Extraordinary exciton conductance induced by strong coupling

We demonstrate that exciton conductance in organic materials can be enhanced by several orders of magnitude when the molecules are strongly coupled to an electromagnetic mode. Using a 1D model system, we show how the formation of a collective polaritonic mode allows excitons to bypass the disordered array of molecules and jump directly from one end of the structure to the other. This finding could have important implications in the fields of exciton transistors, heat transport, photosynthesis, and biological systems in which exciton transport plays a key role.Comment: Main text: 5 pages, 4 figures; Supplemental: 2 pages, 1 figure. Version 2: Updated reference to related work arXiv:1409.2550. Version 3: Updated to version accepted for publication in Physical Review Letter

Cavity-induced modifications of molecular structure in the strong coupling regime

In most theoretical descriptions of collective strong coupling of organic molecules to a cavity mode, the molecules are modeled as simple two-level systems. This picture fails to describe the rich structure provided by their internal rovibrational (nuclear) degrees of freedom. We investigate a first-principles model that fully takes into account both electronic and nuclear degrees of freedom, allowing an exploration of the phenomenon of strong coupling from an entirely new perspective. First, we demonstrate the limitations of applicability of the Born-Oppenheimer approximation in strongly coupled molecule-cavity structures. For the case of two molecules, we also show how dark states, which within the two-level picture are effectively decoupled from the cavity, are indeed affected by the formation of collective strong coupling. Finally, we discuss ground-state modifications in the ultra-strong coupling regime and show that some molecular observables are affected by the collective coupling strength, while others only depend on the single-molecule coupling constant.Comment: 12 pages, 8 figure

Quantum theory of collective strong coupling of molecular vibrations with a microcavity mode

We develop a quantum mechanical formalism to treat the strong coupling between an electromagnetic mode and a vibrational excitation of an ensemble of organic molecules. By employing a Bloch-Redfield-Wangsness approach, we show that the influence of dephasing-type interactions, i.e., elastic collisions with a background bath of phonons, critically depends on the nature of the bath modes. In particular, for long-range phonons corresponding to a common bath, the dynamics of the "bright state" (the collective superposition of molecular vibrations coupling to the cavity mode) is effectively decoupled from other system eigenstates. For the case of independent baths (or short-range phonons), incoherent energy transfer occurs between the bright state and the uncoupled dark states. However, these processes are suppressed when the Rabi splitting is larger than the frequency range of the bath modes, as achieved in a recent experiment [Shalabney et al., Nat. Commun. 6, 5981 (2015)]. In both cases, the dynamics can thus be described through a single collective oscillator coupled to a photonic mode, making this system an ideal candidate to explore cavity optomechanics at room temperature.Comment: 13 pages, 4 figure

Attosecond two-photon interferometry for doubly excited states of helium

We show that the correlation dynamics in coherently excited doubly excited resonances of helium can be followed in real time by two-photon interferometry. This approach promises to map the evolution of the two-electron wave packet onto experimentally easily accessible non-coincident single electron spectra. We analyze the interferometric signal in terms of a semi-analytical model which is validated by a numerical solution of the time-dependent two-electron Schr\"odinger equation in its full dimensionality.Comment: 5 pages, 4 figure

Probing Electron Correlation via Attosecond XUV Pulses in the Two-Photon Double Ionization of Helium

Recent experimental developments of high-intensity, short-pulse XUV light sources are enhancing our ability to study electron-electron correlations. We perform time-dependent calculations to investigate the so-called "sequential" regime (photon energy above 54.4 eV) in the two-photon double ionization of helium. We show that attosecond pulses allow to induce and probe angular and energy correlations of the emitted electrons. The final momentum distribution reveals regions dominated by the Wannier ridge break-up scenario and by post-collision interaction.Comment: 4 pages, 5 figure

Entanglement detection in coupled particle plasmons

When in close contact, plasmonic resonances interact and become strongly correlated. In this work we develop a quantum mechanical model, using the language of continuous variables and quantum information, for an array of coupled particle plasmons. This model predicts that when the coupling strength between plasmons approaches or surpasses the local dissipation, a sizable amount of entanglement is stored in the collective modes of the array. We also prove that entanglement manifests itself in far-field images of the plasmonic modes, through the statistics of the quadratures of the field, in what constitutes a novel family of entanglement witnesses. This protocol is so robust that it is indeed independent of whether our own model is correct. Finally, we estimate the amount of entanglement, the coupling strength and the correlation properties for a system that consists of two or more coupled nanospheres of silver, showing evidence that our predictions could be tested using present-day state-of-the-art technology.Comment: 8 pages (6 main text + 2 supplemental), 3 figure