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Why Cannot All Divalent Cations Completely Substitute the Pb Cations

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Why Cannot All Divalent Cations Completely Substitute the Pb Cations Physics Letters A 383 (2019) 2130–2138 Contents lists available at ScienceDirect Physics Letters A www.elsevier.com/locate/pla Why cannot all divalent cations completely substitute the Pb cations of CH3NH3PbI3 perovskite? ∗ Denghui Ji a, , Shuling Wang b, Hong Zhang b, Huaying Wang b, Buqin Zhang c, Congmin Zhang a, Xiuling Li d a College of Physics, Mechanical and Electronical College, Shijiazhuang University, Shijiazhuang City, 050035, People’s Republic of China b School of Mathematics and Physics, Hebei University of Engineering, Handan city, 056038, People’s Republic of China c Fengfeng Group Co. Ltd., JZEG, Handan city, 056107, People’s Republic of China d College of Physics and Information Engineering, Hebei Advanced Thin Films Laboratory, Hebei Normal University, Shijiazhuang City, 050024, People’s Republic of China a r t i c l e i n f o a b s t r a c t Article history: Organic-inorganic hybrid CH3NH3PbI3 perovskite has a great potential for applications in low-cost Received 3 August 2018 photovoltaic devices. However, the doped and substitution of Pb sites in CH3NH3PbI3 has not been widely Received in revised form 21 December 2018 reported. In this article, a quantum mechanical model was applied to determine why all divalent cations Accepted 8 April 2019 cannot substitute the Pb cations of CH NH PbI perovskite. The evaluation was performed by comparison Available online 12 April 2019 3 3 3 the model with experimental results. On this basis, we carefully examined 42 types of cations and Communicated by R. Wu 2+ 2+ 2+ 2+ 2+ 2+ 2+ 2+ 2+ identified only nine kinds of cations including Ca , Sr , Sc , Ti , V , Y , Zr , Nb and Sn Keywords: for doped into Pb sites. In these cases, it is expected that the corresponding compound would be single Organic-inorganic hybrid phase. Finally, an analysis was performed based on first principle, and the results indicate that divalent Pb site substitution cations substituting the Pb sites modify the band structure and influence the performance of perovskite- Quantum mechanical model based photostatics. The first principle © 2019 Elsevier B.V. All rights reserved. 1. Introduction erties [6]. Michael Saliba et al. achieved a stabilized efficiency of + up to 21.6% for Rb cations doped into the A sites [7]. Burschka, J. = Organic-inorganic hybrid perovskite is widely investigated ow- et al. reported that CH3NH3PbX3 (X Cl, Br, I) perovskite absorbers ing to its excellent structural and optical properties, and its poten- demonstrated power conversion deficiencies over 15% [8]. The ef- tial electronic applications. In particular, CH3NH3PbI3 perovskite fect of Cl substitution on the shift current, and the Cl substitution has been investigated due in part to its high efficiency which ap- at the equatorial site induces a larger response than substitution proaches 22.1% for photovoltaic applications [1]. Perovskites have at the apical site were explored by Fan Zheng et al. [9]. the general formula ABX3, which consists of a network of BX6 oc- Javier Navas et al. [10]first presented results on the synthe- 2+ tahedra where the B atom is a metal cation (typically Sn or sis of the organic-inorganic hybrid perovskite, CH3NH3Pb1−xBxI3, + + + + 2+ − − − = 2 2 2 2 = Pb ), and the X is a monovalent anion (such as F , Cl , Br , B Sn , Sr , Cd and Ca , x 0.05, 0.10, 0.15. The XRD re- − 2+ 2+ 2+ or I ); the A cation is selected to balance the total charge, and it sults showed that the cations Sn , Sr , and Ca can be doped 2+ can be a small molecular species. into the Pb sites and form a single phase, but the cations Cd Doped is widely performed in various areas such as spinel [2], seems to hinder the formation reaction of perovskite, and instead diluted magnetic semiconductors [3], spin systems [4], and inor- formed PbI2 or CdI2 as the second phase. Moreover, DR-UV-Vis ganic perovskites [5], and continues to attract significant attention. spectroscopy revealed a decrease in the band gap with the ad- 2+ 2+ 2+ B. Slimi et al. synthesized formamidinium methylammonium lead dition of the dopants following the trend Sr < Cd < Ca ≈ 2+ 2+ triiodide (NH2CHNH2)1−x(CH3NH2)xPbI3(FA1−xMAxPbI3) thin films < CH3NH3PbI3 Sn . These results indicated that all the Sn , 2+ 2+ 2+ and investigated their morphological, structural and optical prop- Sr , Ca cations and a part of the Cd cations can be doped into the B sites. With the further doped level, the physical mech- anism changed into substituted mechanism. Unfortunately, no ex- * Corresponding author. planation of this behavior is given in the article. In general, there E-mail address: [email protected] (D. Ji). are many reports on CH3NH3PbI3 perovskites doped into the A or https://doi.org/10.1016/j.physleta.2019.04.014 0375-9601/© 2019 Elsevier B.V. All rights reserved. D. Ji et al. / Physics Letters A 383 (2019) 2130–2138 2131 + Fig. 1. The curves of the second ionization energy and the content ratio R versus 42 kinds of cations. The red line represents the second ionization energy of the Pb2 cations. (For interpretation of the colors in the figure(s), the reader is referred to the web version of this article.) X sites [11,12], but there are few reports on B site doped or substi- shapes of the two potential barriers deviate from a square barrier. tution. Naturally, the inability of divalent cations to be doped into The content ratio R between the B-site cations can be obtained the Pb sites of CH3NH3PbI3 perovskite has become a very impor- as: tant physical problem. TB1 V B2 1/2 1/2 In our early investigations [13,14], we proposed a quantum- R = = exp 10.24 rB2 V − c • rB1 V , (2) T V B2 B1 mechanical method for estimating the cation distribution in ABO3 B2 B1 type inorganic perovskites and cubic spinel ferrites. This approach where T B1, T B2 represents the probability of the last ionized elec- 4+ 4+ successfully explained why there are Mn ions, but no La or tron of the B1, B2 cations at the B sites, jumping to the anions 3+ Ca ions in the La1−xCaxMnO3 system. In addition, the difference through the potential barriers with the height V B1, V B2 and width between the observed and the traditional theoretical magnetic mo- rB1, rB2, respectively; V B1 and V B2 are the ionization energies of = ments of the spinel structure ferrites MFe2O4 (M Mn, Fe, Co, Ni, the last ionized electron of the cations B1 and B2, respectively; Cu) was explained, and fitted the dependence of the magnetic mo- and rB1 and rB2 are the distances from the cations B1 and B2 to = ments of the ferrites M1−xZnxFe2O4 (M Mn, Fe, Co, Ni, Cu) on the anions, respectively. the doped level x perfectly. Since both the B1 and B2 cations are at the B sites, rB1 = rB2. 2+ In this paper, we used the quantum-mechanical method to elu- Based on ref. [10], the distance (rB2) between the Pb (B2) cations − + cidate why not all divalent cations substitute the Pb cations of 2 and the I anions is 0.31515 nm. The content ratio R0 of the Pb CH3NH3PbI3 perovskite completely. In addition, the proposed con- cations are shown in Table 1. Because the distance (rB2) becomes cepts were compared with experimental results. Based on our find- smaller or larger when the B1 cations are doped into the B sites, ings, we predict that only 9 kinds of cations can be doped into the we allow the distance to change in the range −5% and +5%, and 2+ 2+ 2+ 2+ 2+ 2+ 2+ 2+ Pb sites, including Ca , Sr , Sc , Ti , V , Y , Zr , Nb the content ratio labeled as R−0.5 and R+0.5 are also shown in Ta- 2+ and Sn . In addition, related physical properties were obtained ble 1. It can be seen that this ratio R increases with a decrease by using the first principle. of the second ionization energy, and decreases with an increase of the distance between the cations B1 and B2 to the anions. This 2. The quantum-mechanical method response results from the increase of the height of the potential barrier and the width of the potential barrier are reported by Tang 2+ We supposed that there is a square potential barrier between et al. [13,14]. In the case of B2 as the Pb cations, R is equal to 2+ a cation-anion pair [13,14]. The height of the potential barrier is 1 because the cations of both B1 and B2 are Pb . This indicates 2+ proportional to the ionization energy of the last ionized electron, that all the Pb cations can be doped into the B sites. Therefore, and the width of the potential barrier is related to the distance be- the value of R greater than or less than 1 is essentially the crite- tween neighboring cations and anions. The content ratio R of the rion which determines whether all the cations can replace the Pb cations. A-site cations to the B-site cations which is related to the probabil- In order to show this idea in a more intuitive manner, Fig. 1 ity of their last ionized electrons penetrating the potential barrier represents the curves of the second ionization energy and the can be derived, and takes the following form: content ratio R for 42 kinds of cations. The content ratio R 2+ 2+ 2+ 2+ 2+ 2+ 2+ 2+ 2+ TA V B 1/2 1/2 of only Ca , Sr , Sc , Ti , V , Y , Zr , Nb , Sn , and = = − • 2+ R exp 10.24 rB V B c rA V A , (1) Pb is greater than or equal to 1, indicating that these 10 kinds TB V A of cations can completely replace the Pb cations.
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