Simulation of structured ⁴T₁?sup>6A₁ emission bands of Mn²⁺ impurity in Zn₂SiO₄: A first-principle methodology

详细信息    查看全文

• 作者：M.K. Kretov^a ; I.M. Iskandarova^b ; B.V. Potapkin^b ; ^c ; A.V. Scherbinin^a ; ^{andrei.scherb@gmail.com} ; A.M. Srivastava^d ; N.F. Stepanov^a
• 关键词：Willemite ; Zn2SiO4 ; Mn2+ emission ; Periodic DFT calculations ; Cluster ab initio calculations ; Vibronic band simulation
• 刊名：Journal of Luminescence
• 出版年：2012
• 出版时间：August, 2012
• 年：2012
• 卷：132
• 期：8
• 页码：2143-2150
• 全文大小：674 K

文摘

A sequential, fully first-principle theoretical study of the Mn²⁺ green emission bands in the Zn₂SiO₄:Mn²⁺ phosphor is presented for the first time. A combined approach is developed based on the modern periodic density-functional theory and cluster ab initio wave-function-based electronic structure methods, the linear response theory for lattice phonons, and generating function formalism of vibronic spectra within the displaced multi-mode harmonic oscillator model. We obtain fairly good agreement between the calculated low- and high-temperature emission band positions, widths, zero-phonon lines and phonon wings and the available experimental emission studies, with special emphasis on Mn²⁺ distribution over two non-equivalent Zn²⁺ sites in the Zn₂SiO₄ material. An interpretation for vibronic structure observed in the low-temperature emission spectrum of this phosphor is suggested based on the present first-principle study.