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Research output: Contribution to Journal/Magazine › Journal article › peer-review
Research output: Contribution to Journal/Magazine › Journal article › peer-review
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TY - JOUR
T1 - Optical excitation of MgO nanoparticles
T2 - a computational perspective
AU - Wobbe, Milena C. C.
AU - Kerridge, Andrew
AU - Zwijnenburg, Martijn A.
N1 - This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.
PY - 2014
Y1 - 2014
N2 - The optical absorption spectra of magnesium oxide (MgO) nanoparticles, along with the atomic centres responsible, are studied using a combination of time-dependent density functional theory (TD-DFT) and coupled-cluster methods. We demonstrate that TD-DFT calculations on MgO nanoparticles require the use of range-separated exchange–correlation (XC-) functionals or hybrid XC-functionals with a high percentage of Hartree–Fock like exchange to circumvent problems related to the description of charge-transfer excitations. Furthermore, we show that the vertical excitations responsible for the experimentally studied range of the spectra of the MgO nanoparticles typically involve both 3-coordinated corner sites and 4-coordinated edge sites. We argue therefore that to label peaks in these absorption spectra exclusively as either corner or edge features does not provide insight into the full physical picture.
AB - The optical absorption spectra of magnesium oxide (MgO) nanoparticles, along with the atomic centres responsible, are studied using a combination of time-dependent density functional theory (TD-DFT) and coupled-cluster methods. We demonstrate that TD-DFT calculations on MgO nanoparticles require the use of range-separated exchange–correlation (XC-) functionals or hybrid XC-functionals with a high percentage of Hartree–Fock like exchange to circumvent problems related to the description of charge-transfer excitations. Furthermore, we show that the vertical excitations responsible for the experimentally studied range of the spectra of the MgO nanoparticles typically involve both 3-coordinated corner sites and 4-coordinated edge sites. We argue therefore that to label peaks in these absorption spectra exclusively as either corner or edge features does not provide insight into the full physical picture.
U2 - 10.1039/C4CP03442B
DO - 10.1039/C4CP03442B
M3 - Journal article
VL - 16
SP - 22052
EP - 22061
JO - Physical Chemistry Chemical Physics
JF - Physical Chemistry Chemical Physics
SN - 1463-9076
IS - 40
ER -