The control and manipulation of quantum-entangled states is crucial for the development of quantum technologies. A promising route is to couple solid-state quantum emitters through their optical dipole-dipole interactions. Entanglement in itself is challenging, as it requires both nanometric distances between emitters and nearly degenerate electronic transitions. Here we implement hyperspectral imaging to identify pairs of coupled dibenzanthanthrene molecules, and find distinctive spectral signatures of maximally entangled superradiant and subradiant electronic states by tuning the molecular optical resonances with Stark effect. We demonstrate far-field selective excitation of the long-lived subradiant delocalized state with a laser field tailored in amplitude and phase. Optical nanoscopy of the coupled molecules unveils spatial signatures that result from quantum interferences in their excitation pathways and reveal the location of each emitter. Controlled electronic-states superposition will help deciphering more complex physical or biological mechanisms governed by the coherent coupling and developing quantum information schemes.
Download full-text PDF |
Source |
---|---|
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC9135760 | PMC |
http://dx.doi.org/10.1038/s41467-022-30672-2 | DOI Listing |
Nanotechnology
December 2024
Department of Physics, King Faisal University, King Faisal University P.O. 380 Ahsaa 31982, Al Ahsa, 31982, SAUDI ARABIA.
An anisotropic plasmonic trimer is proposed as an effective spectroscopic amplifier for the maximum signal enhancement of the Hyper-Raman Scattering (HRS) process. The three-particle system is composed of asymmetric Au nanorings arranged collinearly in a J-aggregate configuration and illuminated by a longitudinally polarized light. The optical properties of the considered trimer have been numerically simulated by the Finite-Difference Time-Domain (FDTD) method.
View Article and Find Full Text PDFPhys Rev Lett
September 2024
Departamento de Física Teórica e Experimental, Universidade Federal do Rio Grande do Norte, Campus Universitário, Lagoa Nova, Natal-RN 59078-970, Brazil.
Confinement is a pivotal phenomenon in numerous models of high-energy and statistical physics. In this study, we investigate the emergence of confined meson excitations within a one-dimensional system, comprising Rydberg-dressed atoms trapped and coupled to a cavity field. This system can be effectively represented by an Ising-Dicke Hamiltonian model.
View Article and Find Full Text PDFSci Rep
August 2024
Department of Chemistry, University of Ulsan, 93 Daehak-ro, Nam-gu, Ulsan, 44610, South Korea.
Herein, we investigated the distinctive scattering properties exhibited by single gold nanorods coated with palladium (AuNRs@Pd), with variations in the Pd shell thicknesses and morphologies. AuNRs@Pd were synthesized through bottom-up epitaxial Pd growth using two different concentrations of Pd precursor. These single AuNRs@Pd displayed the characteristic of subradiant and superradiant localized surface plasmon resonance peaks, characterized by a noticeable gap marked by a Fano dip.
View Article and Find Full Text PDFJ Chem Theory Comput
June 2024
Department of Chemistry, Temple University, Philadelphia, Pennsylvania 19122, United States.
The impact of exciton-vibrational (EV) coupling involving low-energy ("slow") molecular vibrations and higher-energy ("fast") molecular vibrations on the absorption and emission spectra of H- and J-dimers is studied theoretically for a pair of chromophores with excitonic coupling dominated by transition dipole-dipole coupling, . Exact quantum-mechanical solutions based on a Frenkel-Holstein-Peierls Hamiltonian reveal a fascinating interplay between the two coupling sources in determining the spectral line widths, Stoke shifts and radiative decay rates. It is shown that the ratio rules derived from the vibronic progression of the fast mode in molecular dimers remain valid under the influence of slow-mode EV coupling under most conditions.
View Article and Find Full Text PDFNat Commun
February 2024
Niels Bohr Institute, University of Copenhagen, Blegdamsvej 17, Copenhagen, DK-2100, Denmark.
When an inverted ensemble of atoms is tightly packed on the scale of its emission wavelength or when the atoms are collectively strongly coupled to a single cavity mode, their dipoles will align and decay rapidly via a superradiant burst. However, a spread-out dipole phase distribution theory predicts a required minimum threshold of atomic excitation for superradiance to occur. Here we experimentally confirm this predicted threshold for superradiant emission on a narrow optical transition when exciting the atoms transversely and show how to take advantage of the resulting sub- to superradiant transition.
View Article and Find Full Text PDFEnter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!