Kinetic control of molecular assembly on surfaces

Paris, Chiara and Floris, Andrea and Aeschlimann, Simon and Neff, Julia and Kling, Felix and Kühnle, Angelika and Kantorovich, Lev (2018) Kinetic control of molecular assembly on surfaces. Communications Chemistry . ISSN 2399-3669

Full content URL: https://www.nature.com/articles/s42004-018-0069-0

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Abstract

It is usually assumed that molecules deposited on surfaces assume the most thermodynamically
stable structure. Here we show, by considering a model system of dihydroxybenzoic
acid molecules on the (10.4) surface of calcite, that metastable molecular
architectures may also be accessed by choosing a suitable initial state of the molecules
which defines the observed transformation path. Moreover, we demonstrate that the latter
is entirely controlled by kinetics rather than thermodynamics. We argue that molecules
are deposited as dimers that undergo, upon increase of temperature, a series of structural
transitions from clusters to ordered striped and then dense networks, and finally to a
disordered structure. Combining high-resolution dynamic atomic force microscopy experiments
and density-functional theory calculations, we provide a comprehensive analysis of
the fundamental principles driving this sequence of transitions. Our study may open new
avenues based on kinetic control as a promising strategy for achieving tailored molecular
architectures on surfaces.

Additional Information:Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
Keywords:physics, density functional theory, molecular assembly on surfaces, calcite, insulating surfaces, self-assembly, kinetics, thermodynmics, Organic molecules
Subjects:F Physical Sciences > F343 Computational Physics
F Physical Sciences > F200 Materials Science
F Physical Sciences > F170 Physical Chemistry
F Physical Sciences > F300 Physics
Divisions:College of Science > School of Mathematics and Physics
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ID Code:33858
Deposited On:25 Oct 2018 12:51

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