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Title: Spatially dependent H-bond dynamics at interfaces of water/biomimetic self-assembled lattice materials

Abstract

Understanding hydrogen-bond interactions in self-assembled lattice materials is crucial for preparing such materials, but the role of hydrogen bonds (H bonds) remains unclear. To gain insight into H-bond interactions at the materials’ intrinsic spatial scale, we investigated ultrafast H-bond dynamics between water and biomimetic self-assembled lattice materials (composed of sodium dodecyl sulfate and β-cyclodextrin) in a spatially resolved manner. To accomplish this, we developed an infrared pump, vibrational sum-frequency generation (VSFG) probe hyperspectral microscope. With this hyperspectral imaging method, we were able to observe that the primary and secondary OH groups of β-cyclodextrin exhibit markedly different dynamics, suggesting distinct H-bond environments, despite being separated by only a few angstroms. We also observed another ultrafast dynamic reflecting a weakening and restoring of H bonds between bound water and the secondary OH of β-cyclodextrin, which exhibited spatial uniformity within self-assembled domains, but heterogeneity between domains. The restoration dynamics further suggest heterogeneous hydration among the self-assembly domains. The ultrafast nature and meso- and microscopic ordering of H-bond dynamics could contribute to the flexibility and crystallinity of the material––two critically important factors for crystalline lattice self-assemblies––shedding light on engineering intermolecular interactions for self-assembled lattice materials.

Authors:
ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1658999
Grant/Contract Number:  
SC0019333
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 117 Journal Issue: 38; Journal ID: ISSN 0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Country of Publication:
United States
Language:
English

Citation Formats

Wang, Haoyuan, Wagner, Jackson C., Chen, Wenfan, Wang, Chenglai, and Xiong, Wei. Spatially dependent H-bond dynamics at interfaces of water/biomimetic self-assembled lattice materials. United States: N. p., 2020. Web. https://doi.org/10.1073/pnas.2001861117.
Wang, Haoyuan, Wagner, Jackson C., Chen, Wenfan, Wang, Chenglai, & Xiong, Wei. Spatially dependent H-bond dynamics at interfaces of water/biomimetic self-assembled lattice materials. United States. https://doi.org/10.1073/pnas.2001861117
Wang, Haoyuan, Wagner, Jackson C., Chen, Wenfan, Wang, Chenglai, and Xiong, Wei. Wed . "Spatially dependent H-bond dynamics at interfaces of water/biomimetic self-assembled lattice materials". United States. https://doi.org/10.1073/pnas.2001861117.
@article{osti_1658999,
title = {Spatially dependent H-bond dynamics at interfaces of water/biomimetic self-assembled lattice materials},
author = {Wang, Haoyuan and Wagner, Jackson C. and Chen, Wenfan and Wang, Chenglai and Xiong, Wei},
abstractNote = {Understanding hydrogen-bond interactions in self-assembled lattice materials is crucial for preparing such materials, but the role of hydrogen bonds (H bonds) remains unclear. To gain insight into H-bond interactions at the materials’ intrinsic spatial scale, we investigated ultrafast H-bond dynamics between water and biomimetic self-assembled lattice materials (composed of sodium dodecyl sulfate and β-cyclodextrin) in a spatially resolved manner. To accomplish this, we developed an infrared pump, vibrational sum-frequency generation (VSFG) probe hyperspectral microscope. With this hyperspectral imaging method, we were able to observe that the primary and secondary OH groups of β-cyclodextrin exhibit markedly different dynamics, suggesting distinct H-bond environments, despite being separated by only a few angstroms. We also observed another ultrafast dynamic reflecting a weakening and restoring of H bonds between bound water and the secondary OH of β-cyclodextrin, which exhibited spatial uniformity within self-assembled domains, but heterogeneity between domains. The restoration dynamics further suggest heterogeneous hydration among the self-assembly domains. The ultrafast nature and meso- and microscopic ordering of H-bond dynamics could contribute to the flexibility and crystallinity of the material––two critically important factors for crystalline lattice self-assemblies––shedding light on engineering intermolecular interactions for self-assembled lattice materials.},
doi = {10.1073/pnas.2001861117},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 38,
volume = 117,
place = {United States},
year = {2020},
month = {9}
}

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https://doi.org/10.1073/pnas.2001861117

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