Modeling-driven materials by design for conjugated polymers: insights into optoelectronic, conformational, and thermomechanical properties.

Conjugated polymers (CPs) have emerged as pivotal functional materials in the realm of flexible electronics and optoelectronic devices due to their unique blend of mechanical flexibility, solution processability, and tunable optoelectronic properties. This review synthesizes the latest molecular simulation-driven insights obtained from various multiscale modeling techniques, including quantum mechanics (QM), all-atomistic (AA) molecular dynamics (MD), coarse-grained (CG) modeling, and machine learning (ML), to elucidate the optoelectronic, structural, and thermomechanical properties of CPs. By integrating findings from our recent computational work with key experimental studies, we highlight the molecular mechanisms influencing the multifunctional performance of CPs. This comprehensive understanding aims to guide future research directions and applications in the modeling assisted design of high-performance CP-based materials and devices.

A portable elliptical dichroism spectrometer targeting secondary structural features of tumorous protein for pancreatic cancer detection.

Stereochemical analysis is essential for understanding the complex function of biomolecules. Various direct and indirect approaches can be used to explore the allosteric configuration. However, the size, cost, and delicate nature of these systems limit their biomedical usage. Here, we constructed elliptical dichroism (ED) spectrometer for biomedical applications, whose performance is validated by experiment and theoretical simulation (Jones/Mueller calculus and time-dependent density-functional theory). Instead of complicated control of circular polarization, ED spectrometer adopted the absorbance of left- and right-oriented elliptically polarized light. With a simplified design, we demonstrated the potential of ED spectrometry as an alternative for secondary structural analysis of biomolecules, their conformation and chirality. It not only provides a portable, low-cost alternative to the sophisticated instruments currently used for structural analysis of biomolecules but also provides superior translational features: low sample consumption(200 µl), easy operation, and multiple working modes, for noninvasive cancer detection.

Molecular Structure and Conformational Design of Donor-Acceptor Conjugated Polymers to Enable Predictable Optoelectronic Property.

Tuning the optoelectronic properties of donor-acceptor conjugated polymers (D-A CPs) is of great importance in designing various organic optoelectronic devices. However, there remains a critical challenge in precise control of bandgap through synthetic approach, since the chain conformation also affects molecular orbital energy levels. Here, D-A CPs with different acceptor units are explored that show an opposite trend in energy band gaps with the increasing length of oligothiophene donor units. By investigating their chain conformation and molecular orbital energy, it is found that the molecular orbital energy alignment between donor and acceptor units plays a crucial role in dictating the final optical bandgap of D-A CPs. For polymers with staggered orbital energy alignment, the higher HOMO with increasing oligothiophene length leads to a narrowing of the optical bandgap despite decreased chain rigidity. On the other hand, for polymers with sandwiched orbital energy alignment, the increased band gap with increasing oligothiophene length originates from the reduction of bandwidth due to more localized charge density distribution. Thus, this work provides a molecular understanding of the role of backbone building blocks on the chain conformation and bandgaps of D-A CPs for organic optoelectronic devices through the conformation design and segment orbital energy alignment.