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Enhanced nonlinear optomechanics in a coupled-mode photonic crystal device
Get PDFThe nonlinear component of the optomechanical interaction between light and mechanical vibration promises many exciting classical and quantum mechanical applications, but is generally weak. Here we demonstrate enhancement of nonlinear optomechanical measurement of mechanical motion by using pairs of coupled optical and mechanical modes in a photonic crystal device. In the same device we show linear optomechanical measurement with a strongly reduced input power and reveal how both enhancements are related. Our design exploits anisotropic mechanical elasticity to create strong coupling between mechanical modes while not changing optical properties. Additional thermo-optic tuning of the optical modes is performed with an auxiliary laser and a thermally-optimised device design. We envision broad use of this enhancement scheme in multimode phonon lasing, two-phonon heralding and eventually nonlinear quantum optomechanics
The role of Pb oxidation state of the precursor in the formation of 2D perovskite microplates
Get PDFTwo-dimensional (2D) lead halide perovskites are an exciting class of materials currently being extensively explored for photovoltaics and other optoelectronic applications. Their ionic nature makes them ideal candidates for solution processing into both thin films and nanostructured crystals. Understanding how 2D lead halide perovskite crystals form is key towards full control over their physical properties, which may enable new physical phenomena and devices. Here, we investigate the effects of the Pb oxidation state of the initial inorganic precursor on the growth of pure-phase (n = 1) – Popper 2D perovskite BA2PbI4 in single-step synthesis. We examine the different crystallisation routes in exposing PbO2 and PbI2 powders to a BAI : IPA organo-halide solution, by combining in situ optical microscopy, UV–VIS spectroscopy and time-resolved high performance liquid chromatography. So far, works using PbO2 to synthesise 3D LHPs introduce a preceding step to reduce PbO2 into either PbO or PbI2. In this work, we find that BA2PbI4 is directly formed when exposing PbO2 to BAI : IPA without the need for an external reducing agent. We explain this phenomenon by the spontaneous reduction/oxidation of PbO2/BAI that occurs under iodine-rich conditions. We observe differences in the final morphology (rectangles vs. octagons) and nanocrystal growth rate, which we explain through the different chemistry and iodoplumbate complexes involved in each case. As such, this work spans the horizon of usable lead precursors and offers a new turning knob to control crystal growth in single-step LHP synthesis
A universal method for analyzing copolymer growth
Get PDFPolymers consisting of more than one type of monomer, known as copolymers, are vital to both living and synthetic systems. Copolymerization has been studied theoretically in a number of contexts, often by considering a Markov process in which monomers are added or removed from the growing tip of a long copolymer. To date, the analysis of the most general models of this class has necessitated simulation. We present a general method for analyzing such processes without resorting to simulation. Our method can be applied to models with an arbitrary network of sub-steps prior to addition or removal of a monomer, including non-equilibrium kinetic proofreading cycles. Moreover, the approach allows for a dependency of addition and removal reactions on the neighboring site in the copolymer and thermodynamically self-consistent models in which all steps are assumed to be microscopically reversible. Using our approach, thermodynamic quantities such as chemical work; kinetic quantities such as time taken to grow; and statistical quantities such as the distribution of monomer types in the growing copolymer can be directly derived either analytically or numerically from the model definition
Ion Current Rectification and Long-Range Interference in Conical Silicon Micropores
Get PDFFluidic devices exhibiting ion current rectification (ICR), or ionic diodes, are of broad interest for applications including desalination, energy harvesting, and sensing, among others. For such applications a large conductance is desirable, which can be achieved by simultaneously using thin membranes and wide pores. In this paper we demonstrate ICR in micrometer sized conical channels in a thin silicon membrane with pore diameters comparable to the membrane thickness but both much larger than the electrolyte screening length. We show that for these pores the entrance resistance is key not only to Ohmic conductance around 0 V but also for understanding ICR, both of which we measure experimentally and capture within a single analytic theoretical framework. The only fit parameter in this theory is the membrane surface potential, for which we find that it is voltage dependent and its value is excessively large compared to the literature. From this we infer that surface charge outside the pore strongly contributes to the observed Ohmic conductance and rectification by a different extent. We experimentally verify this hypothesis in a small array of pores and find that ICR vanishes due to pore–pore interactions mediated through the membrane surface, while Ohmic conductance around 0 V remains unaffected. We find that the pore–pore interaction for ICR is set by a long-ranged decay of the concentration which explains the surprising finding that the ICR vanishes for even a sparsely populated array with a pore–pore spacing as large as 7 μm
Bending and Stretching: A Practical Examination of Molecules at Aqueous Interfaces
No full textIn this PhD thesis the highly surface-specific technique of vibrational sum-frequency generation (VSFG) spectroscopy is described and applied to several aqueous systems. VSFG allows the specific probing of the vibrational resonances of the molecules embedded in single molecular layers at interfaces. The technique also allows the determination of the orientation of the molecular groups carrying the vibration. A detailed description of the theoretical background of VSFG can be found in chapter 2, while in chapter 3 the experimental implementation of the technique is described. In chapter 4 the technique is used to identify the origin of the VSFG response of the bending vibration of water molecules at the surface of pure water and at charged interfaces. In chapter 5 VSFG is used to study the molecular orientation of urea molecules in water at charged interfaces. In chapter 6 the vibrational response and the molecular orientation of small carboxylate ions at the water/air interface are studied. Chapter 7 discusses the origin of the VSFG signal of small carboxylic acids at the water/air interface, while chapter 8 describes the different freezing behavior of aqueous solutions of small carboxylic acids on ice. Chapter 9 reports on a study of the molecular structure of hyperactive antifreeze proteins adsorbed to the surface of ice. In the final chapter, chapter 10, the molecular structure and surface accumulation dynamics of hyaluronan at the water/air interface are discussed, in dependence of the molecular weight and concentration of hyaluronan, and the properties of the solvent
Confined pulsed diffuse layer charging for nanoscale electrodeposition with an STM
No full textRegulating the state of the solid-liquid interface by means of electric fields is a powerful tool to control electrochemistry. In scanning probe systems, this can be confined closely to a scanning (nano)electrode by means of fast potential pulses, providing a way to probe the interface and control electrochemical reactions locally, as has been demonstrated in nanoscale electrochemical etching. For this purpose, it is important to know the spatial extent of the interaction between pulses applied to the tip, and the substrate. In this paper we use a framework of diffuse layer charging to describe the localization of electrical double layer charging in response to a potential pulse at the probe. Our findings are in good agreement with literature values obtained in electrochemical etching. We show that the pulse can be much more localized by limiting the diffusivity of the ions present in solution, by confined electrodeposition of cobalt in a dimethyl sulfoxide solution, using an electrochemical scanning tunnelling microscope. Finally, we demonstrate the deposition of cobalt nanostructures (<100 nm) using this method. The presented framework therefore provides a general route for predicting and controlling the time-dependent region of interaction between an electrochemical scanning probe and the surface
Simulations of DNA-Origami Self-Assembly Reveal Design-Dependent Nucleation Barriers
Get PDFNucleation is the rate-determining step in the kinetics of many self-assembly processes. However, the importance of nucleation in the kinetics of DNA-origami self-assembly, which involves both the binding of staple strands and the folding of the scaffold strand, is unclear. Here, using Monte Carlo simulations of a lattice model of DNA origami, we find that some, but not all, designs can have a nucleation barrier and that this barrier disappears at lower temperatures, rationalizing the success of isothermal assembly. We show that the height of the nucleation barrier depends primarily on the coaxial stacking of staples that are adjacent on the same helix, a parameter that can be modified with staple design. Creating a nucleation barrier to DNA-origami assembly could be useful in optimizing assembly times and yields, while eliminating the barrier may allow for fast molecular sensors that can assemble/disassemble without hysteresis in response to changes in the environment
Zero-Threshold Optical Gain in Electrochemically Doped Nanoplatelets and the Physics Behind It
Get PDFColloidal nanoplatelets (NPLs) are promising materials for lasing applications. The properties are usually discussed in the framework of 2D materials, where strong excitonic effects dominate the optical properties near the band edge. At the same time, NPLs have finite lateral dimensions such that NPLs are not true extended 2D structures. Here we study the photophysics and gain properties of CdSe/CdS/ZnS core-shell-shell NPLs upon electrochemical n doping and optical excitation. Steady-state absorption and PL spectroscopy show that excitonic effects are weaker in core-shell-shell nanoplatelets due to the decreased exciton binding energy. Transient absorption studies reveal a gain threshold of only one excitation per nanoplatelet. Using electrochemical n doping, we observe the complete bleaching of the band edge exciton transitions. Combining electrochemical doping with transient absorption spectroscopy, we demonstrate that the gain threshold is fully removed over a broad spectral range and gain coefficients of several thousand cm(-1) are obtained. These doped NPLs are the best performing colloidal nanomaterial gain medium reported to date, with the lowest gain threshold and broadest gain spectrum and gain coefficients that are 4 times higher than in n-doped colloidal quantum dots. The low exciton binding energy due to the CdS and ZnS shells, in combination with the relatively small lateral size of the NPLs, results in excited states that are effectively delocalized over the entire platelet. Core-shell NPLs are thus on the border between strong confinement in QDs and dominant Coulombic effects in 2D materials. We demonstrate that this limit is in effect ideal for optical gain and that it results in an optimal lateral size of the platelets where the gain threshold per nm2 is minimal.
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Temporal scaling in C. elegans larval development
Get PDFIt is essential that correct temporal order of cellular events is maintained during animal development. During postembryonic development, the rate of development depends on external conditions, such as food availability, diet, and temperature. How timing of cellular events is impacted when the rate of development is changed at the organism level is not known. We used a unique time-lapse microscopy approach to simultaneously measure timing of oscillatory gene expression, hypodermal stem cell divisions, and cuticle shedding in individual Caenorhabditis elegans larvae, as they developed from hatching to adulthood. This revealed strong variability in timing between isogenic individuals under the same conditions. However, this variability obeyed “temporal scaling,” meaning that events occurred at the same time when measured relative to the total duration of development in each individual. We also observed pervasive changes in timing when temperature, diet, or genotype were varied, but with larval development divided in “epochs” that differed in how event timing was impacted. Yet, these variations in timing were still explained by temporal scaling when time was rescaled by the duration of the respective epochs in each individual. Surprisingly, timing obeyed temporal scaling even in mutants lacking lin-42/Period, presumed a core regulator of timing of larval development, that exhibited strongly delayed, heterogeneous timing. However, shifting conditions middevelopment perturbed temporal scaling and changed event order in a highly condition-specific manner, indicating that a complex machinery is responsible for temporal scaling under constant conditions
Directional quantum dot emission by soft-stamping on silicon Mie resonators
No full textWe present a soft-stamping method to selectively print a homogenous layer of CdSeTe/ZnS core–shell quantum dots (QDs) on top of an array of Si nanocylinders with Mie-type resonant modes. Using this new method, we gain accurate control of the quantum dot's angular emission through engineered coupling of the QDs to these resonant modes. Using numerical simulations we show that the emission into or away from the Si substrate can be precisely controlled by the QD position on the nanocylinder. QDs centered on a 400 nm diameter nanocylinder surface show 98% emission directionality into the Si substrate. Alternatively, for homogenous ensembles placed over the nanocylinder top-surface, the upward emission is enhanced 10-fold for 150 nm diameter cylinders. Experimental PL intensity measurements corroborate the simulated trends with cylinder diameter. PL lifetime measurements reflect well the variations of the local density of states at the QD position due to coupling to the resonant cylinders. These results demonstrate that the soft imprint technique provides a unique manner to directly integrate optical emitters with a wide range of nanophotonic geometries, with potential applications in LEDs, luminescent solar concentrators, and up- and down-conversion schemes for improved photovoltaics