Dynamic Dewetting: Designing and Breaking Novel Morphologies of Liquid Films

Lead Research Organisation: University of Edinburgh
Department Name: Sch of Engineering

Abstract

When a small droplet is deposited on a smooth surface it spreads across the surface until it reaches an equilibrium droplet shape or until it becomes a film. This allows the dynamic wetting process to be studied at a fundamental level enabling the fluid mechanics of contact line motion to be understood. This understanding is important in many industrial processes, such as printing. However, often a process starts with a liquid film, rather than a droplet, and a change of the environment or some other parameter, can initiate a process of de-wetting, i.e. the recoil or break up of a film on a surface into one or more droplets. The initial film state and its de-wetting from a surface are important for industrial processes, such as spin coated films used in lithography, painting/coatings, printing, heat exchangers, etc. One difficulty in understanding the de-wetting is that it is extremely challenging to initiate the breakup of a film of liquid on a surface in a controlled manner that leads to an ideal droplet state. Dewetting usually leads to a mixture of droplets and puddles making it difficult to study the dynamics of the process or to control the final droplet state. In a recent paper (Science Advances, 2016) we showed a new method using a non-uniform electric field to force a liquid to wet a non-wetting surface. By quenching the electric field, a controlled dewetting into a single droplet state can then be initiated.

In this project, we use electric-field induced film formation to study non-naturally occurring film morphologies (e.g. triangular, square and ring droplets) and their de-wetting dynamics into single droplets in a manner, which has never previously been possible. We investigate liquid-in-liquid systems with order of magnitude contrasts in viscosity ratios (from droplets-in-air to liquids-in-liquids to bubbles-in-liquids) thereby elucidating the fundamentals of the fluid mechanics of contact line motion. We also investigate the combination of individually programmable film morphologies into fully programmable arrays of wetting patterns. An ability to finely control liquid films has potential for industrial applications from printing to displays. Finally, we establish a new concept of electric field stabilised surface-localised 2D emulsions where the arrays of droplets or bubbles can be detached from the surface and reattached in a controlled manner.

Planned Impact

(1) Knowledge and Techniques
Being able to reversibly induce a liquid film on a non-wetting surface using a voltage will establish a technique with broad applicability across a range of industrial sectors. This ability has relevance to coatings, films, adhesion and icing properties of surfaces, which can be modified by altering the wetting properties of a surface. For example, one industrial process of interest to one of our collaborators, Huntsman Ltd, is the release of objects from moulds without using a barrier release agent.

Our techniques also have greater flexibility than simply controlling wetting globally across an entire surface. Designing individual shaped areas to become wetting on the application of a voltage extends the potential industrial applications to those that require specific patterns, e.g. printing. Moreover, with the ability for reversible switching of these shaped areas between wetting states, the applicability potentially extends to displays. This ability is similar to electrowetting, which has been the basis for spin-out companies for displays, liquid lenses and digital microfluidics (e.g. Liquavista - now an Amazon company, Varioptic, and Advanced Liquid Logic - now part of Affymetrix).

Beyond the droplet-liquid film control techniques, the project also develops a method to reversibly induce bubble-gas film transitions and to control the position and motion of bubbles and arrays of bubbles along surfaces. Bubble and gas film formation during heat transfer creates an insulating barrier and so is an important industrial problem. The knowledge and techniques developed may inform industrial processes where nucleate boiling and critical heat flux are important.

(2) Economic Impact
This project is at Technology Readiness Level (TRL) 1 generating basic knowledge and developing new techniques. It combines ideas on liquid dielectrophoresis with ideas on surface patterning of wettability and the dynamics of moving contact lines and the hydrodynamics of internal and external flows in wedges and corners. The ability to voltage controllably pattern wettability is a new platform technology. The principles are scalable across large surface areas and the experimental work is fundamental, but includes a scoping element to enable future application oriented projects at lower TRLs. This project may also enable the re-engineering of existing processes (e.g. printing, optics, electronic paper and displays). Ultimately, it will generate enabling knowledge with the potential for high value disruptive technology fundamental to UK economic success.

Two industrial research laboratory collaborators are providing advice on leveraging industrial benefits. These companies have industrial networks and supply chains providing a wider understanding of potential commercial applications. The international basis of these companies means new techniques developed within the UK could have global relevance. Intellectual property will be protected by Collaborative Research Agreements and Invention Disclosures. Annual IPR reviews with transfer to industry will be supported by a Business Development Manager using patents and licences. As appropriate, demonstrator or industrial R&D projects may be initiated.

(3) People Pipeline
The UK skills base would benefit from the training of two multidisciplinary postdocs having skills relevant to high value manufacturing due to the project including work in (i) heat/mass transfer (bubbles/gas films), (ii) instrumentation/measurement, (iii) test-rig construction/operation, (iv) microfabrication/cleanrooms (v) computational modelling. They will also have received public communication training and taken part in our Nature's Raincoats Outreach (http://www.naturesraincoats.com/). Undergraduate summer work placements will promote interest in research thereby helping to ensure a continuing pipeline of future PhD students.

Publications

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Ruiz-Gutiérrez É (2021) Lattice Boltzmann Simulations of Multiphase Dielectric Fluids. in Langmuir : the ACS journal of surfaces and colloids

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Ruiz-Gutiérrez É (2022) Dielectrowetting on curved surfaces in Applied Physics Letters

 
Description The fundamental aim of this project was to investigate and control the de-wetting of liquids on surfaces with patterned and switchable regions of wettability in fluid-fluid systems of widely differing viscosity and density contrasts ranging from liquid-in-air to liquid-in-liquid and air-in-liquid systems. We have produced key findings of interest in our studies of all three of these systems.

1. Liquid in air - Exploration of the dewetting and stability of liquid films of non-circular initial morphologies in air: We used electrostatic forces to create a rectangular shaped spread film of a liquid on a normally liquid repellent flat solid surface. We demonstrated the "dewetting" of this film in which the liquid retracts and changes shape after being released (i.e. we switch the electrostatic forces off) and evolves to become a ball shape ("spherical cap shape") sitting proud on the surface. We found that if we reduce the magnitude of the electrostatic forces, rather than completely removing them, this allowed us to program the degree of repellency of the solid surface as the film retracted and hence we could voltage-select the final contact angle and height of the spherical cap. We found excellent agreement between our experimental prediction of the functional dependence of the retraction timescale on the final contact angle with the theoretically expected scaling, for a wide range of voltage-selected final contact angles. We further demonstrated "dewetting" from square, rectangle and ring shaped films. For example, we showed repeatable switching between a ring shaped film of an electrically insulating liquid and patterns of droplets of well-defined dimensions confined to a ring geometry. We demonstrated here how our programming of the degree of repellancy of the solid surface as the film retracted could select the final number of droplets into which the ring breaks up, between 1 and 7 droplets.

2. Liquid in liquid - Exploration of the dewetting of a liquid film immersed in a second immiscible liquid: We used electrostatic forces to create a disk-shaped spread film of a liquid - liquid 1 - on a liquid repellent flat solid surface, and again demonstrated the "dewetting" of this film of liquid 1 initiated by us switching off the electrostatic forces. Intuitively you might expect that the more repellent the surface is to liquid 1, then the higher the speed with which the film retracts and changes into a ball shape. However, when liquid 1 is immersed in liquid 2, we observed something counter-intuitive. We performed experiments covering five decades of the viscosity of the outer liquid 2 as a ratio of the viscosity of liquid 1. At small viscosity ratio, dewetting is slower on low liquid 1-repellency surfaces, whilst at high viscosity ratios it is the other way around and there is slower dewetting on high liquid 1-repellency surfaces. The switch effect is a consequence of the interplay between the excess energy due to the surface energy, which drives the dewetting process, and the dissipation due to the geometry of the fluid flow, which resists it.

3. Air in liquid - Exploration of the electrostatic forced dewetting of bubbles from solid surfaces and their subsequent actuation: We used electrostatic forces to force a captive air bubble to detach away from an inverted solid surface. We showed that we could then hold the detached bubble stationary in place below the surface at a distance controlled by the voltage. In this "levitated" state, the bubble is separated from the surface by liquid layer with a voltage-selected thickness at which the electrostatic force exactly counterbalances the gravitational buoyancy force. We demonstrated the repeatable ability to cycle between bubble detachment, levitation, and then reattachment. We observed detachment-reattachment hysteresis in which bubble levitation is maintained with voltages in an order of magnitude lower than those used to create detachment.

4. Relevant to all the above systems, particularly Liquid in air and Liquid in Liquid. We have formulated and validated against experimental results a new lattice-Boltzmann method capable of modelling the dynamics of immiscible dielectric fluids coupled with electric fields within a single framework, thus eliminating the need for using separate algorithms to solve the electrostatic and fluid dynamics equations.
Exploitation Route In addition to much enhancing understanding of the science underpinning the dewetting and stability processes for liquid films, the work has relevance to any industry using films of liquid as coatings (e.g. printing, coating and lithographic fabrication in electronics) and it also has relevance to the optics and displays industries where rings and droplets can be optical elements (e.g. apertures, lenses and pixels).
Sectors Chemicals,Digital/Communication/Information Technologies (including Software),Education,Manufacturing, including Industrial Biotechology,Other

URL https://naturesraincoats.com/smart-control-of-wetting/
 
Description Control of liquid film shapes is important in industrial processes such as printing and microscale patterning. The inverse situation of controlling bubbles at surfaces within liquids is important for heat transfer. This project has established a new experimental technique for creating liquid film shapes in precise spatial arrangements, such as squares, semi-circles, ring and other shapes, which are programmable between droplet and film states. It allows novel morphologies to be created which under other circumstances would suffer from instability and break into separate domains of liquid. It also allows pathways to dewetting and instabilities to be controlled and for the formation, detachment and reattachment of bubbles to be controlled. In "Slippery when wet: mobility regimes of confined drops in electrowetting" (doi: 10.1039/C9SM01107B) we were able to use our knowledge to study the directed transport of the liquid droplets using the related technique of electrowetting. In "Electrostatic control of dewetting dynamics" (doi: 10.1063/5.0010443) we were able to show how a stripe of liquid in air dewet surfaces in a similar manner to axisymmetric films of liquids. We were also able to create complex liquid shapes, such as a torus on a solid, and study the competition between dewetting and the Rayleigh-Plateau instability. In "Controlling the breakup of toroidal liquid films on solid surfaces" (doi: 10.1038/s41598-021-87549-5) we demonstrated that electric fields could control and determine the breakup pathways of instabilities. The dewetting dynamics are usually considered to be controlled by the viscous dissipation occurring within a liquid, particularly when the region close to the contact line is an acute wedge-like shape. In "a viscous switch for liquid-liquid dewetting" (doi: 10.1038/s42005-020-0284-8) we were able study dewetting when the outer medium was another viscous liquid. We were able to consider the inner to out liquid viscosity ratio of a remarkable range of five orders of magnitude and do so for both equilibrium droplets with shallow and high contact angles (acute and obtuse shapes near the contact line). This revealed a counter-intuitive effect that, unexpectedly, a surrounding viscous phase can switch the overall dewetting speed so that films retract slower with increasing surface repellency. An effect we were able to both explain theoretically and model numerically. In a further experimental contribution, we were able to study the inverse situation to a droplet in air of a bubble in a liquid. Here we showed that bubbles could be controlled, levitated and manipulated using dielectrophoresis (doi: 10.1002/admi.202001204). To complement experimental work we developed detailed theoretical models validate using lattice-Boltzmann simulations of multiphase dielectric fluids (doi: 10.1021/acs.langmuir.1c00606).
First Year Of Impact 2017
Sector Education,Other
 
Description 2020 - Institute for Multiscale Thermofluids, University of Edinburgh, UK 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Postgraduate students
Results and Impact 2020 - Invited Research Talk - "Smart Slippery Surfaces". Glen McHale. Institute for Multiscale Thermofluids, University of Edinburgh, UK (23/10/2020)
Year(s) Of Engagement Activity 2020
 
Description 2020 - Wetting Dynamics, Bonn, Germany 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Other audiences
Results and Impact 2020 - Wetting Dynamics, Bonn, Germany, 28-30 September 2020. Contributed Research Talk - "Switchable Wetting to Define and Control Liquid Shapes and Instabilities" (29/9/020). Talk given by Glen McHale.
Year(s) Of Engagement Activity 2020
 
Description 2021 - Contributed Research Talk - 7th Micro and Nano Flows Conference 2021, Imperial College London, UK. 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Other audiences
Results and Impact 2021 - 7th Micro and Nano Flows Conference 2021, Mini-Symposium on Transport Phenomena on Superhydrophobic Surfaces, Imperial College London 24/5/21-26/5/21. Contributed Research Talk - "Droplet self-propulsion on hemi-liquid and shaped-liquid surfaces", (24/5/21). Talk given by Glen McHale.
Year(s) Of Engagement Activity 2021
URL https://www.micronanoflows.com/
 
Description 2021 - Dielectrophoresis 2020, Flagstaff, Arizona, USA. 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Other audiences
Results and Impact 2021 - Dielectrophoresis 2020, Flagstaff, Arizona, USA. 26-28 July 2021. Contributed Research Talk - "Lattice Boltzmann Simulations of Dielectrowetting" (27/7/21). Talk given by Élfego Ruiz-Gutiérrez.
Year(s) Of Engagement Activity 2021
URL https://dep2020.org/
 
Description 2021 - Droplets 2021 (5th International Conference on Droplets), Technische Universität Darmstadt, Germany. 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Other audiences
Results and Impact 2021 - Droplets 2021 (5th International Conference on Droplets), Technische Universität Darmstadt, Germany 16-19 September 2021. Contributed Research Talk - "Negative Dielectrowetting of Thick and Thin Films" (27/7/21). Talk given by Andrew M.J. Edwards.
Year(s) Of Engagement Activity 2021
URL https://www.sfb1194.tu-darmstadt.de/droplets_2021/index.en.jsp
 
Description 2021 - Droplets 2021 (5th International Conference on Droplets), Technische Universität Darmstadt, Germany. 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Other audiences
Results and Impact 2021 - Droplets 2021 (5th International Conference on Droplets), Technische Universität Darmstadt, Germany 16-19 September 2021. Contributed Research Talk - "Dynamic dewetting from complex liquid film shapes" (27/7/21). Talk given by Carl Brown.
Year(s) Of Engagement Activity 2021
URL https://www.sfb1194.tu-darmstadt.de/droplets_2021/index.en.jsp
 
Description 2021 - Invited Research Seminar - Collaborative Research Center "Interaction between Transport and Wetting Process", TU Darmstadt, Germany. 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Other audiences
Results and Impact 2021 - Invited Research Seminar - "Controlling Wettability of Solid and Liquid Surfaces". Glen McHale. Collaborative Research Center "Interaction between Transport and Wetting Process", TU Darmstadt, Germany (7/5/2021).
Year(s) Of Engagement Activity 2021
 
Description 2021 - Invited Research Seminar - Continuum Mechanics & Industrial Mathematics Group, University of Strathclyde, Glasgow, UK. 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach Local
Primary Audience Postgraduate students
Results and Impact 2021 - Invited Research Seminar - "Controlling Wettability of Solid and Liquid Surfaces". Glen McHale. Continuum Mechanics & Industrial Mathematics Group, Department of Mathematics & Statistics, University of Strathclyde, Glasgow, UK (16/3/2021).
Year(s) Of Engagement Activity 2021
 
Description 2021 - Invited Research Seminar - Instituto de Fisica, de la Universidad Nacional Autónoma de México (IFUNAM), Mexico. 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Postgraduate students
Results and Impact 2021 - Invited Research Seminar - "Mode-selection pathways in the Plateau-Rayleigh instability on liquid rings. Élfego Ruiz-Gutiérrez. Instituto de Fisica, de la Universidad Nacional Autónoma de México (IFUNAM), Mexico (22/3/21).
Year(s) Of Engagement Activity 2021
 
Description 2021 - UK Fluids Conference 2021, University of Southampton, UK. 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Other audiences
Results and Impact 2021 - UK Fluids Conference 2021, University of Southampton, UK 8-10 September 2021. Contributed Research Talk - "Controlling the breakup of toroidal liquid films on solid surfaces" (10/9/21). Talk given by Glen McHale.
Year(s) Of Engagement Activity 2021
 
Description 2021 - XXVII Congreso de la División de Dinámica de Fluidos, Sociedad Mexicana de Física, Mexico (On-line) 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Other audiences
Results and Impact XXVII Congreso de la División de Dinámica de Fluidos, Sociedad Mexicana de Física
Mexico (On-line) 10/11/2021-12/11/2021

Contributed Research Talk - Theory and Simulations on the Dynamics of Dielectrowetting 10/11/2021
Dr. Elfego Ruiz-Guttierez
Year(s) Of Engagement Activity 2021
URL https://www.fluidos.mx/congreso
 
Description 2022 - NPE International Series Forum XIII (On-line). 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Other audiences
Results and Impact International Forum on Nanotechnology & Precision Engineering (NPE)
NPE International Series Forum XIII (On-line) 8/11/2022

Invited Research Talk - A Tale of Two Surfaces: How do we Make Surfaces Slippery to Liquids? 8/11/2022
Year(s) Of Engagement Activity 2022
URL https://aip.scitation.org/npe/info/webinar
 
Description 2022 - Nature Inspired Surface Engineering (NISE 2022) - Dewetting Topic 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Other audiences
Results and Impact 2022 - Nature Inspired Surface Engineering (NISE 2022)
Seoul, Korea 17/08/2021-19/08/2022
Contributed Research Poster - Wetting and Dewetting on Electrically Switchable Surfaces 17-19/08/2022
Glen McHale
Year(s) Of Engagement Activity 2022
URL https://ameriscience.org/nise-2021/