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This study investigates how steric forces introduced by a pegylated derivative of superfolder green fluorescent protein (sfGFP) that is monofunctional for silica binding modulate the delicate interplay of long\u2010range (electrostatic and van der Waals) and short\u2010range (protein\u2010mediated) interactions in pH\u2010responsive silica nanoparticle (SiNP) assembly by bifunctional silica\u2010binding sfGFP. Increasing the length of the PEG segment and pre\u2010incubating SiNPs with increasing concentrations of pegylated proteins enables precise control over cluster size within the 800\u20131450\u00a0nm range with a sixfold decrease in polydispersity index to a remarkable 0.1 endpoint. Weakening short\u2010range attractive interactions via mutagenesis extends this control to clusters in the 50\u2013250\u00a0nm range and reveals that the F\u00f6rster resonance energy transfer (FRET) efficiency of clusters scales linearly with cluster diameter below 230\u00a0nm but increases only by 15% as clusters grow to 1450\u00a0nm. These findings enable the development of a system that provides an optical readout to dynamic changes in solution conditions enacted by a combination of pH adjustment and ion charge screening.<\/jats:p>","DOI":"10.1002\/smll.202503026","type":"journal-article","created":{"date-parts":[[2025,7,4]],"date-time":"2025-07-04T06:52:34Z","timestamp":1751611954000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Steric Modulation of Protein\u2010Mediated Nanoparticle Assembly: Controlling Cluster Size, Polydispersity, and FRET Responses by Rebalancing Short\u2010 and Long\u2010Range Interactions"],"prefix":"10.1002","volume":"21","author":[{"given":"Yifeng","family":"Cai","sequence":"first","affiliation":[{"name":"Department of Chemical Engineering University of Washington  Seattle WA 98195 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