General role of amorphous aggregates in crystal nucleation

07 July 2023, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

There is mounting evidence that crystal nucleation from supersaturated solution involves the formation and reor-ganisation of pre-nucleation clusters contradicting classical nucleation theory. Here, a wide range of amino acids and peptides is investigated using light scattering, mass spectrometry, and in-situ terahertz Raman spectroscopy to demonstrate that the presence of amorphous aggregates with a wide range of sizes is a general phenomenon in supersaturated solutions. Additionally, these amorphous aggregates act as intermediates for laser-induced crystal nucleation. These observations are inconsistent not only with classical nucleation theory, but also non-classical theories involving liquid-liquid phase separation, requiring a new approach.

Keywords

crystal nucleation
aggregates
prenucleation clusters
laser-induced nucleation
low-frequency Raman spectroscopy
dynamic light scattering
mass spectrometry

Supplementary materials

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Supplementary Movies S1
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Aggregate-assisted laser-induced nucleation of alanine from solution (0.18g/mL in D2O, 5 days old).
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Supplementary Movies S2
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Aggregate-assisted laser-induced nucleation of Gly-Gly from solution (0.2g/mL in H2O, 2 days old).
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Supplementary Movies S3
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Aggregate-assisted laser-induced nucleation of Gly-Gly-Gly from solution (0.1g/mL in D2O, 1 day old).
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Supplementary Movies S4
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Aggregate-assisted laser-induced nucleation of Ala-Ala from solution (0.3g/mL in D2O, 1 day old).
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Supplementary Movies S5
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Aggregate-assisted laser-induced nucleation of serine from solution (0.4g/mL in D2O, 1 day old).
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Supplementary Movies S6
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Aggregate-assisted laser-induced nucleation of glutamic acid from solution (0.13g/mL in H2O, 2 days old).
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Supplementary Movies S7
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Aggregate-assisted laser-induced nucleation of phenylalanine from solution (0.05g/mL in H2O, 2 days old).
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Supplementary Movies S8
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Aggregate-assisted laser-induced nucleation of lysine from solution (0.5g/mL in H2O, 2 days old).
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Supplementary Movies S9
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Aggregate-assisted laser-induced nucleation of histidine from solution (0.13g/mL in H2O, 1 day old).
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