Abstract
We investigated, using DFT calculations, the electronic, optical, polaron properties and estimate the upper light yield of \({\mathrm{Tl}}_{2}{\mathrm{ZrCl}}_{6}\) material. The DFT calculations were performed with GGA+mBJ and GGA+mBJ+SOC approximations to obtain precise electronic, optical and polaron properties. The calculated results showed that \({\mathrm{Tl}}_{2}{\mathrm{ZrCl}}_{6}\) has localized valence and narrow discrete conduction bands with many sharp peaks and low dispersion which reflects the heavier effective mass of electron at CBM, 4.63 \({m}_{e}\), in comparison with that of hole at VBM, 1.05 \({m}_{e}\). Indirect band gap energy of 4.30 eV was observed and which is close to the experimental value, 4.22 eV. Additionally, in the emission range, this material exhibited a high transmittance rate of around 90% which is an advantage of the scintillation properties. Following DFT calculations, polaron properties and also the temperature-dependence of polaron mobility and relaxation time were calculated by solving the Feynman polaron model, variationally, with the free-energies minimization. The obtained results showed that \({\mathrm{Tl}}_{2}{\mathrm{ZrCl}}_{6}\) has a large electron (hole)-phonon coupling, \({\alpha }_{e}=8.55\)(\({\alpha }_{h}=4.1)\), leading to large polaron mass, small relaxation time, high scattering rate and low electron (hole) mobility of 0.13 \({cm}^{2}{V}^{-1}{s}^{-1}\) (4.17 \({cm}^{2}{V}^{-1}{s}^{-1}\)) at room-temperature. Such low mobility has a positive role only in the initial ionization track by increasing the recombination yield. Moreover, using the polaron and simple phenomenological models, the upper light yield was estimated to be 87,757 \(ph/MeV\) and 75,187 \(ph/MeV\). Such findings could have important implications for understanding the scintillation behavior of this material to improve its performance as a potential scintillator for γ- and X-rays detection.
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Data are available from the authors upon reasonable request and with the permission of [Deanship of Scientific Research at King Khalid University].
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Acknowledgements
The authors extend their appreciation to the Deanship of Scientific Research at King Khalid University for funding this work through Small Groups Project under Grant No. (R.G.P.1/193/43).
Funding
This work was supported by [the Deanship of Scientific Research at King Khalid University] (Grant No. [R.G.P.1/193/43]).
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Naji, S., Murshed, M.N., El Sayed, M.E. et al. A computational investigation of electronic, optical, and polaron properties and upper light yield prediction of new self-activated scintillator Tl2ZrCl6 using polaron and simple phenomenological models. Opt Quant Electron 55, 279 (2023). https://doi.org/10.1007/s11082-023-04547-9
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DOI: https://doi.org/10.1007/s11082-023-04547-9