Radenković Slavko, Tomović Željko
University of Kragujevac, Faculty of Science, P. O. Box 60, 34000, Kragujevac, Serbia.
Polymer Performance Materials Group, Department of Chemical Engineering & Chemistry and Institute for Complex Molecular Systems, Eindhoven University of Technology, 5600 MB, Eindhoven, The Netherlands.
Chemphyschem. 2022 Jun 20;23(12):e202200125. doi: 10.1002/cphc.202200125. Epub 2022 Apr 29.
A detailed study of the geometry, aromatic character, electronic and magnetic properties for a series of positively charged N-doped polycyclic aromatic hydrocarbons (PAHs) was performed. Magnetic properties of the examined molecules were analyzed by means of the magnetically induced current density calculated using the diamagnetic-zero version of the continuous transformation of origin of current density (CTOCD-DZ) method. The comparative study of the local aromaticity of the studied molecules was performed using several different indices: energy effect (ef), harmonic oscillator model of aromaticity (HOMA) index, six centre delocalization index (SCI) and nucleus independent chemical shifts (NICS). The presence of N-atoms in the inner rings was found to cause a planarity distortion in the studied N-doped systems. The geometric changes and charged nature of the studied N-doped systems do not significantly influence the current density and the local aromaticity distribution in comparison with the corresponding parent benzenoid hydrocarbons. The present study demonstrates how quantum chemical calculations can be used for rational design of novel PAHs and for fine tuning of their properties.
对一系列带正电荷的氮掺杂多环芳烃（PAHs）的几何结构、芳香性、电子和磁性性质进行了详细研究。通过使用电流密度原点连续变换的抗磁零版本（CTOCD-DZ）方法计算的磁诱导电流密度来分析所研究分子的磁性性质。使用几种不同的指标对所研究分子的局部芳香性进行了比较研究：能量效应（ef）、芳香性的谐振子模型（HOMA）指数、六中心离域指数（SCI）和核独立化学位移（NICS）。发现在内环中存在氮原子会在所研究的氮掺杂体系中引起平面度畸变。与相应的母体苯型烃相比，所研究的氮掺杂体系的几何变化和带电性质对电流密度和局部芳香性分布没有显著影响。本研究展示了如何将量子化学计算用于新型PAHs的合理设计及其性质的微调。
