Polaritonic states in a dielectric nanoguide: localization and strong coupling

Propagation of light through dielectrics lies at the heart of optics. However, this ubiquitous process is commonly described using phenomenological dielectric function $\varepsilon$ and magnetic permeability $\mu$, i.e. without addressing the quantum graininess of the dielectric matter. Here, we present a theoretical study where we consider a one-dimensional ensemble of atoms in a subwavelength waveguide (nanoguide) as fundamental building blocks of a model dielectric. By exploring the roles of the atom-waveguide coupling efficiency, density, disorder, and dephasing, we establish connections among various features of polaritonic light-matter states such as localization, super and subradiance, and strong coupling. In particular, we show that coherent multiple scattering of light among atoms that are coupled via a single propagating mode can gives rise to Rabi splitting. These results provide important insight into the underlying physics of strong coupling reported by recent room-temperature experiments with microcavities and surface plasmons.Comment: 10 pages, 6 figure

Gain-tunable optomechanical cooling in a laser cavity

We study the optical cooling of the resonator mirror in a cavity-optomechanical system that contains an optical gain medium. We find that the optical damping rate is vanishingly small for an incoherently pumped laser above threshold. In the presence of an external coherent drive however, the optical damping rate can be enhanced substantially with respect to that of a passive cavity. We show that the strength of the incoherent pump provides a conduit to tune the damping rate and the minimum attainable phonon number with the same radiation pressure force, and the latter can be lowered from that of a passive cavity if the thermal contribution is nonnegligible. We also show that the system can undergo a transition from the weak optomechanical coupling regime to the strong optomechanical coupling regime as the incoherent pump strength is varied.Comment: 7 pages, 5 figure

Optical tracing of multiple charges in single-electron devices

Single molecules that exhibit narrow optical transitions at cryogenic temperatures can be used as local electric-field sensors. We derive the single charge sensitivity of aromatic organic dye molecules, based on first principles. Through numerical modeling, we demonstrate that by using currently available technologies it is possible to optically detect charging events in a granular network with a sensitivity better than $10^{-5}e/\sqrt{\textrm{Hz}}$ and track positions of multiple electrons, simultaneously, with nanometer spatial resolution. Our results pave the way for minimally-invasive optical inspection of electronic and spintronic nanodevices and building hybrid optoelectronic interfaces that function at both single-photon and single-electron levels.Comment: 7 pages, submitted to Physical Revie

Sensing force and charge at the nanoscale with a single-molecule tether

Measuring the electrophoretic mobility of molecules is a powerful experimental approach for investigating biomolecular processes. A frequent challenge in the context of single-particle measurements is throughput, limiting the obtainable statistics. Here, we present a molecular force sensor and charge detector based on parallelised imaging and tracking of tethered double-stranded DNA functionalised with charged nanoparticles interacting with an externally applied electric field. Tracking the position of the tethered particle with simultaneous nanometre precision and microsecond temporal resolution allows us to detect and quantify electrophoretic forces down to the sub-piconewton scale. Furthermore, we demonstrate that this approach is capable of detecting changes to the particle charge state, as induced by the addition of charged biomolecules or changes to pH. Our approach provides an alternative route to studying structural and charge dynamics at the single-molecule level.Comment: 23 pages, 7 figure

Coherent Interaction of Light and Single Molecules in a Dielectric Nanoguide

We present a new scheme for performing optical spectroscopy on single molecules. A glass capillary with a diameter of 600 nm filled with an organic crystal tightly guides the excitation light and provides a maximum spontaneous emission coupling factor ($\beta$) of 18% for the dye molecules doped in the organic crystal. Combination of extinction, fluorescence excitation and resonance fluorescence spectroscopy with microscopy provides high-resolution spatio-spectral access to a very large number of single molecules in a linear geometry. We discuss strategies for exploring a range of quantum optical phenomena, including coherent cooperative interactions in a mesoscopic ensemble of molecules mediated by a single mode of propagating photons.Comment: 5 pages, 5 figure

Varying the effective refractive index to measure optical transport in random media

We introduce a new approach for measuring both the effective medium and the transport properties of light propagation in heterogeneous media. Our method utilizes the conceptual equivalence of frequency variation with a change in the effective index of refraction. Experimentally, we measure intensity correlations via spectrally resolved refractive index tuning, controlling the latter via changes in the ambient pressure. Our experimental results perfectly match a generalized transport theory that incorporates the effective medium and predicts a precise value for the diffusion constant. Thus, we directly confirm the applicability of the effective medium concept in strongly scattering materials.Comment: 5 pages, 5 figure

Design and synthesis of aromatic molecules for probing electric-fields at the nanoscale

We propose using halogenated organic dyes as nanoprobes for electric field and show their greatly enhanced Stark coefficients using density functional theory (DFT) calculations. We analyse halogenated variants of three molecules that have been of interest for cryogenic single molecule spectroscopy, perylene, terrylene, and dibenzoterrylene, with the zero-phonon optical transitions at blue, red, and near infrared. Out of all the combinations of halides and binding sites that are calculated, we have found that fluorination of the optimum binding site induces a dipole difference between ground and excited states larger than 0.5 D for all three molecules with the highest value of 0.69 D for fluoroperylene. We also report on synthesis of 3-fluoroterrylene and bulk spectroscopy of this compound in liquid and solid organic environments.Comment: Article presented in Faraday Discussions on September 201