title: Ultrafast Exciton Dissociation and Long-Lived Charge Separation in a Photovoltaic Pentacene-MoS2van der Waals Heterojunction.
abstract: van der Waals heterojunctions between two-dimensional (2D) layered materials and nanomaterials of different dimensions present unique opportunities for gate-tunable optoelectronic devices. Mixed-dimensional p-n heterojunction diodes, such as p-type pentacene (0D) and n-type monolayer MoS2(2D), are especially interesting for photovoltaic applications where the absorption cross-section and charge transfer processes can be tailored by rational selection from the vast library of organic molecules and 2D materials. Here, we study the kinetics of excited carriers in pentacene-MoS2p-n type-II heterojunctions by transient absorption spectroscopy. These measurements show that the dissociation of MoS2excitons occurs by hole transfer to pentacene on the time scale of 6.7 ps. In addition, the charge-separated state lives for 5.1 ns, up to an order of magnitude longer than the recombination lifetimes from previously reported 2D material heterojunctions. By studying the fractional amplitudes of the MoS2decay processes, the hole transfer yield from MoS2to pentacene is found to be ∼50%, with the remaining holes undergoing trapping due to surface defects. Overall, the ultrafast charge transfer and long-lived charge-separated state in pentacene-MoS2p-n heterojunctions suggest significant promise for mixed-dimensional van der Waals heterostructures in photovoltaics, photodetectors, and related optoelectronic technologies.
authors.affiliation: Department of Chemistry and ‡Department of Materials Science and Engineering, Northwestern University , Evanston, Illinois 60208, United States.
authors.forename: Stephanie
authors.initials: S
authors.lastname: Bettis Homan
authors.affiliation: Department of Chemistry and ‡Department of Materials Science and Engineering, Northwestern University , Evanston, Illinois 60208, United States.
authors.forename: Vinod K
authors.initials: VK
authors.lastname: Sangwan
authors.affiliation: Department of Chemistry and ‡Department of Materials Science and Engineering, Northwestern University , Evanston, Illinois 60208, United States.
authors.forename: Itamar
authors.identifier: 0000-0002-9358-5743
authors.initials: I
authors.lastname: Balla
authors.affiliation: Department of Chemistry and ‡Department of Materials Science and Engineering, Northwestern University , Evanston, Illinois 60208, United States.
authors.forename: Hadallia
authors.initials: H
authors.lastname: Bergeron
authors.affiliation: Department of Chemistry and ‡Department of Materials Science and Engineering, Northwestern University , Evanston, Illinois 60208, United States.
authors.forename: Emily A
authors.initials: EA
authors.lastname: Weiss
authors.affiliation: Department of Chemistry and ‡Department of Materials Science and Engineering, Northwestern University , Evanston, Illinois 60208, United States.
authors.forename: Mark C
authors.identifier: 0000-0003-4120-1426
authors.initials: MC
authors.lastname: Hersam
keywords: Organic; charge transfer; transient absorption spectroscopy; transition metal dichalcogenide; ultrafast