Template Stripping of Perovskite Thin Films for Dry Interfacing and Surface Structuring.

Combining excellent optoelectronic properties with the benefits of solution processability, metal-halide perovskites are promising materials for photovoltaic and light-emitting technologies. To facilitate the integration of perovskite thin films into optoelectronic devices, a need exists for simple and efficient fabrication methods. Here, we present a template-stripping technique to produce ultraflat and flexible perovskite thin films. We apply a one-step spin-coating procedure to produce high-quality CH3NH3PbBr3 perovskite thin films on top of ultraflat silicon templates. These films can be mechanically cleaved from the template using a polymer adhesive to reveal the ultraflat perovskite surfaces. We demonstrate how the flatness and flexibility of the template-stripped films enable new processing strategies based on dry interfacing, by interfacing them with plasmonic hole arrays. Moreover, we show that by using prepatterned silicon templates, structured perovskite surfaces can be produced with feature sizes down to a micrometer.

Dual-Wavelength Lasing in Quantum-Dot Plasmonic Lattice Lasers.

Arrays of metallic particles patterned on a substrate have emerged as a promising design for on-chip plasmonic lasers. In past examples of such devices, the periodic particles provided feedback at a single resonance wavelength, and organic dye molecules were used as the gain material. Here, we introduce a flexible template-based fabrication method that allows a broader design space for Ag particle-array lasers. Instead of dye molecules, we integrate colloidal quantum dots (QDs), which offer better photostability and wavelength tunability. Our fabrication approach also allows us to easily adjust the refractive index of the substrate and the QD-film thickness. Exploiting these capabilities, we demonstrate not only single-wavelength lasing but dual-wavelength lasing via two distinct strategies. First, by using particle arrays with rectangular lattice symmetries, we obtain feedback from two orthogonal directions. The two output wavelengths from this laser can be selected individually using a linear polarizer. Second, by adjusting the QD-film thickness, we use higher-order transverse waveguide modes in the QD film to obtain dual-wavelength lasing at normal and off-normal angles from a symmetric square array. We thus show that our approach offers various design possibilities to tune the laser output.

Defect-Tolerant Plasmonic Elliptical Resonators for Long-Range Energy Transfer.

Energy transfer allows energy to be moved from one quantum emitter to another. If this process follows the Förster mechanism, efficient transfer requires the emitters to be extremely close (<10 nm). To increase the transfer range, nanophotonic structures have been explored for photon- or plasmon-mediated energy transfer. Here, we fabricate high-quality silver plasmonic resonators to examine long-distance plasmon-mediated energy transfer. Specifically, we design elliptical resonators that allow energy transfer between the foci, which are separated by up to 10 µm. The geometry of the ellipse guarantees that all plasmons emitted from one focus are collected and channeled through different paths to the other focus. Thus, energy can be transferred even if a micrometer-sized defect obstructs the direct path between the focal points. We characterize the spectral and spatial profiles of the resonator modes and show that these can be used to transfer energy between green- and red-emitting colloidal quantum dots printed with subwavelength accuracy using electrohydrodynamic nanodripping. Rate-equation modeling of the time-resolved fluorescence from the quantum dots further confirms the long-distance energy transfer.

Room-Temperature Strong Coupling of CdSe Nanoplatelets and Plasmonic Hole Arrays.

Exciton polaritons are hybrid light-matter quasiparticles that can serve as coherent light sources. Motivated by applications, room-temperature realization of polaritons requires narrow, excitonic transitions with large transition dipoles. Such transitions must then be strongly coupled to an electromagnetic mode confined in a small volume. While much work has explored polaritons in organic materials, semiconductor nanocrystals present an alternative excitonic system with enhanced photostability and spectral tunability. In particular, quasi-two-dimensional nanocrystals known as nanoplatelets (NPLs) exhibit intense, spectrally narrow excitonic transitions useful for polariton formation. Here, we place CdSe NPLs on silver hole arrays to demonstrate exciton-plasmon polaritons at room temperature. Angle-resolved reflection spectra reveal Rabi splittings up to 149 meV for the polariton states. We observe bright, polarized emission arising from the lowest polariton state. Furthermore, we assess the dependence of the Rabi splitting on the hole-array pitch and the number N of NPLs. While the pitch determines the in-plane momentum for which strong coupling is observed, it does not affect the size of the splitting. The Rabi splitting first increases with NPL film thickness before eventually saturating. Instead of the commonly used [Formula: see text] dependence, we develop an analytical expression that includes the transverse confinement of the plasmon modes to describe the measured Rabi splitting as a function of NPL film thickness.

A One-Step Germole to Silole Transformation and a Stable Isomer of a Disilabenzene.

An unusual germole-to-silole transformation is described. As key intermediates hetero-fulvenes are formed which rearrange to more stable bicyclic carbene analogues. The so-formed germylenes undergo a reductive elimination yielding elemental germanium and siloles. In contrast, the analogous silylenes are stable at ambient conditions and were identified by MS spectrometry and NMR spectroscopy supported by the results of quantum mechanical calculations. These bicyclic silylenes are stable derivatives of the global minimum of the C4 Si2 H6 potential energy surface.