Insights into first-principles characterization of the monoclinic VO<sub>2</sub>(B) polymorph <i>via</i> DFT + U calculation: electronic, magnetic and optical properties

Mohebbi, Elaheh; Pavoni, Eleonora; Mencarelli, Davide; Stipa, Pierluigi; Pierantoni, Luca; Laudadio, Emiliano

doi:10.1039/d2na00247g

Cited by 12 publications

(7 citation statements)

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“…As the results of previous studies have underscored that the outcomes are substantially dependent on the magnitude of U, we tested different Hubbard U values for V-3d and O-2p. We set V-3d = 5.20 eV and O-2p = 0.95 eV since these parameters have shown very good agreement with the experimental results, as reported by Mohebbi et al (2022).…”

Section: Methodsmentioning

confidence: 69%

Stability, phonon calculations, electronic structure, and optical properties of a VO2(M) nanostructure: A comprehensive density functional theory study

et al. 2023

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This work aimed to precisely evaluate the physical properties of vanadium dioxide (M), particularly the optical characteristics. We employed different exchange-correlation functionals to determine the phase stability, band gap properties, and optical characteristics of an experimentally recognized monoclinic VO2(M) polymorph. The calculations not only correctly interpreted the VO2(M) origin but also predicted other optical properties including the extinction coefficient (k) and refractive index (n), which have not been reported in experimental measurements. Phonon dispersion calculations confirmed the presence of negative frequencies for acoustic modes in the phononic curves. When the HSE functional correctly reproduced the experimental band gap, here for the first time, our calculations based on PBE and PBEsol yielded non-zero electronic bandgaps of 0.23 and 0.15 eV for bulk VO2(M). Our predictions showed that semi-local functionals can adequately predict the semiconductor properties of VO2(M) and performed better than all previously reported theoretical works on nulled band gaps. In addition to the better prediction of the peak position in the absorption spectra with HSE hybrid functional, this method also reasonably well described the static dielectric constant of 7.54, showing an excellent match to the experimental values. In general, the results of this study reveal that hybrid functionals yield superior outcomes compared to semi-local functionals for optical properties of a VO2(M) polymorph. Our results suggest that the PBEsol + HSE approach allows the efficient characterization of smart materials for electronic and optoelectronic applications.

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Section: Methodsmentioning

confidence: 69%

Stability, phonon calculations, electronic structure, and optical properties of a VO2(M) nanostructure: A comprehensive density functional theory study

et al. 2023

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“…Usually, the conventional DFT, adding a Hubbard U parameter representing the strong electron-electron interaction of strongly correlated materials, can cure the deficiencies of local or semilocal exchange-correlation functions and maintain relatively low computational cost. [41][42][43] As was reported, the accuracy of outcomes by DFT + U is tend to depend on the magnitude of U parameter. In the need of the correct description of strongly correlated system properties, it is necessary to determine a reliable U value firstly.…”

Section: Introductionmentioning

confidence: 70%

“…The widely used approach reported in literature for choosing effective U is adjusting calculated results to fitting experimental data (for instance, fitting the experimental bandgaps, seeback effect or electrical conductivity). [42,44,45] On the other hand, several pure theoretical perspectives have also been developed to determine the U non-empirically, for example, the linear response method based on constrained DFT (CDFT) by Cococcioni and de Gironcoli1, [46] the constrained random-phase approximation (cRPA) method, [47] and self-consistent methods from the local electron density based on the Thomas-Fermi screening mode. [48] However, these methods have shortcomings more or less.…”

Section: Introductionmentioning

confidence: 99%

Determining Hubbard U of VO₂ by the quasi-harmonic approximation

Kong 孔,

Lu 陆,

Zhuang 庄

et al. 2024

Chinese Phys. B

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Vanadium dioxide ($\rm VO_{2}$) is a strongly correlated material that undergoes a metal-to-insulator transition around 340 K. In order to describe the electron correlation effects in $\rm VO_{2}$, the DFT+$U$ method is commonly employed in calculations. However, the choice of the Hubbard $U$ parameter has been a subject of debate and its value has been reported over a wide range. In this paper, taking focus on the phase transition behavior of $\rm VO_{2}$, the Hubbard $U$ parameter for vanadium oxide is determined by using the quasi-harmonic approximation (QHA). First-principles calculations demonstrate that the phase transition temperature can be modulated by varying the $U$ values. The phase transition temperature can be well reproduced by the calculations using the Perdew-Burke-Ernzerhof (PBE) functional combined with the $U$ parameter of 1.5 eV. Additionally, the calculated band structure, insulating or metallic properties, and phonon dispersion with this $U$ value are in line with experimental observations. By employing the QHA to determine the Hubbard $U$ parameter, this study provides valuable insights into the phase transition behavior of $\rm VO_{2}$. The findings highlight the importance of electron correlation effects in accurately describing the properties of this material. The agreement between the calculated results and experimental observations further validates the chosen $U$ value and supports the use of the DFT+$U$ method in studying $\rm VO_{2}$.

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“…For this description, an LCAO basis set was adopted. 39,40 Normconserving Pseudo Dojo pseudopotentials 41 were used to describe the 1s 2 orbitals of C atoms. The energy cut-off was xed at 900 eV and Brillouin-zone integration was performed over a 50 × 50 × 1 k-point grid.…”

Section: Methodsmentioning

confidence: 99%

Towards graphene-based asymmetric diodes: a density functional tight-binding study

Mohebbi,

Pavoni,

Pierantoni

et al. 2024

Nanoscale Adv.

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Insights into first-principles characterization of the monoclinic VO₂(B) polymorph via DFT + U calculation: electronic, magnetic and optical properties

Abstract: We have studied the structural, electronic, magnetic, and optical properties of the VO2(B) polymorph using first-principles calculations based on density functional theory (DFT).

Cited by 12 publications

References 129 publications

Stability, phonon calculations, electronic structure, and optical properties of a VO2(M) nanostructure: A comprehensive density functional theory study

Stability, phonon calculations, electronic structure, and optical properties of a VO2(M) nanostructure: A comprehensive density functional theory study

Determining Hubbard U of VO₂ by the quasi-harmonic approximation

Towards graphene-based asymmetric diodes: a density functional tight-binding study

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Insights into first-principles characterization of the monoclinic VO2(B) polymorph via DFT + U calculation: electronic, magnetic and optical properties

Abstract: We have studied the structural, electronic, magnetic, and optical properties of the VO2(B) polymorph using first-principles calculations based on density functional theory (DFT).

Cited by 12 publications

References 129 publications

Stability, phonon calculations, electronic structure, and optical properties of a VO2(M) nanostructure: A comprehensive density functional theory study

Stability, phonon calculations, electronic structure, and optical properties of a VO2(M) nanostructure: A comprehensive density functional theory study

Determining Hubbard U of VO2 by the quasi-harmonic approximation

Towards graphene-based asymmetric diodes: a density functional tight-binding study

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Product

Resources

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Insights into first-principles characterization of the monoclinic VO₂(B) polymorph via DFT + U calculation: electronic, magnetic and optical properties

Determining Hubbard U of VO₂ by the quasi-harmonic approximation