Conjugated Polyelectrolyte-Based Complex Fluids as Aqueous Exciton Transport Networks

Johnston, Anna R.; Minckler, Eris D.; Shockley, Mia C. J.; Matsushima, Levi N.; Perry, Sarah L.; Ayzner, Alexander L.

doi:10.1002/anie.202117759

Title: Conjugated Polyelectrolyte-Based Complex Fluids as Aqueous Exciton Transport Networks

Journal Article · 27 February 2022 · Angewandte Chemie (International Edition)

DOI: https://doi.org/10.1002/anie.202117759 · OSTI ID:1981388

Johnston, Anna R. ^[1]; Minckler, Eris D. ^[1]; Shockley, Mia C. J. ^[1]; Matsushima, Levi N. ^[1];

^[2];

^[1]

Univ. of California, Santa Cruz, CA (United States)
Univ. of Massachusetts, Amherst, MA (United States)

The ability to assemble artificial systems that mimic aspects of natural light-harvesting functions is fascinating and attractive for materials design. Given the complexity of such a system, a simple design pathway is desirable. Here, we argue that associative phase separation of oppositely charged conjugated polyelectrolytes (CPEs) can provide such a path in an environmentally benign medium: water. We find that complexation between an exciton–donor and acceptor CPE leads to formation of a complex fluid. We interrogate exciton transfer from the donor to the acceptor CPE within the complex fluid and find that transfer is highly efficient. We also find that excess molecular ions can tune the modulus of the inter-CPE complex fluid. Even at high ion concentrations, CPEs remain complexed with significantly delocalized electronic wavefunctions. In conclusion, our work lays the rational foundation for complex, tunable aqueous light-harvesting systems via the intrinsic thermodynamics of associative phase separation.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1981388

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 20 Vol. 61; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (51)

Polyion Charge Ratio Determines Transition between Bright and Dark Excitons in Donor/Acceptor-Conjugated Polyelectrolyte Complexes Hollingsworth, William R.; Magnanelli, Timothy J.; Segura, Carmen The Journal of Physical Chemistry C, Vol. 122, Issue 39 https://doi.org/10.1021/acs.jpcc.8b06195	journal	August 2018
Semiconducting Eggs and Ladders: Understanding Exciton Landscape Formation in Aqueous π-Conjugated Inter-Polyelectrolyte Complexes Hollingsworth, William R.; Williams, Vanessa; Ayzner, Alexander L. Macromolecules, Vol. 53, Issue 7 https://doi.org/10.1021/acs.macromol.0c00029	journal	March 2020
Organic Photovoltaics: Relating Chemical Structure, Local Morphology, and Electronic Properties Wang, Tonghui; Kupgan, Grit; Brédas, Jean-Luc Trends in Chemistry, Vol. 2, Issue 6 https://doi.org/10.1016/j.trechm.2020.03.006	journal	June 2020
Recent progress in the science of complex coacervation Sing, Charles E.; Perry, Sarah L. Soft Matter, Vol. 16, Issue 12 https://doi.org/10.1039/D0SM00001A	journal	January 2020
Structure and Conductivity of Semiconducting Polymer Hydrogels Huber, Rachel C.; Ferreira, Amy S.; Aguirre, Jordan C. The Journal of Physical Chemistry B, Vol. 120, Issue 26 https://doi.org/10.1021/acs.jpcb.6b02202	journal	April 2016
Efficient polymer solar cells that use conjugated polyelectrolyte with a tetravalent amine-end side chain Shi, Yueqin; Lu, Xiaoxiao; Zhang, Yannan Organic Electronics, Vol. 77 https://doi.org/10.1016/j.orgel.2019.105542	journal	February 2020
Get the Basics Right: Jacobian Conversion of Wavelength and Energy Scales for Quantitative Analysis of Emission Spectra Mooney, Jonathan; Kambhampati, Patanjali The Journal of Physical Chemistry Letters, Vol. 4, Issue 19 https://doi.org/10.1021/jz401508t	journal	October 2013
Phase Behavior and Salt Partitioning in Polyelectrolyte Complex Coacervates Li, Lu; Srivastava, Samanvaya; Andreev, Marat Macromolecules, Vol. 51, Issue 8 https://doi.org/10.1021/acs.macromol.8b00238	journal	April 2018
A Review on Emerging Barrier Materials and Encapsulation Strategies for Flexible Perovskite and Organic Photovoltaics Sutherland, Luke J.; Weerasinghe, Hasitha C.; Simon, George P. Advanced Energy Materials, Vol. 11, Issue 34 https://doi.org/10.1002/aenm.202101383	journal	July 2021
Powering the future of molecular artificial photosynthesis with light-harvesting metallosupramolecular dye assemblies Frischmann, Peter D.; Mahata, Kingsuk; Würthner, Frank Chem. Soc. Rev., Vol. 42, Issue 4 https://doi.org/10.1039/C2CS35223K	journal	January 2013
In-Situ Synthesis of TiO2@GO Nanosheets for Polymers Degradation in a Natural Environment Shi, Yueqin; Yu, Zhanyang; Li, Zhengjun Polymers, Vol. 13, Issue 13 https://doi.org/10.3390/polym13132158	journal	June 2021
Multiphase Adhesive Coacervates Inspired by the Sandcastle Worm Kaur, Sarbjit; Weerasekare, G. Mahika; Stewart, Russell J. ACS Applied Materials & Interfaces, Vol. 3, Issue 4 https://doi.org/10.1021/am200082v	journal	March 2011
Molecular weight fractionation and the self-suppression of complex coacervation Veis, Arthur; Bodor, Edward; Mussell, Shirley Biopolymers, Vol. 5, Issue 1 https://doi.org/10.1002/bip.1967.360050106	journal	January 1967
Ambient Processable and Stable All-Polymer Organic Solar Cells Xu, Yalong; Yuan, Jianyu; Zhou, Sijie Advanced Functional Materials, Vol. 29, Issue 8 https://doi.org/10.1002/adfm.201806747	journal	January 2019
Quenching of aromatic hydrocarbon fluorescence by alkylpyridinium halides Davis, Gene A. Journal of the Chemical Society, Chemical Communications, Issue 19 https://doi.org/10.1039/c39730000728	journal	January 1973
A Supramolecular Artificial Light‐Harvesting System with Two‐Step Sequential Energy Transfer for Photochemical Catalysis Hao, Min; Sun, Guangping; Zuo, Minzan Angewandte Chemie, Vol. 132, Issue 25 https://doi.org/10.1002/ange.201912654	journal	November 2019
Effects of Non-Electrostatic Intermolecular Interactions on the Phase Behavior of pH-Sensitive Polyelectrolyte Complexes Li, Lu; Srivastava, Samanvaya; Meng, Siqi Macromolecules, Vol. 53, Issue 18 https://doi.org/10.1021/acs.macromol.0c00999	journal	August 2020
Compartmentalised RNA catalysis in membrane-free coacervate protocells Drobot, Björn; Iglesias-Artola, Juan M.; Le Vay, Kristian Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-06072-w	journal	September 2018
Yield stress fluid flows: A review of experimental data Coussot, P. Journal of Non-Newtonian Fluid Mechanics, Vol. 211 https://doi.org/10.1016/j.jnnfm.2014.05.006	journal	September 2014
Nanocatalysis under Nanoconfinement: A Metal-Free Hybrid Coacervate Nanodroplet as a Catalytic Nanoreactor for Efficient Redox and Photocatalytic Reactions Saini, Bhawna; Singh, Shivendra; Mukherjee, Tushar Kanti ACS Applied Materials & Interfaces, Vol. 13, Issue 43 https://doi.org/10.1021/acsami.1c17106	journal	October 2021
Efficient polymer solar cells utilizing solution‐processed interlayer based on different conjugated backbones Shi, Yueqin; Yu, Zhanyang; Li, Zhengjun Journal of Applied Polymer Science, Vol. 137, Issue 46 https://doi.org/10.1002/app.49527	journal	June 2020
Fluorescent H-Aggregate Vesicles and Tubes of a Cyanine Dye and Their Potential as Light-Harvesting Antennae Reddy, Nitin Ramesh; Aubin, Megan; Kushima, Akihiro The Journal of Physical Chemistry B, Vol. 125, Issue 28 https://doi.org/10.1021/acs.jpcb.1c04262	journal	July 2021
Recent Progress of Organic Photovoltaics with Efficiency over 17% Wang, Xuelin; Sun, Qianqian; Gao, Jinhua Energies, Vol. 14, Issue 14 https://doi.org/10.3390/en14144200	journal	July 2021
Construction of coacervate-in-coacervate multi-compartment protocells for spatial organization of enzymatic reactions Chen, Yufeng; Yuan, Min; Zhang, Yanwen Chemical Science, Vol. 11, Issue 32 https://doi.org/10.1039/D0SC03849K	journal	January 2020
Theory of optical transitions in conjugated polymers. II. Real systems Marcus, Max; Tozer, Oliver Robert; Barford, William The Journal of Chemical Physics, Vol. 141, Issue 16 https://doi.org/10.1063/1.4897985	journal	October 2014
Solar‐Powered Organic Semiconductor–Bacteria Biohybrids for CO ₂ Reduction into Acetic Acid Gai, Panpan; Yu, Wen; Zhao, Hao Angewandte Chemie International Edition, Vol. 59, Issue 18 https://doi.org/10.1002/anie.202001047	journal	March 2020
Solar‐Powered Organic Semiconductor–Bacteria Biohybrids for CO ₂ Reduction into Acetic Acid Gai, Panpan; Yu, Wen; Zhao, Hao Angewandte Chemie, Vol. 132, Issue 18 https://doi.org/10.1002/ange.202001047	journal	March 2020
Effect of Solvent Quality on the Phase Behavior of Polyelectrolyte Complexes Li, Lu; Rumyantsev, Artem M.; Srivastava, Samanvaya Macromolecules, Vol. 54, Issue 1 https://doi.org/10.1021/acs.macromol.0c01000	journal	December 2020
Bioinspiration in light harvesting and catalysis Proppe, Andrew H.; Li, Yuguang C.; Aspuru-Guzik, Alán Nature Reviews Materials, Vol. 5, Issue 11 https://doi.org/10.1038/s41578-020-0222-0	journal	August 2020
Theory of optical transitions in conjugated polymers. I. Ideal systems Barford, William; Marcus, Max The Journal of Chemical Physics, Vol. 141, Issue 16 https://doi.org/10.1063/1.4897984	journal	October 2014
Review of Waterborne Organic Semiconductor Colloids for Photovoltaics Holmes, Alexandre; Deniau, Elise; Lartigau-Dagron, Christine ACS Nano, Vol. 15, Issue 3 https://doi.org/10.1021/acsnano.0c10161	journal	February 2021
Aqueous Formulation of Concentrated Semiconductive Fluid Using Polyelectrolyte Coacervation Le, My Linh; Rawlings, Dakota; Danielsen, Scott P. O. ACS Macro Letters, Vol. 10, Issue 8 https://doi.org/10.1021/acsmacrolett.1c00354	journal	July 2021
Recent progress of organic photovoltaics for indoor energy harvesting Xie, Lin; Song, Wei; Ge, Jinfeng Nano Energy, Vol. 82 https://doi.org/10.1016/j.nanoen.2021.105770	journal	April 2021
Determining exciton coherence from the photoluminescence spectral line shape in poly(3-hexylthiophene) thin films Spano, Frank C.; Clark, Jenny; Silva, Carlos The Journal of Chemical Physics, Vol. 130, Issue 7 https://doi.org/10.1063/1.3076079	journal	February 2009
Polyelectrolyte Complexes Consisting of Macromolecules With Varied Stiffness: Computer Simulation Lazutin, Alexei A.; Semenov, Alexander N.; Vasilevskaya, Valentina V. Macromolecular Theory and Simulations, Vol. 21, Issue 5 https://doi.org/10.1002/mats.201100097	journal	February 2012
Viscoelastic Conjugated Polymer Fluids Shinohara, Akira; Pan, Chengjun; Guo, Zhenfeng Angewandte Chemie International Edition, Vol. 58, Issue 28 https://doi.org/10.1002/anie.201903148	journal	July 2019
Interaction of Tetraethylammonium Ion Derivatives with the Potassium Channels of Giant Axons Armstrong, Clay M. Journal of General Physiology, Vol. 58, Issue 4 https://doi.org/10.1085/jgp.58.4.413	journal	October 1971
Origin of apparent viscosity in yield stress fluids below yielding Møller, P. C. F.; Fall, A.; Bonn, D. EPL (Europhysics Letters), Vol. 87, Issue 3 https://doi.org/10.1209/0295-5075/87/38004	journal	August 2009
Complexation of a Conjugated Polyelectrolyte and Impact on Optoelectronic Properties Danielsen, Scott P. O.; Nguyen, Thuc-Quyen; Fredrickson, Glenn H. ACS Macro Letters, Vol. 8, Issue 1 https://doi.org/10.1021/acsmacrolett.8b00924	journal	January 2019
Nanoscale Strategies for Light Harvesting Kundu, Simanta; Patra, Amitava Chemical Reviews, Vol. 117, Issue 2 https://doi.org/10.1021/acs.chemrev.6b00036	journal	March 2016
Coacervate delivery systems for proteins and small molecule drugs Johnson, Noah R.; Wang, Yadong Expert Opinion on Drug Delivery, Vol. 11, Issue 12 https://doi.org/10.1517/17425247.2014.941355	journal	August 2014
A Supramolecular Artificial Light‐Harvesting System with Two‐Step Sequential Energy Transfer for Photochemical Catalysis Hao, Min; Sun, Guangping; Zuo, Minzan Angewandte Chemie International Edition, Vol. 59, Issue 25 https://doi.org/10.1002/anie.201912654	journal	November 2019
Multiphase Complex Coacervate Droplets Lu, Tiemei; Spruijt, Evan Journal of the American Chemical Society, Vol. 142, Issue 6 https://doi.org/10.1021/jacs.9b11468	journal	January 2020
Solid-to-Liquid Phase Transition in Polyelectrolyte Complexes Meng, Siqi; Ting, Jeffrey M.; Wu, Hao Macromolecules, Vol. 53, Issue 18 https://doi.org/10.1021/acs.macromol.0c00930	journal	August 2020
The role of coacervation and phase transitions in the sandcastle worm adhesive system Stewart, Russell J.; Wang, Ching Shuen; Song, In Taek Advances in Colloid and Interface Science, Vol. 239 https://doi.org/10.1016/j.cis.2016.06.008	journal	January 2017
π⁺–π Interactions between (Hetero)aromatic Amine Cations and the Graphitic Surfaces of Pyrogenic Carbonaceous Materials Xiao, Feng; Pignatello, Joseph J. Environmental Science & Technology, Vol. 49, Issue 2 https://doi.org/10.1021/es5043029	journal	January 2015
Associative Phase Separation of Aqueous π-Conjugated Polyelectrolytes Couples Photophysical and Mechanical Properties Johnston, Anna R.; Perry, Sarah L.; Ayzner, Alexander L. Chemistry of Materials, Vol. 33, Issue 4 https://doi.org/10.1021/acs.chemmater.0c02424	journal	February 2021
Viskoelastische konjugierte polymere Fluide Shinohara, Akira; Pan, Chengjun; Guo, Zhenfeng Angewandte Chemie, Vol. 131, Issue 28 https://doi.org/10.1002/ange.201903148	journal	May 2019
Organic Semiconductor–Organism Interfaces for Augmenting Natural and Artificial Photosynthesis Zhou, Xin; Zeng, Yue; Lv, Fengting Accounts of Chemical Research, Vol. 55, Issue 2 https://doi.org/10.1021/acs.accounts.1c00580	journal	December 2021
Systematic Study of Quaternary Ammonium Cations for Bromine Sequestering Application in High Energy Density Electrolytes for Hydrogen Bromine Redox Flow Batteries Küttinger, Michael; Loichet Torres, Paulette A.; Meyer, Emeline Molecules, Vol. 26, Issue 9 https://doi.org/10.3390/molecules26092721	journal	May 2021
Quenching of fluorescence from pyrene-labeled poly(N-isopropylacrylamide) solutions heated above their lower critical solution temperature Winnik, Francoise M. Macromolecules, Vol. 23, Issue 6 https://doi.org/10.1021/ma00208a014	journal	March 1990

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
chemistry
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energy transfer
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Title: Conjugated Polyelectrolyte-Based Complex Fluids as Aqueous Exciton Transport Networks

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