Measuring self-assembly in solution: Incorporation and dynamics of a "Tailor-made impurity" in precrystalline glucose aggregates

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Abstract

We have studied the onset of crystallization from solution using a fluorescent probe molecule that incorporates selectively into precrystalline glucose aggregates that form in supersaturated aqueous glucose solutions. We achieve incorporation of the fluorophore into the aggregates by virtue of the fluorophore pendant glycosyl moiety and compare the rotational diffusion data for this molecule to that for the nonglycosylated, native probe molecule. This experimental approach, in conjunction with semiempirical calculations to understand the electronic response of the fluorescent probe, provides insight into the formation and size of precrystalline glucose aggregates. Our data indicate that the aggregates effectively isolate the fluorophore from the solution over a range of glucose concentrations spanning the saturation point and that the lifetime of these aggregates is on the order of a nanosecond for aggregates that include the glycosylated probe molecule. The subtle but important differences between these results and those we reported previously for carminic acid in aqueous glucose solutions point to the significant role of labile protons in mediating the formation and dynamics of precrystalline glucose aggregates.

LanguageEnglish (US)
Pages17034-17040
Number of pages7
JournalJournal of Physical Chemistry
Volume100
Issue number42
StatePublished - 1996

Profile

glucose
Self assembly
Glucose
self assembly
Impurities
impurities
Fluorophores
Molecules
probes
Fluorescent Dyes
molecules
Carmine
Crystallization
Protons
crystallization
saturation
life (durability)
acids
protons
Acids

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

Cite this

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title = "Measuring self-assembly in solution: Incorporation and dynamics of a {"}Tailor-made impurity{"} in precrystalline glucose aggregates",
abstract = "We have studied the onset of crystallization from solution using a fluorescent probe molecule that incorporates selectively into precrystalline glucose aggregates that form in supersaturated aqueous glucose solutions. We achieve incorporation of the fluorophore into the aggregates by virtue of the fluorophore pendant glycosyl moiety and compare the rotational diffusion data for this molecule to that for the nonglycosylated, native probe molecule. This experimental approach, in conjunction with semiempirical calculations to understand the electronic response of the fluorescent probe, provides insight into the formation and size of precrystalline glucose aggregates. Our data indicate that the aggregates effectively isolate the fluorophore from the solution over a range of glucose concentrations spanning the saturation point and that the lifetime of these aggregates is on the order of a nanosecond for aggregates that include the glycosylated probe molecule. The subtle but important differences between these results and those we reported previously for carminic acid in aqueous glucose solutions point to the significant role of labile protons in mediating the formation and dynamics of precrystalline glucose aggregates.",
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AB - We have studied the onset of crystallization from solution using a fluorescent probe molecule that incorporates selectively into precrystalline glucose aggregates that form in supersaturated aqueous glucose solutions. We achieve incorporation of the fluorophore into the aggregates by virtue of the fluorophore pendant glycosyl moiety and compare the rotational diffusion data for this molecule to that for the nonglycosylated, native probe molecule. This experimental approach, in conjunction with semiempirical calculations to understand the electronic response of the fluorescent probe, provides insight into the formation and size of precrystalline glucose aggregates. Our data indicate that the aggregates effectively isolate the fluorophore from the solution over a range of glucose concentrations spanning the saturation point and that the lifetime of these aggregates is on the order of a nanosecond for aggregates that include the glycosylated probe molecule. The subtle but important differences between these results and those we reported previously for carminic acid in aqueous glucose solutions point to the significant role of labile protons in mediating the formation and dynamics of precrystalline glucose aggregates.

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