Interaction and coherence of a plasmon-exciton polariton condensate

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. In this work we demonstrate the formation of a non-equilibrium room temperature plasmon-exciton-polariton condensate with a long range spatial coherence, extending a hundred of microns, well over the excitation area, by coupling Frenkel excitons in organic molecules to a multipolar mode in a lattice of plasmonic nanoparticles. Time-resolved experiments evidence the picosecond dynamics of the condensate and a sizeable blueshift, thus measuring for the first time the effect of polariton interactions in plasmonic cavities. Our results pave the way to the observation of room temperature superfluidity and novel nonlinear phenomena in plasmonic systems, challenging the common belief that absorption losses in metals prevent the realization of macroscopic quantum states.Comment: 23 pages, 5 figures, SI 7 pages, 5 figure

Two-dimensional Spectroscopy of Molecular Excitons in a Model Dimer System

The physics of molecular excitons has been the subject of many recent studies using electronic two-dimensional photon-echo spectroscopy (2DPE), particularly in the context of light harvesting in photosynthesis. Since the spectra for multichromophoric aggregates are congested, particularly so at room temperature, we present a study of a model dimer comprised of identical chromophores with a well defined electronic coupling strength, to provide clear signatures for coherences between vibronic excitons in 2D spectra. We begin by describing the design of a broadband passively phase-stabilized interferometer for collection of 2D spectra, which also allows for the investigation of state preparation in 2D spectroscopy by using shaped excitation pulses. In experiments on the model dimer we observe strong oscillating off-diagonal features in the 2D spectra which are present only before the onset of dephasing, which occurs in less than 100 fs due to strong system-bath coupling. This is in contrast with the parent dye, where low amplitude oscillations associated with Raman active vibrations persist for several ps following excitation. The results of this comparative study indicate that the signals observed earlier in photosynthetic proteins likely reflect vibrational motion in isolated pigments, and not delocalized quantum coherence. While long-lived vibrational coherences are of questionable biological relevance at face value, we conclude with a discussion on initial findings using coherently controlled 2D spectroscopy, where we observe long-lived signatures associated to vibronic coherences at room temperature. These results point to new directions of study using multidimensional spectroscopy to unravel the role of coherence in excitation energy transfer in molecular aggregates in an experimentally direct fashion.Ph.D

Broadband characterization of congruent lithium niobate from mHz to optical frequencies

Lithium niobate (LiNbO3) is a well known uniaxial ferroelectric material. Using impedance measurement, quasi-optical free-space characterization, THz time domain spectroscopy (THz-TDS) and ellipsometry, its dielectric permittivity/refractive index was characterized depending on the crystal orientation over a broad frequency range: 1 mHz to 1 PHz ( nm). Three different frequency ranges, separated by well identified resonances, are observed: low frequency 'free-piezoelectric' response, intermediate frequency 'clamped-ionic' response and high frequency 'electronic' response. These features are discussed with an emphasis on the role of the crystallographic structure and piezoelectric response.</p

Diffraction enhanced transparency (DET) using frequency detuned and displaced resonant rods

In this contribution, we demonstrate that a periodic lattice of frequency-detuned and displaced resonant rods can suppress the THz extinction at the central resonant frequency, leading to an enhanced spectral window of near perfect transparency. The system consists of a periodic lattice of metallic rods of two different sizes. Each of the rods supports a strong half-wavelength (λ/2) resonance which are detuned with respect to each other. Furthermore, both the rods are spatially displaced within each unit cell of the lattice. The group-index obtained from far-field measurements shows that the THz field is strongly delayed by more than four orders of magnitude at the spectral transparency window. Using micro-spectroscopic measurements of the electric near fields, we show that this transparency window has its origin in the interference between two surface lattice resonances, arising from the diffractively enhanced radiative coupling of the two λ/2 resonances in the lattice. Thus, we term this phenomenon as Diffraction Enhanced Transparency (DET). Since DET does not involve near-field coupling between resonators, the fabrication tolerance to imperfections is expected to be very high. This remarkable response and ease of fabrication renders these systems as very interesting components for THz communicatio

Ultrafast dynamics of nonequilibrium organic exciton-polariton condensates

Exciton-polariton condensation in organic materials, arising from the coupling of Frenkel excitons to the electromagnetic field in cavities, is a phenomenon resulting in low-threshold coherent light emission among other fascinating properties. The exact mechanisms leading to the thermalization of organic exciton-polaritons toward condensation are not yet understood, partly due to the complexity of organic molecules and partly to the canonical microcavities used in condensation studies, which limit broadband studies. Here, we exploit an entirely different cavity design, i.e., an array of plasmonic nanoparticles strongly coupled to organic molecules, to successfully measure the broadband ultrafast dynamics of the strongly coupled system. Sharp features emerge in the transient spectrum originating from the formation of a condensate with a well-defined molecular vibrational composition. These measurements represent the first direct experimental evidence that molecular vibrations drive condensation in organic systems and provide a benchmark for modeling the dynamics of organic-based exciton-polariton condensates

Visualizing near-field coupling in terahertz dolmens

Strong interactions between resonant structures in the near-field occur at length scales shorter than the wavelength, and can be exploited for modifying the propagation of electromagnetic radiation. Dolmen-like structures, formed by a rod supporting a dipolar (bright) resonance and two orthogonal rods with a quadrupolar (dark) resonance at the same frequency, represent a geometry of significant interest for near-field electromagnetic coupling. These structures demonstrate electromagnetically induced transparency (EIT) through coupling between these resonances, concurrently providing a sharp spectral selectivity in transmission and large group velocity reduction. We use near-field terahertz scanning microscopy to map the electric fields in the vicinity of a metallic dolmen in both amplitude and phase. In this way, we directly measure the interaction between bright and dark modes in the time-domain, revealing the physics resulting in EIT. We experimentally demonstrate the hybridization of bright and dark modes accompanying the near-field coupling, as well as the excitation of the dark mode at the frequency of the far-field transparency