We derive the closure relation for $N$ polaritons made of three different types of excitons: bosonized excitons, Frenkel or Wannier excitons. In the case of polaritons made of Wannier excitons, we show how this closure relation, which appears as non-diagonal, may reduce to the one of $N$ elementary bosons, the photons, with its $1/N!$ prefactor, or to the one of $N$ Wannier excitons, with its $(1/N!)^2$ prefactor. Widely different forms of closure relations are thus found depending on the composite bosons at hand. Comparison with closure relations of excitons, either bosonized or kept composite as Frenkel or Wannier excitons, allows us to discuss the influence of a reduction of the number of internal degrees of freedom, as well as the importance of the composite nature of the particles and the existence of fermionic components.
Optical measurements and first-principles calculations of the band structure and exciton states in direct-gap bulk and few-layer PbI2 indicate that the n = 1 exciton is Frenkel-like in nature in that its energy exhibits a weak dependence on thickness down to atomic-length scales. Results reveal large increases of the gap and exciton binding energy with decreasing number of layers, and a transition of the fundamental gap, which becomes indirect for 1-2 monolayers. Calculated values are in reasonable agreement with a particle-in-a-box model relying on the Wannier-Mott theory of exciton formation…
In this work electronic structures and optical properties of organic-inorganic exciton and polaritons in two-dimensional heterostructures combining both organic and semiconductor materials are studied. In those systems, Wannier-Frenkel hybrid exciton has unique and interesting properties that can improve the efficiency of optical materials. When an organic-semiconductor combined heterostructure is illuminated by high-intensity electromagnetic radiation with the frequency of the photons at or near the resonance frequency of the Wannier-Frenkel exciton, we obtain a macroscopically occupied syste…
Frenkel polaritons, hybrid light-matter quasiparticles, offer promises for the designing of new opto-electronic devices. However, their technological implementations are hindered by sensitivity to imperfections. Topology has raised as a way to circumvent defects and fabrication limitations. Here, we propose a lattice of cavities to realize the one-dimensional Su-Schrieffer-Heeger model (SSH) for topological Frenkel polaritons. By engineering the configuration of the cavities we demonstrate that the SSH topological and trivial phases can be accessed, which we unravel by complementary classical …
We present a many-body theory for Frenkel excitons which takes into account their composite nature exactly. Our approach is based on four commutators similar to the ones we previously proposed for Wannier excitons. They allow us to calculate any physical quantity dealing with $N$ excitons in terms of "Pauli scatterings" for carrier exchange in the absence of carrier interaction and "interaction scatterings" for carrier interaction in the absence of carrier exchange. We show that Frenkel excitons have a novel "transfer assisted exchange scattering", specific to these excitons. It comes from ind…
Exciton-polaritons are quasiparticles consisting of a linear superposition of photonic and excitonic states, offering potential for nonlinear optical devices. The excitonic component of the polariton provides a finite Coulomb scattering cross section, such that the different types of exciton found in organic materials (Frenkel) and inorganic materials (Wannier-Mott) produce polaritons with different interparticle interaction strength. A hybrid polariton state with distinct excitons provides a potential technological route towards in-situ control of nonlinear behaviour. Here we demonstrate a de…
Plasmonic structures are known to support the modes with subwavelength volumes in which the field matter interactions are greatly enhanced. Coupling between the molecular excitations and plasmons leading to formation of plexcitons has been investigated for a number of organic molecules. However, plasmon-exciton coupling in metal semiconductor structures have not experienced the same degree of attention. In this work we show that the very strong coupling regime in which the Rabi energy exceeds the exciton binding energy is attainable in semiconductor cladded plasmonic nanoparticles and leads to…
Exciton-polariton propagation in a quantum well, under centre-of-mass quantization, is computed by a variational self-consistent microscopic theory. The Wannier exciton envelope functions basis set is given by the simple analytical model of ref. [1], based on pure states of the centre-of-mass wave vector, free from fitting parameters and "ad hoc" (the so called additional boundary conditions-ABCs) assumptions. In the present paper, the former analytical model is implemented in order to reproduce the centre-of-mass quantization in a large range of quantum well thicknesses (5a_B < L < inf.). The…
By using the composite many-body theory for Frenkel excitons we have recently developed, we here derive the ground state energy of $N$ Frenkel excitons in the Born approximation through the Hamiltonian mean value in a state made of $N$ identical $\mathbf{Q=0}$ excitons. While this quantity reads as a density expansion in the case of Wannier excitons, due to many-body effects induced by fermion exchanges between $N$ composite particles, we show that the Hamiltonian mean value for $N$ Frenkel excitons only contains a first order term in density, just as for elementary bosons. Such a simple resul…
We propose a new model to implement organic exciton-semiconductor exciton hybridization by embedding a semiconductor quantum dot array into an organic medium. A Wannier-Mott transfer exciton is formed when the exciton in each semiconductor dot interacts via the multipole-multipole coupling with other excitons in the different dtos of the array. A new hybrid exciton appears in the system owing to strong dipole-dipole interaction of the Frenkel exciton of the organic molecules with the Wannier Mott transfer exciton of the quantum dot array. This hybrid exciton has both a large oscillator strengt…
We have developed a model in order to account for electron-vibrational effects on absorption, luminescence of molecular aggregates and exciton-polaritons in nanofibers. The model generalizes the mean-field electron-vibrational theory developed by us earlier to the systems with spatial symmetry, exciton luminescence and the exciton-polaritons with spatial dispersion. The correspondence between manifestation of electron-vibrational interaction in monomers, molecular aggregates and exciton-polariton dispersion in nanofibers is obtained by introducing the aggregate line-shape functions in terms of…
Interacting bosonic particles in artificial lattices have proven to be a powerful tool for the investigation of exotic phases of matter as well as phenomena resulting from non-trivial topology. Exciton-polaritons, bosonic quasi-particles of light and matter, have shown to combine the on-chip benefits of optical systems with strong interactions, inherited form their matter character. Technologically significant semiconductor platforms, however, strictly require cryogenic temperatures for operability. In this paper, we demonstrate exciton-polariton lasing for topological defects emerging form th…
We report on the origin of energy-shifts in organic polariton condensates. The localised nature of Frenkel excitons in molecular semiconductors precludes interparticle Coulomb exchange interactions -the latter being the dominant mechanism for blueshifts in inorganic semiconductor microcavities that bear Wannier-Mott excitons. We examine the contribution of optically induced change of the intracavity non-linear refractive index, gain induced frequency-pulling and quenching of the Rabi splitting, as well as the role of polariton-exciton and polariton-polariton scattering in the energy-shift of t…
We theoretically investigate the nonlinearity of trion-polaritons in a two-dimensional material that arises from Coulomb interaction between quasiparticles. To evaluate the interaction constant, we solve a three-body Wannier equation precisely by expanding trion wavefunctions into a Gaussian basis. Using these wavefunctions, we calculate the trion-polariton interaction energies for the exchange processes, resolving the outstanding question of trion-trion scattering. We find that the nonlinearity is the result of the competition between different scattering channels. Such a cancellation effect …
We study Frenkel exciton-polariton Bose-Einstein condensation in a two-dimensional defect-free triangular photonic crystal with an organic semiconductor active medium containing bound excitons with dipole moments oriented perpendicular to the layers. We find photonic Bloch modes of the structure and consider their strong coupling regime with the excitonic component. Using the Gross- Pitaevskii equation for exciton polaritons and the Boltzmann equation for the external exciton reservoir, we demonstrate the formation of condensate at the points in reciprocal space where photon group velocity equ…
Polaritons are quasiparticles arising from the strong coupling of electromagnetic waves in cavities and dipolar oscillations in a material medium. In this framework, localized surface plasmon in metallic nanoparticles defining optical nanocavities have attracted increasing interests in the last decade. This interest results from their sub-diffraction mode volume, which offers access to extremely high photonic densities by exploiting strong scattering cross-sections. However, high absorption losses in metals have hindered the observation of collective coherent phenomena, such as condensation. I…
Under adequate conditions, cavity-polaritons form a macroscopic coherent quantum state, known as Bose-Einstein condensate (BEC). Compared to Wannier-Mott excitons in inorganic semiconductors, the localized Frenkel excitons in organic emitter materials show weaker interaction but stronger coupling, which recently enabled the first realization of BEC at room temperature. However, this required ultrafast optical pumping which limits the applications of organic BECs. Here, we demonstrate room-temperature BEC of cavity-polaritons in simple laminated microcavities filled with the biologically produc…
Coherent interaction of WS$_2$ and quasi-2D perovskite excitons over micrometer distances via a cavity field
Carl von Ossietzky Universität Oldenburg（奥尔登堡卡尔·冯·奥西埃茨基大学）；Philipps-Universität Marburg（马尔堡菲利普斯大学）；Wroclaw University of Science and Technology（弗罗茨瓦夫科技大学）；University of Applied Sciences Emden/Leer（埃姆登/莱尔应用科学大学）；Fraunhofer-Institute for Applied Optics and Precision Engineering IOF（弗劳恩霍夫应用光学和精密工程研究所IOF）；Friedrich Schiller University, Jena（耶拿弗里德里希·席勒大学）；University of Chemistry and Technology Prague（布拉格化学技术大学）；Massachusetts Institute of Technology（麻省理工学院）；Vidyasirimedhi Institute of Science and Technology (VISTEC)（维他西亚米德科学与技术学院(VISTEC)）；Laboratoire National des Champs Magnétiques Intenses, EMFL, CNRS UPR, 3228, University Grenoble Alpes, University Toulouse, University Toulouse 3, INSA-T Grenoble（强磁场国家实验室，EMFL，CNRS UPR 3228，格勒诺布尔阿尔卑斯大学，图卢兹大学，图卢兹第三大学，INSA-T格勒诺布尔）
We consider the resonant energy transfer from a two-dimensional Wannier exciton (donor) to a Frenkel exciton of a molecular crystal overlayer (acceptor) when the active medias are separated by a metallic layer, possibly an electrode. We characterize the effect of the surface plasmon on this process. Using realistic values of material parameters, we show that it is possible to change the transfer rate within typically a factor of 5 (up to 44 according to geometrical configuration). We then take into account the quenching of the organic luminescence due to the proximity with the metal. This latt…
Tunable Magneto-Excitonic Coupling in Alloyed van der Waals Antiferromagnet
Wroclaw University of Science and Technology（弗罗茨瓦夫科技大学）；University of Warsaw（华沙大学）；Laboratoire National des Champs Magnétiques Intenses（强磁场国家实验室）；Université Grenoble Alpes（格勒诺布尔阿尔卑斯大学）；Université Toulouse（图卢兹大学）；King’s College London（伦敦国王学院）
