Abstract

Self-assembled molecular nanostructures embody an enormous potential for new technologies, therapeutics, and understanding of molecular biofunctions. Their structure and function are dependent on local environments, necessitating in-situ/operando investigations for the biggest leaps in discovery and design. However, the most advanced of such investigations involve laborious labeling methods that can disrupt behavior or are not fast enough to capture stimuli-responsive phenomena. We utilize X-rays resonant with molecular bonds to demonstrate an in-situ nanoprobe that eliminates the need for labels and enables data collection times within seconds. Our analytical spectral model quantifies the structure, molecular composition, and dynamics of a copolymer micelle drug delivery platform using resonant soft X-rays. We additionally apply this technique to a hydrocarbon sequestrating polysoap micelle and discover that the critical organic-capturing domain does not coalesce upon aggregation but retains distinct single-molecule cores. This characteristic promotes its efficiency of hydrocarbon sequestration for applications like oil spill remediation and drug delivery. Such a technique enables operando, chemically sensitive investigations of any aqueous molecular nanostructure, label-free.

In-situ methods are important for investigating the local structure and function in molecular nanostructures but such investigations often involve laborious labeling methods that can disrupt behavior or are not fast enough to capture stimuli-responsive phenomena. Here, the authors use X-rays resonant with molecular bonds to demonstrate an in-situ nanoprobe that eliminates the need for labels and enables data collection times within seconds.

Details

Title
Label-free characterization of organic nanocarriers reveals persistent single molecule cores for hydrocarbon sequestration
Author
McAfee, Terry 1 ; Ferron, Thomas 2 ; Cordova, Isvar A 3   VIAFID ORCID Logo  ; Pickett, Phillip D 4   VIAFID ORCID Logo  ; McCormick, Charles L 4 ; Wang, Cheng 3 ; Collins, Brian A 2   VIAFID ORCID Logo 

 Washington State University, Department of Physics and Astronomy, Pullman, USA (GRID:grid.30064.31) (ISNI:0000 0001 2157 6568); Lawrence Berkeley National Laboratory, Advanced Light Source, Berkeley, USA (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551) 
 Washington State University, Department of Physics and Astronomy, Pullman, USA (GRID:grid.30064.31) (ISNI:0000 0001 2157 6568) 
 Lawrence Berkeley National Laboratory, Advanced Light Source, Berkeley, USA (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551) 
 University of Southern Mississippi, School of Polymer Science and Engineering, Hattiesburg, USA (GRID:grid.267193.8) (ISNI:0000 0001 2295 628X) 
Publication year
2021
Publication date
2021
Publisher
Nature Publishing Group
e-ISSN
20411723
Source type
Scholarly Journal
Language of publication
English
ProQuest document ID
2531843608
Copyright
© The Author(s) 2021. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.