Mikaël Kepenekian1,B, Cucco1,G. Volonakis1,Claudine Katan1,Jacky Even2
Univ Rennes, ENSCR, CNRS, ISCR-UMR 62261,Univ Rennes, INSA Rennes, CNRS, Institut FOTON − UMR 60822
Mikaël Kepenekian1,B, Cucco1,G. Volonakis1,Claudine Katan1,Jacky Even2
Univ Rennes, ENSCR, CNRS, ISCR-UMR 62261,Univ Rennes, INSA Rennes, CNRS, Institut FOTON − UMR 60822
If 3-dimensional (3D) halide perovskites AMX<sub>3</sub> (A: organic cation, M: metal ion, X: halide) have shown spectacular results in optoelectronic devices, they offer limited choice of metals and organic cations. This is not the case of the other shapes that impose far less constraints over the chemical design of the organic spacer, such as layered (2D) halide perovskites A<sub>2</sub>MX<sub>4</sub> [1]. In addition to strictly 2D and 3D materials, there is a wealth of compounds with features of both dimensionality and intriguing properties. Among those, one can find the ‘deficient’ or ‘hollow’ perovskites [2], but also perovskitoids consisting of not-only corner-shared octahedra [3] down to 1D materials. Another direction recently explored aims at moving away from toxic lead using double perovskites structures [4] or even by making a side-step towards cousin structures of perovskites where [MX<sub>6</sub>] octahedra are no longer corner-shared [5]. These compounds often present attractive properties beyond optoelectronic and are used for electronic component, spinorbitronic or photocatalytic devices [6].<br/>However, once the 3D structural lock is lifted, the number of suitable candidates for A becomes so large that guidelines would be desirable for the design of future devices. Here, based on computational investigations conducted on experimental and model systems, we propose to contribute to the writing of those rules. In this contribution, we will navigate this wide range of materials and highlight how modelling and computational investigations, in close contact with experimental approaches, can help rationalize the electronic, optical, magnetic and ionic transport properties of compounds but also lay done rules for the design of new materials for targeted applications [7].<br/> <br/>[1] B. Saparov, D. B. Mitzi, <i>Chem. Rev. </i><b>2016</b>, <i>116</i>, 4558; L. Pedesseau, M.K. <i>et al.</i>, <i>ACS Nano</i> <b>2016</b>, <i>10</i>, 9776; C. Katan, N. Mercier, J. Even, <i>Chem. Rev.</i> <b>2019</b>, <i>119</i>, 3140.<br/>[2] A. Leblanc <i>et al.</i>, <i>Angew. </i><i>Chem. Int. Ed.</i> <b>2017</b>, <i>56</i>, 16067; I. Spanopoulos <i>et al.</i>, <i>J. Am. </i><i>Chem. Soc.</i> <b>2018</b>, <i>140</i>, 5728; A. Leblanc, M.K. <i>et al.</i>, <i>ACS Appl. </i><i>Mater. Interfaces</i> <b>2019</b>, <i>11</i>, 20743.<br/>[3] J. M. Hoffman, M.K. <i>et al.</i>, <i>J. Am. Chem. Soc.</i> <b>2019</b>, <i>141</i>, 10661; X. Li, M.K. <i>et al.</i>, <i>J. Am. Chem. Soc.</i> <b>2022</b>, <i>144</i>, 3902.<br/>[4] G. Volonakis <i>et al.</i>, <i>J. Phys. </i><i>Chem. Lett.</i> <b>2017</b>, <i>8</i>, 772; X. Li, M.K. <i>et al.</i>, <i>Chem. </i><i>Mater.</i> <b>2021</b>, <i>33</i>, 5085; B. Cucco, M.K. <i>et al.</i>, <i>Appl. Phys. Lett.</i> <b>2021</b>, <i>119</i>, 181903.<br/>[5] I. Turkevych <i>et al.</i>, <i>ChemSusChem</i> <b>2017</b>, <i>10</i>, 3754; B. Cucco, M.K. <i>et al.</i>, <i>Solar RRL</i> <b>2022</b>, doi: 10.1002/solr.202200718.<br/>[6] R. A. John <i>et al.</i>, <i>Nat. Commun.</i> <b>2021</b>, <i>12</i>, 3681; M. Kepenekian, J. Even, <i>J. Phys. Chem. Lett.</i> <b>2017</b>, <i>8</i>, 3362; Y. Zhou, J. Chen, O. M. Bakr, O. F. Mohammed, <i>ACS Energy Lett.</i> <b>2021</b>, <i>6</i>, 739.<br/>[7] M. Kepenekian <i>et al.</i>, <i>Nano Lett.</i> <b>2018</b>, <i>18</i>, 5603; X. Li, M.K. <i>et al.</i>, <i>J. Am. Chem. Soc.</i> <b>2022</b>, <i>144</i>, 3902; R. A. John, M.K. <i>et al.</i>, manuscript submitted.