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Two-Dimensional Conducting Polymers: Synthesis and Charge Transport
摘要： Current technological advances and prolific endeavors have entrenched two-dimensional conducting polymers as the rapidly emerging interface across a diversity of functional materials for flexible electronics, sensors, ion-exchange membranes, biotechnology, catalysis, energy storage, and conversion. Rational design and fabrication of polymeric nanostructures enriched with well-ordered geometry are appealing and endorse significant impact on their inbuilt electrical, optical, and mechanical properties. In particular, recent interest in controlled hierarchical assembly of monomers/oligomers proved the free-standing sheet-like structures with exotic features of high conductivity and flexibility. Yet, the ongoing research to make nanometer-thick polymers suffers from limitations to access large-area, mechanical stability, and high-range internal ordering. In this perspective, we focus on the radical approaches that highlight confinement-entitled features of two-dimensional polymeric materials correlating to their interface or template-assisted synthesis, structure–property relationship, charge transport properties, and future scopes for relevant practical enactments.
关键词： 2D assembly,self-organization,conjugated polymers,charge transport,interfacial synthesis
更新于2025-09-23 15:22:29
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Preparing Semiconducting Nanoribbons with Tunable Length and Width via Crystallization-Driven Self-Assembly of a Simple Conjugated Homopolymer
摘要： Precise control of width and length of one-dimensional (1D) semiconducting nanostructures has attracted much attention owing to its potential for optoelectronic applications. However, regulating both their length and width using conjugated polymers or even block copolymers is a huge challenge. To solve this problem, we synthesized a unique conjugated polyacetylene homopolymer by living cyclopolymerization, which spontaneously formed 1D nanoribbons via in situ nanoparticlization. Interestingly, their widths could be controlled from 8 to 41 nm, which were directly proportional to their degree of polymerization. Furthermore, a self-seeding technique via crystallization-driven self-assembly (CDSA) was used to control the length of the nanoribbons up to 5.2 μm with narrow distributions less than 1.1. Interestingly, adding a block copolymer unimer to these nanoribbons produced triblock comicelles by the living CDSA mechanism. Finally, these nanoribbons were visualized directly by super-resolution optical fluorescence microscopy. Now, one can modulate both length and width of 1D nanoribbons simultaneously.
关键词： semiconducting nanostructures,crystallization-driven self-assembly,nanoribbons,optoelectronic applications,conjugated polymers
更新于2025-09-23 15:21:21
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Conjugated Polymers Based on Thiazole Flanked Naphthalene Diimide for Unipolar n-Type Organic Field-Effect Transistors
摘要： This paper reports the rational design and synthesis of a novel electron-withdrawing building block, thiazole flanked naphthalene diimide (TzNDI), which offers a coplanar conformation and deep-lying highest occupied molecular orbitals energy level in resulting conjugated polymers. A series of conjugated polymers (PTzNDI-2FT, PTzNDI-T, PTzNDI-Se, and PTzNDI-2T) consisting of TzNDI and different donor units were synthesized and characterized. The polymers all possess a high molecular weight and excellent thermal property. Their intense light absorption in low energy bands suggests an enhanced intramolecular charge transfer. The organic field-effect transistors (OFETs) based on these polymers exhibit unipolar n-type transport characteristics with low off current and high on–off current ratio. More importantly, all the devices exhibit near ideal transfer curves with kink-free transfer characteristics. Among these polymers, PTzNDI-2FT exhibits the highest electron mobility (μe) of 0.57 cm2 V?1 s?1, outperforming the commercial n-type polymer N2200 (0.41 cm2 V?1 s?1) under the same conditions. These results demonstrate that TzNDI is a promising building block for high performance unipolar n-type conjugated polymers in OFETs.
关键词： Unipolar n-Type,Thiazole Flanked Naphthalene Diimide,Conjugated Polymers,Organic Field-Effect Transistors
更新于2025-09-23 15:21:21
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Tuning the Cross-Linker Crystallinity of a Stretchable Polymer Semiconductor
摘要： The cross-linking of conjugated polymers has been demonstrated to be an effective strategy to improve its elastic properties to give deformable semiconductors for plastic electronics. While there have been extensive studies of the structural requirements of the polymer host for good film ductility, no work to date has focused on the relevance of the structural design or chemistry of these cross-linker additives. In this study, urethane groups and tertiary carbon atoms are inserted into the alkyl backbone of perfluorophenyl azide-based cross-linkers to investigate the importance of cross-linker crystallinity with respect to polymer morphology and hence mechanical and electrical properties. Linear cross-linkers with hydrogen bonding from urethane groups readily phase separate and recrystallize in the polymer network to form cross-linked domains that obstruct the strain distribution of the polymer film. Branch cross-linkers with tertiary carbon on the other hand form an evenly cross-linked network in the polymer blend stemming from excellent miscibility and show a 4-fold increase in fracture strain. Furthermore, a stable hole mobility of 0.2 cm2 V?1 s?1 is achieved up to ε = 100%, and a stable hole mobility of 0.1 cm2 V?1 s?1 after 2000 cycles of ε = 25% on fully stretchable organic field-effect transistors.
关键词： cross-linking,deformable semiconductors,cross-linker crystallinity,electrical properties,polymer morphology,elastic properties,plastic electronics,conjugated polymers,mechanical properties
更新于2025-09-23 15:21:21
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p-Doping Poly(3-hexylthiophene) in Solvent Mixtures
摘要： One method to improve the conductivity of conjugated polymers, like poly(3-hexylthiophene) (P3HT), is to “chemically dope” them analogous to inorganic materials. One electron acceptor that has been used in tandem to p-doped P3HT is 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4TCNQ), and recently there has been much interest in the nature of the interactions between F4TCNQ and P3HT in the solution phase. To date, however, there are few reports that investigate the behavior of F4TCNQ-doped P3HT in binary solvent mixtures. The study reported herein is an investigation of F4TCNQ-doped P3HT in mixtures of chloroform (CF) with dichloromethane (DCM) or acetonitrile (AcN), wherein variations in the doping efficiency in these mixtures are observed using UV–vis absorption, Raman, and electron paramagnetic resonance spectroscopic techniques. The contrasting solubility and charge transfer behavior of F4TCNQ-doped P3HT in CF:DCM and CF:AcN show that judicious selection of solvent mixtures may be exploited to improve the doping efficiency and solution processability of p-doped P3HT dispersions.
关键词： dispersions,charge transfer,conjugated polymers,self-assembly
更新于2025-09-23 15:21:21
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Unraveling Doping Capability of Conjugated Polymers for Strategic Manipulation of Electric Dipole Layer toward Efficient Charge Collection in Perovskite Solar Cells
摘要： Developing electrical organic conductors is challenging because of the difficulties involved in generating free charge carriers through chemical doping. To devise a novel doping platform, the doping capabilities of four designed conjugated polymers (CPs) are quantitatively characterized using an AC Hall-effect device. The resulting carrier density is related to the degree of electronic coupling between the CP repeating unit and 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4-TCNQ), and doped PIDF-BT provides an outstanding electrical conductivity, exceeding 210 S cm?1, mainly due to the doping-assisted facile carrier generation and relatively fast carrier mobility. In addition, it is noted that a slight increment in the electron-withdrawing ability of the repeating unit in each CP diminishes electronic coupling with F4-TCNQ, and severely deteriorates the doping efficiency including the alteration of operating doping mechanism for the CPs. Furthermore, when PIDF-BT with high doping capability is applied to the hole transporting layer, with F4-TCNQ as the interfacial doping layer at the interface with perovskite, the power conversion efficiency of the perovskite solar cell improves significantly, from 17.4% to over 20%, owing to the ameliorated charge-collection efficiency. X-ray photoelectron spectroscopy and Kelvin probe analyses verify that the improved solar cell performance originates from the increase in the built-in potential because of the generation of electric dipole layer.
关键词： conjugated polymers,conducting polymers,doping,molecular electronics,solar cells
更新于2025-09-23 15:21:01
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Nonlinear Optics || Molecular Origin of the Nonlinear Optical Response
摘要： In Chapter 3, we presented a general quantum-mechanical theory of the nonlinear optical susceptibility. This calculation was based on time-dependent perturbation theory and led to explicit predictions for the complete frequency dependence of the linear and nonlinear optical susceptibilities. Unfortunately, however, these quantum-mechanical expressions are typically far too complicated to be of use for practical calculations. In this chapter we review some of the simpler approaches that have been implemented to develop an understanding of the nonlinear optical characteristics of various materials. Many of these approaches are based on understanding the optical properties at the molecular level. We also present brief descriptions of the nonlinear optical characteristics of conjugated polymers, chiral molecules, and liquid crystals.
关键词： chiral molecules,nonlinear optical susceptibility,liquid crystals,quantum-mechanical theory,conjugated polymers,time-dependent perturbation theory
更新于2025-09-23 15:21:01
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Alignment of Lyotropic Liquid Crystalline Conjugated Polymers in Floating Films
摘要： Directed alignment of polymer chains plays an indispensable role in charge transport properties. We focus not only on a specific method to induce the alignment but also on the design of a liquid crystalline (LC) conjugated polymer to take advantage of an intrinsic self-assembly characteristic. We synthesized a lyotropic LC conjugated polymer, CP1-P, having o-nitrobenzyl (ONB) esters as photocleavable side chains and adopted a floating film transfer method to induce the polymer chain alignment through a lyotropic LC phase transition. An optimum amount of a high boiling point solvent (1,2-dichlorobenzene) in chloroform turned out to be an important factor to maximize the polymer chain alignment. The hole transport mobility along the polymer chain alignment direction was 13?14 times higher than that in the direction perpendicular to the alignment. In addition, the removal of side chains resulted in the solvent resistivity while maintaining the alignment feature in organic thin-film transistors.
关键词： floating films,liquid crystalline conjugated polymers,photocleavable side chains,polymer chain alignment,charge transport properties
更新于2025-09-23 15:21:01
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Recent Advances in Isoindigo-Inspired Organic Semiconductors
摘要： Over the past decade, isoindigo has become a widely used electron-deficient subunit in donor-acceptor organic semiconductors, and these isoindigo-based materials have been widely used in both organic photovoltaic (OPV) devices and organic field effect transistors (OFETs). Shortly after the development of isoindigo-based semiconductors, researchers began to modify the isoindigo structure in order to change the optoelectronic properties of the resulting materials. This led to the development of many new isoindigo-inspired compounds; since 2012, the Kelly Research Group has synthesized a number of these isoindigo analogues and produced a variety of new donor-acceptor semiconductors. In this Personal Account, recent progress in the field is reviewed. We describe how the field has evolved from relatively simple donor-acceptor small molecules to structurally complex, highly planarized polymer systems. The relevance of these materials in OPV and OFET applications is highlighted, with particular emphasis on structure-property relationships.
关键词： isoindigo,organic field effect transistors,organic materials,organic photovoltaics,conjugated polymers
更新于2025-09-23 15:21:01
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Perdeuterated conjugated polymers for ultralowa??frequency magnetic resonance of OLEDs
摘要： Formation of excitons in OLEDs is spin dependent and can be controlled by electron-paramagnetic resonance, affecting device resistance and electroluminescence yield. We explore electrically detected magnetic resonance in the regime of very low magnetic fields (<1mT). A pronounced feature emerges at zero field in addition to the conventional spin-? Zeeman resonance for which the Larmor frequency matches that of the incident radiation. By comparing a conventional π-conjugated polymer as the active material to a perdeuterated analogue, we demonstrate the interplay between zero-field feature and local hyperfine fields. The zero-field peak results from a quasistatic magnetic-field effect of the RF radiation for periods comparable to the carrier-pair lifetime. Zeeman resonances are resolved down to 3.2MHz, approximately twice the Larmor frequency of an electron in Earth’s field. However, since reducing hyperfine fields sharpens the Zeeman peak at the cost of an increased zero-field peak, we suggest that this result constitutes a fundamental low-field limit of magnetic resonance in carrier-pair-based systems. OLEDs offer an alternative solid-state platform to investigate the radical-pair mechanism of magnetic-field effects in photochemical reactions, allowing models of biological magnetoreception to be explored by measuring spin decoherence directly in the time domain.
关键词： Deuteration,Magnetic resonance,Isotopes,Conjugated Polymers,Organic light-emitting diodes
更新于2025-09-23 15:19:57