Molecular dynamics simulations of droplet evaporation in the non-linear response regime


Prof. Dr. rer. nat. Florian Müller-Plathe
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Dr. Eunsang Lee
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The study of molecular processes in heat- and mass- transfer is becoming increasingly important. The understanding of basic mechanisms in heat transfer, such as phase transitions, requires a good knowledge of the phenomena of liquid-solid contact on a nanometer scale. Despite many efforts using continuum approaches to evaluate microscopic problems in terms of space, time or speed, such extrapolations find quickly their limits. For example, the characteristic length in the vicinity of the 3-phase contact line is so small that it reaches molecular dimensions and that microscopic models are needed in order to provide independent information in addition to a macroscopic approach. Molecular dynamic simulations can investigate these phenomena on a molecular scale. The simulations have been successfully used in statistical mechanics and in many areas of chemistry. In this project they will be expanded methodically to investigate heat and mass transfer under extreme conditions.

This subproject uses molecular dynamic simulations with large numbers of particles to simulate liquid droplets of submicron size in a homogeneous environment and in contact with surfaces. These droplets should be systematically subjected to changes in their thermodynamic state or non-equilibrium conditions. These should cause or alter evaporation rates, heat transfer rates, etc. and will be analyzed, in a linear and nonlinear regime. Changes in state should be made quickly and stationary nonequilibrium simulations should reach to a non-linear response area. Nonequilibrium molecular dynamic methods are specially adapted for the region far from equilibrium and for the existing geometries and need to be redeveloped. The objective of these simulations is to understand the molecular processes under extreme conditions and the identification of appropriate quantitative indicators, such as transport parameters or contact angle. These models should be available for partners in the SFB-TRR 75.

In particular the following processes are simulated:

1. Droplet evaporation due to a sudden change of environmental conditions

2. Droplet evaporation on a hot surface and evaporation close to the 3-phase contact line

The investigations in the first funding period are focused on molecular dynamic simulations of evaporation under extreme conditions. In the first funding period only one-component fluids are investigated. An extension to multicomponent and complex fluids and the simulation of droplet impact on overheated surfaces is reserved for later funding periods.



Tianhang Zhuo, Hari Krishna Chilukoti, Zhenghao Wu, Florian Müller-Plathe:
Effect of Defects on the Interfacial Thermal Conductance between n-Heneicosane in Solid and Liquid Phases and a Graphene Monolayer
J. Phys. Chem. C 2021, 125, 14149–14162
DOI: 10.1021/acs.jpcc.1c04676

Eunsang Lee, Hari Krishna Chilukoti, Florian Müller-Plathe:
Suppressing the rebound of impacting droplets from solvophobic surfaces by polymer additives: polymer adsorption and molecular mechanisms
Soft Matter, 2021, 17, 6952-6963
DOI: 10.1039/D1SM00558H

E. Lee, H. K. Chilukoti, and F. Müller-Plathe:
Rebound suppression of a droplet impacting on a supersolvophobic surface by a small amount of polymer additives
ACS Macro Lett. 10, 192−196 (2021)
DOI: 10.1021/acsmacrolett.0c00808


D. Surblys, F. Müller-Plathe, and T. Ohara:
Dry-surface 法による遮蔽クーロン相互作用を有する系の固液界面の付着仕事算出 (Computing the work of adhesion of solid-liquid interfaces in systems with damped Coulomb interactions via the dry-surface method)
日本流体力学会年会 (The Japan Society of Fluid Mechanics annual meeting) Yamaguchi University, 18-20 Sep 2020.


H. K. Chilukoti, T. Zhou, V. R. Ardham, M. C. Böhm, and F. Müller-Plathe:
Thermal Energy Transport across the Interface between Phase Change Material n-Heneicosane in Solid and Liquid Phases and Few-Layer Graphene
J. Phys. Chem. C 123, 29192–29202 (2019)
DOI: 10.1021/acs.jpcc.9b07054


H. K. Chilukoti, F. Müller-Plathe, and H. Yang:
Application of Reverse Non-equilibrium Molecular Dynamics to the Calculation of the Mutual Diffusion Coefficient of Alkane Mixtures
J. Phys. Chem. B 122, 9210−9217 (2018)
DOI: 10.1021/acs.jpcb.8b06886

D. Surblys, F. Leroy, Y. Yamaguchi, and F. Müller-Plathe:
Molecular dynamics analysis of the influence of Coulomb and van der Waals interactions on the work of adhesion at the solid-liquid interface
J. Chem. Phys. 148, 134707 (2018)
DOI: 10.1063/1.5019185


H. Han, S. Mérabia, and F. Müller-Plathe:
Thermal transport at solid-liquid interface: From the increase of thermal resistance towards the shift of rapid boiling
Nanoscale 9, 8314−8320 (2017)
DOI: 10.1039/C7NR01215B

H. Han, C. Schlawitschek, N. Katyal, P. Stephan, T. Gambaryan-Roisman, F. Leroy, and F. Müller-Plathe:
Solid-liquid interface thermal resistance affects the evaporation rate of droplets from a surface: A study of perfluorohexane on chromium using molecular dynamics and continuum theory
Langmuir 33, 5336–5343 (2017)
DOI: 10.1021/acs.langmuir.7b01410

H. Jiang, F. Müller-Plathe, and A.Z. Panagiotopoulos
Contact Angles from Young’s Equation in Molecular Dynamics Simulations
J. Chem. Phys. 147, 084708 (2017)
DOI: 10.1063/1.4994088

J. Zhang, J. Milzetti, F. Müller-Plathe, and F. Leroy
Formation of Coffee-Stain Patterns at the Nanoscale: The Role of Nanoparticle Solubility and Solvent Evaporation Rate
J. Chem. Phys. 146, 114503 (2017).
DOI: 10.1063/1.4978284

H. Han, S. Mérabia, and F. Müller-Plathe
Thermal transport at solid-liquid interfaces: high pressure facilitates heat flow through non-local liquid structuring
J. Phys. Chem. Lett. 8, 1946−1951 (2017).
DOI: 10.1021/acs.jpclett.7b00227


Metya, A.K., Singh, J. K., Müller-Plathe, F.:
Ice nucleation on nanotextured surfaces: Influence of surface fraction, pillar height and wetting states,
In: Phys. Chem. Chem. Phys. 18 (2016) 26796–26806.

Yang, H., Zhang, J., Müller-Plathe, F.:
Extending reverse nonequilibrium molecular dynamics to the calculation of mutual diffusion coefficients in molecular fluid mixtures,
In: Mol. Sim. 42 (2016) 1379–1384.
DOI: 10.1080/08927022.2015.1114178


Yang, H., Zhang, J., Müller-Plathe, F., Yang, Y.:
A Reverse Nonequilibrium Molecular Dynamics Method for Calculating the Mutual Diffusion Coefficient for Binary Fluids,
In: Chem. Eng. Sci. 130 (2015) 1–7.
DOI: 10.1016/j.ces.2015.03.006

Leroy, F., Müller-Plathe, F.:
Dry-Surface Simulation Method for the Determination of the Work of Adhesion of Solid-Liquid Interfaces,
Langmuir 31 (2015) 8335–8345 (2015).
DOI: 10.1021/acs.langmuir.5b01394

J. Zhang, F. Müller-Plathe, F. Leroy.
Pinning of the contact line during evaporation on heterogeneous surfaces: slowdown or temporary immobilization?
Insights from a nanoscale study, Langmuir, 2015, 31 (27), pp 7544-7552.


Ramírez, R., Singh, J. K., Müller-Plathe, F., Böhm, M. C.:
Ice and water droplets on graphite: a comparison of quantum and classical simulations,
In: J. Chem. Phys. 141 (2014) 204701; featured article and issue front cover.
DOI: 10.1063/1.4901562

Zhang, J., Leroy, F., Müller-Plathe, F.:
Influence of the contact-line curvature on the evaporation of nanodroplets from solid substrates,
In: Phys. Rev. Lett. 113 (2014) 046101

Singh, J. K., Müller-Plathe, F.:
On the characterization of crystallization and ice adhesion on smooth and rough surfaces using molecular dynamics,
In: Appl. Phys. Lett. 104 (2014) 021603.
DOI: 10.1063/1.4862257


Zhang, J., Leroy, F. , Müller-Plathe, F.
Evaporation of nanodroplets on heated substrates: A molecular dynamics study
Langmuir 29, 9770-9782 (2013)

Zhang, J., Müller-Plathe, F., Yahia-Ouahmed, M., Leroy, F.
A steady-state non-equilibrium molecular dynamics approach for the study of evaporation processes
The Journal of Chemical Physics 139, 134701 (2013)


Leroy, F.; Müller-Plathe, F.
Can Continuum Thermodynamics Characterize Wenzel Wetting States of Water at the Nanometer Scale?
Journal of Chemical Theory and Computation, 2012


Leroy, F.; Müller-Plathe, F.
Rationalization of the behavior of solid-liquid surface free energy of water in Cassie and Wenzel wetting states on rugged solid surfaces at the nanometer scale.
Langmuir The ACS Journal Of Surfaces And Colloids, 27(2), 637-645, 2011


Leroy, F.; Müller-Plathe, F.
Solid-liquid surface free energy of Lennard-Jones liquid on smooth and rough surfaces computed by molecular dynamics using the phantom-wall method.
The Journal of Chemical Physics, 133(4), 044110, 2010