{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,9,21]],"date-time":"2026-09-21T03:21:05Z","timestamp":1789960865417,"version":"4.0.1"},"reference-count":73,"publisher":"National Academy of Sciences","issue":"12","license":[{"start":{"date-parts":[[2025,3,17]],"date-time":"2025-03-17T00:00:00Z","timestamp":1742169600000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by-nc-nd\/4.0\/"}],"funder":[{"name":"NIH","award":["S10OD018516"],"award-info":[{"award-number":["S10OD018516"]}]},{"name":"NSF","award":["DMR-1719875"],"award-info":[{"award-number":["DMR-1719875"]}]},{"name":"DOE","award":["DE-SC0020179"],"award-info":[{"award-number":["DE-SC0020179"]}]}],"content-domain":{"domain":["www.pnas.org"],"crossmark-restriction":true},"short-container-title":["Proc. Natl. Acad. Sci. U.S.A."],"published-print":{"date-parts":[[2025,3,25]]},"abstract":"\n Integrating the optoelectronic properties of quantum dots (QDs) with biological enzymatic systems to form microbe-semiconductor biohybrids offers promising prospects for both solar-to-chemical conversion and light-modulated biochemical processes. Developing these nano\u2013bio hybrid systems necessitates a deep understanding of charge-transfer dynamics at the nano\u2013bio interface. Photoexcited carrier transfer from QDs to microbes is driven by complex interactions, with emerging insights into the relevant thermodynamic and kinetic factors. The heterogeneities of both microbes and QD ensembles pose significant challenges in mechanistic understanding, which is critical for designing advanced nano\u2013bio hybrids. We used fluorescence lifetime imaging microscopy to analyze charge transfer between a CdSe QD film and\n Shewanella oneidensis<\/jats:italic>\n microbes. We correlated the spatiotemporal fluorescence data with an analytical model. Our analysis revealed two distinct distributions of QD de-excitation pathways. The characteristics of these distributions: 1) a faster transfer rate (\n \n \n \n \n k<\/mml:mi>\n \u00af<\/mml:mo>\n <\/mml:mover>\n \n E<\/mml:mi>\n T<\/mml:mi>\n 1<\/mml:mn>\n <\/mml:mrow>\n <\/mml:msub>\n =<\/mml:mo>\n 1.5<\/mml:mn>\n \u00a0<\/mml:mo>\n \n \n \n 10<\/mml:mn>\n 9<\/mml:mn>\n <\/mml:msup>\n <\/mml:mrow>\n <\/mml:mfenced>\n \u00a0<\/mml:mo>\n \n s<\/mml:mi>\n \n -<\/mml:mo>\n 1<\/mml:mn>\n <\/mml:mrow>\n <\/mml:msup>\n <\/mml:math>\n <\/jats:inline-formula>\n ), with a lower acceptor number (\n \n \n \n \n \n \n N<\/mml:mi>\n <\/mml:mrow>\n \n \u00af<\/mml:mo>\n <\/mml:mrow>\n <\/mml:mover>\n \n a<\/mml:mi>\n 1<\/mml:mn>\n <\/mml:mrow>\n <\/mml:msub>\n =<\/mml:mo>\n 0.03<\/mml:mn>\n <\/mml:mrow>\n <\/mml:math>\n <\/jats:inline-formula>\n ) and 2) a slower transfer rate (\n \n \n \n \n k<\/mml:mi>\n \u00af<\/mml:mo>\n <\/mml:mover>\n \n E<\/mml:mi>\n T<\/mml:mi>\n 2<\/mml:mn>\n <\/mml:mrow>\n <\/mml:msub>\n =<\/mml:mo>\n 4.1<\/mml:mn>\n \u00a0<\/mml:mo>\n \n \n \n 10<\/mml:mn>\n 8<\/mml:mn>\n <\/mml:msup>\n <\/mml:mrow>\n <\/mml:mfenced>\n \u00a0<\/mml:mo>\n \n s<\/mml:mi>\n \n -<\/mml:mo>\n 1<\/mml:mn>\n <\/mml:mrow>\n <\/mml:msup>\n <\/mml:math>\n <\/jats:inline-formula>\n ) with a higher acceptor number (\n \n \n \n \n \n \n N<\/mml:mi>\n <\/mml:mrow>\n \n \u00af<\/mml:mo>\n <\/mml:mrow>\n <\/mml:mover>\n \n a<\/mml:mi>\n 2<\/mml:mn>\n <\/mml:mrow>\n <\/mml:msub>\n =<\/mml:mo>\n 0.18<\/mml:mn>\n <\/mml:mrow>\n <\/mml:math>\n <\/jats:inline-formula>\n ). We assign these distributions to the indirect and direct electron transfer mechanisms, respectively. Our findings demonstrate how spectroscopic imaging can uncover fundamental electron transfer mechanisms at complex interfaces, offering valuable design principles for future nano\u2013bio hybrids.\n <\/jats:p>","DOI":"10.1073\/pnas.2407987122","type":"journal-article","created":{"date-parts":[[2025,3,17]],"date-time":"2025-03-17T15:32:56Z","timestamp":1742225576000},"update-policy":"https:\/\/doi.org\/10.1073\/pnas.cm10313","source":"Crossref","is-referenced-by-count":11,"title":["Spatially resolved charge-transfer kinetics at the quantum dot\u2013microbe interface using fluorescence lifetime imaging microscopy"],"prefix":"10.1073","volume":"122","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-0398-5725","authenticated-orcid":false,"given":"Mokshin","family":"Suri","sequence":"first","affiliation":[{"name":"Department of Materials Science and Engineering, Cornell University","place":["Ithaca"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Farshid","family":"Salimi Jazi","sequence":"additional","affiliation":[{"name":"Department of Biological and Environmental Engineering, Cornell University","place":["Ithaca"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4220-8152","authenticated-orcid":false,"given":"Jack C.","family":"Crowley","sequence":"additional","affiliation":[{"name":"Department of Applied and Engineering Physics, Cornell University","place":["Ithaca"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0681-6487","authenticated-orcid":false,"given":"Youngchan","family":"Park","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Chemical Biology, Cornell University","place":["Ithaca"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9952-2244","authenticated-orcid":false,"given":"Bing","family":"Fu","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Chemical Biology, Cornell University","place":["Ithaca"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8582-7661","authenticated-orcid":false,"given":"Peng","family":"Chen","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Chemical Biology, Cornell University","place":["Ithaca"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2640-329X","authenticated-orcid":false,"given":"Warren R.","family":"Zipfel","sequence":"additional","affiliation":[{"name":"Department of Applied and Engineering Physics, Cornell University","place":["Ithaca"]},{"name":"Meinig School of Biomedical Engineering, Cornell University","place":["Ithaca"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2218-6152","authenticated-orcid":false,"given":"Buz","family":"Barstow","sequence":"additional","affiliation":[{"name":"Department of Biological and Environmental Engineering, Cornell University","place":["Ithaca"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5782-4666","authenticated-orcid":false,"given":"Tobias","family":"Hanrath","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering, Cornell University","place":["Ithaca"]},{"name":"Robert F. 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