The Stockmayer fluid, composed of dipolar spheres, has a well-known isotropic-ferroelectric phase transition at high dipole densities. However, there has been little investigation of the ferroelectric transition in nearly spherical fluids at dipole densities corresponding to those found in many polar solvents and in guest-host organic electro-optic materials. In this work, we examine the transition to ordered phases of low-aspect-ratio spheroids under both unperturbed and poled conditions, characterizing both the static dielectric response and thermodynamic properties of spheroidal systems. Spontaneous ferroelectric ordering was confined to a small region of aspect ratios about unity, indicating that subtle changes in sterics can have substantial influence on the behavior of coarse-grained liquid models. Our results demonstrate the importance of molecular shape in obtaining even qualitatively correct dielectric responses and provide an explanation for the success of the Onsager model as a phenomenological representation for the dielectric behavior of polar organic liquids.
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http://dx.doi.org/10.1021/acs.jpcb.5b00009 | DOI Listing |
J Phys Chem A
January 2025
Liaoning Key Laboratory of Manufacturing System and Logistics Optimization, Shenyang 110819, China.
Artificial intelligence technology has introduced a new research paradigm into the fields of quantum chemistry and materials science, leading to numerous studies that utilize machine learning methods to predict molecular properties. We contend that an exemplary deep learning model should not only achieve high-precision predictions of molecular properties but also incorporate guidance from physical mechanisms. Here, we propose a framework for predicting molecular properties based on data-driven electron density images, referred to as D3-ImgNet.
View Article and Find Full Text PDFSci Rep
January 2025
Department of Chemistry, University of Massachusetts Boston, 100 Morrissey Blvd, Boston, MA, 02125, USA.
Oxidative stress, associated with excessive production of reactive oxygen and nitrogen species (ROS, RNS), contributes to the development and progression of many ailments, such as aging, cardiovascular diseases, Alzheimer's disease, Parkinson's disease, diabetes, cancer, preeclampsia or multiple sclerosis. While phenols and polyphenols are the most studied antioxidants structurally similar compounds such as anilines or thiophenols are sporadically analyzed despite their radical scavenging potential. This work assesses the impact of structural features of phenols and thiophenols on their antioxidant activity.
View Article and Find Full Text PDFJ Chem Phys
January 2025
Department of Chemistry, University of Waterloo, Waterloo, Ontario N2L 3G1, Canada.
In this work, we propose a path integral Monte Carlo approach based on discretized continuous degrees of freedom and rejection-free Gibbs sampling. The ground state properties of a chain of planar rotors with dipole-dipole interactions are used to illustrate the approach. Energetic and structural properties are computed and compared to exact diagonalization and numerical matrix multiplication for N ≤ 3 to assess the systematic Trotter factorization error convergence.
View Article and Find Full Text PDFAdv Mater
December 2024
The Soft2D Lab, State Key Laboratory of Metal Matrix Composites, Shanghai Key Laboratory of Electrical Insulation and Thermal Ageing, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China.
The electrochemical conversion of carbon dioxide (CO) into hydrocarbon products emerges as a pivotal sustainable strategy for carbon utilization. Cu-based catalysts are currently prioritized as the most effective means for this process, yet it remains a long-term goal to achieve high product selectivity at elevated current densities. This study delved into exploring the influence of a topological poly(2-aminoazulene) with a substantial dipole moment on modulating the Cu surface dipole field to augment the catalytic activity involved in CO reduction.
View Article and Find Full Text PDFNat Commun
December 2024
Key Laboratory for Quantum Materials of Zhejiang Province, Department of Physics, School of Science, Westlake University, 18 Shilongshan Road, Hangzhou, 310024, Zhejiang Province, China.
Extending ferroelectric materials to two-dimensional limit provides versatile applications for the development of next-generation nonvolatile devices. Conventional ferroelectricity requires materials consisting of at least two constituent elements associated with polar crystalline structures. Monolayer graphene as an elementary two-dimensional material unlikely exhibits ferroelectric order due to its highly centrosymmetric hexagonal lattices.
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