Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 8, Issue 5, Pages 975-983Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.6b02978
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Funding
- European Research Council under European Union's Seventh Framework Programme [279632]
- European Research Council (ERC) [279632] Funding Source: European Research Council (ERC)
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We present an atomistic understanding of the evolution of the size distribution with temperature and number of cycles in atomic layer deposition (ALD) of Pt nanoparticles (NPs). Atomistic modeling of our experiments teaches us that the NPs grow mostly via NP diffusion and coalescence rather than through single-atom processes such as precursor chemisorption, atom attachment, and Ostwald ripening. In particular, our analysis shows that the NP aggregation takes place during the oxygen half-reaction and that the NP mobility exhibits a size and temperature dependent scaling. Finally, we show that contrary to what has been widely reported, in general, one cannot simply control the NP size by the number of cycles alone. Instead, while the amount of Pt deposited can be precisely controlled over a wide range of temperatures, ALD-like precision over the NP size requires low deposition temperatures (e.g., T<100 degrees C) when growth is dominated by atom attachment.
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