Unified calculations of spin-Hamiltonian parameters and optical band positions for Ni+ ion in AgGaSe2 crystal

作者：Zhang Xin-Xin; Mei Yang; Liu Gang; Zheng Wen-Chen^*

来源：Molecular Physics, 2015, 113(22): 3384-3388.

DOI：10.1080/00268976.2015.1025881

• electron paramagnetic resonance
• optical spectra
• crystal- and ligand-field theory
• Ni+
• AgGaSe2
• 71
• 70Ch
• 76
• 30Fc
• 55Ht
• 78
• 40Ha

The complete diagonalisation (of energy matrix) method based on the two-spin-orbit-parameter model is applied to unifiedly calculate the spin-Hamiltonian parameters (g factors g(//), g(perpendicular to) and hyperfine structure constants A(//), A(perpendicular to)) and optical band positions for Ni+ ion in silver gallium selenide (AgGaSe2) crystal. In the model, besides the contribution due to the spin-orbit parameter of central d(n) ion (i.e., the one-spin-orbit-parameter model in the traditional crystal-field theory), that of ligand ions are taken into account. The calculated results are reasonably consistent with the experimental values. The local structure of Ni+ centre in AgGaSe2 is estimated through the calculation. The complete diagonalisation method based on the one-spin-orbit-parameter model is also applied to calculate these electron paramagnetic resonance and optical data. It is found that although the calculated optical band positions are close to those based on the two-spin-orbit-parameter model and hence to the experimental values, the calculated spin-Hamiltonian parameters (in particular, the g factors) are in disagreement with the experimental values. The latter point is further confirmed from the calculations with the perturbation method. So, for the rational calculations of spin-Hamiltonian parameters of d(n) clusters with ligand having large spin-orbit parameter, the contributions due to spin-orbit parameters of both the central d(n) ion and ligand ion should be contained.

• 出版日期2015-11-17
• 单位四川大学; 绵阳师范学院