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Plasmonic nanopatch antennas that incorporate dielectric gaps hundreds of picometers to several nanometers thick have drawn increasing attention over the past decade because they confine electromagnetic fields to grossly sub-diffraction-limited volumes. Substantial control over the optical properties of excitons and color centers confined within these plasmonic cavities has already been demonstrated with far-field optical spectroscopies, but near-field optical spectroscopies are essential for an improved understanding of the plasmon–emitter interaction at the nanoscale. Here, we characterize the intensity and phase-resolved plasmonic response of isolated nanopatch antennas by cathodoluminescence microscopy. Furthermore, we explore the distinction between optical and electron beam spectroscopies of coupled plasmon–exciton heterostructures to identify constraints and opportunities for future nanoscale characterization and control of hybrid nanophotonic structures. While we observe substantial Purcell enhancement in time-resolved photoluminescence spectroscopies, negligible Purcell enhancement is observed in cathodoluminescence spectroscopies of hybrid nanophotonic structures. The substantial differences in measured Purcell enhancement for electron beam and laser excitation can be understood as a result of the different selection rules for these complementary experiments. These results provide a fundamentally new understanding of near-field plasmon–exciton interactions in nanopatch antennas, which is essential for myriad emerging quantum photonic devices. 

Abstract Radiation as a heat transfer mode inside a bulk material is usually negligible in comparison to conduction. Here, the contribution of radiation to energy transport inside a hyperbolic material, hexagonal boron nitride (hBN), is investigated. With hyperbolic dispersion, i.e., opposite signs of dielectric components along principal directions, phonon polaritons contribute significantly to energy transport due to a much greater number of propagating modes compared to that in a normal material. A many‐body model is developed to account for radiative heat transfer in a material with a nonuniform temperature distribution. The total radiative heat transfer through hBN is found to be largely contributed by the high‐κ modes within the Reststrahlen bands, and is comparable to phonon conduction. Experimental measurements of temperature‐dependent thermal transport also show that radiative contribution to thermal transport is of the same order as that from phonons. Therefore, this work shows, for the first time, radiative heat transfer inside a material can be comparable to phonon conductive heat transfer. 

ABSTRACT Printing of high‐resolution three‐dimensional nanostructures utilizing two‐photon polymerization has gained significant attention recently. In particular, isopropyl thioxanthone (ITX) has been implemented as a photoinitiator due to its capability of initiating and depleting polymerization on demand, but new photoinitiating materials are still needed in order to reduce the power requirements for the high‐throughput creation of 3D structures. To address this point, a suite of new thioxanthone‐based photoinitiators were synthesized and characterized. Then two‐photon polymerization was performed using the most promising photoinitiating molecule. Importantly, one of the initiators, 2,7‐bis[(4‐(dimethylamino)phenyl ethynyl)‐9H‐thioxanthen‐9‐one] (BDAPT), showed a fivefold improvement in the writing threshold over the commonly used ITX molecule. To elucidate the fundamental mechanism, the excitation and inhibition behavior of the BDAPT molecule were evaluated using density functional theory (DFT) calculations, low‐temperature phosphorescence spectroscopy, ultra‐fast transient absorption spectroscopy, and the two‐photon Z‐scan spectroscopic technique. The improved polymerization threshold of this new photoinitiator presents a clear pathway for the modification of photoinitiators in 3D nanoprinting. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys.2019,57, 1462–1475