to their potential to control nanoscale molecular processes by harnessing electromagnetic coherence. Although recent experiments with liquid-phase vibrational polaritons have shown…

Confined electromagnetic modes strongly couple to collective excitations in ensembles of quantum emitters, producing light-matter hybrid states known as polaritons. Under such conditions, the discrete multilevel spectrum of molecular…

Quantum Physics · Physics 2022-06-01 Jorge A. Campos-Gonzalez-Angulo , Joel Yuen-Zhou

Multidimensional coherent spectroscopy directly unravels multiply excited states that overlap in a linear spectrum. We report multidimensional coherent optical photocurrent spectroscopy in a semiconductor polariton diode and explore the…

We investigate the two-dimensional motion of polaritons injected into a planar microcavity by a continuous wave optical pump in presence of a static perturbation, e.g. a point defect. By finding the stationary solutions of the nonlinear…

Other Condensed Matter · Physics 2007-05-23 Iacopo Carusotto , Cristiano Ciuti

Strong coupling of molecular vibrations to an infrared cavity mode affects their nature by creating dressed polariton states. We show how the single and double vibrational polariton manifolds may be controlled by varying the cavity coupling…

Quantum Physics · Physics 2016-05-10 Prasoon Saurabh , Shaul Mukamel

We propose a three-pulse coherent ultrafast optical technique that is particularly sensitive to two-exciton correlations. Two Liouville-space pathways for the density matrix contribute to this signal which reveals double quantum coherences…

Mesoscale and Nanoscale Physics · Physics 2009-11-13 Lijun Yang , Shaul Mukamel

We theoretically propose a multidimensional high-harmonic echo spectroscopy technique which utilizes strong optical fields to resolve coherent electron dynamics spanning an energy range of multiple electron Volts. Using our recently…

We devise a phase-coherent three-pulse protocol to probe the polariton dynamics in a trapped-ion quantum simulation. In contrast to conventional nonlinear signals, the presented scheme does not change the number of excitations in the…

Quantum Physics · Physics 2015-09-09 Manuel Gessner , Frank Schlawin , Andreas Buchleitner

High harmonic spectroscopy has the potential to combine attosecond temporal with sub-Angstrom spatial resolution of the early nuclear and multielectron dynamics in molecules. It involves strong field ionization of the molecule by the IR…

Atomic Physics · Physics 2013-08-08 Valeria Serbinenko , Olga Smirnova

We investigate symmetric oscillators, and in particular their quantization, by employing semiclassical and quantum phase functions introduced in the context of Liouville-Green transformations of the Schr\"{o}dinger equation. For anharmonic…

Quantum Physics · Physics 2011-11-10 A. Matzkin , M. Lombardi

Strong coupling between vibrational transitions in molecules within a resonant optical microcavity leads to the formation of collective, delocalized vibrational polaritons. There are many potential applications of "polaritonic chemistry,"…

Chemical Physics · Physics 2021-11-05 Rong Duan , Joseph N. Mastron , Yin Song , Kevin J. Kubarych

We develop a fully quantum mechanical methodology to describe the static properties and the dynamics of a single anharmonic vibrational mode interacting with a quantized infrared cavity field in the strong and ultrastrong coupling regimes.…

Chemical Physics · Physics 2020-06-22 Johan F. Triana , Federico J. Hernández , Felipe Herrera

We theoretically propose a biphoton entanglement-enhanced multidimensional spectroscopic technique as a probe for the dissipative polariton dynamics in the ultrafast regime. It is applied to the cavity-confined monomeric photosynthetic…

Quantum Physics · Physics 2022-09-07 Arunangshu Debnath , Angel Rubio

Recently the possibility of generating nonclassical polariton states by means of parametric scattering has been demonstrated. Excitonic polaritons propagate in a complex interacting environment and contain real electronic excitations…

Mesoscale and Nanoscale Physics · Physics 2007-10-16 S. Portolan , O. Di Stefano , S. Savasta , F. Rossi , R. Girlanda

We introduce a general approach for the simulation of quantum vibrational states of (symmetric and asymmetric) double-well potentials in molecules and materials for thermodynamic and spectroscopic applications. The method involves solving…

High harmonic generation in solids provides us compact and coherent UV sources. Our simulations illustrate abnormal harmonic yield dependence on the intensity of driving or pre-excitation pulses. A multielectron interference model is…

Optics · Physics 2020-01-01 Ling-Jie Lü , Xue-Bin Bian
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