一类非常规富勒烯C64X4（X = H; F;Cl;Br）的结构、电子性质、光谱和吸波单分子膜相
Structures, Electronic Properties, Spectroscopies and Hexagonal Monolayer Phase of a Family of Unconventional Fullerenes C64X4 (X = H; F;Cl;Br)
摘要：
采用密度泛函理论对非常规富勒烯C64及其衍生物C64 X4（X = H; F;Cl;Br）的几何结构和电子性质进行了系统的第一性原理研究.通过对C64的3465个异构体的搜索，发现C64的基态是具有D2对称性的球形结构，而最近合成的C64 H4的母体笼是具有C3 v对称性的梨形结构.我们发现在C64笼的五角-五角融合顶点上加入F、Cl、Br等卤素原子可以提高稳定性，形成非常规的富勒烯C64 X4。计算了Mulliken电荷布居数、LUMO-HOMO能隙和态密度，结果表明：不同卤素原子的引入会导致C64 X4分子的电荷布居数发生显著变化，化学衍生会使C64 X4分子的能隙增大，对电子结构产生明显影响.发现C64 F4比C64 H4更稳定，因为前者的C-X键能高于后者。C64 H4分子的计算光谱与实验数据吻合较好，C64 X4（X = F;Cl;Br）分子的IR、Raman、NMR光谱也进行了计算，以促进进一步的实验研究。最后，通过总能量计算发现，C64 X4可以形成稳定的六方单分子层。
英文摘要：
A systematic first-principles study within density functional theory on the geometrical structures and electronic properties of unconventional fullerene C64 and its derivatives C64X4 (X = H; F;Cl;Br) has been performed. By searching through all 3465 isomers of C64, the ground state of C64 is found to be spherical shape with D2 symmetry, which differs from the parent cage of the recently synthesized C64H4 that is pear-shaped with C3v symmetry. We found that the addition of the halogen atoms like F;Cl;Br to the pentagon-pentagon fusion vertex of C64 cage could enhance the stability, forming the unconventional fullerenes C64X4. The Mulliken charge populations, LUMO-HOMO gap energies and density of states are calculated, showing that different halogen atoms added to C64 will cause remarkably different charge populations of the C64X4 molecule; the chemical deriving could enlarge the energy gaps and affect the electronic structures distinctly. It is unveiled that C64F4 is even more stable than C64H4, as the C-X bond energy of the former is higher than that of the latter. The computed spectra of C64H4 molecules agree well with the experimental data; the IR, Raman, NMR spectra of C64X4 (X = F;Cl;Br) are also calculated to stimulate further experimental investigations. Finally, it is uncovered by total energy calculations that C64X4 could form a stable hexagonal monolayer.
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