Total non-lewis structures: An application to predict the stability and reactivity of linear and angular polyacenes

Manassir, Mohammad; Pakiari, A.H.

doi:10.1016/j.jmgm.2020.107643

Cited by 5 publications

(2 citation statements)

References 47 publications

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“…Owing to its computational efficiency and decent accuracy for exploring the properties of electronic systems at the nanoscale, TAO-DFT has recently been adopted to investigate the electronic properties (Wu and Chai, 2015;Seenithurai and Chai, 2016, 2017, 2020Wu et al, 2016;Yeh and Chai, 2016;Yeh et al, 2018;Chung and Chai, 2019;Deng and Chai, 2019;Huang et al, 2020;Manassir and Pakiari, 2020), hydrogen storage properties (Seenithurai and Chai, 2016, 2017, and vibrational frequencies (Hanson-Heine, 2020) of several electronic systems at the nanoscale, especially for those possessing a radical nature.…”

Section: Introductionmentioning

confidence: 99%

TAO-DFT-Based Ab Initio Molecular Dynamics

Chai

2020

Front. Chem.

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Recently, AIMD (ab initio molecular dynamics) has been extensively employed to explore the dynamical information of electronic systems. However, it remains extremely challenging to reliably predict the properties of nanosystems with a radical nature using conventional electronic structure methods (e.g., Kohn-Sham density functional theory) due to the presence of static correlation. To address this challenge, we combine the recently formulated TAO-DFT (thermally-assisted-occupation density functional theory) with AIMD. The resulting TAO-AIMD method is employed to investigate the instantaneous/average radical nature and infrared spectra of n-acenes containing n linearly fused benzene rings (n = 2-8) at 300 K. According to the TAO-AIMD simulations, on average, the smaller n-acenes (up to n = 5) possess a nonradical nature, and the larger n-acenes (n = 6-8) possess an increasing radical nature, showing remarkable similarities to the ground-state counterparts at 0 K. Besides, the infrared spectra of n-acenes obtained with the TAO-AIMD simulations are in qualitative agreement with the existing experimental data.

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Section: Introductionmentioning

confidence: 99%

TAO-DFT-Based Ab Initio Molecular Dynamics

Chai

2020

Front. Chem.

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“…Besides, to improve the overall accuracy of TAO-DFT for diverse applications, an approach that determines the self-consistent value of

in TAO-DFT has been recently formulated [ 44 ]. Also, to comment on its applicability, TAO-DFT has been widely adopted for electronic structure calculations [ 5 , 12 , 15 , 45 , 46 , 47 , 48 , 49 , 50 , 51 , 52 , 53 ], hydrogen storage applications [ 46 , 48 , 49 ], and vibrational analysis [ 54 ], especially for nanosystems possessing radical character. Furthermore, in several recent investigations [ 5 , 37 , 39 , 40 , 42 , 45 ], the occupation numbers of orbitals from TAO-DFT have been shown to be close to the occupation numbers of natural orbitals obtained with the variational two-electron reduced-density-matrix-driven CASSCF (v2RDM-CASSCF) method, which is an accurate MR electronic structure method, leading to a qualitatively similar tendency in describing the radical nature associated with various PAHs.…”

Section: Introductionmentioning

confidence: 99%

TAO-DFT Study on the Electronic Properties of Diamond-Shaped Graphene Nanoflakes

2020

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At the nanoscale, it has been rather troublesome to properly explore the properties associated with electronic systems exhibiting a radical nature using traditional electronic structure methods. Graphene nanoflakes, which are graphene nanostructures of different shapes and sizes, are typical examples. Recently, TAO-DFT (i.e., thermally-assisted-occupation density functional theory) has been formulated to tackle such challenging problems. As a result, we adopt TAO-DFT to explore the electronic properties associated with diamond-shaped graphene nanoflakes with n = 2–15 benzenoid rings fused together at each side, designated as n-pyrenes (as they could be expanded from pyrene). For all the n values considered, n-pyrenes are ground-state singlets. With increasing the size of n-pyrene, the singlet-triplet energy gap, vertical ionization potential, and fundamental gap monotonically decrease, while the vertical electron affinity and symmetrized von Neumann entropy (which is a quantitative measure of radical nature) monotonically increase. When n increases, there is a smooth transition from the nonradical character of the smaller n-pyrenes to the increasing polyradical nature of the larger n-pyrenes. Furthermore, the latter is shown to be related to the increasing concentration of active orbitals on the zigzag edges of the larger n-pyrenes.

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Benzothiophene and benzosulfone fused pyrazino[2,3-g]quinoxaline: Synthesis and semiconducting properties

Ding

Xia

et al. 2023

Chinese Chemical Letters

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Total non-lewis structures: An application to predict the stability and reactivity of linear and angular polyacenes

Cited by 5 publications

References 47 publications

TAO-DFT-Based Ab Initio Molecular Dynamics

TAO-DFT-Based Ab Initio Molecular Dynamics

TAO-DFT Study on the Electronic Properties of Diamond-Shaped Graphene Nanoflakes

Benzothiophene and benzosulfone fused pyrazino[2,3-g]quinoxaline: Synthesis and semiconducting properties

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