zhpsЖурнал прикладной спектроскопииZhurnal Prikladnoii Spektroskopii0514-7506B. I. Stepanov Institute of Physics of the National Academy of Scienceszhps-1281Research ArticleАННОТАЦИИ АНГЛОЯЗЫЧНЫХ СТАТЕЙABSTRACTS ENGLISH-LANGUAGE ARTICLESВлияние упаковки двумерных перовскитов на основе хлорида свинца в вертикальные гетероструктуры на интенсивность фотолюминесценцииEffect of Stacking 2D Lead Chloride Perovskites into Vertical Heterostructures on Photoluminescence IntensityGraupnerD. R.GraupnerD. R.

Фарго, Северная Дакота

Department of Chemistry and Biochemistry

Fargo, North Dakota

KilinD. S.KilinD. S.

Фарго, Северная Дакота

Department of Chemistry and Biochemistry

Fargo, North Dakota

dmitri.kilin@ndsu.eduУниверситет штата Северная ДакотаNorth Dakota State University20232503202390234810Copyright © Graupner D.R., Kilin D.S., 20232023Graupner D.R., Kilin D.S.Graupner D.R., Kilin D.S.Данная работа распространяется под лицензией Creative Commons Attribution 4.0.This work is licensed under a Creative Commons Attribution 4.0 License.https://zhps.ejournal.by/jour/article/view/1281

С использованием теории функционала плотности и динамики возбужденного состояния, обработанного методом приведенной матрицы плотности, изучено влияние изменения толщины слоя перовскита на фотофизические свойства 2D-перовскитов на основе галогенидов свинца в основном и возбужденном состояниях, далее исследованы эффекты вертикальной гетероструктуры слоев перовскита. Неадиабатические взаимодействия рассчитаны на основе подхода on-the-fly по траектории молекулярной динамики при температуре окружающей среды. Уравнение движения электронных степеней свободы на основе матрицы плотности используется для расчета динамики электронных степеней свободы. Обнаружено, что вертикальная укладка двумерных перовскитов в гетероструктуры приводит к увеличению интенсивности фотолюминесценции на два порядка по сравнению с отдельными двумерными перовскитами.

Two-dimensional organic-inorganic hybrid lead halide perovskites are of interest for photovoltaic and light emitting devices due to their relative stability when compared to bulk lead halide perovskites and favorable properties that can be tuned. Tuning of the material can be performed by adjusting halide composition or by taking advantage of confinement effects. Here we use density functional theory and excited state dynamics treated by reduced density matrix method to examine the effects that varying the thickness of the perovskite layer has on the ground state and excited state photo-physical properties of the materials, further we explore the effects of a vertical heterostructure of perovskite layers. Nonadiabatic couplings were computed based on the on-the-fly approach along a molecular dynamic trajectory at ambient temperatures. Density matrix-based equation of motion for electronic degrees of freedom is used to calculate the dynamics of electronic degrees of freedom. We find that the vertical stacking of two-dimensional perovskites into heterostructures shows an increase in photoluminescence intensity by two orders of magnitude when compared to the individual two-dimensional perovskites.

фотолюминесценциягетероструктурадвумерные перовскитыphotoluminescenceheterostructuretwo-dimensional perovskitesD.G. Thanks NSF CHE-2004197 for support. D.K. acknowledges the support of the National Science Foundation under Grant CHE-1944921. Authors thank the DOE BES NERSC facility for computational resources, allocation award “Computational Modeling of Photo-catalysis and Photoinduced Charge Transfer Dynamics on Surfaces”, supported by the Office of Science of the DOE under Contract DE-AC02-05CH11231.ReferencesL. Protesescu, S. Yakunin, M. I. Bodnarchuk, F. Krieg, R. Caputo, C. H. Hendon, R. X. Yang, A. Walsh, M. V. Kovalenko, Nano Lett., 15, No. 6, 3692 (2015), doi: 10.1021/nl5048779.L. Protesescu, S. Yakunin, M. I. Bodnarchuk, F. Krieg, R. Caputo, C. H. Hendon, R. X. Yang, A. Walsh, M. V. Kovalenko, Nano Lett., 15, No. 6, 3692 (2015), doi: 10.1021/nl5048779.B. R. Sutherland, E. H. Sargent, Nat. Photonics, 10, No. 5, 295 (2016), doi: 10.1038/nphoton.2016.62.B. R. Sutherland, E. H. Sargent, Nat. Photonics, 10, No. 5, 295 (2016), doi: 10.1038/nphoton.2016.62.3. X. Chen, H. Zhou, H. Wang, Front. Chem., 9 (2021), doi: 10.3389/fchem.2021.715157.3. X. Chen, H. Zhou, H. Wang, Front. Chem., 9 (2021), doi: 10.3389/fchem.2021.715157.E.-B. Kim, M. S. Akhtar, H.-S. Shin, S. Ameen, M. K. Nazeeruddin, J. Photochem. Photobiol., C 48, 100405 (2021), doi: 10.1016/j.jphotochemrev.2021.100405.E.-B. Kim, M. S. Akhtar, H.-S. Shin, S. Ameen, M. K. Nazeeruddin, J. Photochem. Photobiol., C 48, 100405 (2021), doi: 10.1016/j.jphotochemrev.2021.100405.C. Ma, C. Leng, Y. Ji, X. Wei, K. Sun, L. Tang, J. Yang, W. Luo, C. Li, Y. Deng, S. Feng, J. Shen, S. Lu, C. Du, H. Shi, Nanoscale, 8, No. 43, 18309 (2016), doi: 10.1039/C6NR04741F.C. Ma, C. Leng, Y. Ji, X. Wei, K. Sun, L. Tang, J. Yang, W. Luo, C. Li, Y. Deng, S. Feng, J. Shen, S. Lu, C. Du, H. Shi, Nanoscale, 8, No. 43, 18309 (2016), doi: 10.1039/C6NR04741F.F. Arabpour Roghabadi, M. Alidaei, S. M. Mousavi, T. Ashjari, A. S. Tehrani, V. Ahmadi, S. M. Sadrameli, J. Mater. Chem. A, 7, No. 11, 5898 (2019), doi:10.1039/C8TA10444A.F. Arabpour Roghabadi, M. Alidaei, S. M. Mousavi, T. Ashjari, A. S. Tehrani, V. Ahmadi, S. M. Sadrameli, J. Mater. Chem. A, 7, No. 11, 5898 (2019), doi:10.1039/C8TA10444A.G. E. Eperon, S. D. Stranks, C. Menelaou, M. B. Johnston, L. M. Herz, H. J. Snaith, Energy Environ. Sci., 7, No. 3, 982 (2014), doi:10.1039/C3EE43822H.G. E. Eperon, S. D. Stranks, C. Menelaou, M. B. Johnston, L. M. Herz, H. J. Snaith, Energy Environ. Sci., 7, No. 3, 982 (2014), doi:10.1039/C3EE43822H.T. M. Koh, V. Shanmugam, J. Schlipf, L. Oesinghaus, P. Muller-Buschbaum, N. Ramakrishnan, V. Swamy, N. Mathews, P. P. Boix, S. G. Mhaisalkar, Adv. Mater., 28, No. 19, 3653 (2016), doi: 10.1002/adma.201506141.T. M. Koh, V. Shanmugam, J. Schlipf, L. Oesinghaus, P. Muller-Buschbaum, N. Ramakrishnan, V. Swamy, N. Mathews, P. P. Boix, S. G. Mhaisalkar, Adv. Mater., 28, No. 19, 3653 (2016), doi: 10.1002/adma.201506141.Z.-K. Tan, R. S. Moghaddam, M. L. Lai, P. Docampo, R. Higler, F. Deschler, M. Price, A. Sadhanala, M. Pazos, D. Credgington, F. Hanusch, T. Bein, H. J. Snaith, R. H. Friend, Nat. Nanotechnol., 9, No. 9, 687 (2014), doi: 10.1038/nnano.2014.149.Z.-K. Tan, R. S. Moghaddam, M. L. Lai, P. Docampo, R. Higler, F. Deschler, M. Price, A. Sadhanala, M. Pazos, D. Credgington, F. Hanusch, T. Bein, H. J. Snaith, R. H. Friend, Nat. Nanotechnol., 9, No. 9, 687 (2014), doi: 10.1038/nnano.2014.149.Y. Miao, L. Cheng, W. Zou, L. Gu, J. Zhang, Q. Guo, Q. Peng, M. Xu, Y. He, S. Zhang, Y. Cao, R. Li, N. Wang, W. Huang, J. Wang, Light: Sci. Appl., 9, No. 1, 89 (2020), doi: 10.1038/s41377-020-0328-6.Y. Miao, L. Cheng, W. Zou, L. Gu, J. Zhang, Q. Guo, Q. Peng, M. Xu, Y. He, S. Zhang, Y. Cao, R. Li, N. Wang, W. Huang, J. Wang, Light: Sci. Appl., 9, No. 1, 89 (2020), doi: 10.1038/s41377-020-0328-6.L. Zhang, C. Sun, T. He, Y. Jiang, J. Wei, Y. Huang, M. Yuan, Light: Sci. Appl., 10, No. 1, 61 (2021), doi: 10.1038/s41377-021-00501-0.L. Zhang, C. Sun, T. He, Y. Jiang, J. Wei, Y. Huang, M. Yuan, Light: Sci. Appl., 10, No. 1, 61 (2021), doi: 10.1038/s41377-021-00501-0.C. Zhao, D. Zhang, C. Qin, CCS Chem., 2, No. 4, 859 (2020), doi: 10.31635/ccschem.020.202000216.C. Zhao, D. Zhang, C. Qin, CCS Chem., 2, No. 4, 859 (2020), doi: 10.31635/ccschem.020.202000216.L. Mao, W. Ke, L. Pedesseau, Y. Wu, C. Katan, J. Even, M. R. Wasielewski, C. C. Stoumpos, M. G. Kanatzidis, J. Am. Chem. Soc., 140, No. 10, 3775 (2018), doi: 10.1021/jacs.8b00542.L. Mao, W. Ke, L. Pedesseau, Y. Wu, C. Katan, J. Even, M. R. Wasielewski, C. C. Stoumpos, M. G. Kanatzidis, J. Am. Chem. Soc., 140, No. 10, 3775 (2018), doi: 10.1021/jacs.8b00542.M. Dion, M. Ganne, M. Tournoux, Mater. Res. Bull., 16, No. 11, 1429 (1981), doi: 10.1016/00255408(81)90063-5.M. Dion, M. Ganne, M. Tournoux, Mater. Res. Bull., 16, No. 11, 1429 (1981), doi: 10.1016/00255408(81)90063-5.A. J. Jacobson, J. W. Johnson, J. T. Lewandowski, Inorg. Chem., 24, No. 23, 3727 (1985), doi: 10.1021/ic00217a006.A. J. Jacobson, J. W. Johnson, J. T. Lewandowski, Inorg. Chem., 24, No. 23, 3727 (1985), doi: 10.1021/ic00217a006.C. C. Stoumpos, D. H. Cao, D. J. Clark, J. Young, J. M. Rondinelli, J. I. Jang, J. T. Hupp, L. G. Kanatzidis, Chem. Mater., 28, No. 8, 2852 (2016), doi: 10.1021/acs.chemmater.6b00847.C. C. Stoumpos, D. H. Cao, D. J. Clark, J. Young, J. M. Rondinelli, J. I. Jang, J. T. Hupp, L. G. Kanatzidis, Chem. Mater., 28, No. 8, 2852 (2016), doi: 10.1021/acs.chemmater.6b00847.K. R. Kendall, C. Navas, J. K. Thomas, H.-C. zur Loye, Chem. Mater., 8, No. 3, 642 (1996), doi: 10.1021/cm9503083.K. R. Kendall, C. Navas, J. K. Thomas, H.-C. zur Loye, Chem. Mater., 8, No. 3, 642 (1996), doi: 10.1021/cm9503083.C. M. M. Soe, C. C. Stoumpos, M. Kepenekian, B. Traoré, H. Tsai, W. Nie, B. Wang, C. Katan, R. Seshadri, A. D. Mohite, J. Even, T. J. Marks, M. G. Kanatzidis, J. Am. Chem. Soc., 139, No. 45, 16297 (2017), doi: 10.1021/jacs.7b09096.C. M. M. Soe, C. C. Stoumpos, M. Kepenekian, B. Traoré, H. Tsai, W. Nie, B. Wang, C. Katan, R. Seshadri, A. D. Mohite, J. Even, T. J. Marks, M. G. Kanatzidis, J. Am. Chem. Soc., 139, No. 45, 16297 (2017), doi: 10.1021/jacs.7b09096.K. Wang, J. Y. Park, Akriti, L. Dou, EcoMat, 3, No. 3, e12104 (2021), doi: 10.1002/eom2.12104.K. Wang, J. Y. Park, Akriti, L. Dou, EcoMat, 3, No. 3, e12104 (2021), doi: 10.1002/eom2.12104.J. C. Blancon, A. V. Stier, H. Tsai, W. Nie, C. C. Stoumpos, B. Traoré, L. Pedesseau, M. Kepenekian, F. Katsutani, G. T. Noe, J. Kono, S. Tretiak, S. A. Crooker, C. Katan, M. G. Kanatzidis, J. J. Crochet, J. Even, A. D. Mohite, Nat. Commun., 9, No. 1, 2254 (2018), doi: 10.1038/s41467-018-04659-x.J. C. Blancon, A. V. Stier, H. Tsai, W. Nie, C. C. Stoumpos, B. Traoré, L. Pedesseau, M. Kepenekian, F. Katsutani, G. T. Noe, J. Kono, S. Tretiak, S. A. Crooker, C. Katan, M. G. Kanatzidis, J. J. Crochet, J. Even, A. D. Mohite, Nat. Commun., 9, No. 1, 2254 (2018), doi: 10.1038/s41467-018-04659-x.L. N. Quan, M. Yuan, R. Comin, O. Voznyy, E. M. Beauregard, S. Hoogland, A. Buin, A. R. Kirmani, K. Zhao, A. Amassian, D. H. Kim, E. H. Sargent, J. Am. Chem. Soc., 138, No. 8, 2649 (2016), doi: 10.1021/jacs.5b11740.L. N. Quan, M. Yuan, R. Comin, O. Voznyy, E. M. Beauregard, S. Hoogland, A. Buin, A. R. Kirmani, K. Zhao, A. Amassian, D. H. Kim, E. H. Sargent, J. Am. Chem. Soc., 138, No. 8, 2649 (2016), doi: 10.1021/jacs.5b11740.C. P. Clark, J. E. Mann, J. S. Bangsund, W.-J. Hsu, E. S. Aydil, R. J. Holmes, ACS Energy Lett., 5, No. 11, 3443 (2020), doi: 10.1021/acsenergylett.0c01609.C. P. Clark, J. E. Mann, J. S. Bangsund, W.-J. Hsu, E. S. Aydil, R. J. Holmes, ACS Energy Lett., 5, No. 11, 3443 (2020), doi: 10.1021/acsenergylett.0c01609.J. P. Perdew, K. Burke, M. Ernzerhof, Phys. Rev. Lett., 78, No. 7, 1396 (1997), doi: 10.1103/PhysRevLett.78.1396.J. P. Perdew, K. Burke, M. Ernzerhof, Phys. Rev. Lett., 78, No. 7, 1396 (1997), doi: 10.1103/PhysRevLett.78.1396.G. Kresse, D. Joubert, Phys. Rev. B, 59, No. 3, 1758 (1999), doi: 10.1103/PhysRevB.59.1758.G. Kresse, D. Joubert, Phys. Rev. B, 59, No. 3, 1758 (1999), doi: 10.1103/PhysRevB.59.1758.P. E. Blöchl, Phys. Rev. B, 50, No. 24, 17953 (1994), doi: 10.1103/PhysRevB.50.17953.P. E. Blöchl, Phys. Rev. B, 50, No. 24, 17953 (1994), doi: 10.1103/PhysRevB.50.17953.G. Kresse, J. Furthmüller, Comput. Mater. Sci., 6, No. 1, 15 (1996), doi: 10.1016/0927-0256(96)00008-0.G. Kresse, J. Furthmüller, Comput. Mater. Sci., 6, No. 1, 15 (1996), doi: 10.1016/0927-0256(96)00008-0.J. Kubler, K. H. Hock, J. Sticht, A. R. Williams, J. Phys. F: Met. Phys., 18, No. 3, 469 (1988), doi: 10.1088/0305-4608/18/3/018.J. Kubler, K. H. Hock, J. Sticht, A. R. Williams, J. Phys. F: Met. Phys., 18, No. 3, 469 (1988), doi: 10.1088/0305-4608/18/3/018.U. V. Barth, L. Hedin, J. Phys. C: Solid State Phys., 5, No. 13, 1629 (1972), doi: 10.1088/00223719/5/13/012.U. V. Barth, L. Hedin, J. Phys. C: Solid State Phys., 5, No. 13, 1629 (1972), doi: 10.1088/00223719/5/13/012.A. G. Redfield, IBM J. Res. Dev. 1, No. 1, 19 (1957), doi: 10.1147/rd.11.0019.A. G. Redfield, IBM J. Res. Dev. 1, No. 1, 19 (1957), doi: 10.1147/rd.11.0019.J. M. Jean, R. A. Friesner, G. R. Fleming, J. Chem. Phys., 96, No. 8, 5827 (1992), doi: 10.1063/1.462858.J. M. Jean, R. A. Friesner, G. R. Fleming, J. Chem. Phys., 96, No. 8, 5827 (1992), doi: 10.1063/1.462858.A. Einstein, Phys. Z., 18, 121 (1917).A. Einstein, Phys. Z., 18, 121 (1917).M. Kasha, Discuss. Faraday Soc., 9, 14 (1950), doi: 10.1039/DF9500900014.M. Kasha, Discuss. Faraday Soc., 9, 14 (1950), doi: 10.1039/DF9500900014.Y. Fu, W. Zheng, X. Wang, M. P. Hautzinger, D. Pan, L. Dang, J. C. Wright, A. Pan, S. Jin, J. Am. Chem. Soc., 140, No. 46, 15675 (2018), doi: 10.1021/jacs.8b07843.Y. Fu, W. Zheng, X. Wang, M. P. Hautzinger, D. Pan, L. Dang, J. C. Wright, A. Pan, S. Jin, J. Am. Chem. Soc., 140, No. 46, 15675 (2018), doi: 10.1021/jacs.8b07843.

The authors declare that there are no conflicts of interest present.