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Register a new userVacuum-enhanced optical nonlinearities with organic molecular photoswitches
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We propose a cavity QED scheme to enable cross-phase modulation between two arbitrarily weak classical fields in the optical domain, using organic molecular photoswitches as a disordered intracavity nonlinear medium. We show that a long-lived vibrational Raman coherence between the $cis$ and $trans$ isomer states of the photoswitch can be exploited to establish the phenomenon of vacuum-induced transparency (VIT) in high-quality microcavities. We exploit this result to derive an expression for the cross-phase modulation signal and demonstrate that it is possible to surpass the detection limit imposed by absorption losses, even in the presence of strong natural energetic and orientational disorder in the medium. Possible applications of the scheme include the development of organic nanophotonic devices for all-optical switching with low photon numbers.
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We study the full field and frequency filtered output photon statistics of a resonator in thermal equilibrium with a bath and containing an arbitrarily large quartic nonlinearity. According to the general theory of photodetection, we derive general input-output relations valid for the ultra-anharmonic regime, where the nonlinearity becomes comparable to the energy of the resonator, and show how the emission properties are modified as compared to the generally assumed simple anharmonic regime. We analyse the impact of the nonlinearity on the full statistics of the emission and its spectral properties. In particular we derive a semi-analytical expression for the frequency resolved two-photon correlations or two-photon spectrum of the system in terms of the master equation coefficients and density matrix. This provides a very clear insight into the level structure and emission possibilities of the system.
Prospects of using metal hole arrays for the enhanced optical detection of molecular chirality in nanosize volumes are investigated. Light transmission through the holes filled with an optically active material is modeled and the activity enhancement by more than an order of magnitude is demonstrated. The spatial resolution of the chirality detection is shown to be of a few tens of nanometers. From comparing the effect in arrays of cylindrical holes and holes of complex chiral shape, it is concluded that the detection sensitivity is determined by the plasmonic near field enhancement. The intrinsic chirality of the arrays due to their shape appears to be less important.
The interaction of organic molecules and molecular aggregates with electromagnetic fields that are strongly confined inside optical cavities within nanoscale volumes, has allowed the observation of exotic quantum regimes of light-matter interaction at room temperature, for a wide variety of cavity materials and geometries. Understanding the universal features of such organic cavities represents a significant challenge for theoretical modelling, as experiments show that these systems are characterized by an intricate competition between coherent and dissipative processes involving entangled nuclear, electronic and photonic degrees of freedom. In this review, we discuss a new theoretical framework that can successfully describe organic cavities under strong light-matter coupling. The theory combines standard concepts in chemical physics and quantum optics to provide a microscopic description of vibronic organic polaritons that is fully consistent with available experiments, and yet is profoundly different from the common view of organic polaritons. We show that by introducing a new class of vibronic polariton wave functions with a photonic component that is dressed by intramolecular vibrations, the new theory can offer a consistent solution to some of the long-standing puzzles in the interpretation of organic cavity photoluminescence. Throughout this review, we confront the predictions of the model with spectroscopic observations, and describe the conditions under which the theory reduces to previous approaches. We finally discuss possible extensions of the theory to account for realistic complexities of organic cavities such spatial inhomogeneities and the multi-mode nature of confined electromagnetic fields.
We combine top-down and bottom-up nanolithography to optimize the coupling of small molecular spin ensembles to $1.4$ GHz on-chip superconducting resonators. Nanoscopic constrictions, fabricated with a focused ion beam at the central transmission line, locally concentrate the microwave magnetic field. Drops of free-radical molecules have been deposited from solution onto the circuits. For the smallest ones, the molecules were delivered at the relevant circuit areas by means of an atomic force microscope. The number of spins $N_{rm eff}$ effectively coupled to each device was accurately determined combining Scanning Electron and Atomic Force Microscopies. The collective spin-photon coupling constant has been determined for samples with $N_{rm eff}$ ranging between $2 times 10^{6}$ and $10^{12}$ spins, and for temperatures down to $44$ mK. The results show the well-known collective enhancement of the coupling proportional to the square root of $N_{rm eff}$. The average coupling of individual spins is enhanced by more than four orders of magnitude (from $4$ mHz up to above $180$ Hz) when the transmission line width is reduced from $400$ microns down to $42$ nm, and reaches maximum values near $1$ kHz for molecules located on the smallest nanoconstrictions. This result opens promising avenues for the realization of magnetic spectroscopy experiments at the nanoscale and for the development of hybrid quantum computation architectures based on molecular spin qubits.
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.
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