Electronic and Optical Properties of VSc₂N@C₆₈ Fullerene

Abstract

We report a detailed investigation of structural, electronic, and spectroscopic properties of VSc 2 N@C 68 endohedral fullerene. First, the candidate structures of the ground state are obtained using a systematic approach in which 900 isomers of endohedral fullerenes were screened for their energetic stability. The stability of some of the most promising isomers was studied using density functional theory at the all-electron level using large polarized Gaussian basis sets. Although the dopant vanadium atom is also in the same charge state as Sc, the doping changes the structure and the spin state from that of Sc 3 N@C 68 . The d-orbitals of the V atom lead to a spin state with spin moment of 2 μ B for the endohedral fullerene. The spin− orbit coupling strength is, however, weak, leading to vanishingly small zero-field splitting of the spin levels. The ionization energy, electron affinity, and the quasi-particle gap of the most stable isomer are comparable to those of C 60 . The vibrational frequency analysis shows that the structure is stable. Finally, the infrared, Raman, and optical spectra of the most stable fullerene are calculated, which can aid in identification of the cluster in experiments.

Electronic structure calculation of vanadium‐and scandium‐based endohedral fullerenes VSc2N@C2n (2n = 70, 76, 78, 80)

“…A very elaborate search for the most stable structure showed isomer 6079 to be the most stable candidate having significant chemical stability among all the 6332 isomers of C 68 . Vanadium doped fullerenes have spin magnetic moment but the spin‐orbit coupling is found to be weak . The most important finding of this study was that the most stable isomer of VSc 2 N@C 68 has a cage structure different from the one for the Sc 3 N@C 68 fullerene.…”

“…From the optimized database of hexanionic fullerenes, the lowest 300 isomers were selected as initial parent cages for the encapsulation of the VSc 2 N unit. In the endohedral fullerenes where six electrons are transferred from the endohedral fullerene to host fullerene cages, the hexanions of such fullerene cages provide a useful starting guess in search of the most stable endohedral fullerenes …”

“…In our recent study, we examined the possibility of encapsulation of the VSc 2 N unit inside C 68 fullerenes. A very elaborate search for the most stable structure showed isomer 6079 to be the most stable candidate having significant chemical stability among all the 6332 isomers of C 68 . Vanadium doped fullerenes have spin magnetic moment but the spin‐orbit coupling is found to be weak .…”

“…We computationally studied the properties of those fullerenes with a VSc 2 N endohedral unit at the density functional level. Using the procedure outlined recently, we performed a large scale search that involves thousands of optimizations to identify the most favorable isomers of VSc 2 N@C 70 , VSc 2 N@C 76 , VSc 2 N@C 78 , and VSc 2 N@C 80 . Subsequently, detailed density functional calculations using large basis sets were performed to obtain the information about the electronic and structural properties of the most stable isomers.…”

Confinement Effects of a Noble Gas Dimer Inside a Fullerene Cage: Can It Be Used as an Acceptor in a DSSC?

“…Ever since the discovery of fullerene (Kroto et al, 1985), it has been studied extensively due to its fascinating properties, leading to versatile applications in various fields of nano and optoelectronics (Bhusal et al, 2016;Paul et al, 2017Paul et al, , 2018aQu et al, 2019), besides being used as sensors (Jaroš et al, 2019;Parey et al, 2019) and hydrogen storage devices (Chandrakumar and Ghosh, 2008;Srinivasu and Ghosh, 2012). Fullerenes are also known to exist in different isomeric forms (Małolepsza et al, 2007;Zhao et al, 2018).…”