Hydration-Shell Transformation of Thermosensitive Aqueous Polymers

Kenji Mochizuki, Dor Ben-Amotz

Research output: Contribution to journalArticlepeer-review

33 Citations (Scopus)


Although water plays a key role in the coil-globule transition of polymers and biomolecules, it is not clear whether a change in water structure drives or follows polymer collapse. Here, we address this question by using Raman multivariate curve resolution (Raman-MCR) spectroscopy to investigate the hydration shell structure around poly(N-isopropylacrylamide) (PNIPAM) and poly(propylene oxide) (PPO), both below and above the cloud point temperature at which the polymers collapse and form mesoscopic polymer-rich aggregates. We find that, upon clouding, the water surrounding long PNIPAM chains transforms to a less ordered and more weakly hydrogen bonded structure, while the water surrounding short PNIPAM and PPO chains remains similar above and below the cloud point. Furthermore, microfluidic temperature jump studies demonstrate that the onset of clouding precedes the hydration-shell structural transformation, and thus the observed water structural transformation is associated with ripening of aggregates composed of long-chain polymers, on a time scale that is long compared to the onset of clouding.

Original languageEnglish
Pages (from-to)1360-1364
Number of pages5
JournalJournal of Physical Chemistry Letters
Issue number7
Publication statusPublished - Apr 6 2017
Externally publishedYes

ASJC Scopus subject areas

  • General Materials Science
  • Physical and Theoretical Chemistry


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