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These heterojunctions have shown unique interfacial properties not found in either individual component. Here, we use femtosecond transient absorption to reveal photoinduced charge transfer and interlayer exciton formation in a mixed-dimensional type-II heterojunction between monolayer MoS2 and vanadyl phthalocyanine (VOPc). Selective excitation of the MoS2 exciton leads to hole transfer from the MoS2 valence band to VOPc highest occupied molecular orbit in \u223c710\u00a0fs. On the contrary, selective photoexcitation of the VOPc layer leads to instantaneous electron transfer from its excited state to the conduction band of MoS2 in less than 100\u00a0fs. This light-initiated ultrafast separation of electrons and holes across the heterojunction interface leads to the formation of an interlayer exciton. These interlayer excitons formed across the interface lead to longer-lived charge-separated states of up to 2.5\u00a0ns, longer than in each individual layer of this heterojunction. Thus, the longer charge-separated state along with ultrafast charge transfer times provide promising results for photovoltaic and optoelectronic device applications.<\/jats:p>","DOI":"10.1063\/5.0107791","type":"journal-article","created":{"date-parts":[[2022,10,20]],"date-time":"2022-10-20T15:35:37Z","timestamp":1666280137000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":16,"title":["Charge transfer dynamics and interlayer exciton formation in MoS2\/VOPc mixed dimensional heterojunction"],"prefix":"10.1063","volume":"157","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-9716-513X","authenticated-orcid":false,"given":"Madison C.","family":"Schwinn","sequence":"first","affiliation":[{"name":"Department of Chemistry, Northwestern University 1 , Evanston, Illinois 60208, USA"},{"name":"Graduate Program in Applied Physics, Northwestern University 2 , Evanston, Illinois 60201, USA"},{"name":"Chemical Science and Engineering Division, Argonne National Laboratory 3 , Lemont, Illinois 60439, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Shahnawaz R.","family":"Rather","sequence":"additional","affiliation":[{"name":"Department of Chemistry, Northwestern University 1 , Evanston, Illinois 60208, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9676-4141","authenticated-orcid":false,"given":"Changmin","family":"Lee","sequence":"additional","affiliation":[{"name":"Department of Chemistry, Northwestern University 1 , Evanston, Illinois 60208, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Matthew P.","family":"Bland","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering, Northwestern University 4 , Evanston, Illinois 60208, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Thomas W.","family":"Song","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering, Northwestern University 4 , Evanston, Illinois 60208, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5623-5285","authenticated-orcid":false,"given":"Vinod K.","family":"Sangwan","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering, Northwestern University 4 , Evanston, Illinois 60208, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4120-1426","authenticated-orcid":false,"given":"Mark C.","family":"Hersam","sequence":"additional","affiliation":[{"name":"Department of Chemistry, Northwestern University 1 , Evanston, Illinois 60208, USA"},{"name":"Graduate Program in Applied Physics, Northwestern University 2 , Evanston, Illinois 60201, USA"},{"name":"Department of Materials Science and Engineering, Northwestern University 4 , Evanston, Illinois 60208, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8450-6687","authenticated-orcid":false,"given":"Lin X.","family":"Chen","sequence":"additional","affiliation":[{"name":"Department of Chemistry, Northwestern University 1 , Evanston, Illinois 60208, USA"},{"name":"Graduate Program in Applied Physics, Northwestern University 2 , Evanston, Illinois 60201, USA"},{"name":"Chemical Science and Engineering Division, Argonne National Laboratory 3 , Lemont, Illinois 60439, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"317","published-online":{"date-parts":[[2022,11,8]]},"reference":[{"key":"2024022101054698500_c1","doi-asserted-by":"publisher","first-page":"320","DOI":"10.3389\/fchem.2020.00320","volume":"8","year":"2020","journal-title":"Front. 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