Coherent photoexcitation of entangled triplet pair states

Juno Kim; David C. Bain; Vivian Ding; Kanad Majumder; Dean Windemuller; Jiaqi Feng; Jishan Wu; Satish Patil; John Anthony; Woojae Kim; Andrew J. Musser

doi:10.1038/s41557-024-01556-3

Coherent photoexcitation of entangled triplet pair states

Juno Kim, David C. Bain, Vivian Ding, Kanad Majumder, Dean Windemuller, Jiaqi Feng, Jishan Wu, Satish Patil, John Anthony, Woojae Kim, Andrew J. Musser

Research output: Contribution to journal › Article › peer-review

13 Scopus citations

Abstract

The functional properties of organic semiconductors are defined by the interplay between optically bright and dark states. Organic devices require rapid conversion between these bright and dark manifolds for maximum efficiency, and one way to achieve this is through multiexciton generation (S₁→¹TT). The dark state ¹TT is typically generated from bright S₁ after optical excitation; however, the mechanistic details are hotly debated. Here we report a ¹TT generation pathway in which it can be coherently photoexcited, without any involvement of bright S₁. Using <10-fs transient absorption spectroscopy and pumping sub-resonantly, ¹TT is directly generated from the ground state. Applying this method to a range of pentacene dimers and thin films of various aggregation types, we determine the critical material properties that enable this forbidden pathway. Through a strikingly simple technique, this result opens the door for new mechanistic insights into ¹TT and other dark states in organic materials. (Figure presented.)

Original language	English
Pages (from-to)	1680-1686
Number of pages	7
Journal	Nature Chemistry
Volume	16
Issue number	10
DOIs	https://doi.org/10.1038/s41557-024-01556-3
State	Published - Oct 2024

Bibliographical note

Publisher Copyright:
© The Author(s), under exclusive licence to Springer Nature Limited 2024.

Funding

This work made use of the Cornell Center for Materials Research Shared Facilities, which are supported through the NSF MRSEC programme (DMR-1719875). This work was supported by the College of Arts and Sciences at Cornell University (A.J.M.), the US Department of Energy, Office of Science, Basic Energy Sciences, Condensed Phase and Interfacial Molecular Science, Early Career Research Program DE-SC0021941 (A.J.M.), the Alfred P. Sloan Foundation (A.J.M.), Cornell Atkinson Center for Sustainability (A.J.M.), the National Research Foundation of Korea funded by the Ministry of Education 2022R1A6A3A03072477 (J.K.), a National Research Foundation of Korea Grant funded by the Korean Government RS-2023-00210400 (W.K.), National Science Foundation grant no. DMR-1627428 (J.A.), and the Science and Engineering Research Board (SERB), India, through IRHPA grant IPA/2020/000033 and core research grant CRG/2022/004523 (S.P.).

Funders	Funder number
National Research Foundation of Korea
College of Arts and Sciences, Cornell University
Cornell Atkinson Center for Sustainability, Cornell University
U.S. Department of Energy EPSCoR
Alfred P Sloan Foundation
Office of Science Programs
National Science Foundation Arctic Social Science Program	DMR-1627428
DOE Basic Energy Sciences	DE-SC0021941
Science and Engineering Research Board	CRG/2022/004523, IPA/2020/000033
Materials Research Science and Engineering Center, Harvard University	DMR-1719875
Ministry of Education China	RS-2023-00210400, 2022R1A6A3A03072477

ASJC Scopus subject areas

General Chemistry
General Chemical Engineering

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title = "Coherent photoexcitation of entangled triplet pair states",

abstract = "The functional properties of organic semiconductors are defined by the interplay between optically bright and dark states. Organic devices require rapid conversion between these bright and dark manifolds for maximum efficiency, and one way to achieve this is through multiexciton generation (S1→1TT). The dark state 1TT is typically generated from bright S1 after optical excitation; however, the mechanistic details are hotly debated. Here we report a 1TT generation pathway in which it can be coherently photoexcited, without any involvement of bright S1. Using <10-fs transient absorption spectroscopy and pumping sub-resonantly, 1TT is directly generated from the ground state. Applying this method to a range of pentacene dimers and thin films of various aggregation types, we determine the critical material properties that enable this forbidden pathway. Through a strikingly simple technique, this result opens the door for new mechanistic insights into 1TT and other dark states in organic materials. (Figure presented.)",

author = "Juno Kim and Bain, \{David C.\} and Vivian Ding and Kanad Majumder and Dean Windemuller and Jiaqi Feng and Jishan Wu and Satish Patil and John Anthony and Woojae Kim and Musser, \{Andrew J.\}",

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AU - Kim, Juno

AU - Bain, David C.

AU - Ding, Vivian

AU - Majumder, Kanad

AU - Windemuller, Dean

AU - Feng, Jiaqi

AU - Wu, Jishan

AU - Patil, Satish

AU - Anthony, John

AU - Kim, Woojae

AU - Musser, Andrew J.

PY - 2024/10

Y1 - 2024/10

N2 - The functional properties of organic semiconductors are defined by the interplay between optically bright and dark states. Organic devices require rapid conversion between these bright and dark manifolds for maximum efficiency, and one way to achieve this is through multiexciton generation (S1→1TT). The dark state 1TT is typically generated from bright S1 after optical excitation; however, the mechanistic details are hotly debated. Here we report a 1TT generation pathway in which it can be coherently photoexcited, without any involvement of bright S1. Using <10-fs transient absorption spectroscopy and pumping sub-resonantly, 1TT is directly generated from the ground state. Applying this method to a range of pentacene dimers and thin films of various aggregation types, we determine the critical material properties that enable this forbidden pathway. Through a strikingly simple technique, this result opens the door for new mechanistic insights into 1TT and other dark states in organic materials. (Figure presented.)

AB - The functional properties of organic semiconductors are defined by the interplay between optically bright and dark states. Organic devices require rapid conversion between these bright and dark manifolds for maximum efficiency, and one way to achieve this is through multiexciton generation (S1→1TT). The dark state 1TT is typically generated from bright S1 after optical excitation; however, the mechanistic details are hotly debated. Here we report a 1TT generation pathway in which it can be coherently photoexcited, without any involvement of bright S1. Using <10-fs transient absorption spectroscopy and pumping sub-resonantly, 1TT is directly generated from the ground state. Applying this method to a range of pentacene dimers and thin films of various aggregation types, we determine the critical material properties that enable this forbidden pathway. Through a strikingly simple technique, this result opens the door for new mechanistic insights into 1TT and other dark states in organic materials. (Figure presented.)

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Coherent photoexcitation of entangled triplet pair states

Abstract

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