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