Strong light-matter coupling for optical switching through the fluorescence and FRET control

Resonant interaction between excitonic transitions of molecules and localized electromagnetic field forms the hybrid polaritonic states. Tuneable microresonators may change the light-matter coupling strength and modulate them from weak to strong and ultra-strong coupling regimes. In this work we have realised strong coupling between the tuneable open-access cavity mode and the excitonic transitions in oligonucleotide-based molecular beacons with their terminus labelled with a pair of organic dye molecules demonstrating an efficient donor-to-acceptor Förster resonance energy transfer (FRET). We show that the predominant strong coupling of the cavity photon to the exciton transition in the donor dye molecule can lead to such a large an energy shift that the energy transfer from the acceptor exciton reservoir to the mainly donor lower polaritonic state can be achieved, thus yielding the chromophores’ donor–acceptor role reversal or “carnival effect”. The data show the possibility for confined electromagnetic fields to control and mediate polariton-assisted remote energy transfer. Obtained results open the avenues to quantum optical switching and other applications.

Chemical Tuning on Resonance Coupling in Gold Nanorod−Monolayer WS2 Heterostructures

Resonance coupling between plasmonic resonances in metallic nanostructures and excitons in two-dimensional (2D) semiconductors has attracted much recent attention. The 2D semiconductor excitons are sensitive to external stimulus, enabling active tuning on the resonance couplings by physical, such as applying electrostatic gating, thermal scanning, etc., or chemical approaches. Among the others, chemical tuning approach has the advantage of facile implementation, high efficiency, and being capable of large-area tuning. Here, we report on chemical tuning of resonance coupling in heterostructures consisted of individual gold nanorods integrated with monolayer WS2. We showed that by incubating the heterostructures into a bis (trifluoro-methane) sulfonimide (TFSI) solution, the exciton transition strength of the WS2 will be enhanced significantly. As a result, the resonance coupling in the heterostructures evolved from a weak coupling regime to a strong coupling one, with the mode splitting energy increases from 94.96 to 105.32 meV. These findings highlight the potential of chemical treatment as an efficient technique for tailoring the interactions between plasmonic nanostructures and 2D semiconductors.

The Relationship between the Spatial Arrangement of Pigments and Exciton Transition Moments in Photosynthetic Light-Harvesting Complexes

Considering bacteriochlorophyll molecules embedded in the protein matrix of the light-harvesting complexes of purple bacteria (known as LH2 and LH1-RC) as examples of systems of interacting pigment molecules, we investigated the relationship between the spatial arrangement of the pigments and their exciton transition moments. Based on the recently reported crystal structures of LH2 and LH1-RC and the outcomes of previous theoretical studies, as well as adopting the Frenkel exciton Hamiltonian for two-level molecules, we performed visualizations of the LH2 and LH1 exciton transition moments. To make the electron transition moments in the exciton representation invariant with respect to the position of the system in space, a system of pigments must be translated to the center of mass before starting the calculations. As a result, the visualization of the transition moments for LH2 provided the following pattern: two strong transitions were outside of LH2 and the other two were perpendicular and at the center of LH2. The antenna of LH1-RC was characterized as having the same location of the strongest moments in the center of the complex, exactly as in the B850 ring, which actually coincides with the RC. Considering LH2 and LH1 as supermolecules, each of which has excitation energies and corresponding transition moments, we propose that the outer transitions of LH2 can be important for inter-complex energy exchange, while the inner transitions keep the energy in the complex; moreover, in the case of LH1, the inner transitions increased the rate of antenna-to-RC energy transfer.

Excitonic States and Related Optical Susceptibility in InN/AlN Quantum Well Under the Effects of the Well Size and Impurity Position

Based on the finite difference method, linear optical susceptibility, photoluminescence peak and binding energies of three first states of an exciton trapped by a positive charge donor-impurity ( ) confined in InN/AlN quantum well are investigated in terms of well size and impurity position. The electron, heavy hole free and bound excitons allowed eigen-values and corresponding eigen-functions are obtained numerically by solving one-dimensional time-independent Schrödinger equation. Within the parabolic band and effective mass approximations, the calculations are made considering the coupling of the electron in the n-th conduction subband and the heavy hole in the m-th valence subband under the impacts of the well size and impurity position. The obtained results show clearly that the energy, binding energy and photoluminescence peak energy show a decreasing behavior according to well size for both free and bound cases. Moreover, the optical susceptibility associated to exciton transition is strongly red-shift (blue-shifted) with enhancing the well size (impurity position).

Localization-limited exciton oscillator strength in colloidal CdSe nanoplatelets revealed by the optically induced stark effect

Abstract2D materials are considered for applications that require strong light-matter interaction because of the apparently giant oscillator strength of the exciton transitions in the absorbance spectrum. Nevertheless, the effective oscillator strengths of these transitions have been scarcely reported, nor is there a consistent interpretation of the obtained values. Here, we analyse the transition dipole moment and the ensuing oscillator strength of the exciton transition in 2D CdSe nanoplatelets by means of the optically induced Stark effect (OSE). Intriguingly, we find that the exciton absorption line reacts to a high intensity optical field as a transition with an oscillator strength FStark that is 50 times smaller than expected based on the linear absorption coefficient. We propose that the pronounced exciton absorption line should be seen as the sum of multiple, low oscillator strength transitions, rather than a single high oscillator strength one, a feat we assign to strong exciton center-of-mass localization. Within the quantum mechanical description of excitons, this 50-fold difference between both oscillator strengths corresponds to the ratio between the coherence area of the exciton’s center of mass and the total area, which yields a coherence area of a mere 6.1 nm2. Since we find that the coherence area increases with reducing temperature, we conclude that thermal effects, related to lattice vibrations, contribute to exciton localization. In further support of this localization model, we show that FStark is independent of the nanoplatelet area, correctly predicts the radiative lifetime, and lines up for strongly confined quantum dot systems.

Нетривиальная зависимость спектральных характеристик экситонов в квантовых ямах от мощности резонансного оптического возбуждения

Basic exciton parameters, the energy of exciton transition and the radiative and nonradiative broadenings, are experimentally studied by means of reflectance spectroscopy for a heterostructure with the 14-nm GaAs/AlGaAs quantum well. Particular attention is paid to the nonradiative broadening which is sensitive to optical creation of free carriers and long-lived nonradiative excitons. A sublinear increase of the broadening of the heavy-hole and light-hole exciton resonances is observed when the light-hole exciton resonance is excited with increasing power. A simple model is developed, which allows one to well reproduce the observed dependence.