Pressure-Treated Luminescent and Structural Evolution With Irreversible Control of Emission in Through-Space Charge Transfer Emitter.

Λεπτομέρειες βιβλιογραφικής εγγραφής
Τίτλος: Pressure-Treated Luminescent and Structural Evolution With Irreversible Control of Emission in Through-Space Charge Transfer Emitter.
Συγγραφείς: Li A; School of Physical Science and Information Technology, Liaocheng University, Liaocheng, China., Chen Z; School of Physical Science and Information Technology, Liaocheng University, Liaocheng, China., Fu R; School of Physical Science and Information Technology, Liaocheng University, Liaocheng, China., Song X; Institute of Molecular Aggregation Science, Tianjin University, Tianjin, China., Song Z; Institute of Molecular Aggregation Science, Tianjin University, Tianjin, China., Wang J; Institute of Molecular Aggregation Science, Tianjin University, Tianjin, China., Li Q; School of Physical Science and Information Technology, Liaocheng University, Liaocheng, China., Wang K; School of Physical Science and Information Technology, Liaocheng University, Liaocheng, China., Xie Y; Institute of Molecular Aggregation Science, Tianjin University, Tianjin, China., Li Z; Institute of Molecular Aggregation Science, Tianjin University, Tianjin, China.; Hubei Key Lab on Organic and Polymeric Opto-Electronic Materials, Department of Chemistry, Wuhan University, Wuhan, China.; College of Chemistry and Chemical Engineering, Hubei University, Wuhan, China.
Πηγή: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2026 Oct 05; Vol. 65 (41), pp. e9247211. Date of Electronic Publication: 2026 Aug 12.
Τύπος έκδοσης: Journal Article
Γλώσσα: English
Στοιχεία περιοδικού: Publisher: Wiley-VCH Country of Publication: Germany NLM ID: 0370543 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1521-3773 (Electronic) Linking ISSN: 14337851 NLM ISO Abbreviation: Angew Chem Int Ed Engl Subsets: MEDLINE; PubMed not MEDLINE
Imprint Name(s): Publication: <2004-> : Weinheim : Wiley-VCH
Original Publication: Weinheim/Bergstr. : New York, : Verlag Chemie ; Academic Press, c1962-
Περίληψη: Through-space charge transfer (TSCT) is gaining prominence for developing solid-state luminophores, owing to its tunable and dynamically regulable luminescence. In this work, a novel TSCT emitter with a spatially segregated donor-acceptor (D-A) architecture is designed and synthesized, which exhibits high-efficiency blue-violet emission at 410 nm with a narrow 37 nm FWHM and minimal Stokes shift due to molecular rigidity and suppressed structural reorganization. DMAC-CBO crystal demonstrates remarkable mechanochromism through grinding-induced amorphization and a pronounced piezochromic response showing a 156 nm redshift in the range of 14.0 GPa due to the decreased distance between D and A units. As a result, pressure-induced the enhancement of intramolecular and intermolecular interactions promote excimer formation, leading to redshifted emission and enabling the modulation of the dominant emissive state from a local excited (LE) state to an excimer. Impressively, upon decompression from high pressure, DMAC-CBO retains a metastable phase, resulting in irreversibly shifted and broadened luminescence derived from excimers. These findings not only demonstrate that pressure can continuously regulate the distance between D and A units of TSCT-based materials, but also effectively establish a structure-property framework for TSCT-based smart materials with tunable and persistent emission, offering promising applications in data storage, sensing, and optoelectronics.
(© 2026 Wiley‐VCH GmbH.)
References: R. R. Palem, G. Shimoga, S.‐H. Lee, H.‐S. Kim, and C. Nathula, “Recent Advances in OLED Applications of TADF Materials With Decreased Singlet‐Triplet Energy Gaps,” Coordination Chemistry Reviews 556 (2026): 217679, https://doi.org/10.1016/j.ccr.2026.217679.
S. Shao and L. Wang, “Through‐Space Charge Transfer Polymers for Solution‐Processed Organic Light‐Emitting Diodes,” Aggregate 1 (2020): 45–56, https://doi.org/10.1002/agt2.4.
J. Zhang, D. Li, W. Li, et al., “Highly Efficient Through‐Space Charge Transfer TADF Molecule Employed in TADF‐ and TADF‐Sensitized Organic Light‐Emitting Diodes,” Science China Chemistry 67 (2024): 1270–1276, https://doi.org/10.1007/s11426‐023‐1894‐1.
S. Ye, D. Fuglistaller, T. Tian, et al., “Lighting up Aggregate Emission of Perylene Diimide by Leveraging Polymerization‐Mediated Through‐Space Charge Transfer and π‐π stacking,” Science China Chemistry 67 (2024): 4218–4233, https://doi.org/10.1007/s11426‐024‐2032‐6.
Q. Li, J. Hu, J. Lv, et al., “Through‐Space Charge‐Transfer Polynorbornenes With Fixed and Controllable Spatial Alignment of Donor and Acceptor for High‐Efficiency Blue Thermally Activated Delayed Fluorescence,” Angewandte Chemie International Edition 59 (2020): 20174–20182, https://doi.org/10.1002/anie.202008912.
Y. K. Qu, Q. Zheng, D. Y. Zhou, L. S. Cui, L. S. Liao, and Z. Q. Jiang, “Unraveling the Configuration Modulation in Spiro‐Based Through‐Space Charge Transfer Materials,” Angewandte Chemie International Edition 64 (2025): e202418008, https://doi.org/10.1002/anie.202418008.
Z. Shuai, Q. Sun, J. Ren, T. Jiang, and W. Li, “Excited State Structure and Decay Rates for Aggregates,” Aggregate 6 (2025): e70013, https://doi.org/10.1002/agt2.70013.
J. Xu, J. Xue, Y. Dai, et al., “π‐Bridge Mediated Coupling Between Inter‐ and Intra‐Molecular Charge Transfer in Aggregates For Highly Efficient Near‐Infrared Emission,” Aggregate 5 (2024): e634, https://doi.org/10.1002/agt2.634.
D. J. Cram and H. Steinberg, “Macro Rings. I. Preparation and Spectra of the Paracyclophanes,” Journal of the American Chemical Society 73 (1951): 5691–5704, https://pubs.acs.org/doi/abs/10.1021/ja01156a059.
D. J. Cram, N. L. Allinger, and H. Steinberg, “Macro Rings. VII. The Spectral Consequences of Bringing Two Benzene Rings Face to Face 1,” Journal of the American Chemical Society 76 (1954): 6132–6141, https://doi.org/10.1021/ja01652a081.
A. Batra, G. Kladnik, H. Vázquez, et al., “Quantifying Through‐Space Charge Transfer Dynamics in π‐Coupled Molecular Systems,” Nature Communications 3 (2012): 1086, https://doi.org/10.1038/ncomms2083.
J. Zhang, Z. Xiong, J. W. Y. Lam, J. Z. Sun, H. Zhang, and B. Z. Tang, “Through‐Space Interactions of Optoelectronic Materials,” Chemical Society Reviews 55 (2026): 2493–2573, https://doi.org/10.1039/d3cs00996c.
S. Y. Yang, Y. K. Qu, L. S. Liao, Z. Q. Jiang, and S. T. Lee, “Research Progress of Intramolecular π‐Stacked Small Molecules for Device Applications,” Advanced Materials 34 (2022): 2104125, https://doi.org/10.1002/adma.202104125.
P. Shen, H. Liu, Z. Zhuang, J. Zeng, Z. Zhao, and B. Z. Tang, “Through‐Space Conjugated Electron Transport Materials for Improving Efficiency and Lifetime of Organic Light‐Emitting Diodes,” Advanced Science 9 (2022): 2200374, https://doi.org/10.1002/advs.202200374.
C. Yin, D. Zhang, Y. Zhang, et al., “High‐Efficiency Narrow‐Band Electro‐Fluorescent Devices With Thermally Activated Delayed Fluorescence Sensitizers Combined Through‐Bond and Through‐Space Charge Transfers,” CCS Chemistry 2 (2020): 1268–1277, https://doi.org/10.31635/ccschem.020.202000243.
W. Tu, Z. Xiong, L. Wang, et al., “The Superiority of Nonconjugated Structures in Fluorescence: Through‐Space vs. Through‐Bond Charge Transfer,” Science China Chemistry 67 (2024): 3121–3130, https://doi.org/10.1007/s11426‐024‐2015‐9.
J. Chen, X. Zhang, Z. Xie, and B. Liu, “Ultralong Thermally Activated Delayed Fluorescence Based on Intermolecular Charge Transfer Induced by Isomer in Carbazole Derivative,” Aggregate 5 (2024): e638, https://doi.org/10.1002/agt2.638.
J. Guo, C. Shi, Y. Zhen, and W. Hu, “Rational Control of Packing Arrangements in Organic Semiconducting Materials Toward High‐Performance Optoelectronics,” Accounts of Materials Research 5 (2024): 907–919, https://doi.org/10.1021/accountsmr.4c00054.
Y. Sagara, S. Yamane, M. Mitani, C. Weder, and T. Kato, “Mechanoresponsive Luminescent Molecular Assemblies: An Emerging Class of Materials,” Advanced Materials 28 (2016): 1073–1095, https://doi.org/10.1002/adma.201504125.
Y. Chen, G. Mellot, D. van Luijk, C. Creton, and R. P. Sijbesma, “Mechanochemical Tools for Polymer Materials,” Chemical Society Reviews 50 (2021): 4100–4140, https://doi.org/10.1039/D0CS00940G.
N. Kazuhiko, S. Shohei, Y. Hitoshi, et al., “Distinct Responses to Mechanical Grinding and Hydrostatic Pressure in Luminescent Chromism of Tetrathiazolylthiophene,” Journal of the American Chemical Society 135 (2013): 10322–10325, https://doi.org/10.1021/ja4055228.
Y. Liu, Q. Zeng, B. Zou, Y. Liu, B. Xu, and W. Tian, “Piezochromic Luminescence of Donor–Acceptor Cocrystals: Distinct Responses to Anisotropic Grinding and Isotropic Compression,” Angewandte Chemie International Edition 57 (2018): 15670–15674, https://doi.org/10.1002/anie.201810149.
A. Li, J. Wang, and Z. Li, “Strategies to Achieve Luminescence Enhancement for Piezochromic Materials Under High Pressure,” Cell Reports Physical Science 6 (2025): 102733, https://doi.org/10.1016/j.xcrp.2025.102733.
L. Tu, Y. Fan, C. Bi, et al., “How Temperature and Hydrostatic Pressure Impact Organic Room Temperature Phosphorescence From H‐Aggregation of Planar Triarylboranes and the Application in Bioimaging,” Science China Chemistry 66 (2023): 816–825, https://doi.org/10.1007/s11426‐022‐1469‐2.
A. Li, Z. Liu, M. Gao, et al., “Conformation‐Determined Emission Enhancement of Phenothiazine Derivatives Under High Pressure,” Materials Chemistry Frontiers 8 (2024): 2420–2427, https://doi.org/10.1039/D4QM00110A.
J. Zou, Y. Fang, Y. Shen, et al., “Piezochromic Tetracoordinate Boron Complex: Blue‐Shifted and Enhanced Luminescence,” Angewandte Chemie International Edition 61 (2022): e202207426, https://doi.org/10.1002/anie.202207426.
J. Ruan, Y. Wang, X. Yang, et al., “Pressure‐Tailored π‐π Stacking in Dimers Enhances Blue Photoluminescence in Boron‐Based Organic Molecules,” Laser & Photonics Reviews 19 (2025): 2401537, https://doi.org/10.1002/lpor.202401537.
Q. Yang, X. Yang, Y. Wang, et al., “Brightening Triplet Excitons Enable High‐Performance White‐Light Emission in Organic Small Molecules via Integrating n–π*/π–π* transitions,” Nature Communications 15 (2024): 7778, https://doi.org/10.1038/s41467‐024‐52196‐7.
S. Hu, X. Yin, S. Liu, et al., “Lighting up Nonemissive Azobenzene Derivatives by Pressure,” Journal of the American Chemical Society 146 (2024): 28961–28972, https://doi.org/10.1021/jacs.4c09784.
S. Y. Yang, Z. Q. Feng, Z. Fu, et al., “Highly Efficient Sky‐Blue π‐Stacked Thermally Activated Delayed Fluorescence Emitter With Multi‐Stimulus Response Properties,” Angewandte Chemie International Edition 61 (2022): e202206861, https://doi.org/10.1002/anie.202206861.
Q. Qi, J. Qian, X. Tan, et al., “Remarkable Turn‐on and Color‐Tuned Piezochromic Luminescence: Mechanically Switching Intramolecular Charge Transfer in Molecular Crystals,” Advanced Functional Materials 25 (2015): 4005–4010, https://doi.org/10.1002/adfm.201501224.
A. Li, Z. Ma, J. Wu, et al., “Pressure‐Induced Wide‐Range Reversible Emission Shift of Triphenylamine‐Substituted Anthracene via Hybridized Local and Charge Transfer (HLCT) Excited State,” Advanced Optical Materials 6 (2018): 1700647, https://doi.org/10.1002/adom.201700647.
Q. Pan, S. Long, J. Li, et al., “Spin Orbit Charge Transfer Enhances Intermolecular Hydrogen Atom Transfer Catalyzed Polymerization for Conductive Elastomers Syntheses,” Chemical Engineering Journal 524 (2025): 169584, https://doi.org/10.1016/j.cej.2025.169584.
L. Xing, J. Wang, W.‐C. Chen, et al., “Highly Efficient Pure‐Blue Organic Light‐Emitting Diodes Based on Rationally Designed Heterocyclic Phenophosphazinine‐Containing Emitters,” Nature Communications 15 (2024): 6175, https://doi.org/10.1038/s41467‐024‐50370‐5.
J. Liu, X. Yin, M. Huang, et al., “High‐Performance Narrowband Pure‐Green OLEDs With Gamut Approaching BT.2020 Standard: Deuteration Promotes Device Efficiency and Lifetime Simultaneously,” Advanced Materials 37 (2025): 2411610, https://doi.org/10.1002/adma.202411610.
J. Dong, L. Chen, Q. Feng, and D.‐T. Yang, “Near‐Infrared‐Emitting Helically Twisted Conjugated Frameworks Consisting of Alternant Donor‐π‐Acceptor Units and Multiple Boron Atoms,” Angewandte Chemie International Edition 64 (2025): e202417200, https://doi.org/10.1002/anie.202417200.
J. Wu, Y. Cheng, J. Lan, et al., “Molecular Engineering of Mechanochromic Materials by Programmed C–H Arylation: Making a Counterpoint in the Chromism Trend,” Journal of the American Chemical Society 138 (2016): 12803–12812, https://doi.org/10.1021/jacs.6b03890.
S. Xu, Y. Duan, and B. Liu, “Precise Molecular Design for High‐Performance Luminogens With Aggregation‐Induced Emission,” Advanced Materials 32 (2020): 1903530, https://doi.org/10.1002/adma.201903530.
J. Mei, N. L. C. Leung, R. T. K. Kwok, J. W. Y. Lam, and B. Z. Tang, “Aggregation‐Induced Emission: Together We Shine, United We Soar!,” Chemical Reviews 115 (2015): 11718–11940, https://doi.org/10.1021/acs.chemrev.5b00263.
Z. Chi, X. Zhang, B. Xu, et al., “Recent Advances in Organic Mechanofluorochromic Materials,” Chemical Society Reviews 41 (2012): 3878, https://doi.org/10.1039/c2cs35016e.
T. Mutai, H. Satou, and K. Araki, “Reproducible on–off Switching of Solid‐State Luminescence by Controlling Molecular Packing Through Heat‐Mode Interconversion,” Nature Materials 4 (2005): 685–687, https://doi.org/10.1038/nmat1454.
Y. Gong, S. He, Y. Li, et al., “Partially Controlling Molecular Packing to Achieve off–on Mechanochromism Through Ingenious Molecular Design,” Advanced Optical Materials 8 (2020): 1902036, https://doi.org/10.1002/adom.201902036.
A. Li, S. Xu, C. Bi, Y. Geng, H. Cui, and W. Xu, “Piezochromic Mechanism of Organic Crystals Under Hydrostatic Pressure,” Materials Chemistry Frontiers 5 (2021): 2588–2606, https://doi.org/10.1039/d0qm00975j.
S. Dai, X. Z. Li, J. Liu, et al., “Conformation‐Confined Organic Butterfly‐Molecule With High Photoluminescence Efficiency, Deep‐Blue Amplified Spontaneous Emission, and Unique Piezochromic Luminescence,” Angewandte Chemie International Edition 64 (2025): e202417734, https://doi.org/10.1002/anie.202414960.
W. Yang, C. Xie, T. Chen, et al., “Dynamic Reversible Full‐Color Piezochromic Fluorogens Featuring Through‐Space Charge‐Transfer Thermally Activated Delayed Fluorescence and their Application as X‐Ray Imaging Scintillators,” Angewandte Chemie International Edition 63 (2024): e202402704, https://doi.org/10.1002/anie.202402704.
Q. Luo, C. Lv, H. Sheng, et al., “Highly Bright Fluorescence From Dispersed Dimers: Deep‐Red Polymorphs and Wide‐Range Piezochromism,” Advanced Optical Materials 8 (2020): 1901836, https://doi.org/10.1002/adom.201901836.
A. Jaffe, Y. Lin, W. L. Mao, and H. I. Karunadasa, “Pressure‐Induced Metallization of the Halide Perovskite (CH3NH3)PbI3,” Journal of the American Chemical Society 139 (2017): 4330–4333, https://doi.org/10.1021/jacs.7b01162.
S. Tong, J. Dai, J. Sun, et al., “Fluorescence‐Based Monitoring of the Pressure‐Induced Aggregation Microenvironment Evolution for an AIEgen Under Multiple Excitation Channels,” Nature Communications 13 (2022): 5234, https://doi.org/10.1038/s41467‐022‐32968‐9.
J. Mei, Y. Hong, J. W. Y. Lam, A. Qin, Y. Tang, and B. Z. Tang, “Aggregation‐Induced Emission: The Whole Is More Brilliant Than the Parts,” Advanced Materials 26 (2014): 5429–5479, https://doi.org/10.1002/adma.201401356.
Y. Wang, Z. Xiong, Y. Wang, et al., “Pressure‐Engineered Through‐Space Conjugation for Precise Control of Clusteroluminescence,” Angewandte Chemie International Edition 64 (2025): e202420502, https://doi.org/10.1002/anie.202420502.
C. Zhao, Z. Ding, Y. Zhang, et al., “Thermally Activated Delayed Fluorescence With Dual‐Emission And Pressure‐Induced Bidirectional Shifting: Cooperative Effects of Intramolecular and Intermolecular Energy Transfer,” Chemical Science 14 (2023): 1089–1096, https://doi.org/10.1039/d2sc05792a.
Y. Wang, S. Guo, H. Luo, et al., “Reaching 90% Photoluminescence Quantum Yield in One‐Dimensional Metal Halide C4N2H14PbBr4 by Pressure‐Suppressed Nonradiative Loss,” Journal of the American Chemical Society 142 (2020): 16001–16006, https://doi.org/10.1021/jacs.0c07166.
B. R. Fisher, H.‐J. Eisler, N. E. Stott, and M. G. Bawendi, “Emission Intensity Dependence and Single‐Exponential Behavior in Single Colloidal Quantum Dot Fluorescence Lifetimes,” Journal of Physical Chemistry B 108 (2004): 143–148, https://doi.org/10.1021/jp035756.
A. Li, J. Wang, C. Bi, et al., “New Insight Into π–π Interactions: Realization of Full Color Emission From Blue to Red Under Hydrostatic Pressure Without Exogenous Intramolecular Charge Transfer,” Journal of Materials Chemistry C 12 (2024): 17377–17385, https://doi.org/10.1039/d4tc03810j.
Y. Xu, W. Zhao, X. Wang, et al., “Pressure‐Induced Emission Luminogens From Antimony Chloride Dimers Toward White‐Light Emission Harvesting,” Laser & Photonics Reviews 19 (2025): 2501683, https://doi.org/10.1002/lpor.202501683.
Q. Li, S. Li, K. Wang, Z. Quan, Y. Meng, and B. Zou, “High‐Pressure Study of Perovskite‐Like Organometal Halide: Band‐Gap Narrowing and Structural Evolution of [NH3‐(CH2)4‐NH3]CuCl4,” Journal of Physical Chemistry Letters 8 (2017): 500–506, https://doi.org/10.1021/acs.jpclett.6b02786.
J. Jiang, X. Li, P. Zhu, et al., “Effect of Pressure on 4‐Toluenesulfonyl Azide Studied by Raman Scattering and Synchrotron X‐Ray Diffraction,” Journal of Physical Chemistry C 121 (2017): 1032–1039, https://doi.org/10.1021/acs.jpcc.6b11016.
Q. Yang, W. Wang, Y. Yang, et al., “Pressure Treatment Enables White‐Light Emission in Zn‐IPA MOF via Asymmetrical Metal‐Ligand Chelate Coordination,” Nature Communications 16 (2025): 696, https://doi.org/10.1038/s41467‐025‐55978‐9.
K. Dziubek, M. Citroni, S. Fanetti, A. B. Cairns, and R. Bini, “High‐Pressure High‐Temperature Structural Properties of Urea,” Journal of Physical Chemistry C 121 (2017): 2380–2387, https://doi.org/10.1021/acs.jpcc.6b11059.
W. Humphrey, A. Dalke, and K. Schulten, “VMD: Visual Molecular Dynamics,” Journal of Molecular Graphics 14 (1996): 33–38, https://doi.org/10.1016/0263‐7855(96)00018‐5.
T. Lu and F. Chen, “Multiwfn: A Multifunctional Wavefunction Analyzer,” Journal of Computational Chemistry 33 (2012): 580–592, https://doi.org/10.1002/jcc.22885.
T. Lu and Q. Chen, “Independent Gradient Model Based on Hirshfeld Partition: A New Method for Visual Study of Interactions in Chemical Systems,” Journal of Computational Chemistry 43 (2022): 539–555, https://doi.org/10.1002/jcc.26812.
T. Lu, “A Comprehensive Electron Wavefunction Analysis Toolbox for Chemists, Multiwfn,” Journal of Chemical Physics 161 (2024): 082503, https://doi.org/10.1063/5.0216272.
Y. Yang, X. Zhao, J. Liang, et al., “Pressure‐Promoted Self‐Trapped Exciton Emission and White‐Light Harvesting in Lead Halide Metal–Organic Frameworks at Ambient Conditions,” Laser & Photonics Reviews 19 (2025): 2401961, https://doi.org/10.1002/lpor.202401961.
T. Ohsaka, F. Izumi, and Y. Fujiki, “Raman Spectrum of Anatase TiO2,” Journal of Raman Spectroscopy 7 (1978): 321–324, https://doi.org/10.1002/jrs.1250070606.
A. Kailer, Y. G. Gogotsi, and K. G. Nickel, “Raman Microspectroscopy of Nanocrystalline and Amorphous Phases in Hardness Indentations,” Journal of Raman Spectroscopy 30 (1999): 939–946, https://doi.org/10.1002/(sici)1097‐4555(199910)30.
Grant Information: 22205157 National Natural Science Foundation of China; W2411008 National Natural Science Foundation of China; 12174146 National Natural Science Foundation of China; ZR2024QA167 Shandong Provincial Natural Science Foundation Youth Fund project; ZR2023MA009 Shandong Provincial Natural Science Foundation Youth Fund project; 318052381 Liaocheng University High-Level Talents Start-Up Fund for Scientific Research; 318042301 Liaocheng University High-Level Talents Start-Up Fund for Scientific Research; 318042305 Liaocheng University High-Level Talents Start-Up Fund for Scientific Research; 2025-skllmd-13 Open Fund of the State Key Laboratory of Luminescent Materials and Devices; LUGYTD2023-01 Guangyue Young Scholar Innovation Team of Liaocheng University
Contributed Indexing: Keywords: excimer; irreversible transformation; mechanochromism; piezochromism; through‐space charge transfer
Entry Date(s): Date Created: 20260812 Latest Revision: 20261005
Update Code: 20261006
DOI: 10.1002/anie.9247211
PMID: 42584985
Βάση Δεδομένων: MEDLINE
Περιγραφή
ISSN:1521-3773
DOI:10.1002/anie.9247211