School of Physics - Research Publications
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ItemTuning Single Quantum Dot Emission with a Micromirror(AMER CHEMICAL SOC, 2018-02)The photoluminescence of single quantum dots fluctuates between bright (on) and dark (off) states, also termed fluorescence intermittency or blinking. This blinking limits the performance of quantum dot-based devices such as light-emitting diodes and solar cells. However, the origins of the blinking remain unresolved. Here, we use a movable gold micromirror to determine both the quantum yield of the bright state and the orientation of the excited state dipole of single quantum dots. We observe that the quantum yield of the bright state is close to unity for these single QDs. Furthermore, we also study the effect of a micromirror on blinking, and then evaluate excitation efficiency, biexciton quantum yield, and detection efficiency. The mirror does not modify the off-time statistics, but it does change the density of optical states available to the quantum dot and hence the on times. The duration of the on times can be lengthened due to an increase in the radiative recombination rate.
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ItemThe Degradation and Blinking of Single CsPbl3 Perovskite Quantum Dots(AMER CHEMICAL SOC, 2018-06-28)We demonstrate using single molecule spectroscopy that inorganic CsPbI3 perovskite quantum dots (PQDs) undergo an irreversible, photoaccelerated reaction with water that results in a blue-shift of the photoluminescence (PL) and ultimately to complete quenching of the emission. We find that decomposition does not take place in the presence of oxygen alone but that it requires light and water. We also analyze the blinking for some stable PQDs and find a continuous distribution of emission states with a linear correlation between intensity and lifetime. We postulate that, in addition to charging and discharging processes, blinking arises from the activation and deactivation of nonradiative recombination centers in the PQDs.
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ItemNear-Perfect Absorption of Light by Coherent Plasmon-Exciton States(AMER CHEMICAL SOC, 2021-05-12)We experimentally demonstrate and theoretically study the formation of coherent plasmon-exciton states which exhibit absorption of >90% of the incident light (at resonance) and cancellation of absorption. These coherent states result from the interaction between a material supporting an electronic excitation and a plasmonic structure capable of (near) perfect absorption of light. We illustrate the potential implications of these coherent states by measuring the charge separation attainable after photoexcitation. Our study opens the prospect for realizing devices that exploit coherent effects in applications.
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ItemA Tunable Polymer-Metal Based Anti-Reflective Metasurface(WILEY-V C H VERLAG GMBH, 2020-01)Anti-reflective surfaces are of great interest for optical devices, sensing, photovoltaics, and photocatalysis. However, most of the anti-reflective surfaces lack in situ tunability of the extinction with respect to wavelength. This communication demonstrates a tunable anti-reflective surface based on colloidal particles comprising a metal core with an electrochromic polymer shell. Random deposition of these particles on a reflective surface results in a decrease in the reflectance of up to 99.8% at the localized surface plasmon resonance frequency. This narrow band feature can be tuned by varying the pH or by application of an electric potential, resulting in wavelength shifts of up to 30 nm. Electrophoretic particle deposition is shown to be an efficient method for controlling the interparticle distance and thereby further optimizing the overall efficiency of the anti-reflective metasurface.
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ItemBroadband High-Efficiency Chiral Splitters and Holograms from Dielectric Nanoarc Metasurfaces(WILEY-V C H VERLAG GMBH, 2019-05)Simultaneous broadband and high efficiency merits of designer metasurfaces are currently attracting widespread attention in the field of nanophotonics. However, contemporary metasurfaces rarely achieve both advantages simultaneously. For the category of transmissive metadevices, plasmonic or conventional dielectric metasurfaces are viable for either broadband operation with relatively low efficiency or high efficiency at only a selection of wavelengths. To overcome this limitation, dielectric nanoarcs are proposed as a means to accomplish two advantages. Continuous nanoarcs support different electromagnetic resonant modes at localized areas for generating phase retardation. Meanwhile, the geometric nature of nanoarc curvature endows the nanoarcs with full phase coverage of 0-2π due to the Pancharatnam-Berry phase principle. Experimentally incorporated with the chiral-detour phase principle, a few compelling functionalities are demonstrated, such as chiral beamsplitting, broadband holography, and helicity-selective holography. The continuous nanoarc metasurfaces prevail over plasmonic or dielectric discretized building block strategies and the findings lead to novel designs of spin-controllable metadevices.
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ItemA new method to position and functionalize metal-organic framework crystals(NATURE PUBLISHING GROUP, 2011-03)With controlled nanometre-sized pores and surface areas of thousands of square metres per gram, metal-organic frameworks (MOFs) may have an integral role in future catalysis, filtration and sensing applications. In general, for MOF-based device fabrication, well-organized or patterned MOF growth is required, and thus conventional synthetic routes are not suitable. Moreover, to expand their applicability, the introduction of additional functionality into MOFs is desirable. Here, we explore the use of nanostructured poly-hydrate zinc phosphate (α-hopeite) microparticles as nucleation seeds for MOFs that simultaneously address all these issues. Affording spatial control of nucleation and significantly accelerating MOF growth, these α-hopeite microparticles are found to act as nucleation agents both in solution and on solid surfaces. In addition, the introduction of functional nanoparticles (metallic, semiconducting, polymeric) into these nucleating seeds translates directly to the fabrication of functional MOFs suitable for molecular size-selective applications.
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ItemDipole-field-assisted charge extraction in metal-perovskite-metal back-contact solar cells(NATURE PUBLISHING GROUP, 2017-09-20)Hybrid organic-inorganic halide perovskites are low-cost solution-processable solar cell materials with photovoltaic properties that rival those of crystalline silicon. The perovskite films are typically sandwiched between thin layers of hole and electron transport materials, which efficiently extract photogenerated charges. This affords high-energy conversion efficiencies but results in significant performance and fabrication challenges. Herein we present a simple charge transport layer-free perovskite solar cell, comprising only a perovskite layer with two interdigitated gold back-contacts. Charge extraction is achieved via self-assembled monolayers and their associated dipole fields at the metal-perovskite interface. Photovoltages of ~600 mV generated by self-assembled molecular monolayer modified perovskite solar cells are equivalent to the built-in potential generated by individual dipole layers. Efficient charge extraction results in photocurrents of up to 12.1 mA cm-2 under simulated sunlight, despite a large electrode spacing.Simplified device concepts may become important for the development of low cost photovoltaics. Lin et al. report solar cells based on interdigitated gold back-contacts and metal halide perovskites where charge extraction is assisted via a dipole field generated by self-assembled molecular monolayers.
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ItemPhotoexcited Pd(ii) auxiliaries enable light-induced control in C(sp3)-H bond functionalisation(ROYAL SOC CHEMISTRY, 2020-03-07)Herein we report the photophysical and photochemical properties of palladacycle complexes derived from 8-aminoquinoline ligands, commonly used auxiliaries in C-H activation. Spectroscopic, electrochemical and computational studies reveal that visible light irradiation induces a mixed LLCT/MLCT charge transfer providing access to synthetically relevant Pd(iii)/Pd(iv) redox couples. The Pd(ii) complex undergoes photoinduced electron transfer with alkyl halides generating C(sp3)-H halogenation products rather than C-C bond adducts. Online photochemical ESI-MS analysis implicates participation of a mononuclear Pd(iii) species which promotes C-X bond formation via a distinct Pd(iii)/Pd(iv) pathway. To demonstrate the synthetic utility, we developed a general method for inert C(sp3)-H bond bromination, chlorination and iodination with alkyl halides. This new strategy in auxiliary-directed C-H activation provides predictable and controllable access to distinct reactivity pathways proceeding via Pd(iii)/Pd(iv) redox couples induced by visible light irradiation.
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ItemPlasmonic Metasurfaces for Optical Information Processing(SPIE-INT SOC OPTICAL ENGINEERING, 2019-01-01)Optical spatial frequency filtering is a key method for information processing in biological and technical imaging. While conventional approaches rely on bulky components to access and filter the Fourier plane content of a wavefield, nanophotonic approaches for spatial frequency filtering have recently gained attention. Here computational and experimental progress towards the design and demonstration of metasurfaces with spatial frequency filtering capability for optical image processing will be presented. Using the example of a metasurface consisting of radial rod trimers we demonstrate its potential to perform edge enhancement in an amplitude image and conversion of phase gradients in a wavefield into intensity modulations. The presented results indicate a potential avenue for ultra-compact image processing devices with applications in biological live-cell imaging.
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ItemTuning the asymmetric response of metasurfaces for optical spatial filtering(SPIE-INT SOC OPTICAL ENGINEERING, 2019-01-01)The spatial filtering of optical signals has been demonstrated previously with metasurface thin-films created from arrays of structured optical elements. We consider the problem of changing the symmetry of their response with changes to the in-plane wavevector kI→-kI and show it can be tailored or even dynamically tuned. Our work is based on a general theory of metasurfaces constructed from non-diffracting arrays of coupled metal particles. We present the optical transfer function of such a metasurface, identify the physical properties essential for asymmetry and demonstrate its behaviour experimentally.