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Controlled n‐Doping of Naphthalene‐Diimide‐Based 2D Polymers

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dc.creator Evans, Austin M
dc.creator Collins, Kelsey A
dc.creator Xun, Sangni
dc.creator Allen, Taylor G
dc.creator Jhulki, Samik
dc.creator Castano, Ioannina
dc.creator Smith, Hannah L
dc.creator Strauss, Michael J
dc.creator Oanta, Alexander K
dc.creator Liu, Lujia
dc.creator Sun, Lei
dc.creator Reid, Obadiah G
dc.creator Sini, Gjergji
dc.creator Puggioni, Danilo
dc.creator Rondinelli, James M
dc.creator Rajh, Tijana
dc.creator Gianneschi, Nathan C
dc.creator Kahn, Antoine
dc.creator Freedman, Danna E
dc.creator Li, Hong
dc.creator Barlow, Stephen
dc.creator Rumbles, Garry
dc.creator Brédas, Jean-Luc
dc.creator Marder, Seth R
dc.creator Dichtel, William R
dc.date 2022-12-05T19:24:26Z
dc.date 2022-12-05T19:24:26Z
dc.date 2022
dc.date 2022-12-05T19:20:52Z
dc.date.accessioned 2023-03-01T18:11:55Z
dc.date.available 2023-03-01T18:11:55Z
dc.identifier https://hdl.handle.net/1721.1/146761
dc.identifier Evans, Austin M, Collins, Kelsey A, Xun, Sangni, Allen, Taylor G, Jhulki, Samik et al. 2022. "Controlled n‐Doping of Naphthalene‐Diimide‐Based 2D Polymers." Advanced Materials, 34 (22).
dc.identifier.uri http://localhost:8080/xmlui/handle/CUHPOERS/279120
dc.description 2D polymers (2DPs) are promising as structurally well-defined, permanently porous, organic semiconductors. However, 2DPs are nearly always isolated as closed shell organic species with limited charge carriers, which leads to low bulk conductivities. Here, the bulk conductivity of two naphthalene diimide (NDI)-containing 2DP semiconductors is enhanced by controllably n-doping the NDI units using cobaltocene (CoCp2 ). Optical and transient microwave spectroscopy reveal that both as-prepared NDI-containing 2DPs are semiconducting with sub-2 eV optical bandgaps and photoexcited charge-carrier lifetimes of tens of nanoseconds. Following reduction with CoCp2 , both 2DPs largely retain their periodic structures and exhibit optical and electron-spin resonance spectroscopic features consistent with the presence of NDI-radical anions. While the native NDI-based 2DPs are electronically insulating, maximum bulk conductivities of >10-4  S cm-1 are achieved by substoichiometric levels of n-doping. Density functional theory calculations show that the strongest electronic couplings in these 2DPs exist in the out-of-plane (π-stacking) crystallographic directions, which indicates that cross-plane electronic transport through NDI stacks is primarily responsible for the observed electronic conductivity. Taken together, the controlled molecular doping is a useful approach to access structurally well-defined, paramagnetic, 2DP n-type semiconductors with measurable bulk electronic conductivities of interest for electronic or spintronic devices.
dc.format application/pdf
dc.language en
dc.publisher Wiley
dc.relation 10.1002/ADMA.202101932
dc.relation Advanced Materials
dc.rights Creative Commons Attribution-Noncommercial-Share Alike
dc.rights http://creativecommons.org/licenses/by-nc-sa/4.0/
dc.source DOE repository
dc.title Controlled n‐Doping of Naphthalene‐Diimide‐Based 2D Polymers
dc.type Article
dc.type http://purl.org/eprint/type/JournalArticle


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