Ju, Meng Xiao, Yang Zhong, MingMin Sun, Weiguo Xia, Xinxin Yeung, Yau-yuen Lu, Cheng New Theoretical Insights into the Crystal-Field Splitting and Transition Mechanism for Nd<sup>3+</sup>-Doped Y<sub>3</sub>Al<sub>5</sub>O<sub>12</sub> There has been considerable research interest paid to rare-earth transition-metal-doped Y<sub>3</sub>Al<sub>5</sub>O<sub>12</sub>, which has great potential for application as a laser crystal of new-type laser devices because of its unique optoelectronic and photophysical properties. Here, we present new research conducted on the structural evolution and crystal-field characteristics of a rare-earth Nd-doped Y<sub>3</sub>Al<sub>5</sub>O<sub>12</sub> laser crystal by using the CALYPSO structure search method and our newly developed WEPMD method. A novel cage-like structure with a Nd<sup>3+</sup> concentration of 4.16% is uncovered, which belongs to the standardized <i>C</i><sub>222</sub> space group. Our results indicate that the impurity Nd<sup>3+</sup> ions are likely to substitute the Y<sup>3+</sup> at the central site of the host Y<sub>3</sub>Al<sub>5</sub>O<sub>12</sub> crystal lattice. The laser emission <sup>4</sup>F<sub>3/2</sub> ⃗ <sup>4</sup>I<sub>11/2</sub> occurring at 1077 nm is in accord with that of the experimental data. By introducing the proper correlation crystal field, three transitions, <sup>4</sup>G<sub>5/2</sub> ⃗ <sup>4</sup>I<sub>9/2</sub>, <sup>4</sup>F<sub>7/2</sub> ⃗ <sup>4</sup>I<sub>9/2</sub>, and <sup>4</sup>S<sub>3/2</sub> ⃗ <sup>4</sup>I<sub>9/2</sub>, are predicted to be good candidates for laser action. These findings can provide powerful guidelines for further experiments of rare-earth-metal-doped laser crystals. WEPMD method;research interest;Doped Y 3 Al 5 O 12;rare-earth transition-metal-doped Y 3 Al 5 O 12;new-type laser devices;1077 nm;rare-earth Nd-doped Y 3 Al 5 O 12 laser crystal;laser crystal;Transition Mechanism;rare-earth-metal-doped laser crystals;laser action;photophysical properties;correlation crystal field;C 222 space group;CALYPSO structure search method;host Y 3 Al 5 O 12 crystal lattice;novel cage-like structure;Crystal-Field Splitting;crystal-field characteristics 2019-02-21
    https://acs.figshare.com/articles/journal_contribution/New_Theoretical_Insights_into_the_Crystal-Field_Splitting_and_Transition_Mechanism_for_Nd_sup_3_sup_-Doped_Y_sub_3_sub_Al_sub_5_sub_O_sub_12_sub_/7804433
10.1021/acsami.9b00973.s001