Numerical simulation of super-square patterns in Faraday waves

We report the first simulations of the Faraday instability using the full three-dimensional Navier-Stokes equations in domains much larger than the characteristic wavelength of the pattern. We use a massively parallel code based on a hybrid Front-Tracking/Level-set algorithm for Lagrangian tracking of arbitrarily deformable phase interfaces. Simulations performed in rectangular and cylindrical domains yield complex patterns. In particular, a superlattice-like pattern similar to those of [Douady & Fauve, Europhys. Lett. 6, 221-226 (1988); Douady, J. Fluid Mech. 221, 383-409 (1990)] is observed. The pattern consists of the superposition of two square superlattices. We conjecture that such patterns are widespread if the square container is large compared to the critical wavelength. In the cylinder, pentagonal cells near the outer wall allow a square-wave pattern to be accommodated in the center

Broadband visible two-dimensional spectroscopy of molecular dyes

Two-dimensional Fourier transform spectroscopy is a promising technique to study ultrafast molecular dynamics. Similar to transient absorption spectroscopy, a more complete picture of the dynamics requires broadband laser pulses to observe transient changes over a large enough bandwidth, exceeding the inhomogeneous width of electronic transitions, as well as the separation between the electronic or vibronic transitions of interest. Here, we present visible broadband 2D spectra of a series of dye molecules and report vibrational coherences with frequencies up to ∼1400 cm−1 that were obtained after improvements to our existing two-dimensional Fourier transform setup [Al Haddad et al., Opt. Lett. 40, 312–315 (2015)]. The experiment uses white light from a hollow core fiber, allowing us to acquire 2D spectra with a bandwidth of 200 nm, in a range between 500 and 800 nm, and with a temporal resolution of 10–15 fs. 2D spectra of nile blue, rhodamine 800, terylene diimide, and pinacyanol iodide show vibronic spectral features with at least one vibrational mode and reveal information about structural motion via coherent oscillations of the 2D signals during the population time. For the case of pinacyanol iodide, these observations are complemented by its Raman spectrum, as well as the calculated Raman activity at the ground- and excited-state geometry

Energy relaxation pathways between light-matter states revealed by coherent two-dimensional spectroscopy

Coupling matter excitations to electromagnetic modes inside nano-scale optical resonators leads to the formation of hybrid light-matter states, so-called polaritons, allowing the controlled manipulation of material properties. Here, we investigate the photo-induced dynamics of a prototypical strongly-coupled molecular exciton-microcavity system using broadband two-dimensional Fourier transform spectroscopy and unravel the mechanistic details of its ultrafast photo-induced dynamics. We find evidence for a direct energy relaxation pathway from the upper to the lower polariton state that initially bypasses the excitonic manifold of states, which is often assumed to act as an intermediate energy reservoir, under certain experimental conditions. This observation provides new insight into polariton photophysics and could potentially aid the development of applications that rely on controlling the energy relaxation mechanism, such as in solar energy harvesting, manipulating chemical reactivity, the creation of Bose–Einstein condensates and quantum computing

Effect of surfactants during drop formation in a microfluidic channel: a combined experimental and computational fluid dynamics approach

The effect of surfactants on the flow characteristics during rapid drop formation in a microchannel is investigated using high-speed imaging, micro-particle image velocimetry and numerical simulations; the latter are performed using a three- dimensional multiphase solver that accounts for the transport of soluble surfactants in the bulk and at the interface. Drops are generated in a flow-focusing microchannel, using silicone oil ( 4.6 mPa s) as the continuous phase and a 52 % w/w glycerol solution as the dispersed phase. A non-ionic surfactant (Triton X-100) is dissolved in the dispersed phase at concentrations below and above the critical micelle concentration. Good agreement is found between experimental and numerical data for the drop size, drop formation time and circulation patterns. The results reveal strong circulation patterns in the forming drop in the absence of surfactants, whose intensity decreases with increasing surfactant concentration. The surfactant concentration profiles in the bulk and at the interface are shown for all stages of drop formation. The surfactant interfacial concentration is large at the front and the back of the forming drop, while the neck region is almost surfactant free. Marangoni stresses develop away from the neck, contributing to changes in the velocity profile inside the drop

Carbon K-edge x-ray emission spectroscopy of gas phase ethylenic molecules

We report on the C K-edge x-ray absorption spectra and the resonant (RXES) and non-resonant (NXES) x-ray emission spectra of ethylene, allene and butadiene in the gas phase. The RXES and NXES show clear differences for the different molecules. Overall both types of spectra are more structured for ethylene and allene, than for butadiene. Using density functional theory–restricted open shell configuration interaction single calculations, we simulate the spectra with remarkable agreement with the experiment. We identify the spectral features as being due to transitions involving localised 1s orbitals. For allene, there are distinct spectral bands that reflect transitions predominantly from either the central or terminal carbon atoms. These results are discussed in the context of ultrafast x-ray studies aimed at detecting the passage through conical intersections in polyatomic molecules

Numerical study of oil–water emulsion formation in stirred vessels: effect of impeller speed

The mixing of immiscible oil and water by a pitched blade turbine in a cylindrical vessel is studied numerically. Three-dimensional simulations combined with a hybrid front-tracking/level-set method are employed to capture the complex flow and interfacial dynamics. A large eddy simulation approach, with a Lilly–Smagorinsky model, is employed to simulate the turbulent two-phase dynamics at large Reynolds numbers Re=1802−18 026 . The numerical predictions are validated against previous experimental work involving single-drop breakup in a stirred vessel. For small Re , the interface is deformed but does not reach the impeller hub, assuming instead the shape of a Newton's Bucket. As the rotating speed increases, the deforming interface attaches to the impeller hub which leads to the formation of long ligaments that subsequently break up into small droplets. For the largest Re studied, the system dynamics becomes extremely complex wherein the creation of ligaments, their breakup and the coalescence of drops occur simultaneously. The simulation outcomes are presented in terms of spatio-temporal evolution of the interface shape and vortical structures. The results of a drop size analysis in terms of the evolution of the number of drops, and their size distribution, is also presented as a parametric function of Re

Dynamics of a surfactant-laden bubble bursting through an interface

We study the effect of surfactant on the dynamics of a bubble bursting through an interface. We perform fully three-dimensional direct numerical simulations using a hybrid interface-tracking/level-set method accounting for surfactant-induced Marangoni stresses, sorption kinetics and diffusive effects. We select an initial bubble shape corresponding to a large Laplace number and a vanishingly small Bond number in order to neglect gravity, and isolate the effects of surfactant on the flow. Our results demonstrate that the presence of surfactant affects the dynamics of the system through Marangoni-induced flow, driving motion from high to low concentration regions, which is responsible for the onset of a recirculation zone close to the free surface. These Marangoni stresses rigidify the interface, delay the cavity collapse and influence the jet breakup process

The transition to aeration in turbulent two-phase mixing in stirred vessels

We consider the mixing dynamics of an air–liquid system driven by the rotation of a pitched blade turbine (PBT) inside an open, cylindrical tank. To examine the flow and interfacial dynamics, we use a highly parallelised implementation of a hybrid front-tracking/level-set method that employs a domain-decomposition parallelisation strategy. Our numerical technique is designed to capture faithfully complex interfacial deformation, and changes of topology, including interface rupture and dispersed phase coalescence. As shown via transient, a three-dimensional (3-D) LES (large eddy simulation) using a Smagorinsky–Lilly turbulence model, the impeller induces the formation of primary vortices that arise in many idealised rotating flows as well as several secondary vortical structures resembling Kelvin–Helmholtz, vortex breakdown, blade tip vortices and end-wall corner vortices. As the rotation rate increases, a transition to ‘aeration’ is observed when the interface reaches the rotating blades leading to the entrainment of air bubbles into the viscous fluid and the creation of a bubbly, rotating, free surface flow. The mechanisms underlying the aeration transition are probed as are the routes leading to it, which are shown to exhibit a strong dependence on flow history

Harmonium: A pulse preserving source of monochromatic extreme ultraviolet (30–110 eV) radiation for ultrafast photoelectron spectroscopy of liquids

A tuneable repetition rate extreme ultraviolet source (Harmonium) for time resolved photoelectron spectroscopy of liquids is presented. High harmonic generation produces 30-110 eV photons, with fluxes ranging from similar to 2 x 10(11) photons/s at 36 eV to similar to 2 x 10(8) photons/s at 100 eV. Four different gratings in a time-preserving grating monochromator provide either high energy resolution (0.2 eV) or high temporal resolution (40 fs) between 30 and 110 eV. Laser assisted photoemission was used to measure the temporal response of the system. Vibrational progressions in gas phase water were measured demonstrating the similar to 0.2 eV energy resolution. (C) 2015 Author(s)