arXiv subjects

Hans-Jürgen Butt

Publications and source records attributed to Hans-Jürgen Butt.

At least 19 recordsLinked to original sources

arXiv2026

Drop Spray Electrification

Charge separation during the breakup of water drop has been recognized since the early studies of waterfall and spray electrification, yet the role of controlled drop fragmentation at structured liquid-repellent surfaces remains unclear. Here we show that water drops impacting superhydrophobic meshes generate charged secondary droplets as liquid penetrates and fragments through the mesh pores. By combining Faraday-cup charge measurements with high-speed imaging, we identify how the charge depends on the Weber number and on the pathway of spray formation. No measurable charge is detected below the penetration threshold. At low Weber numbers, recoil jet formation gives a high charge per unit spray mass, whereas at intermediate Weber numbers both recoil jets and impact-induced jets contribute to charging. At higher Weber numbers, pancake bouncing suppresses recoil jet formation, so charging is dominated by impact induced penetration and the total charge approaches a saturated value. We further show that smaller mesh pores enhance the charge-to-mass ratio and that conductive meshes provide stable charging under repeated impacts by dissipating residual surface charge. These findings provide design principles for superhydrophobic mesh platforms for spray charging and rain-driven energy harvesting.

physics.flu-dyn↗

arXiv2026

Mechanisms in Slide Electrification of Liquid and Frozen Drops on Hydrophobic Surfaces

The microscopic and fundamental origin of slide electrification, where droplets of water move across insulating surfaces accumulating and depositing electrical charges, is still debated. Charge transfer is often attributed to ion transfer at the receding contact line. However, it is still unclear whether ion transfer alone can fully account for the observed charge separation. We examined slide electrification of two polar, self-ionizing liquids (water, formamide) and two non-polar liquids (diiodomethane, bromonaphthalene). By cooling below the melting temperature, we were able to compare this process to tribocharging of the respective frozen components. Despite reduced ion mobility at sub-freezing temperatures, the frozen polar compounds continue to accumulate significant charge. Non-polar liquids exhibit lower charging (<25% of polar liquids) and nearly identical charging behaviour in both their liquid and frozen phases on five different substrates. Since non-polar liquids contain few free ions, these observations indicate an alternative charging mechanism, which could be electron transfer. Our findings suggest that slide electrification operates through at least two mechanisms, with the dominant charge transfer pathway shifting between ions and electron transfer depending on the electronegativity, phase, and temperature.

cond-mat.soft↗

arXiv2026

Pre-charging polymer surfaces enhances droplet mobility and electrification

Surface-bound electric charge on polymer materials can strongly influence droplet behaviour and solid-liquid charge transfer, but the mechanisms and the means to control these effects remain unclear. In this work, we systematically controlled the surface charge on polymer surfaces, including polytetrafluoroethylene (PTFE) and Nylon-66, by first neutralising the surfaces with an anti-static ion blower and then applying charge using an ion gun. We find that droplets pick up pre-deposited surface ions during the first wetting of the surface, and that the transferred charge directly correlates with the deposited charge encountered by the wetted area for moderate deposited densities (|σ_d |<40 μC/m2) independent of material properties. We also demonstrate that the deposited charge reduces contact angle and increases contact-line mobility in a manner consistent with an increase in effective solid surface energy. For higher surface charge densities, we observe instabilities such as droplet splitting or detachment. This work demonstrates an effective approach to control solid-liquid electrification, enabling amplification or suppression of surface charge and the directed manipulation of fluid motion on surfaces.

cond-mat.soft↗

arXiv2026

Polyelectrolyte adsorption at the solid-liquid interface favors receding contact line instability

Controlling the motion of non-Newtonian drops on surfaces is crucial for applications ranging from inkjet printing to biomedical devices and food processing. While the macroscopic behavior of viscoelastic drops sliding on tilted hydrophobic surfaces has been characterized, showing reduced velocities and elongation compared to Newtonian fluids, the underlying microscopic mechanisms remain poorly understood. To address this gap, we developed a high-speed, high-resolution reflection microscope that enables direct visualization of the contact line of sliding drops. We used water/soluble polyelectrolyte solutions based on polyacrylamide and let drops sliding on hydrophobic substrates composed of Teflon AF- and PDMS-coated glass slides. The substrate tilting angle was varied between 20° and 45°. We reveal how viscoelasticity influences the dynamics of the receding contact line and drop motion. Our experiments demonstrate that viscoelasticity can destabilize the receding contact line, triggering filament formation. This instability previously observed in the coating of thin viscoelastic films, is reported here for the first time in sliding drops. We further highlight the critical role of polymer charge in this process: while cationic and non-ionic polymers promote filament formation, anionic polymers do not, a difference we attribute to the distinct wetting properties of the solutions. In conclusion, we clarify the interplay between rheology, surface interactions, and drop dynamics.

cond-mat.soft↗

arXiv2026

How Spontaneous Electrowetting and Surface Charge affect Drop Motion

Water drops sliding on hydrophobic surfaces spontaneously separate charges at their rear. It is unclear how this charge separation affects the contact angles of a sliding drop. We slide grounded and insulated drops on hydrophobic surfaces at low capillary numbers (\leq 10^{-4}). We find that drop charge leads to spontaneous electrowetting, which decreases the contact angles. Additionally, the deposited charges lead to a surface charge effect and decrease the contact angle. Both phenomena compensate each other at the receding contact line, resulting in an insignificant change in the receding contact angle of a sliding drop.

physics.flu-dyn↗

arXiv2025

Stood-up drop to measure receding contact angles

The wetting behavior of drops on natural and industrial surfaces is determined by the advancing and receding contact angles. They are commonly measured by the sessile drop technique, also called goniometry, which doses liquid through a solid needle. Consequently, this method requires substantial drop volumes, long contact times, tends to be user-dependent, and is difficult to automate. Here, we propose the stood-up drop (SUD) technique as an alternative to measure receding contact angles. The method consists of depositing a liquid drop on a surface by a short liquid jet, at which it spreads radially forming a pancake-shaped film. Then the liquid retracts, forming a spherical cap drop shape (stood-up drop). At this quasi-equilibrium state, the contact angle ($θ_\text{SUD}$) closely resembles the receding contact angle measured by goniometry. Our method is suitable for a wide variety of surfaces from hydrophilic to hydrophobic, overcoming typical complications of goniometry such as needle-induced distortion of the drop shape, and it reduces user dependence. We delineate when the receding contact angle can be obtained by the stood-up method using Volume-of-Fluid (VoF) simulations that systematically vary viscosity, contact angle, and deposited drop volume. Finally, we provide simple scaling criteria to predict when the stood-up drop technique works.

physics.flu-dyn↗

arXiv2025

Three-phase contact line dynamics on moving fibers measured by X-ray holography

Wetting of solid surfaces by a liquid is important for many natural and industrial processes such as printing, painting and coating. However, a quantitative description of the dynamic receding and advancing contact angle is still debated, in particular for aqueous solutions. One reason for our lack of quantitative understanding is the limited spatial resolution of currently used optical methods. We therefore present a new approach to access the sub-microscopic region. We use X-ray phase contrast imaging to measure the dynamic receding contact angle on a moving glass fiber of 17 um diameter. The fiber was pulled out of a liquid bath which was filled with a mixture of glycerol and Milli-Q water. The dynamic receding contact angle decreased with increasing contact line velocity for all mixtures. In the holograms we achieved a resolution of 50 nm/pixel with a spatial error of 450 nm. This spatial error is due to an extended surface region of the fiber and the liquid surface in the holograms. Our results demonstrate the feasibility of X-ray holography as a method to investigate dynamic contact angle phenomena and thereby opening pathways to higher spatial and temporal resolution.

physics.chem-ph↗

arXiv2025

Surfactants Screen Slide Electrification

Water drops spontaneously accumulate charges when they move on hydrophobic dielectric surfaces by slide electrification. On the one hand, slide electrification generates electricity with possible applications on tiny devices. On the other hand, the potential of up to 1 KV generated by slide electrification alters wetting and drop motion. Therefore, it is important to know the factors that affect slide electrification. To find out how surfactants affect slide electrification, we measured drop charges of aqueous drops containing cationic CTAB, anionic SDS and neutral C8E3 sliding on different hydrophobic surfaces. The result is: addition of surfactant significantly reduces the spontaneous charging of moving water drops. Based on zeta potential measurements, confocal microscopy of deposited surface-active dyes and drop impact studies, we propose that several factors contribute to this suppression of charge separation: (1) Surfactants tend to lower the contact angles, which reduces charge separation. (2) Surfactant adsorption at the solid-liquid interface can reduce the density of primary ions, particularly for anionic surfactants. (3) Anionic and neutral surfactants are mostly transferred to the liquid-air interface at the rear of the sliding drop, retaining primary ions within the drop. (4) Deposited cationic surfactant directly reduces the charge of the drop.

cond-mat.soft↗

arXiv2024

Adaptive two capacitor model to describe slide electrification in moving water drops

Slide electrification is a spontaneous charge separation between a surface and a sliding drop. Here, we describe this effect in terms of a voltage generated at the three-phase contact line. This voltage moves charges between capacitors, one formed by the drop and one on the surface. By introducing an adaptation of the voltage upon water contact, we can model drop charge experiments on many surfaces, including more exotic ones with drop-rate dependent charge polarity. Thus, the adaptive two capacitor model enables new insights into the molecular details of the charge separation mechanism.

cond-mat.soft↗

arXiv2024

Chemical Physics of Controlled Wettability and Super Surfaces

Wetting phenomena are widespread in both natural and technological contexts. Despite the well-established nature of this scientific field and our extensive knowledge of its underlying principles, wetting remains a dynamic and vibrant area of study. It continues to pose fundamental questions while offering innovative avenues for controlling these phenomena to develop novel applications. By tailoring the wetting properties of surfaces, researchers and engineers can design materials with specific functionalities, such as self-cleaning surfaces, anti-fog coatings, and enhanced slipperiness. Recent years have witnessed significant advancements in wetting research, owing to the exquisite control achieved in surface topography and chemistry and to the development of novel experimental techniques. Additionally, simulations and theory have played a crucial role in these advancements. They provid the fundamental knowledge and quantitative tools to control wettability and design surfaces with enhanced properties. Given these recent breakthroughs, this special collection Chemical Physics of Controlled Wettability and Super Surfaces becomes particularly timely and significant. It serves as a platform to showcase some of the latest developments in the field of wetting. It highlights the exciting progress and potential applications in controlling wetting properties that are enabled by the synergy between theory, simulations, and experiments.

cond-mat.soft↗

arXiv2023

Durable, ultrathin, and antifouling polymer brush coating for efficient condensation heat transfer

Heat exchangers are made of metals because of their high heat conductivity and mechanical stability. Metal surfaces are inherently hydrophilic, leading to inefficient filmwise condensation. It is still a challenge to coat these metal surfaces with a durable, robust and thin hydrophobic layer, which is required for efficient dropwise condensation. Here, we report the non-structured and ultrathin (~6 nm) polydimethylsiloxane (PDMS) brushes on copper that sustain high-performing dropwise condensation in high supersaturation. Due to the flexible hydrophobic siloxane polymer chains, the coating has low resistance to drop sliding and excellent chemical stability. The PDMS brushes can sustain dropwise condensation for up to ~8 h during exposure to 111 °C saturated steam flowing at 3 m/s, with a 5-7 times higher heat transfer coefficient compared to filmwise condensation. The surface is self-cleaning and can reduce bacterial attachment by 99%. This low-cost, facile, fluorine-free, and scalable method is suitable for a great variety of condensation heat transfer applications.

cond-mat.mtrl-sci↗

arXiv2023

Experimental Study of Condensation of Water on Polydimethylsiloxane-Coated Copper Surfaces

Modification of surfaces to enable dropwise condensation is a promising approach for achieving high condensation rates. In this work, we present an experimental study on condensation of water on copper surfaces coated with an ultrathin, 5 nm - 10 nm thick polydimethylsiloxane (PDMS) layer. This hydrophobic coating possesses a very low thermal resistance, which in combination with copper substrate enables achieving high condensation rates in heat transfer applications. The PDMS-coated copper substrates have been fabricated with a newly developed method, which involves turning, sanding, polishing, oxidation, and polymer coating steps. The measured static contact angle was 110°, and a the contact angle hysteresis was 2°. The achieved very low hysteresis is advantageous for promoting dropwise condensation. The surface showed no ageing effects during 100 repetitions of advancing and receding contact angle (ARCA) measurements. Condensation heat transfer on uncoated and PDMS-coated copper surfaces surfaces has been studied experimentally in a saturated water vapor atmosphere at 60°C. An enhancement factor for heat flux and heat transfer coefficient of up to 1.6 was found on PDMS-coated copper surfaces compared to uncoated surfaces, which decreased to 1.1 on second and third day of condensation operation. Images of the condensation surface were recorded while conducting condensation experiments and post processed to evaluate drop departure diameter and frequency of drop sweeping events. It has been shown that the behavior of the heat transfer coefficient correlates with the frequency of the sweeping events.

physics.flu-dyn↗

arXiv2023

How charges separate when surfaces are dewetted

Charge separation at moving three-phase contact lines is observed in nature as well as technological processes. Despite the growing number of experimental investigations in recent years, the physical mechanism behind the charging remains obscure. Here we identify the origin of charge separation as the dewetting of the bound surface charge within the electric double layer by the receding contact line. This charge depends strongly on the local electric double layer structure close to the contact line, which is affected by the gas-liquid interface and the internal flow of the liquid. We summarize the charge separation mechanism in an analytical model that captures parametric dependencies in agreement with our experiments and numerical simulations. Charge separation increases with increasing contact angle and decreases with increasing dewetting velocity. Our findings reveal the universal mechanism of charge separation at receding contact lines, relevant to many dynamic wetting scenarios, and provide a theoretical foundation for both fundamental questions, like contact angle hysteresis, and practical applications.

cond-mat.soft↗

arXiv2023

Surface charge deposition by moving drops reduces contact angles

Slide electrification - the spontaneous charge separation by sliding water drops - can lead to an electrostatic potential of 1 kV and change drop motion substantially. To find out, how slide electrification influences the contact angles of moving drops, we analyzed the dynamic contact angles of aqueous drops sliding down tilted plates with insulated surfaces, grounded surfaces, and while grounding the drop. The observed decrease in dynamic contact angles at different salt concentrations is attributed to two effects: An electrocapillary reduction of contact angles caused by drop charging and a change in the free surface energy of the solid due to surface charging.

cond-mat.soft↗

arXiv2023

Charging of dielectric surfaces in contact with aqueous electrolyte -- the influence of CO$_2$

The charge state of dielectric surfaces in aqueous environments is of fundamental and technological importance. Here, we study the influence of dissolved molecular CO$_2$ on the charging of three, chemically different surfaces (SiO$_2$, Polystyrene, Perfluorooctadecyltrichlorosilane). We determine their charge state from electrokinetic experiments. We compare an ideal, CO$_2$-free reference system to a system equilibrated against ambient CO$_2$ conditions. In the reference system, the salt-dependence is weakened for SiO$_2$ and inverted for the organic surfaces. We show that screening and pH-driven charge regulation alone cannot explain the observed effects. As additional cause, we tentatively suggest dielectric regulation of surface charges due to a diffusively adsorbed thin layer of molecular CO$_2$. The formation of such a dynamic layer even at the hydrophilic and partially ionized silica surfaces is supported by a minimal theoretical model and results from molecular simulations.

cond-mat.soft↗

arXiv2021

Enhancing condensation on soft substrates through bulk lubricant infusion

Soft substrates such as polydimethylsiloxane (PDMS) enhance droplet nucleation during the condensation of water vapour, because their deformability inherently reduces the energetic threshold for heterogeneous nucleation relative to rigid substrates. However, this enhanced droplet nucleation is counteracted later in the condensation cycle, when the viscoelastic dissipation inhibits condensate droplet shedding from the substrate. Here, we show that bulk lubricant infusion in the soft substrate is a potential pathway for overcoming this limitation. We demonstrate that even 5% bulk lubricant infusion in PDMS reduces viscoelastic dissipation in the substrate by more than 30 times and more than doubles the droplet nucleation density. We correlate the droplet nucleation and growth rate with the material properties controlled by design, i.e. the fraction and composition of uncrosslinked chains, shear modulus, and viscoelastic dissipation. Through in-situ, microscale condensation on the substrates, we show that the increase in nucleation density and reduction in pre-coalescence droplet growth rate is insensitive to the percentage of lubricant in PDMS. Our results indicate the presence of a lubricant layer on the substrate surface that cloaks the growing condensate droplets. We visualize the cloaking effect and show that lubricant infusion in PDMS significantly increases the rate of cloaking compared to PDMS without any lubricant infusion. Finally, we show that the overall enhanced condensation due to bulk lubricant infusion in PDMS leads to more than 40% increase in dewing on the substrate.

cond-mat.soft↗

arXiv2021

Flow profiles near receding three--phase contact lines: Influence of surfactants

The dynamics of wetting and dewetting is largely determined by the velocity field near the contact lines. For water drops it has been observed that adding surfactant decreases the dynamic receding contact angle even at a concentration much lower than the critical micelle concentration (CMC). To better understand why surfactants have such a drastic effect on drop dynamics, we constructed a dedicated a setup on an inverted microscope, in which an aqueous drop is held stationary while the transparent substrate is moved horizontally. Using astigmatism particle tracking velocimetry, we track the 3D displacement of the tracer particles in the flow. We study how surfactants alter the flow dynamics near the receding contact line of a moving drop for capillary numbers in the order of $10^{-6}$. Even for surfactant concentrations $c$ far below the critical micelle concentration ($c \ll$ CMC) Marangoni stresses change the flow drastically. We discuss our results first in a 2D model that considers advective and diffusive surfactant transport and deduce estimates of the magnitude and scaling of the Marangoni stress from this. Modeling and experiment agree that a tiny gradient in surface tension of a few $μN \, m^{-1}$ is enough to alter the flow profile significantly. The variation of the Marangoni stress with the distance from the contact line suggests that the 2D advection-diffusion model has to be extended to a full 3D model. The effect is ubiquitous, since surfactant is present in many technical and natural dewetting processes either deliberately or as contamination.

physics.flu-dyn↗

arXiv2019

Versatile high-speed confocal microscopy using a single laser beam

We present a new flexible high speed laser scanning confocal microscope and its extension by an astigmatism particle tracking device (APTV). Many standard confocal microscopes use either a single laser beam to scan the sample at relatively low overall frame rate, or many laser beam to simultaneously scan the sample and achieve a high overall frame rate. Single-laser-beam confocal microscope often use a point detector to acquire the image. To achieve high overall frame rates, we use, next to the standard 2D probe scanning unit, a second 2D scan unit projecting the image directly on a 2D CCD-sensor (re-scan configuration). Using only a single laser beam eliminates cross-talk and leads to an imaging quality that is independent of the frame rate with a lateral resolution of 0.235\unit{μm}. The design described here is suitable for high frame rate, i.e., for frame rates well above video rate (full frame) up to a line rate of 32kHz. The dwell time of the laser focus on any spot in the sample (122ns) is significantly shorter than in standard confocal microscopes (in the order of milli or microseconds). This short dwell time reduces phototoxicity and bleaching of fluorescent molecules. The new design opens further flexibility and facilitates coupling to other optical methods. The setup can easily be extended by an APTV device to measure three dimensional dynamics while being able to show high resolution confocal structures. Thus one can use the high resolution confocal information synchronized with an APTV dataset.

physics.optics↗