Electrically induced liquid-liquid phase transition in water at room temperature.

In this work we expand on findings previously reported [Wexler et al., Phys. Chem. Chem. Phys., 2016, 18, 16281] on the experimental observation of a phase transition in a hydrogen bonded liquid manifesting in long range dipole-dipole interactions. The studied system, liquid water stressed by an electric field, exhibits collective oscillations brought about through spontaneous breakdown of symmetry. Raman spectroscopy identifies the primary excitation of the emergent phase as transverse optically active phonon-like sidebands that appear on the hydrogen bonded asymmetric stretch mode. The phase transition is observed throughout the entire volume of liquid. The system also exhibits a self-similarity relation between the scattered Raman intensity and the electric field strength which further supports the conclusion that collective behavior persists against thermal disruption. The experimental findings are discussed in terms of a quantum field theory for macroscopic quantum systems.

Non-equilibrium thermodynamics and collective vibrational modes of liquid water in an inhomogeneous electric field.

In this experiment liquid water is subject to an inhomogeneous electric field (∇(2)Ea≈ 10(10) V m(2)) using a high voltage (20 kV) point-plane electrode system. Using interferometry it was found that the application of a strong electric field gradient to water generates local changes in the refractive index of the liquid, polarizes the surface and creates a downward moving electro-convective jet. A maximum temperature difference of 1 °C is measured in the immediate vicinity of the point electrode. Raman spectroscopy performed on water reveals an enhancement of the vibrational collective modes (3250 cm(-1)) as well as an increase in the local mode (3490 cm(-1)) energy. This bimodal enhancement indicates that the spectral changes are not due to temperature changes. The intense field gradient thus establishes an excited subpopulation of vibrational oscillators far from thermal equilibrium. Delocalization of the collective vibrational mode spatially expands this excited population beyond the microscale. Hindered rotational freedom due to electric field pinning of molecular dipoles retards the heat flow and generates a chemical potential gradient. These changes are responsible for the observed changes in the refractive index and temperature. It is demonstrated that polar liquids can thus support local non-equilibrium thermodynamic transient states critical to biochemical and environmental processes.

Preparation of Free-Surface Hyperbolic Water Vortices.

Free surface vortices are present in industry in flow regulation, energy dissipation, and energy generation. Although investigated extensively, detailed experimental data regarding free surface vortices are lacking, particularly regarding the turbulence at the interface. The present paper reports on a special type of free surface vortex first proposed by Walter Schauberger in the 1960s that has an oxygen volumetric mass transfer coefficient exceeding the value of similar systems. This special type of vortex forms in a hyperbolic funnel. Different stable regimes can be stabilized with different hydraulic characteristics. Other advantages of this technology are its energy efficiency, simple design, and scalability. The flow in this hyperbolic funnel is characterized by strong turbulence and an increased surface area of the air-water interface. The local pressure strongly varies along the surface, resulting in a pronounced wavey air-water boundary layer. Due to the helical flow, these perturbations move inward, pulling the boundary layer with them. The resultant pressure gradient draws a certain air volume into the water vortex. The construction of the basic hyperbolic funnel setup and operational examples, including high-speed visualization for three different stable regimes, are presented in this work.

Quantitative measurement of density fluctuations with a full-field laser interferometric vibrometer.

ABSTRACT: Modern, lean and premixed gas turbine combustion concepts for low NOx emissions are prone to combustion instabilities. In a previous work it was shown that laser interferometric vibrometry (LIV) can be used to record global as well as local heat release fluctuations in swirl-stabilized premixed methane flames quantitatively, if other effects influencing density are small. In this work a newly developed camera-based full-field LIV system (CLIV) was applied to a lean, confined, premixed and swirl-stabilized methane flame under atmospheric conditions. Instead of time-consuming pointwise scanning of the flame, CLIV records full-field line-of-sight density fluctuations with high spatio-temporal resolution. With a recording rate of 200 kHz, CLIV enables the visualization of highly unsteady processes in fluid dynamics and combustion research. As an example for an unsteady process, the propagation of the flame front through a lean, premixed gas volume is visualized during an ignition process. A discussion of algorithms and assumptions necessary to calculate heat release oscillations from density oscillations is presented and applied to phase-averaged data recorded with CLIV for this type of flame. As reference, OH* chemiluminescence data were recorded simultaneously. While density gradients travelling with the flow are recorded by LIV and CLIV, chemiluminescence imaging will show nothing in the absence of chemical reaction. GRAPHIC ABSTRACT: a Time-averaged density gradient within the combustor in lateral direction. b Density fluctuations along line-of-sight 7 ms after ignition. c Phase-averaged and local heat release fluctuations at 225 Hz perturbation frequency.

Nuclear Magnetic Relaxation Mapping of Spin Relaxation in Electrically Stressed Glycerol.

This work discusses nuclear magnetic relaxation effects in glycerol subject to a strong electric field. The methods used are 1.5 T magnetic resonance imaging (MRI), referenced by 9.4 T nuclear magnetic resonance (NMR). While MRI allows a glycerol probe to be sampled with a high voltage (HV) of 16 kV applied to the probe, NMR provides precise molecular data from the sample, but the sample cannot be tested under HV. Using MRI, the recording of magnetic relaxation times was possible while HV was applied to the glycerol. NMR spectroscopy was used to confirm that MRI provides a reasonably accurate estimation of temperature. The applied HV was observed to have a negligible effect on the spin-lattice relaxation time T 1, which represents the energy release to the thermal bath or system enthalpy. In contrast to that, the spin-spin relaxation time T 2, which does represent the local entropy of the system, shows a lower response to temperature while the liquid is electrically stressed. These observations point toward a proton population in electrically stressed glycerol that is more mobile than that found in the bulk, an observation that is in agreement with previously published results for water.

A Quasi-Elastic Neutron Scattering Study of the Dynamics of Electrically Constrained Water.

We have measured the quasi-elastic neutron scattering (QENS) of an electrohydrodynamic liquid bridge formed between two beakers of pure water when a high voltage is applied, a setup allowing to investigate water under high-voltage without high currents. From this experiment two proton populations were distinguished: one consisting of protons strongly bound to oxygen atoms (immobile population, elastic component) and a second one of quasi-free protons (mobile population, inelastic component) both detected by QENS. The diffusion coefficient of the quasi-free protons was found to be D = (26 ± 10) × 10(-5) cm(2) s(-1) with a jump length lav ∼ 3 Å and an average residence time of τ0 = 0.55 ± 0.08 ps. The associated proton mobility in the proton channel of the bridge is ∼9.34 × 10(-7) m(2) V(-1) s(-1), twice as fast as diffusion-based proton mobility in bulk water. It also matches the so-called electrohydrodynamic or "apparent" charge mobility, an experimental quantity which so far has lacked molecular interpretation. These results further corroborate the proton channel model for liquid water under high voltage and give new insights into the molecular mechanisms behind electrohydrodynamic charge transport phenomena and delocalization of protons in liquid water.

The preparation of electrohydrodynamic bridges from polar dielectric liquids.

Horizontal and vertical liquid bridges are simple and powerful tools for exploring the interaction of high intensity electric fields (8-20 kV/cm) and polar dielectric liquids. These bridges are unique from capillary bridges in that they exhibit extensibility beyond a few millimeters, have complex bi-directional mass transfer patterns, and emit non-Planck infrared radiation. A number of common solvents can form such bridges as well as low conductivity solutions and colloidal suspensions. The macroscopic behavior is governed by electrohydrodynamics and provides a means of studying fluid flow phenomena without the presence of rigid walls. Prior to the onset of a liquid bridge several important phenomena can be observed including advancing meniscus height (electrowetting), bulk fluid circulation (the Sumoto effect), and the ejection of charged droplets (electrospray). The interaction between surface, polarization, and displacement forces can be directly examined by varying applied voltage and bridge length. The electric field, assisted by gravity, stabilizes the liquid bridge against Rayleigh-Plateau instabilities. Construction of basic apparatus for both vertical and horizontal orientation along with operational examples, including thermographic images, for three liquids (e.g., water, DMSO, and glycerol) is presented.