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Structural Diversity in White-Light Emitting Hybrid Lead Bromide

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Structural Diversity in White-Light Emitting Hybrid Lead Bromide Structural Diversity in White-light Emitting Hybrid Lead Bromide Perovskites Lingling Mao, Peijun Guo, Mikael Kepenekian, Ido Hadar, Claudine Katan, Jacky Even, Richard Schaller, Constantinos Stoumpos, Mercouri Kanatzidis To cite this version: Lingling Mao, Peijun Guo, Mikael Kepenekian, Ido Hadar, Claudine Katan, et al.. Structural Diversity in White-light Emitting Hybrid Lead Bromide Perovskites. Journal of the American Chemical Society, American Chemical Society, 2018, 140 (40), pp.13078-13088. 10.1021/jacs.8b08691. hal-01874092 HAL Id: hal-01874092 https://hal.archives-ouvertes.fr/hal-01874092 Submitted on 29 Nov 2018 HAL is a multi-disciplinary open access L’archive ouverte pluridisciplinaire HAL, est archive for the deposit and dissemination of sci- destinée au dépôt et à la diffusion de documents entific research documents, whether they are pub- scientifiques de niveau recherche, publiés ou non, lished or not. The documents may come from émanant des établissements d’enseignement et de teaching and research institutions in France or recherche français ou étrangers, des laboratoires abroad, or from public or private research centers. publics ou privés. Page 1 of 12 1 2 3 4 5 6 7 Structural Diversity in White-light Emitting Hybrid Lead Bromide 8 Perovskites 9 10 Lingling Mao1, Peijun Guo2, Mikaël Kepenekian3, Ido Hadar1, Claudine Katan3, Jacky Even4, Richard 11 D. Schaller1,2, Constantinos C. Stoumpos1* and Mercouri G. Kanatzidis1* 12 13 1Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States 14 15 2Center for Nanoscale Materials, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United 16 States 17 18 3Univ Rennes, ENSCR, INSA Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes) − UMR 6226, Rennes F- 19 35000, France 20 4 21 Univ Rennes, INSA Rennes, CNRS, Institut FOTON − UMR 6082, Rennes F-35000, France 22 23 ABSTRACT: Hybrid organic-inorganic halide perovskites are under intense investigations because of their astounding physical 24 properties and promises for optoelectronics. Lead bromide and chloride perovskites exhibit intrinsic whitelight emission believed 25 to arise from self-trap excitons (STEs). Here, we report a series of new structurally diverse hybrid lead bromide perovskites that 26 have broadband emission at room temperature. They feature Pb/Br structures which vary from 1D facesharing structures to 3D 27 corner- and edgesharing structures. Through single -crystal X-ray diffraction and low frequency Raman spectroscopy, we have 2+ 28 identified the local distortion level of the octahedral environments of Pb within the structures. The band gaps of these compound 29 range from 2.92 to 3.50 eV, following the trend of “corner-sharing< edgesharing< facesharing”. Density functional theory (DFT) 30 calculations suggest the electronic structure is highly dependent on the connectivity mode of the PbBr6 octahedra, where the edge and corner-sharing 1D structure of (2,6-dmpz) Pb Br exhibits more disperse bands and smaller band gap (2.49 eV) than the face 31 3 2 10 Manuscript sharing 1D structure of (hep)PbBr3 (3.10 eV). Using photoemission spectroscopy, we measured the energies of the valence band of 32 these compounds and found them to remain almost constant, while the energy of conduction bands varies. Temperature dependent 33 PL measurements reveal the 2D and 3D compounds have narrower PL emission at low temperature (~5K), whereas the 1D com- 34 pounds have both free exciton emission and STEs emission. The 1D compound (2,6-dmpz)3Pb2Br10 has the highest photolumines- 35 cence quantum yield (PLQY) of 12%, owing to its unique structure that allows efficient charge carrier relaxation and light emis- 36 sion. 37 38 39 40 Introduction 41 42 Accepted 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 Page 2 of 12 the dimensionality (0D to 3D) of the structure. For the three 1 dimensional (3D) structures, the general formula is ABX3, 2 where A is methylammonium (MA+), formamidinium (FA+) 3 or Cs+, B is Pb2+, Sn2+ or Ge2+, and X is halide (Cl-, Br- or I- 16 4 ). Lowering the dimensionality to two-dimensions (2D) with 5 corner-sharing octahedral layers and bulky organic cations 6 separating the perovskite layers, gives rise to increased struc tural diversity. The general perovskite formula then becomes 7 + + + A′2An-1BnX3n+1 (A′ = 1+ cation, A = MA , FA or Cs ), in the 8 17 Ruddlesden−Popper (RP) phases, A′An-1MnX3n+1, in the Di- 9 on-Jacobson phases (A′ = 2+ cation, A = MA+, FA+ or Cs+).18 10 Further reducing the dimensionality to onedimension (1D), 11 the formula is then dictated by the connectivity modes of the 4- 12 [BX6] octahedra, with the most common connectivity modes 13 being facesharing, followed by corner-sharing as well as rare 14 edgesharing connectivity. Notably, a single compound can have one connectivity mode or a combination of connectivity 15 19 16 modes, thus producing extremely rich and diverse structural types. Zero-dimensional (0D) compounds composed of iso- 17 4- lated [MX6] octahedra have also been reported, with repre 18 4+ 20 21-22 sentative examples being Cs2SnI6 (Sn ), Cs4PbBr6 and 19 possibly the mixed-metal double perovskites.23 20 21 Broadband whitelight emission at room temperature from 22 hybrid perovskite materials is an attractive optical property and has received tremendous attention, given the poorly un- 23 derstood and apparently unique photo-physics that gives rise 24 Figure 1. (a) Organic cations used in this work. mpz =1- to this phenomenon.24 It was discovered in various (110)- 25 methylpiperazine, epz =1-ethylpiperazine, 4amp = 4- oriented 2D lead bromide perovskites, such as (aminomethyl)piperidine, 2,6-dmpz = 2,6-dimethylpiperazine , hmp = 25 26 (C6H13N3)PbBr4, (N-MEDA)[PbBr4] (N-MEDA = N1- meth- homopiperazine , hex = hexamethyleneimine, hep = heptamethylene- 26 27 imine . (b) Optical microscopic images of the hybrid perovskite com- ylethane1,2-diammonium) and (EDBE)[PbBr4] (EDBE = 27 28 pounds synthesized using the cations listed above. 2,2′-(ethylenedioxy)bis(ethylammonium)). Subsequent stud- 29 ies have focused on the correlation between the lattice distor- 28-30 30 Hybrid organicinorganic perovskites are emerging semicon- tion in order to explain the origins of the broad emission. 31 ducting crystalline materials that are solution-processable, ManuscriptThe currently debated broadband emission model has been 32 low-cost and can be easily synthesized.1-3 The diverse nature connected to the highly deformed/deformable crystal lattice that induces electron-phonon coupling associated with excited 33 of the organic cationic templates lend these materials to be highly tunable, which, in conjunction with the variable dimen- states (i.e., polarons), generating the so-called self-trapped 34 exciton (STE) states.28 Interestingly, the broad-band emission 35 sionalities of these materials ranging from single crystals to nanocrystals and thin-films,4 have provided a solid foundation does not only exist in layered structures, but also in lower 36 of a wide range of optoelectronic devices such as photovolta dimensional structures, such as the recent report on 1D perov- 37 ics5-7,8-11 and light-emitting diodes (LEDs). 12-15 Hybrid per- skite that exhibits bluish whitelight emission and a higher 38 ovskites can be tuned “by design” for specific applications. photoluminescence quantum yield (PLQY) compared to the 39 2D perovskites.31 Because of this, the concept of dimensional The energy band gap is associated with choices of different 32-34 40 metal ions (Pb2+, Sn2+, Ge2+), halide anions (Cl-, Br- and I-) and reduction provides a new materials’ design principle to 41 Table 1. Summary of structural characteristics and band gaps of (2,6-dmpz)3Pb2Br10, (epz)PbBr4, (4amp)PbBr4, (hmp)PbBr4, 42 (mpz) Pb Br , (hep)PbBr and (hex)PbBrAccepted. 2 3 10 3 3 43 44 Cations Formula Dimensionality space group connectivity modes Eg (eV) 45 46 2,6-dmpz (C6H16N2)3Pb2Br10 1D P1 corner and edgesharing 3.16 47 48 epz (C6H16N2)PbBr4 (110)oriented 2D Pc cornersharing 3.12 49 4amp (C H N )PbBr (100)oriented 2D Pca2 cornersharing 2.92 50 6 16 2 4 1 51 mpz (C5H14N2)2Pb3Br10 threelayered 2D C2/c corner and edgesharing 2.97 52 53 hmp (C5H14N2)PbBr4 3D C2/m corner and edgesharing 3.04 54 hep (C H N)PbBr 1D Cc facesharing 3.50 55 7 16 3 56 hex (C6H14N)PbBr3 1D P21 facesharing 3.41 57 58 59 2 60 Page 3 of 12 access a broader variety of white light-emitting materials.35-39 1 In general, lower-dimensional structures possess more vibra 2 tional degrees of freedom and are more easily polarizable un- 3 der photo-excitation, thus leading to enhancements in the STE process and to the amplification of the broad-band emission.40- 4 41 5 6 Exploring the above concepts, we report here a variety of 7 new hybrid lead bromide perovskites, representative of each 8 kind, focusing on their whitelight emission properties. We 9 investigate the templating effect42 of asymmetric diammonium 10 organic cations based on the piperazinium and piperidinium 11 backbone as seen in Figure 1a in the lead bromide system, 12 since these types of cations are known to interact strongly with 18, 43 13 the anionic perovskite lattice. The resulting compounds 14 present a library that includes 1D facesharing structures, 1D 15 corner- and edgesharing structure, 2D (100)-oriented and (110)-oriented corner-sharing structures, to 3D corner- and 16 edgesharing structures as summarized in Table 1. We find 17 that all the compounds reported here have broad-band PL 18 emission at room temperature with different emission charac 19 teristics. We investigate the temperaturedependence of the PL 20 emission and find the width of the broad-band emission for 2D 21 and 3D structures becomes narrower when the temperature 22 decreases, presumably due to deactivation of some STE states.
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