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We show that individual vibrational modes in single-molecule junctions with asymmetric molecule-lead coupling can be selectively excited by applying an external bias voltage. Thereby, a non-statistical distribution of vibrational energy can…

Mesoscale and Nanoscale Physics · Physics 2017-09-13 R. Volkovich , R. Härtle , M. Thoss , U. Peskin

Molecular polaritons within the mid-infrared regime have emerged as a source for modifying and manipulating molecular and photonic properties. However, the development of new methodologies for photon generation is still a challenge in…

Quantum Physics · Physics 2025-09-17 Arley Flórez López , Johan F. Triana , José Luis Sanz-Vicario

Nonlinear interactions between phonon modes govern the behavior of vibrationally highly excited solids and molecules. Here, we demonstrate theoretically that optical cavities can be used to control the redistribution of energy from a highly…

Materials Science · Physics 2021-08-25 Dominik M. Juraschek , Tomáš Neuman , Johannes Flick , Prineha Narang

Multi-level exciton-polariton systems offer an attractive platform for studies of non-linear optical phenomena. However, studies of such consequential non-linear phenomena as polariton condensation and lasing in planar microcavities have so…

Microcavity polaritons are bosonic light-matter particles that can emit coherent radiation without electronic population inversion via bosonic scattering. This phenomenon, known as polariton lasing, strongly depends on the polaritons'…

Optics · Physics 2021-02-09 U. Czopak , M. Prilmüller , C. Schneider , S. Höfling , G. Weihs

A remote energy transfer pathway from electronic to vibrational degrees of freedom is identified inside an infrared optical cavity under vibrational strong coupling conditions. This mechanism relies on the dynamical Casimir effect, whereby…

Quantum Physics · Physics 2024-03-19 Tao E. Li

Exciton-polaritons in semiconductor microcavities exhibit large two-body interactions that, thanks to ever refined nanotechnology techniques, are getting closer and closer to the quantum regime where single-photon nonlinearities start being…

There is growing interest in using strongly coupled organic microcavities to tune molecular dynamics, including the electronic and vibrational properties of molecules. However, very little attention has been paid to the utility of cavity…

Materials Science · Physics 2024-06-12 Bin Liu , Vinod M. Menon , Matthew Y. Sfeir

A general theory of electronic excitations in aggregates of molecules coupled to intramolecular vibrations and the harmonic environment is developed for simulation of the third-order nonlinear spectroscopy signals. The model is applied in…

Chemical Physics · Physics 2014-01-17 Vytautas Butkus , Leonas Valkunas , Darius Abramavicius

The emerging field of molecular cavity polaritons has stimulated a surge of experimental and theoretical activities and presents a unique opportunity to develop the many-body simulation methodology. This paper presents a numerical scheme…

Quantum Physics · Physics 2024-03-12 Andrew Wu , Javier Cerrillo , Jianshu Cao

By using a propagation scheme for current matrices and an auxiliary mode expansion method, we investigate the transient dynamics of a single molecular junction coupled with a vibrational mode. Our approach is based on the Anderson-Holstein…

Mesoscale and Nanoscale Physics · Physics 2016-02-17 Guo-Hui Ding , Bo Xiong , Bing Dong

We derive a many-site version of the non-Markovian time-convolutionless polaron master equation [S. Jang et al., J. Chem Phys. 129, 101104 (2008)] to describe electronic excitation dynamics in multichromophoric systems. By treating…

Quantum Physics · Physics 2015-05-28 Avinash Kolli , Ahsan Nazir , Alexandra Olaya-Castro

In this work, we combine the density functional tight-binding (DFTB) approach with a light-matter Hamiltonian beyond the long-wavelength approximation to propagate the dynamics of vibrational polaritons formed by coupling molecular…

Chemical Physics · Physics 2026-04-13 Sachith Wickramasinghe , Amirhosein Amini , Arkajit Mandal

The emission dynamics of a GaAs microcavity at different angles of observation with respect to the sample normal under conditions of nonresonant picosecond-pulse excitation is measured. At sufficiently high excitation densities, the decay…

Mesoscale and Nanoscale Physics · Physics 2011-05-11 V. V. Belykh , V. A. Tsvetkov , M. L. Skorikov , N. N. Sibeldin

Nonadiabatic phenomena are investigated in the rovibrational motion of molecules confined in an infrared cavity. Conical intersections (CIs) between vibrational polaritons, similar to CIs between electronic polaritonic surfaces, are found.…

Quantum Physics · Physics 2021-02-24 Tamás Szidarovszky , Péter Badankó , Gábor J. Halász , Ágnes Vibók

Molecular exciton polaritons are hybrid states resulting from the strong coupling of molecular electronic excitations with an optical cavity mode, presenting a promising approach for controlling photophysical and photochemical properties in…

Chemical Physics · Physics 2025-03-04 Nguyen Thanh Phuc

Realizing nonlinear coupling across space can enable new scientific and technological advances, including ultrafast operation and propagation of information in IR photonic circuitry, remote triggering or catalyzing of chemical reactions,…

Optics · Physics 2019-12-13 Jiaxi Wang , Bo Xiang , Wei Xiong

Recent experiments have revealed the profound effect of strong light-matter interactions in optical cavities on the electronic ground state of molecular systems. This phenomenon, known as vibrational strong coupling (VSC), can modify…

Quantum Physics · Physics 2023-12-19 Thomas Schnappinger , Markus Kowalewski

In this work we investigate anharmonic vibrational polaritons formed due to strong light-matter interactions in an optical cavity between radiation modes and anharmonic vibrations beyond the long-wavelength limit. We introduce a…

Quantum Physics · Physics 2024-09-13 Dipti Jasrasaria , Arkajit Mandal , David R. Reichman , Timothy C. Berkelbach

Rotational excitation of polar molecules trapped in an optical lattice gives rise to rotational excitons. Here we show that non-linear interactions of such excitons can be controlled by an electric field. The exciton--exciton interactions…

Mesoscale and Nanoscale Physics · Physics 2012-06-20 Ping Xiang , Marina Litinskaya , Roman V. Krems