Two-dimensional materials and surfactants: exfoliation, controlled stacks, targeted particle growth and functional heterostructures
Solid State and Surface Chemistry, Material Synthesis
Physical Chemistry of Molecules, Liquids and Interfaces, Biophysical Chemistry
Final Report Abstract
Two-dimensional crystals received a lot of attention in the past years, as they offer unique properties that are unprecedented in their directly related layered bulk phase. In this project, we have studied the interaction of 2D nanocrystals with surfactant molecules. One research direction is on the shape-controlled synthesis of 2D nanocrystals, the other is on the electronic properties of 2D nanocrystals under the influence of surfactants. The research contained a methodological part for the well-founded choice of the computational methods and an applied part, in which the interactions between selected surfactants and 2D nanocrystals was monitored and assessed. Central to the methodological part of the project was the use of dispersion-corrected DFT methods, particularly the SCAN-rVV10 and PBE-rVV10L functionals, to accurately predict interlayer distances, interaction energies, and electronic properties. These quantities are crucial for a thorough description of stacking properties and were assessed across a wide range of 2D materials in both homogeneous and heterostructured forms. For instance, in homogeneous and heterostructured layered systems, SCAN-rVV10 accurately predicts interlayer distances and interaction energetics, aligning closely with experimental and higher-level theoretical RPA results. Within the more applied part of the project, it was illustrated how molecular orientation and surface structure influence ligand-binding characteristics, particularly for {Mo,Ti}S2 nanostructures interacting with selected organic molecules. This research emphasizes that molecule interactions at edge and basal plane sites are crucial for controlling the shape and growth of these nanostructures. Molecules often bind more strongly to edge sites, promoting edge passivation and vertical stacking, while basal plane interactions would favour lateral growth. In conclusion, this project not only advances our understanding of the fundamental properties of 2D materials but also provides crucial insights into the accuracy of DFT methods in predicting these properties. By identifying the strengths and limitations of different dispersion-corrected DFT methods, we open the way for more accurate computational research and practical applications of these materials. The comprehensive analysis bridges theoretical predictions with potential industrial applications, underscoring the transformative impact of 2D materials in science and technology.
Publications
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Performance of London Dispersion Corrected DFT Functionals for Two-Dimensional Materials, European Conference on Chemistry of Two-Dimensional Materials, Dresden, Germany (September 2019), Poster
Birkan Emrem, Kati Finzel & Thomas Heine
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London Dispersion Corrected Density Functional Theory Made Layered Materials Simple, Saxonian Theoretical Chemistry Symposium, Leipzig, Germany (October 2021), Talk
Birkan Emrem
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Performance of London Dispersion Corrected DFT Functionals and Their Impacts on Electronic Band Structure Calculations, European Conference on Chemistry of Two-Dimensional Materials (virtual), Bologna, Italy (September 2021), Poster
Birkan Emrem, Kati Finzel & Thomas Heine
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London Dispersion‐Corrected Density Functionals Applied to van der Waals Stacked Layered Materials: Validation of Structure, Energy, and Electronic Properties. Advanced Theory and Simulations, 5(7).
Emrem, Birkan; Kempt, Roman; Finzel, Kati & Heine, Thomas
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Shape and Growth Control of {Mo,Ti}S2 Nanoplatelets, Condensed Matter Division (CMD29) Conference, Manchester, UK (August 2022), Poster
Birkan Emrem, Jan-Ole Joswig & Thomas Heine
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The structural and electronic richness of buckled honeycomb AsP bilayers. Nanoscale, 14(28), 10136-10142.
Arcudia, Jessica; Emrem, Birkan; Heine, Thomas & Merino, Gabriel
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Precise structure and energy of group 6 transition metal dichalcogenide homo- and heterobilayers in high-symmetry configurations. 2D Materials, 11(3), 035011.
Emrem, Birkan; Joswig, Jan-Ole & Heine, Thomas
