Optical characterization of surface adlayers and their compositional demixing at the nanoscale

Limin Xiang, Michal Wojcik, Samuel J. Kenny, Rui Yan, Seonah Moon, Wan Li and Ke Xu ()
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Limin Xiang: University of California
Michal Wojcik: University of California
Samuel J. Kenny: University of California
Rui Yan: University of California
Seonah Moon: University of California
Wan Li: University of California
Ke Xu: University of California

Nature Communications, 2018, vol. 9, issue 1, 1-9

Abstract: Abstract Under ambient conditions, the behavior of a solid surface is often dominated by a molecularly thin adsorbed layer (adlayer) of small molecules. Here we develop an optical approach to unveil the nanoscale structure and composition of small-molecule adlayers on glass surfaces through spectrally resolved super-resolution microscopy. By recording the images and emission spectra of millions of individual solvatochromic molecules that turn fluorescent in the adlayer phase, we obtain ~30 nm spatial resolution and achieve concurrent measurement of local polarity. This allows us to establish that the adlayer dimensionality gradually increases through a sequence of 0D (nanodroplets), 1D (nano-lines), and 2D (films) for liquids of increasing polarity. Moreover, we find that in adlayers, a solution of two miscible liquids spontaneously demixes into nanodroplets of different compositions that correlate strongly with droplet size and location. We thus reveal unexpectedly rich structural and compositional behaviors of surface adlayers at the nanoscale.

Date: 2018
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DOI: 10.1038/s41467-018-03820-w

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