Conductivity in organic semiconductors hybridized with the vacuum field

Organic semiconductors have generated considerable interest for their potential for creating inexpensive and flexible devices easily processed on a large scale [1-11]. However technological applications are currently limited by the low mobility of the charge carriers associated with the disorder in these materials [5-8]. Much effort over the past decades has therefore been focused on optimizing the organisation of the material or the devices to improve carrier mobility. Here we take a radically different path to solving this problem, namely by injecting carriers into states that are hybridized to the vacuum electromagnetic field. These are coherent states that can extend over as many as 10^5 molecules and should thereby favour conductivity in such materials. To test this idea, organic semiconductors were strongly coupled to the vacuum electromagnetic field on plasmonic structures to form polaritonic states with large Rabi splittings ca. 0.7 eV. Conductivity experiments show that indeed the current does increase by an order of magnitude at resonance in the coupled state, reflecting mostly a change in field-effect mobility as revealed when the structure is gated in a transistor configuration. A theoretical quantum model is presented that confirms the delocalization of the wave-functions of the hybridized states and the consequences on the conductivity. While this is a proof-of-principle study, in practice conductivity mediated by light-matter hybridized states is easy to implement and we therefore expect that it will be used to improve organic devices. More broadly our findings illustrate the potential of engineering the vacuum electromagnetic environment to modify and to improve properties of materials.Comment: 16 pages, 13 figure

Science and applications of wafer-scale crystalline carbon nanotube films prepared through controlled vacuum filtration

Carbon nanotubes (CNTs) make an ideal one-dimensional (1D) material platform for the exploration of exotic physical phenomena under extremely strong quantum confinement. The 1D character of electrons, phonons and excitons in individual CNTs features extraordinary electronic, thermal and optical properties. Since the first discovery, they have been continuing to attract interest in various disciplines, including chemistry, materials science, physics, and engineering. However, the macroscopic manifestation of such properties is still limited, despite significant efforts for decades. Recently, a controlled vacuum filtration method has been developed for the preparation of wafer-scale films of crystalline chirality-enriched CNTs, and such films immediately enable exciting new fundamental studies and applications. In this review, we will first discuss the controlled vacuum filtration technique, and then summarize recent discoveries in optical spectroscopy studies and optoelectronic device applications using films prepared by this technique.Comment: 24 pages, 14 figure

Ultrafast flow of interacting organic polaritons

The strong-coupling of an excitonic transition with an electromagnetic mode results in composite quasi-particles called exciton-polaritons, which have been shown to combine the best properties of their bare components in semiconductor microcavities. However, the physics and applications of polariton flows in organic materials and at room temperature are still unexplored because of the poor photon confinement in such structures. Here we demonstrate that polaritons formed by the hybridization of organic excitons with a Bloch Surface Wave are able to propagate for hundreds of microns showing remarkable third-order nonlinear interactions upon high injection density. These findings pave the way for the studies of organic nonlinear light-matter fluxes and for a technological promising route of dissipation-less on-chip polariton devices working at room temperature.Comment: Improved version with polariton-polariton interactions. 13 pages, 4 figures, supporting 6 pages, 6 figure

Inverting Singlet and Triplet Excited States using Strong Light-Matter Coupling

In organic microcavities, hybrid light-matter states can form with energies that differ from the bare molecular excitation energies by nearly 1 eV. A timely question, given recent advances in the development of thermally activated delayed fluorescence materials, is whether strong light-matter coupling can be used to invert the ordering of singlet and triplet states and, in addition, enhance reverse intersystem crossing (RISC) rates. Here, we demonstrate a complete inversion of the singlet lower polariton and triplet excited states. We also unambiguously measure the RISC rate in strongly-coupled organic microcavities and find that, regardless of the large energy level shifts, it is unchanged compared to films of the bare molecules. This observation is a consequence of slow RISC to the lower polariton due to the delocalized nature of the state across many molecules and an inability to compete with RISC to the dark exciton reservoir, which occurs at a rate comparable to that in bare molecules

Multivalley engineering in semiconductor microcavities

We consider exciton-photon coupling in semiconductor microcavities in which separate periodic potentials have been embedded for excitons and photons. We show theoretically that this system supports degenerate ground-states appearing at non-zero in-plane momenta, corresponding to multiple valleys in reciprocal space, which are further separated in polarization corresponding to a polarization-valley coupling in the system. Aside forming a basis for valleytronics, the multivalley dispersion is predicted to allow for spontaneous momentum symmetry breaking and two-mode squeezing under non-resonant and resonant excitation, respectively.Comment: Manuscript: 7 pages, 7 figures, published in Scientific Reports 7, 45243 (2017

Zero Dimensional Polariton Laser in a Sub-Wavelength Grating Based Vertical Microcavity

Semiconductor exciton-polaritons in planar microcavities form coherent two-dimensional condensates in non-equilibrium. However, coupling of multiple lower-dimensional polariton quantum systems, critically needed for polaritonic quantum device applications and novel cavity-lattice physics, has been limited due to the conventional cavity structures. Here we demonstrate full confinement of the polaritons non-destructively using a hybrid cavity made of a single-layer sub-wavelength grating mirror and a distributed Bragg reflector. Single-mode polariton lasing was observed at a chosen polarization. Incorporation of a designable slab mirror into the conventional vertical cavity, when operating in the strong-coupling regime, enables confinement, control and coupling of polariton gasses in a scalable fashion. It may open a door to experimental implementation of polariton-based quantum photonic devices and coupled cavity quantum electrodynamics systems.Comment: http://www.nature.com/lsa/journal/v3/n1/full/lsa201416a.htm

Room temperature Bloch surface wave polaritons

Polaritons are hybrid light-matter quasi-particles that have gathered a significant attention for their capability to show room temperature and out-of-equilibrium Bose-Einstein condensation. More recently, a novel class of ultrafast optical devices have been realized by using flows of polariton fluids, such as switches, interferometers and logical gates. However, polariton lifetimes and propagation distance are strongly limited by photon losses and accessible in-plane momenta in usual microcavity samples. In this work, we show experimental evidence of the formation of room temperature propagating polariton states arising from the strong coupling between organic excitons and a Bloch surface wave. This result, which was only recently predicted, paves the way for the realization of polariton devices that could allow lossless propagation up to macroscopic distances