Tuning and Switching a Plasmonic Quantum Dot Sandwich in a Nematic Line Defect

We study the quantum-mechanical effects arising in a single semiconductor core/shell quantum dot controllably sandwiched between two plasmonic nanorods. Control over the position and the sandwich confinement structure is achieved by the use of a linear-trap, liquid-crystal line defect and laser tweezers that push the sandwich together. This arrangement allows for the study of exciton plasmon interactions in a single structure, unaltered by ensemble effects or the complexity of dielectric interfaces. We demonstrate the effect of plasmonic confinement on the photon-antibunching behavior of the quantum dot and its luminescence lifetime. The quantum dot behaves as a single emitter when nanorods are far away from the quantum dot but shows possible multiexciton emission and a significantly decreased lifetime when tightly confined in a plasmonic sandwich. These findings demonstrate that liquid crystal defects, combined with laser tweezers, enable a versatile platform to study plasmonic coupling phenomena in a nanoscale laboratory, where all elements can be arranged almost at will.Comment: Supporting information at the en

Temperature Dependence of the Electron Diffusion Coefficient in Electrolyte-Filled TiO2 Nanoparticle Films: Evidence Against Multiple Trapping in Exponential Conduction-Band Tails

The temperature and photoexcitation density dependences of the electron transport dynamics in electrolytefilled mesoporous TiO2 nanoparticle films were investigated by transient photocurrent measurements. The thermal activation energy of the diffusion coefficient of photogenerated electrons ranged from 0.19–0.27 eV, depending on the specific sample studied. The diffusion coefficient also depends strongly on the photoexcitation density; however, the activation energy has little, if any, dependence on the photoexcitation density. The light intensity dependence can be used to infer temperature-independent dispersion parameters in the range 0.3–0.5. These results are inconsistent with the widely used transport model that assumes multiple trapping of electrons in an exponential conduction-band tail. We can also exclude a model allowing for widening of a band tail with increased temperature. Our results suggest that structural, not energetic, disorder limits electron transport in mesoporous TiO2. The analogy between this material and others in which charge transport is limited by structural disorder is discussed

Comprehensive device modeling of plasmon-enhanced and optical field-dependent photocurrent generation in organic bulk heterojunctions

We present a comprehensive numerical model to describe the coupled optical and electrical behavior of plasmon-enhanced polymer/fullerene bulk heterojunction solar cells. We incorporate a bound electron/hole pair generation rate that is dependent on both the 2-dimensional position within the P3HT:PCBM active layer, and the solar spectral irradiance. By considering the absorption and plasmonic properties of two different popular device architectures, and applying the Poisson, current continuity, and drift/diffusion equations, we are able to predict quantum efficiency, short-circuit current density, and desired carrier mobility ratios for devices possessing strongly non-uniform optical fields commonly produced by nanostructures.4 page(s

Integrated optical and electrical modeling of plasmon-enhanced thin film photovoltaics : a case-study on organic devices

The nanoscale light control for absorption enhancement of organic photovoltaic (OPV) devices inevitably produces strongly non-uniform optical fields. These non-uniformities due to the localized optical modes are a primary route toward absorption enhancement in OPV devices. Therefore, a rigorous modeling tool taking into account the spatial distribution of optical field and carrier generation is necessary. Presented here is a comprehensive numerical model to describe the coupled optical and electrical behavior of plasmon-enhanced polymer:fullerene bulk heterojunction (BHJ) solar cells. In this model, a position-dependent electron-hole pair generation rate that could become highly non-uniform due to photonic nanostructures is directly calculated from the optical simulations. By considering the absorption and plasmonic properties of nanophotonic gratings included in two different popular device architectures, and applying the Poisson, current continuity, and drift/diffusion equations, the model predicts quantum efficiency, short-circuit current density, and desired carrier mobility ratios for bulk heterojunction devices incorporating nanostructures for light management. In particular, the model predicts a significant degradation of device performance when the carrier species with lower mobility are generated far from the collecting electrode. Consequently, an inverted device architecture is preferred for materials with low hole mobility. This is especially true for devices that include plasmonic nanostructures. Additionally, due to the incorporation of a plasmonic nanostructure, we use simulations to theoretically predict absorption band broadening of a BHJ into energies below the band gap, resulting in a 4.8% increase in generated photocurrent.8 page(s