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Aaron Forde1 Talgat Inerbaev2 Dmitri Kilin1

1, North Dakota State University, Fargo, North Dakota, United States
2, L.N. Gumilev Eurasian National University, Astana, , Kazakhstan

Computational modeling of photoexcited dynamics in perovskite quantum dots materials doped by low concentration transition metal ions of Mn(2+), demonstrates how excitation thermalizes to the doping site and participate in the radiative PL processes independent on existence of surface trap sites. The computation is based on dissipative propagation of the excited state by Redfield equation of motion. The nonadiabatic transitions betweeen electronic states are facilitated by nuclear motion and are computed in the basis of non-collinear spin DFT,[1] which accounts for the spin-orbit interactions. The quantum yileld is numerically estimated by comparing rates of radiative and nonradiative recombination pathways [2]The presence of surface traps and surface charge transfer[3] is found to have minimal influence of the doping-related PL.

[1]
Barth, U. v.; Hedin, L., A local exchange-correlation potential for the spin polarized case. i. J. Phys. C: Solid State Phys. 1972, 5 (13), 1629-1642.
[2] Vogel, D. J.; Kryjevski, A.; Inerbaev, T.; Kilin, D. S., Photoinduced Single- and Multiple-Electron Dynamics Processes Enhanced by Quantum Confinement in Lead Halide Perovskite Quantum Dots. J. Phys. Chem. Lett. 2017, 8 (13), 3032-3039.
[3] Forde, A.; Kilin, D. Hole Transfer in Dye-Sensitized Cesium Lead Halide Perovskite Photovoltaics: Effect of Interfacial Bonding. The Journal of Physical Chemistry C 2017, 121, 20113-20125.

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