Computational design of a ferroelectric framework material based on dipolar rotors

Area of Science:

• Materials Science
• Chemistry
• Physics

Background:

• Ferroelectric materials are crucial for electronic devices.
• Designing novel ferroelectric materials with tunable properties remains a challenge.
• Covalent organic frameworks (COFs) offer a versatile platform for materials design.

Purpose of the Study:

• To present a hierarchical computational approach for generating ferroelectric covalent frameworks.
• To demonstrate the design of a specific COF with predicted ferroelectric properties.
• To validate the ferroelectric behavior across different levels of theoretical sophistication.

Main Methods:

• A multi-step workflow was employed, starting from a point dipole model to a full 3D framework.
• Molecular dynamics and Monte Carlo Metropolis sampling were utilized.
• The Universal Force Field for Metall-Organic-Frameworks (UFF4MOF) and GFN1-xTB were used for energy calculations.

Main Results:

• A hierarchical strategy successfully generated a unit cell with predicted ferroelectric behavior.
• The computational workflow confirmed desired ferroelectric attributes at each step.
• A novel covalent organic framework exhibiting a ferroelectric ground state stable above 100 K was demonstrated.

Conclusions:

• The hierarchical approach provides a robust method for designing ferroelectric COFs.
• The developed framework shows promise for applications requiring switchable polarization.
• This work opens new avenues for exploring functional porous materials.