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On the Nature of Fluorescence Modification Induced by Deformation in Regenerated Silk Fibroin

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dc.contributor.authorSantoro, Gonzalo
dc.contributor.authorToledano Sanz, Óscar
dc.contributor.authorHorcajo Peribáñez, Iván
dc.contributor.authorRebollar, Esther
dc.contributor.authorEzquerra, Tiberio A.
dc.contributor.authorSena-Fernández, Jose
dc.contributor.authorSolano, Eduardo
dc.contributor.authorGarcía-Gutiérrez, Mari Cruz
dc.contributor.funderAgencia Estatal de Investigación. España
dc.contributor.funderMinisterio de Ciencia, Innovación y Universidades de España
dc.date.accessioned2025-12-15T18:20:40Z
dc.date.available2025-12-15T18:20:40Z
dc.date.issued2025-09-25
dc.descriptionThe registered version of this article, first published in ACS Applied Bio Materials, is available online at the publisher's website: American Chemical Society, https://doi.org/10.1021/acsabm.5c01392
dc.descriptionLa versión registrada de este artículo, publicado por primera vez en ACS Applied Bio Materials, está disponible en línea en el sitio web del editor: American Chemical Society, https://doi.org/10.1021/acsabm.5c01392
dc.description.abstractThe mechanical deformation of regenerated silk fibroin (RSF) films induces notable changes in their fluorescence properties, yet the underlying molecular mechanisms remain poorly understood. In this work, we investigate the interplay between mechanical, structural, and optical response of RSF films processed with glycerol (gly) and with polyethylene glycol (PEG) as a plasticizer. PEG-containing films exhibited enhanced ductility, a significant increase of the absorption coefficient in the UV spectral range and narrower fluorescence spectra, with reduced intensity at longer wavelengths, suggesting fewer cross-links. These differences in the mechanical and optical properties of the investigated polymers may be due to the higher amorphous phase content of the samples with PEG, as it is revealed by wide-angle X-ray scattering (WAXS). Ab initio calculations of model systems confirmed that fluorescence, primarily due to tryptophan residues, is highly sensitive to local conformation and hydrogen-bonding interactions. To elucidate the effect of deformation on silk fibroin fluorescence, WAXS patterns, using synchrotron radiation, and fluorescence spectra were acquired while simultaneous tensile measurements were performed. Notably, strain-induced backbone alignment favors the formation of electronically coupled cross-links, which give rise to the observed changes in fluorescence. These findings provide further insights into the structure–property relationships governing RSF fluorescence, with potential implications for the design of deformation-responsive biomaterials.en
dc.description.provenanceMade available in DSpace on 2025-12-15T18:20:40Z (GMT). No. of bitstreams: 1 On the Nature of Fluorescence Modification.pdf: 4077605 bytes, checksum: 8330d843698b7a90cbcb4bd7cba639b9 (MD5) Previous issue date: 2025-09-25en
dc.description.sponsorshipThis work has been funded by grants: TED2021-129845B−I00 funded by MCIN/AEI/10.13039/501100011033 and by “ERDF A way of making Europe”, by PID2022-138635NBI00/AEI/10.13039/501100011033, and by the Regional Government of Madrid through the project TEC MATRIXCM (TEC-2024/TEC-85).
dc.description.versionversión publicada
dc.identifier.citationSantoro, G., Toledano, Ó., Horcajo Peribáñez, I., Rebollar, E., Ezquerra, T. A., Sena-Fernández, J., Solano, E., & García-Gutiérrez, M. C. (2025). On the Nature of Fluorescence Modification Induced by Deformation in Regenerated Silk Fibroin. ACS Applied Bio Materials, 8(10), 9268-9276. https://doi.org/10.1021/ACSABM.5C01392
dc.identifier.doihttps://doi.org/10.1021/acsabm.5c01392
dc.identifier.issn2576-6422
dc.identifier.urihttps://hdl.handle.net/20.500.14468/31149
dc.journal.issue10
dc.journal.titleACS Applied Bio Materials
dc.journal.volume8
dc.language.isoen
dc.page.final9276
dc.page.initial9268
dc.publisherAmerican Chemical Society
dc.relation.centerFacultad de Ciencias
dc.relation.departmentFísica Interdisciplinar
dc.relation.projectidinfo:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2022-138635NB-I00
dc.relation.projectidS2024/TEC-2024/TEC-85
dc.rightsinfo:eu-repo/semantics/openAccess
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/deed.es
dc.subject22 Física
dc.subject.keywordssilk fibroinen
dc.subject.keywordsfluorescenceen
dc.subject.keywordsX-ray scatteringen
dc.subject.keywordsmechanical propertiesen
dc.subject.keywordssynchrotron lighten
dc.subject.keywordsab initio calculationsen
dc.titleOn the Nature of Fluorescence Modification Induced by Deformation in Regenerated Silk Fibroinen
dc.typeartículoes
dc.typejournal articleen
dspace.entity.typePublication
relation.isAuthorOfPublication72b031b9-d091-4c35-b48f-b97c34b9d539
relation.isAuthorOfPublication.latestForDiscovery72b031b9-d091-4c35-b48f-b97c34b9d539
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