Review
Polymer Science
Alexander Schmitt, Barry C. C. Thompson
Summary: Non-conjugated pendant electroactive polymers (NCPEPs) offer the potential of combining desirable optoelectronic properties of conjugated polymers with stability of non-conjugated polymers. This review showcases selected reports on NCPEP homopolymers and copolymers, highlighting the impact of structural variables on the optical, electronic, and physical properties of the polymers. The correlation of structural features with improved pi-stacking and charge carrier mobility serves as a guideline for the targeted design of novel NCPEPs.
MACROMOLECULAR RAPID COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Jun Guan, Zejun Sun, Ramin Ansari, Yujia Liu, Aimi Endo, Masafumi Unno, Armelle Ouali, Shahrea Mahbub, Joseph C. Furgal, Nuttapon Yodsin, Siriporn Jungsuttiwong, Daniel Hashemi, John Kieffer, Richard M. Laine
Summary: Multiple studies have explored the use of cage silsesquioxanes as backbone elements in hybrid polymers, and unexpected photophysical properties of copolymers derived from double decker silsesquioxanes were discovered, suggesting unconventional conjugation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Polymer Science
Zhi-Chao Yan, Yanan Li, Zhenfeng Guo, Akira Shinohara, Takashi Nakanishi, Guangming Chen, Chengjun Pan, Florian J. Stadler
Summary: This study examines the linear viscoelasticity of viscoelastic conjugated polymers based on dialkyl-fluorene and dialkoxybenzene over a wide temperature range. Three dynamic transition temperatures are identified and attributed to different parts of the polymer structure. The findings suggest that the properties of different components of the polymer exhibit distinct behaviors under varying temperature conditions.
Article
Polymer Science
Alexander Schmitt, Negar Kazerouni, Barry C. Thompson
Summary: Recent reports have shown that altering structural variables of non-conjugated pendant electroactive polymers (NCPEPs), such as stereoregularity, nature of the pendant group, and length of the spacer, is significant for tuning their optoelectronic properties. The post-polymerization functionalization method allows for selectively studying the effects of tuning these variables, but its scope for tuning the pendant group itself remains largely unexplored. This work investigates the compatibility of the photochemical thiol-ene post-polymerization method with various pendant groups and discusses the limitations and effects on the optoelectronic properties of the functionalized NCPEPs.
Article
Engineering, Electrical & Electronic
Madison Mooney, Yunfei Wang, Ekaterini Iakovidis, Xiaodan Gu, Simon Rondeau-Gagne
Summary: Organic semiconducting polymers offer good mechanical and optoelectronic properties, with solution processability for cost-effective device fabrication compared to silicon-based electronics. This study incorporates environmentally friendly carbohydrate side chains to enhance processability, and introduces a mild postprocessing treatment for solvent resistance. The environmentally friendly approach improves solubility in eco-friendly solvents without negatively impacting electronic performance.
ACS APPLIED ELECTRONIC MATERIALS
(2022)
Review
Chemistry, Physical
Tao Wang, Yiwen Bao, Mengdi Zhuang, Jiacheng Li, Juncheng Chen, Hangxun Xu
Summary: Soft electronics benefit greatly from soft and stretchable conducting polymers with exceptional mechanical compliance and electrical performance. Strategies to enhance the performance of conducting polymers through nanostructuring have been developed in recent years, improving key parameters such as electrical conductivity, stretchability, sensitivity, and self-healing property in soft electronic devices. Future challenges and directions in engineering nanostructured conducting polymers for soft electronics are also discussed.
Article
Nanoscience & Nanotechnology
Manish Pandey, Heriyanto Syafutra, Nikita Kumari, Shyam S. Pandey, Ryo Abe, Hiroaki Benten, Masakazu Nakamura
Summary: The layer-by-layer fabrication of large-area uniformly oriented PQT thin films using the UFTM method resulted in highly oriented films with optical dichroic ratio of around 15 and charge transport anisotropy of 8.9. The fabricated bottom-gated OFETs demonstrated good field-effect mobilities along the width of the film, indicating the potential for high-performance organic circuits. The film thickness could be easily tuned and the reproducibility of field-effect mobility was maintained even at very thin thicknesses.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Polymer Science
Haoyu Zhao, Jordan J. Shanahan, Stephanie Samson, Zhaofan Li, Guorong Ma, Nathaniel Prine, Luke Galuska, Yunfei Wang, Wenjie Xia, Wei You, Xiaodan Gu
Summary: The morphological stability of an organic photovoltaic device can be improved by cleaving the side chains, which raises the glass transition temperature (Tg) of the conjugated polymers. Experimental results showed that isothermal annealing with controlled side chain cleavage increased the Tg and maintained the crystalline structure. Coarse grain molecular dynamics simulations supported these findings.
MACROMOLECULAR RAPID COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Yongfeng Zhang, Wei Zhang, Junming Xia, Chenchen Xiong, Gengchen Li, Xiaodong Li, Peng Sun, Jianbing Shi, Bin Tong, Zhengxu Cai, Yuping Dong
Summary: A breakthrough in room-temperature phosphorescence (RTP) emission performance was realized in a poly(vinylidene fluoride) (PVDF) matrix with a low glass transition temperature. Polymorph-dependent RTP emission in the PVDF matrix endows a 2.45 GHz microwave stimulus responsiveness to the material.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Polymer Science
Junpei Kuwabara, Takaki Kanbara
Summary: Conjugated polymers have immense potential in organic optoelectronic devices as semiconducting materials. To achieve mass production, synthetic methods must consider cost and environmental concerns, with simplification of synthetic steps being an efficient approach.
MACROMOLECULAR RAPID COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Mingfei Xiao, Aditya Sadhanala, Mojtaba Abdi-Jalebi, Tudor H. Thomas, Xinglong Ren, Tao Zhang, Hu Chen, Remington L. Carey, Qijing Wang, Satyaprasad P. Senanayak, Cameron Jellett, Ada Onwubiko, Maximilian Moser, Hailiang Liao, Wan Yue, Iain McCulloch, Mark Nikolka, Henning Sirringhaus
Summary: The glass transition temperature (T-g) of a range of conjugated polymers with different crystallinity levels was determined using dynamical mechanical analysis. The comparison between measured and theoretically predicted T-g values revealed that the consistency is influenced by the length of monomer units and sub-bandgap optical absorption.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Review
Polymer Science
Tengfei Qu, Guangming Nan, Yan Ouyang, Bahaerguli. Bieketuerxun, Xiuling Yan, Yunpeng Qi, Yi Zhang
Summary: This review focuses on the structure-property relationship, glass transition, and crystallization behaviors of conjugated polymers. Understanding the relationship between the molecular structure of conjugated polymers and their properties is essential for optimizing their performance. The glass transition temperature (Tg) plays a key role in determining the processability and application of conjugated polymers. The crystallization behavior of conjugated polymers significantly impacts their mechanical and electrical properties. Advanced characterization techniques provide insights into molecular ordering and polymer-crystal interfaces.
Article
Materials Science, Multidisciplinary
Nan Li, Yahao Dai, Yang Li, Shilei Dai, Joseph Strzalka, Qi Su, Nickolas De Oliveira, Qingteng Zhang, P. Blake J. St Onge, Simon Rondeau-Gagne, Yunfei Wang, Xiaodan Gu, Jie Xu, Sihong Wang
Summary: Polymer semiconductors have great potential for human-integrated electronics due to their solution processability and mechanical softness. The click-to-polymer (CLIP) synthesis strategy developed by the authors allows for the attachment of diverse functional units to pre-synthesized conjugated-polymer precursors, resulting in functionalized polymers with good charge-carrier mobility. This approach can advance the state of the art by enriching the functional properties of conjugated polymers.
Review
Chemistry, Multidisciplinary
Qingpei Wan, Barry C. Thompson
Summary: This review addresses the use of hydrogen-bonding in conjugated polymers, including the synthetic methods for introducing hydrogen-bonding functional groups and the impact on electronic and materials properties. Recent progress in balancing electronic performance and mechanical durability is highlighted, and prospects for future development are discussed.
Article
Polymer Science
Cameron M. Cole, Susanna V. Kunz, Thomas Baumann, James P. Blinco, Prashant Sonar, Christopher Barner-Kowollik, Soniya D. Yambem
Summary: Thermally activated delayed fluorescent (TADF) emitters are the leading materials for efficient OLEDs. A simple OLED with fully solution-processed organic layers is introduced, where the TADF emissive layer is ink-jet printed. The self-hosted TADF polymer shows potential for flexible ink-jet printed OLEDs, enabling a more scalable fabrication process.
MACROMOLECULAR RAPID COMMUNICATIONS
(2023)
Article
Polymer Science
Gustavo Munoz, Kari M. Chamberlain, Sumudu Athukorale, Guorong Ma, Xiaodan Gu, Charles U. Pittman, Dennis W. Smith
Summary: A new method for synthesizing semi-fluorinated polyaryl ethers was reported, which involved electrophilic polymerization under interfacial conditions. The resulting polyaryl ethers exhibited high regioselectivity, high molecular weight, and unique properties such as crystallinity, solubility, thermal stability, and optical transparency.
MACROMOLECULAR RAPID COMMUNICATIONS
(2023)
Article
Polymer Science
Madison Mooney, Audithya Nyayachavadi, Angela Awada, Ekaterini Iakovidis, Yunfei Wang, Mei-Nung Chen, Yuzi Liu, Jie Xu, Yu-Cheng Chiu, Xiaodan Gu, Simon Rondeau-Gagne
Summary: Organic semiconducting polymers have excellent optoelectronic properties and solution processability, making them a powerful platform for next-generation technologies. However, their extended pi-conjugation leads to low solubility and the use of toxic solvents. This study introduces a new approach using asymmetric side-chain engineering to improve processability and maintain electronic performance. Characterization techniques are used to study the solid-state morphologies and solution state aggregation of the polymer.
Article
Chemistry, Physical
Haoyu Zhao, Nathaniel Prine, Guorong Ma, Yongcao Zhang, Md Azimul Haque, Derya Baran, Xiaodan Gu
Summary: Thermal conductivity has a direct impact on the performance of organic thermoelectric devices. This study uses fast scanning calorimetry to quantitatively measure the thermal conductivity of conjugated polymer films, and reveals the effect of doping on thermal conductivity. By optimizing thermal conductivity, rational design of future organic thermoelectric materials can be achieved.
SUSTAINABLE ENERGY & FUELS
(2023)
Article
Chemistry, Multidisciplinary
Yunfei Wang, Kai-Lin Chen, Nathaniel Prine, Simon Rondeau-Gagne, Yu-Cheng Chiu, Xiaodan Gu
Summary: Researchers have developed a highly stretchable and self-healable semiconductor elastomer, which can be used to create self-healing flexible electronic devices.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Zhiqiang Cao, Sara A. Tolba, Zhaofan Li, Gage T. Mason, Yang Wang, Changwoo Do, Simon Rondeau-Gagne, Wenjie Xia, Xiaodan Gu
Summary: Tuning the optoelectronic properties of donor-acceptor conjugated polymers is important in designing organic optoelectronic devices. This study investigates the role of acceptor units and oligothiophene donor units on the energy band gaps of these polymers. The alignment of molecular orbital energy between donor and acceptor units plays a crucial role in determining the final optical bandgap of the polymers. The findings provide molecular insights into the design of D-A CPs for organic optoelectronic devices.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Naresh Eedugurala, Michael E. Steelman, Paramasivam Mahalingavelar, Daniel J. Adams, Kevin S. Mayer, Chih-Ting Liu, Anthony Benasco, Guorong Ma, Xiaodan Gu, Michael K. Bowman, Jason D. Azoulay
Summary: Open-shell conjugated polymers offer new opportunities to integrate the spin degree of freedom within emerging technologies. This study demonstrates a high-spin conjugated polymer composed of alternating benzo[1,2-b:4,5-b']dithiophene donors and a new, strongly electron-withdrawing 6,7,8,9-tetrachloro-[1,2,5]thiadiazolo[3,4-b]phenazine acceptor. The use of annulation and chlorination facilitates a transition between closed-shell aromatic and high-spin quinoidal forms, resulting in reduced bandgap, high electron affinity, delocalization of spin density, and n-type conduction. These insights allow for the development of a broader range of open-shell conjugated polymers and enable manipulation of important properties.
CHEMISTRY OF MATERIALS
(2023)
Article
Multidisciplinary Sciences
Min Woo Jeong, Jin Hyun Ma, Jae Seung Shin, Jun Su Kim, Guorong Ma, Tae Uk Nam, Xiaodan Gu, Seong Jun Kang, Jin Young Oh
Summary: Three highly stretchable primary light-emitting films made from a polymer blend of conventional RGB light-emitting polymers and a nonpolar elastomer have been reported in this study. The blend films consist of multidimensional nanodomains of light-emitting polymers that are interconnected in an elastomer matrix for efficient light-emitting under strain. The RGB blend films exhibited over 1000 cd/m(2) luminance with low turn-on voltage (V-on), and the selectively stretched blend films on rigid substrate maintained stable light-emitting performance up to 100% strain even after 1000 multiple stretching cycles.
Article
Polymer Science
Xiaohong Wang, Chenyin Xu, Ning Xu, Longlong Jiang, Yunfei Wang, Fan Ni, Guobing Zhang, Xiaodan Gu, Longzhen Qiu
Summary: Introducing hydrogen bonding structures into semiconducting polymers is an effective method to improve their performance. In this study, DPP-based random copolymers with quadruple hydrogen bonding were constructed by copolymerization of a ring-like UPy with alkyl chain-substituted DPP. The resulting polymers showed improved mechanical properties and retained 27.9% mobility under 100% stretching. This study also introduced quadruple intramolecular hydrogen bonding into the backbone of conjugated polymers, providing a new strategy for the introduction of multiple intramolecular hydrogen bonds into stretchable semiconducting polymers.
Article
Polymer Science
Kyle D. Mehringer, Parth K. Vagholkar, Brad J. Davis, Lisa K. Kemp, Guorong Ma, Robson F. Storey, Xiaodan Gu, Travis L. Thornell, Dane N. Wedgeworth, Yoan C. Simon, Sarah E. Morgan
Summary: Polymer architecture is crucial for controlling the morphology and mechanochemical response. Graft copolymers with mechanophores at the backbone-arm junction were synthesized through post-polymerization modification and controlled radical polymerization. The morphologies of these polymers are disordered but show decreasing domain size with shorter arm lengths, and greater domain mixing with more PS side chains. Backbone scission is more prevalent in polymers with a greater number of short grafts, and mechanophore activation is higher for samples with arm molecular weights ≥13 kg/mol, surpassing the cutoff molecular weight for PS.
JOURNAL OF POLYMER SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Nathaniel Prine, Camille Cardinal, Xiaodan Gu
Summary: Atomic force microscopy paired with infrared spectroscopy (AFM-IR) is used to investigate nanoscale surface topography and chemical composition of complex polymer blends and composites. The study explores the effect of laser power, frequency, and pulse width on the depth sensitivity of the technique. It demonstrates the capability to control the depth sensitivity of the AFM-IR tool by controlling the laser parameters.
Article
Chemistry, Multidisciplinary
Nathaniel Prine, Zhiqiang Cao, Song Zhang, Tianyu Li, Changwoo Do, Kunlun Hong, Camille Cardinal, Travis L. Thornell, Sarah E. Morgan, Xiaodan Gu
Summary: Atomic-force microscopy coupled with infrared spectroscopy (AFM-IR) simultaneously maps surface morphology and chemical composition of thin-film polymer blends and composites. Overlapping infrared absorption bands between different species make quantitative analysis challenging. Isotope labeling with carbon-deuterium vibration allows distinguishing blend phases and enables nanoscale domain composition analysis.
Article
Chemistry, Physical
Zhiqiang Cao, Zhaofan Li, Sara A. Tolba, Gage T. Mason, Miao Xiong, Michael U. Ocheje, Amirhadi Alesadi, Changwoo Do, Kunlun Hong, Ting Lei, Simon Rondeau-Gagne, Wenjie Xia, Xiaodan Gu
Summary: We studied the chain conformation and optical properties of high-performance donor-acceptor conjugated polymers at the single-chain level. The length of side chains and the presence of branch points play a critical role in the chain conformation and optical absorption. Considering the rigidity and coplanarity of the polymer backbone is important for achieving desired optoelectronic properties.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Shaochuan Luo, Yukun Li, Nan Li, Zhiqiang Cao, Song Zhang, Michael U. Ocheje, Xiaodan Gu, Simon Rondeau-Gagne, Gi Xue, Sihong Wang, Dongshan Zhou, Jie Xu
Summary: Modulating the segmental order in the morphology of conjugated polymers is crucial for achieving optimal electronic properties and mechanical deformability. However, a comprehensive understanding of how anisotropic conjugated polymers form segmentally ordered structures during crystallization is currently lacking. In this study, a novel approach combining stage-type fast scanning calorimetry and micro-Raman spectroscopy was developed to capture the evolution of segmental order in real-time. The findings suggest that the degree of segmental order saturates before reaching maximum crystallinity, allowing for good charge carrier mobility and segmental dynamic mobility in tailored conjugated polymers. The crystallization temperature for optimal segmental order can be predicted based on the glass transition temperature and melting temperature of the polymers. This characterization study provides fundamental insights for designing and controlling the optoelectronic and mechanical properties of conjugated polymers.
MATERIALS HORIZONS
(2023)
Article
Polymer Science
Guorong Ma, Song Zhang, Luke A. Galuska, Xiaodan Gu
Summary: Conjugated polymers with complex backbone structures and side-chain moieties have been studied for their mechanical properties and the development of new polymers with low modulus and high-crack onset strain. However, the mechanical stability of thin films under long-term external tensile strain is less investigated. In this study, we performed mechanical stress relaxation tests on both free-standing and water-floated thin films of high-Tg and low-Tg conjugated polymers, as well as a reference polystyrene sample. We found an enthalpy-entropy compensation effect for glassy polymer thin films and observed that crystalline morphology and higher modulus reduce the relaxation rate. These insights into the mechanical creep behavior of conjugated polymers will have implications for the design of stable organic electronics.
JOURNAL OF POLYMER SCIENCE
(2023)