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Stimuli-Responsive Electronic Reconfiguration in Benzo(ghi)perylene-TCNQ Donor–Acceptor Crystalline Networks

Gubanov, Kirill ; Reva, Yana ; Bo, Yifan ; Hampel, Frank ; Späth, Andreas ; Beinik, Igor LU orcid ; Thånell, Karina LU ; Brzhezinskaya, Maria ; Furxhiu, Stevie and Uhlein, Timo , et al. (2025) In Chemistry of Materials 37(17). p.6932-6942
Abstract

Template-assisted crystal engineering provides a powerful strategy for constructing ordered networks tailored to organic electronic applications. We introduce a solution-based strategy to fabricate crystalline needle-like arrays of charge-transfer complexes (CTCs) between electron-donating benzo(ghi)perylene (BP) and electron-accepting TCNQ. Well-defined square-crystals of BP polymorphs were employed as templates for the spatially controlled anisotropic growth of CTC needle-like arrays. By tuning concentration and deposition rates, we modulated BP crystal dimensions and hence controlled the growth of needle-networks mimicking the template spatial scale. In solution, these free-standing flexible meshes were detached from the BPs and... (More)

Template-assisted crystal engineering provides a powerful strategy for constructing ordered networks tailored to organic electronic applications. We introduce a solution-based strategy to fabricate crystalline needle-like arrays of charge-transfer complexes (CTCs) between electron-donating benzo(ghi)perylene (BP) and electron-accepting TCNQ. Well-defined square-crystals of BP polymorphs were employed as templates for the spatially controlled anisotropic growth of CTC needle-like arrays. By tuning concentration and deposition rates, we modulated BP crystal dimensions and hence controlled the growth of needle-networks mimicking the template spatial scale. In solution, these free-standing flexible meshes were detached from the BPs and redeposited onto variable substrates, while the BP templates remain undissolved, enabling repeated fabrication cycles. CTC formation induces an electronic redistribution with thermally reversible modulation of characteristic electronic states. Such transformation modifies the BP luminescence character: while bare BP exhibits a strong green emission, it is quenched in the presence of TCNQ and replaced by a weaker blueish CTC emission, establishing a charge-transfer-mediated photonic response. Our study provides a combination of crystal engineering with microspectroscopic insights offering a highly sensitive handle for elucidating charge redistribution and modulation of electronic states in CTC upon external stimuli.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Chemistry of Materials
volume
37
issue
17
pages
11 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • scopus:105015553962
ISSN
0897-4756
DOI
10.1021/acs.chemmater.5c01859
language
English
LU publication?
yes
id
a5daa364-50a4-4b01-87e1-d2296098a74d
date added to LUP
2025-10-15 11:48:36
date last changed
2025-10-15 11:49:53
@article{a5daa364-50a4-4b01-87e1-d2296098a74d,
  abstract     = {{<p>Template-assisted crystal engineering provides a powerful strategy for constructing ordered networks tailored to organic electronic applications. We introduce a solution-based strategy to fabricate crystalline needle-like arrays of charge-transfer complexes (CTCs) between electron-donating benzo(ghi)perylene (BP) and electron-accepting TCNQ. Well-defined square-crystals of BP polymorphs were employed as templates for the spatially controlled anisotropic growth of CTC needle-like arrays. By tuning concentration and deposition rates, we modulated BP crystal dimensions and hence controlled the growth of needle-networks mimicking the template spatial scale. In solution, these free-standing flexible meshes were detached from the BPs and redeposited onto variable substrates, while the BP templates remain undissolved, enabling repeated fabrication cycles. CTC formation induces an electronic redistribution with thermally reversible modulation of characteristic electronic states. Such transformation modifies the BP luminescence character: while bare BP exhibits a strong green emission, it is quenched in the presence of TCNQ and replaced by a weaker blueish CTC emission, establishing a charge-transfer-mediated photonic response. Our study provides a combination of crystal engineering with microspectroscopic insights offering a highly sensitive handle for elucidating charge redistribution and modulation of electronic states in CTC upon external stimuli.</p>}},
  author       = {{Gubanov, Kirill and Reva, Yana and Bo, Yifan and Hampel, Frank and Späth, Andreas and Beinik, Igor and Thånell, Karina and Brzhezinskaya, Maria and Furxhiu, Stevie and Uhlein, Timo and Ng, Siowwoon and Guldi, Dirk M. and Fink, Rainer H.}},
  issn         = {{0897-4756}},
  language     = {{eng}},
  number       = {{17}},
  pages        = {{6932--6942}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{Chemistry of Materials}},
  title        = {{Stimuli-Responsive Electronic Reconfiguration in Benzo(ghi)perylene-TCNQ Donor–Acceptor Crystalline Networks}},
  url          = {{http://dx.doi.org/10.1021/acs.chemmater.5c01859}},
  doi          = {{10.1021/acs.chemmater.5c01859}},
  volume       = {{37}},
  year         = {{2025}},
}