Non-Hermitian Hamiltonians for Linear and Nonlinear Optical Response: a
Model for Plexcitons
- URL: http://arxiv.org/abs/2206.13265v2
- Date: Mon, 8 May 2023 22:30:52 GMT
- Title: Non-Hermitian Hamiltonians for Linear and Nonlinear Optical Response: a
Model for Plexcitons
- Authors: Daniel Finkelstein-Shapiro, Pierre-Adrien Mante, Sinan Balci, Donatas
Zigmantas and T\~onu Pullerits
- Abstract summary: In polaritons, the properties of matter are modified by mixing the molecular transitions with light modes inside a cavity.
Non-Hermitian Hamiltonians have been derived to describe the excited states of molecules coupled to surface plasmons.
- Score: 0.0
- License: http://creativecommons.org/licenses/by/4.0/
- Abstract: In polaritons, the properties of matter are modified by mixing the molecular
transitions with light modes inside a cavity. Resultant hybrid light-matter
states exhibit energy level shifts, are delocalized over many molecular units
and have a different excited-state potential energy landscape which leads to
modified exciton dynamics. Previously, non-Hermitian Hamiltonians have been
derived to describe the excited states of molecules coupled to surface plasmons
(i.e. plexcitons), and these operators have been successfully used in the
description of linear and third order optical response. In this article, we
rigorously derive non-Hermitian Hamiltonians in the response function formalism
of nonlinear spectroscopy by means of Feshbach operators, and apply them to
explore spectroscopic signatures of plexcitons. In particular we analyze the
optical response below and above the exceptional point that arises for matching
transition energies for plasmon and molecular components, and study their
decomposition using double-sided Feynman diagrams. We find a clear distinction
between interference and Rabi splitting in linear spectroscopy, and a
qualitative change in the symmetry of the lineshape of the nonlinear signal
when crossing the exceptional. This change corresponds to one in the symmetry
of the eigenvalues of the Hamiltonian. Our work presents an approach for
simulating the optical response of sublevels within an electronic system, and
opens new applications of nonlinear spectroscopy to examine the different
regimes of the spectrum of non-Hermitian Hamiltonians.
Related papers
- Josephson bifurcation readout: beyond the monochromatic approximation [49.1574468325115]
We analyze properties of bifurcation quantum detectors based on weakly nonlinear superconducting resonance circuits.
This circuit can serve as an efficient detector of the quantum state of superconducting qubits.
arXiv Detail & Related papers (2024-05-25T22:22:37Z) - Coherent multidimensional spectroscopy in polariton systems [0.0]
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 spectra for molecules.
Our theoretical method provides a deeper insight in those processes that yield relevant signals in multidimensional molecular spectroscopy.
arXiv Detail & Related papers (2024-03-07T18:37:52Z) - An Exact Expression for Multidimensional Spectroscopy of a Spin-Boson
Hamiltonian [0.0]
We provide an exact expression for multidimensional spectra of a spin-boson Hamiltonian up to arbitrary order of electric field interaction.
We demonstrate the utility of this expression by modeling polaron formation and coherent exciton-phonon coupling in quantum dots.
arXiv Detail & Related papers (2023-11-09T15:49:37Z) - Linear response of molecular polaritons [0.0]
We show that the collective light-matter strong coupling regime, where $N$ molecular emitters couple to the photon mode of an optical cavity, can be mapped to a quantum impurity model.
We derive simple analytical expressions for linear optical spectra (transmission, reflection, and absorption) where the only molecular input required is the molecular linear susceptibility.
This formalism is applied to a series of illustrative examples showcasing the role of temperature, disorder, vibronic coupling, and optical saturation of the molecular ensemble.
arXiv Detail & Related papers (2023-10-24T00:41:20Z) - Nonlinear opto-vibronics in molecular systems [0.0]
We analytically tackle opto-vibronic interactions in molecular systems driven by either classical or quantum light fields.
We present analytical expressions based on a quantum Langevin equations approach to describe the emission and absorption spectra of such nonlinear molecular systems.
arXiv Detail & Related papers (2023-10-13T13:52:25Z) - Probing the symmetry breaking of a light--matter system by an ancillary
qubit [50.591267188664666]
Hybrid quantum systems in the ultrastrong, and even more in the deep-strong, coupling regimes can exhibit exotic physical phenomena.
We experimentally observe the parity symmetry breaking of an ancillary Xmon artificial atom induced by the field of a lumped-element superconducting resonator.
This result opens a way to experimentally explore the novel quantum-vacuum effects emerging in the deep-strong coupling regime.
arXiv Detail & Related papers (2022-09-13T06:14:08Z) - Exact solutions of interacting dissipative systems via weak symmetries [77.34726150561087]
We analytically diagonalize the Liouvillian of a class Markovian dissipative systems with arbitrary strong interactions or nonlinearity.
This enables an exact description of the full dynamics and dissipative spectrum.
Our method is applicable to a variety of other systems, and could provide a powerful new tool for the study of complex driven-dissipative quantum systems.
arXiv Detail & Related papers (2021-09-27T17:45:42Z) - Stochastic Variational Approach to Small Atoms and Molecules Coupled to
Quantum Field Modes [55.41644538483948]
We present a variational calculation (SVM) of energies and wave functions of few particle systems coupled to quantum fields in cavity QED.
Examples for a two-dimensional trion and confined electrons as well as for the He atom and the Hydrogen molecule are presented.
arXiv Detail & Related papers (2021-08-25T13:40:42Z) - Designing Kerr Interactions for Quantum Information Processing via
Counterrotating Terms of Asymmetric Josephson-Junction Loops [68.8204255655161]
static cavity nonlinearities typically limit the performance of bosonic quantum error-correcting codes.
Treating the nonlinearity as a perturbation, we derive effective Hamiltonians using the Schrieffer-Wolff transformation.
Results show that a cubic interaction allows to increase the effective rates of both linear and nonlinear operations.
arXiv Detail & Related papers (2021-07-14T15:11:05Z) - Molecular Interactions Induced by a Static Electric Field in Quantum
Mechanics and Quantum Electrodynamics [68.98428372162448]
We study the interaction between two neutral atoms or molecules subject to a uniform static electric field.
Our focus is to understand the interplay between leading contributions to field-induced electrostatics/polarization and dispersion interactions.
arXiv Detail & Related papers (2021-03-30T14:45:30Z) - Generalization of the Tavis-Cummings model for multi-level anharmonic
systems [0.0]
We study a collective ensemble of identical multi-level anharmonic emitters and their dipolar interaction with a photonic cavity mode.
The permutational properties of the system allow identifying symmetry classified submanifolds in the energy spectrum.
We expect these findings to be applicable in the study of non-linear spectroscopy and chemistry of polaritons.
arXiv Detail & Related papers (2021-01-23T10:40:00Z)
This list is automatically generated from the titles and abstracts of the papers in this site.
This site does not guarantee the quality of this site (including all information) and is not responsible for any consequences.