Stephan Gekle

University of Bayreuth, Bayreuth, Bavaria, Germany

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Publications (32)111.09 Total impact

  • Klaus F Rinne, Stephan Gekle, Roland R Netz
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    ABSTRACT: Using extensive equilibrium molecular dynamics simulations we determine the dielectric spectra of aqueous solutions of NaF, NaCl, NaBr, and NaI. The ion-specific and concentration-dependent shifts of the static dielectric constants and the dielectric relaxation times match experimental results very well, which serves as a validation of the classical and non-polarizable ionic force fields used. The purely ionic contribution to the dielectric response is negligible, but determines the conductivity of the salt solutions. The ion-water cross correlation contribution is negative and reduces the total dielectric response by about 5%-10% for 1 M solutions. The dominating water dielectric response is decomposed into different water solvation shells and ion-pair configurations, by this the spectral blue shift and the dielectric decrement of salt solutions with increasing salt concentration is demonstrated to be primarily caused by first-solvation shell water. With rising salt concentration the simulated spectra show more pronounced deviations from a single-Debye form and can be well described by a Cole-Cole fit, in quantitative agreement with experiments. Our spectral decomposition into ionic and different water solvation shell contributions does not render the individual contributions more Debye-like, this suggests the non-Debye-like character of the dielectric spectra of salt solutions not to be due to the superposition of different elementary relaxation processes with different relaxation times. Rather, the non-Debye-like character is likely to be an inherent spectral signature of solvation water around ions.
    The Journal of Chemical Physics 12/2014; 141(21):214502. DOI:10.1063/1.4901927 · 3.12 Impact Factor
  • Klaus F Rinne, Stephan Gekle, Roland R Netz
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    ABSTRACT: Recent femtosecond-resolved spectroscopy experiments demonstrate the single-water orientational dynamics in the first solvation shell around monatomic ions to be slowed down. In contrast, dielectric spectroscopy experiments exhibit a blue shift of the water dielectric relaxation time with rising salt concentration, indicative of faster water dynamics. Using molecular dynamics simulations employing nonpolarizable and thermodynamically optimized ion force fields, we reproduce both experimental trends and resolve these conflicting experimental findings by the simultaneous analysis of single-water and collective-water dynamics in the ion solvation shells. While the single-molecule reorientational dynamics of first solvation shell water around ions indeed slows down, the collective dynamics, which furnishes the dominant contribution to the dielectric response, accelerates. This collective acceleration is rationalized by a dramatically decreasing water cooperativity around ions when compared to bulk water, quantified by the Kirkwood dielectric enhancement factor. The static dielectric decrement of salt solutions is thus reinterpreted as a dielectric structure breaking rather than a water alignment effect. Both the dielectric blue shift and the dielectric decrement become stronger with increasing anion size, meaning larger halide ions such as iodide are more efficient dielectric structure breakers than small halide ions such as fluoride.
    The Journal of Physical Chemistry A 12/2014; 118(50). DOI:10.1021/jp5066874 · 2.78 Impact Factor
  • Stephan Gekle, Roland R Netz
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    ABSTRACT: Radio-frequency (RF) electromagnetic fields are readily absorbed in biological matter and lead to dielectric heating. To understand how RF radiation interacts with macromolecular structures and possibly influences biological function, a quantitative description of dielectric absorption and heating at nanometer resolution beyond the usual effective medium approach is crucial. We report an exemplary multiscale theoretical study for biomembranes that combines (i) atomistic simulations for the spatially resolved absorption spectrum at a single planar DPPC lipid bilayer immersed in water, (ii) calculation of the electric field distribution in planar and spherical cell models, and (iii) prediction of the nanometer resolved temperature profiles under steady RF radiation. Our atomistic simulations show that the only 2 nm thick lipid hydration layer strongly absorbs in a wide RF range between 10 MHz and 100 GHz. The absorption strength, however, strongly depends on the direction of the incident wave. This requires modeling of the electric field distribution using tensorial dielectric spectral functions. For a spherical cell model, we find a strongly enhanced RF absorption on an equatorial ring, which gives rise to temperature gradients inside a single cell under radiation. Although absolute temperature elevation is small under conditions of typical telecommunication usage, our study points to hitherto neglected temperature gradient effects and allows thermal RF effects to be predicted on an atomistically resolved level. In addition to a refined physiological risk assessment of RF fields, technological applications for controlling temperature profiles in nanodevices are possible.
    The Journal of Physical Chemistry B 04/2014; 118(18). DOI:10.1021/jp501562p · 3.38 Impact Factor
  • Yann von Hansen, Stephan Gekle, Roland R Netz
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    ABSTRACT: The diffusional water dynamics in the hydration layer of a dipalmitoylphosphatidylcholine bilayer is studied using molecular dynamics simulations. By mapping the perpendicular water motion on the ordinary diffusion equation, we disentangle free energetic and friction effects and show that perpendicular diffusion is strongly reduced. The lateral water motion exhibits anomalous diffusion up to several nanoseconds and is characterized by even further decreased diffusion coefficients, which by comparison with coarse-grained simulations are explained by the transient corrugated effective free energy landscape imposed by the lipids. This is in contrast to homogenous surfaces, where boundary hydrodynamic theory quantitatively predicts the anisotropy of water diffusion.
    Physical Review Letters 09/2013; 111(11):118103. DOI:10.1103/PhysRevLett.111.118103 · 7.73 Impact Factor
  • Stephan Gekle, Axel Arnold
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    ABSTRACT: A Comment on the Letter by H. Zhu et al., Phys. Rev. Lett. 109, 107801 (2012). The authors of the Letter offer a Reply.
    Physical Review Letters 08/2013; 111(8):089801. DOI:10.1103/PhysRevLett.111.089801 · 7.73 Impact Factor
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    ABSTRACT: We experimentally study the airflow in a collapsing cavity created by the impact of a circular disk on a water surface. We measure the air velocity in the collapsing neck in two ways: Directly, by means of employing particle image velocimetry of smoke injected into the cavity and indirectly, by determining the time rate of change of the volume of the cavity at pinch-off and deducing the air flow in the neck under the assumption that the air is incompressible. We compare our experiments to boundary integral simulations and show that close to the moment of pinch-off, compressibility of the air starts to play a crucial role in the behavior of the cavity. Finally, we measure how the air flow rate at pinch-off depends on the Froude number and explain the observed dependence using a theoretical model of the cavity collapse.
    Physics of Fluids 02/2013; 25(3). DOI:10.1063/1.4794125 · 2.04 Impact Factor
  • Stephan Gekle, Roland R Netz
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    ABSTRACT: Proteins, molecules, and macromolecular assemblies in water are surrounded by a nanometer-sized hydration layer with properties very different from bulk water. Here, we use classical molecular dynamics simulations to study the dielectric response of hydration water next to hydrophobic and hydrophilic planar surfaces. We find the interfacial dielectric absorption of water to be strongly anisotropic: compared to bulk water, which shows a broad dielectric absorption maximum around 15 GHz in the imaginary part of the dielectric function, the absorption for electric fields parallel to the surface is of similar strength and shows a slight redshift, while for perpendicular electric fields it is strongly attenuated and blueshifted. This anisotropy is generic for hydrophobic and hydrophilic surfaces. From our spatially resolved dielectric functions and a modified Maxwell-Garnett theory that accounts for anisotropic hydration layers around spherical particles, the dielectric absorption of solutions of organic molecules and micelles is derived to exhibit the experimentally known attenuation in combination with a redshift. These two features are traced back to the subtle interplay of interfacial depolarization effects and the dielectric anisotropy in the hydration layer. By a detailed analysis of the individual water molecule dynamics the perpendicular blueshift is shown not to be linked to accelerated water reorientation, but rather to dielectric boundary effects. Carefully conducted angularly resolved experiments at planar aqueous interfaces will be able to resolve this dielectric anisotropy and thus to confirm the subtle connection between spectral absorption features and the molecular water dynamics in hydration layers.
    The Journal of Chemical Physics 09/2012; 137(10):104704. DOI:10.1063/1.4749380 · 3.12 Impact Factor
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    ABSTRACT: The axisymmetric collapse of a cylindrical air cavity in water follows a universal power law with logarithmic corrections. Nonetheless, it has been suggested that the introduction of a small azimuthal disturbance induces a long term memory effect, reflecting in oscillations which are no longer universal but remember the initial condition. In this work, we create non-axisymmetric air cavities by driving a metal disc through an initially-quiescent water surface and observe their subsequent gravity-induced collapse. The cavities are characterized by azimuthal harmonic disturbances with a single mode number $m$ and amplitude $a_m$. For small initial distortion amplitude (1 or 2% of the mean disc radius), the cavity walls oscillate linearly during collapse, with nearly constant amplitude and increasing frequency. As the amplitude is increased, higher harmonics are triggered in the oscillations and we observe more complex pinch-off modes. For small amplitude disturbances we compare our experimental results with the model for the amplitude of the oscillations by Schmidt et al. (2009) and the model for the collapse of an axisymmetric impact-created cavity previously proposed by Bergmann et al. (2009b). By combining these two models we can reconstruct the three-dimensional shape of the cavity at any time before pinch-off.
    Journal of Fluid Mechanics 05/2012; 701:40-58. DOI:10.1017/jfm.2012.130 · 2.29 Impact Factor
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    ABSTRACT: We derive the theoretical framework to calculate the dielectric response tensor and determine its components for water adjacent to hydrophilic and hydrophobic surfaces using molecular dynamics simulations. For the nonpolarizable water model used, linear response theory is found to be applicable up to an external perpendicular field strength of ∼2 V/nm, which is well beyond the experimental dielectric breakdown threshold. The dipole contribution dominates the dielectric response parallel to the interface, whereas for the perpendicular component it is essential to keep the quadrupole and octupole terms. Including the space-dependent dielectric function in a mean-field description of the ion distribution at a single charged interface, we reproduce experimental values of the interfacial capacitance. At the same time, the dielectric function decreases the electrostatic part of the disjoining pressure between two charged surfaces, unlike previously thought. The difference in interfacial polarizability between hydrophilic and hydrophobic surfaces can be quantized in terms of the dielectric dividing surface. Using the dielectric dividing surface and the Gibbs dividing surface positions to estimate the free energy of a single ion close to an interface, ion-specific adsorption effects are found to be more pronounced at hydrophobic surfaces than at hydrophilic surfaces, in agreement with experimental trends.
    Langmuir 03/2012; 28(20):7679-94. DOI:10.1021/la2051564 · 4.38 Impact Factor
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    ABSTRACT: Using molecular dynamics simulations we demonstrate pumping of water through a carbon nanotube by time-dependent electric fields. The fields are generated by electrodes with oscillating charges in a broad gigahertz frequency range that are attached laterally to the tube. The key ingredient is a phase shift between the electrodes to break the spatiotemporal symmetry. A microscopic theory based on a polarization-dragging mechanism accounts quantitatively for our numerical findings.
    Nano Letters 03/2012; 12(4):1780-3. DOI:10.1021/nl203614t · 12.94 Impact Factor
  • Stephan Gekle, José Manuel Gordillo
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    ABSTRACT: We present a multiscale approach to simulate the impact of a solid object on a liquid surface: upon impact a thin liquid sheet is thrown upwards all around the rim of the impactor while in its wake a large surface cavity forms. Under the influence of hydrostatic pressure the cavity immediately starts to collapse and eventually closes in a single point from which a thin, needle-like jet is ejected. Existing numerical treatments of liquid impact either consider the surrounding air as an incompressible fluid or neglect air effects altogether. In contrast, our approach couples a boundary-integral method for the liquid with a Roe scheme for the gas domain and is thus able to handle the fully \emph{compressible} gas stream that is pushed out of the collapsing impact cavity. Taking into account air compressibility is crucial, since, as we show in this work, the impact crater collapses so violently that the air flow through the cavity neck attains supersonic velocities already at cavity diameters larger than 1 mm. Our computational results are validated through corresponding experimental data.
    International Journal for Numerical Methods in Fluids 12/2011; 67(11):1456-1469. DOI:10.1002/fld.2426 · 1.33 Impact Factor
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    ABSTRACT: The framework for deriving tensorial interfacial dielectric profiles from bound charge distributions is established and applied to molecular dynamics simulations of water at hydrophobic and hydrophilic surfaces. In conjunction with a modified Poisson-Boltzmann equation, the trend of experimental double-layer capacitances is well reproduced. We show that the apparent Stern layer can be understood in terms of the dielectric profile of pure water.
    Physical Review Letters 10/2011; 107(16):166102. DOI:10.1103/PhysRevLett.107.166102 · 7.73 Impact Factor
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    ABSTRACT: The axisymmetric collapse of a cylindrical air cavity in water follows a universal power law with logarithmic corrections. Nonetheless, it has been suggested that the introduction of a small azimuthal disturbance induces a long term memory effect, reflecting in oscillations which are no longer universal but remember the initial condition. In this work, we create non-axisymmetric air cavities by driving a metal disc through an initially-quiescent water surface and observe their subsequent gravity-induced collapse. The cavities are characterized by azimuthal harmonic disturbances with a single mode number $m$ and amplitude $a_m$. For small initial distortion amplitude (1 or 2% of the mean disc radius), the cavity walls oscillate linearly during collapse, with nearly constant amplitude and increasing frequency. As the amplitude is increased, higher harmonics are triggered in the oscillations and we observe more complex pinch-off modes. For small amplitude disturbances we compare our experimental results with the model for the amplitude of the oscillations by Schmidt et al. (2009) and the model for the collapse of an axisymmetric impact-created cavity previously proposed by Bergmann et al. (2009b). By combining these two models we can reconstruct the three-dimensional shape of the cavity at any time before pinch-off.
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    Physics of Fluids 09/2011; 23(9). DOI:10.1063/1.3640021 · 2.04 Impact Factor
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    ABSTRACT: Discharging a liquid from a nozzle at sufficient large velocity leads to a continuous jet that due to capillary forces breaks up into droplets. Here we investigate the formation of microdroplets from the breakup of micron-sized jets with ultra high-speed imaging. The diminutive size of the jet implies a fast breakup time scale $\tau_\mathrm{c} = \sqrt{\rho r^3 / \gamma}$ of the order of 100\,ns{}, and requires imaging at 14 million frames per second. We directly compare these experiments with a numerical lubrication approximation model that incorporates inertia, surface tension, and viscosity [Eggers and Dupont, J. Fluid Mech. 262, 205 (1994); Shi, Brenner, and Nagel, Science 265, 219 (1994)]. The lubrication model allows to efficiently explore the parameter space to investigate the effect of jet velocity and liquid viscosity on the formation of satellite droplets. In the phase diagram we identify regions where the formation of satellite droplets is suppressed. We compare the shape of the droplet at pinch-off between the lubrication approximation model and a boundary integral (BI) calculation, showing deviations at the final moment of the pinch-off. Inspite of this discrepancy, the results on pinch-off times and droplet and satellite droplet velocity obtained from the lubrication approximation agree with the high-speed imaging results.
    Physics of Fluids 11/2010; 22(12). DOI:10.1063/1.3524533 · 2.04 Impact Factor
  • J. M. Gordillo, Stephan Gekle
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    ABSTRACT: The capillary breakup of the high-speed Worthington jets ejected after a cavity collapse in water occurs due to the high-Reynolds-number version of the capillary end-pinching mechanism first described, in the creeping flow limit, by Stone & Leal (J. Fluid Mech., vol. 198, 1989, p. 399). Using potential flow numerical simulations and theory, we find that the resulting drop ejection process does not depend on external noise and can be described as a function of a single dimensionless parameter, WeS = ρ R30S20/σ, which expresses the ratio of the capillary time to the inverse of the local strain rate, S0. Here, ρ and σ indicate the liquid density and the interfacial tension coefficient, respectively, and R0 is the initial radius of the jet. Our physical arguments predict the dimensionless size of the drops to scale as Ddrop/R0 ~ We−1/7S and the dimensionless time to break up as TS0 ~ We2/7S. These theoretical predictions are in good agreement with the numerical results
    Journal of Fluid Mechanics 11/2010; 663:331-346. DOI:10.1017/S0022112010003538 · 2.29 Impact Factor
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    Stephan Gekle, J. M. Gordillo
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    ABSTRACT: Helped by the careful analysis of their experimental data, Worthington (1897) described roughly the mechanism underlying the formation of high-speed jets ejected after the impact of an axisymmetric solid on a liquid-air interface. In this work we combine detailed boundary-integral simulations with analytical modeling to describe the formation and break-up of such Worthington jets in two common physical systems: the impact of a circular disc on a liquid surface and the release of air bubbles from an underwater nozzle. We first show that the jet base dynamics can be predicted for both systems using our earlier model in Gekle, Gordillo, van der Meer and Lohse. Phys. Rev. Lett. 102 (2009). Nevertheless, our main point here is to present a model which allows us to accurately predict the shape of the entire jet. Good agreement with numerics and some experimental data is found. Moreover, we find that, contrarily to the capillary breakup of liquid cylinders in vacuum studied by Rayleigh, the breakup of stretched liquid jets at high values of both Weber and Reynolds numbers is not triggered by the growth of perturbations coming from an external source of noise. Instead, the jet breaks up due to the capillary deceleration of the liquid at the tip which produces a corrugation to the jet shape. This perturbation, which is self-induced by the flow, will grow in time promoted by a capillary mechanism. We are able to predict the exact shape evolution of Worthington jets ejected after the impact of a solid object - including the size of small droplets ejected from the tip due to a surface-tension driven instability - using as the single input parameters the minimum radius of the cavity and the flow field before the jet emerges.
    Journal of Fluid Mechanics 11/2010; 663:293-330. DOI:10.1017/S0022112010003526 · 2.29 Impact Factor
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    ABSTRACT: A round disk with a harmonic disturbance impacts on a water surface and creates a non-axisymmetric cavity which collapses under the influence of hydrostatic pressure. We use disks deformed with mode m=2 to m=6. For all mode numbers we find clear evidence for a phase inversion of the cavity wall during the collapse. We present a fluid dynamics video showing high speed imaging of different modes, pointing out the characteristic features during collapse.
    Physics of Fluids 09/2010; 22(9). DOI:10.1063/1.3481432 · 2.04 Impact Factor
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    ABSTRACT: A solid object impacting on liquid creates a liquid jet due to the collapse of the impact cavity. Using visualization experiments with smoke particles and multiscale simulations, we show that in addition, a high-speed air jet is pushed out of the cavity. Despite an impact velocity of only 1 m/s, this air jet attains supersonic speeds already when the cavity is slightly larger than 1 mm in diameter. The structure of the air flow closely resembles that of compressible flow through a nozzle-with the key difference that here the "nozzle" is a liquid cavity shrinking rapidly in time.
    Physical Review Letters 01/2010; 104(2):024501. DOI:10.1103/PhysRevLett.104.024501 · 7.73 Impact Factor
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    ABSTRACT: When an object impacts on a water surface a sizeable cavity is formed below the surface which subsequently collapses due to hydrostatic pressure. The surrounding air is first sucked into the expanding cavity while at a later stage it is squeezed out of the - then shrinking - cavity. We measure this air flow using high-speed imaging of fine smoke particles. Numerical simulations combining a boundary-integral method with a fully compressible Euler solver reveal the intricate structure of the gas dynamics. Despite an impact velocity of merely 1 m/s and a cavity overpressure of only 0.02 atmospheres the air flow is shown to attain supersonic speeds. Consequently, there are significant effects of this air flow close to pinch-off which can be observed consistently in experiment and numerics: (i) the cavity wall is not smoothly curved but exhibits a kink and (ii) the cavity neck is pushed upwards.

Publication Stats

373 Citations
111.09 Total Impact Points

Institutions

  • 2013–2014
    • University of Bayreuth
      • Institute of Physics
      Bayreuth, Bavaria, Germany
  • 2011–2013
    • University of Technology Munich
      • Faculty of Physics
      München, Bavaria, Germany
  • 2007–2012
    • Universiteit Twente
      • Group of Physics of Fluids
      Enschede, Overijssel, Netherlands
  • 2006–2007
    • Universität Stuttgart
      Stuttgart, Baden-Württemberg, Germany