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• W3191194165 abstract "Halide perovskites offer a unique blend of useful semiconductor properties with defect tolerance and facile solution processing, making them attractive for a broad range of optoelectronic applications. These materials can be prepared at relatively mild conditions and yet attain remarkable device performances. Their low formation energy and soft ionic nature make them easy to synthesize but also susceptible to changes and degradation. Such dynamic behavior enables halide perovskites to readily undergo reversible chemical and structural transformations on exposure to external stimuli such as light, temperature, electric field, and chemical environment. The optoelectronic performance, processability, and reconfigurability of halide perovskites, viewed together, make a potentially winning combination of traits for stimuli-responsive materials (SRMs) for switchable applications that are driving energy efficiency, autonomy, and digitization. This review introduces the reader to both fundamental and applied aspects of the emerging class of SRMs based on halide perovskites. We highlight the significant progress in the field, showcasing halide perovskite systems of switchable optical and electrical properties for practical applications, such as smart (photovoltaic) windows, memory devices, data storage, and sensors. The current challenges associated with the switching characteristics of stimuli-responsive halide perovskites and their future potential for various smart technologies are also discussed. Halide perovskites have recently shown potential as stimuli-responsive materials (SRMs) for a range of important technologies such as smart windows, memory devices, data storage, and sensors. Here, we overview these emerging SRMs that are based on halide perovskite systems of switchable optical and electrical properties as well as discuss their switching characteristics and practical applications. We summarize the reversible chemical and structural transformations of these materials and categorize them by their switching mechanisms. Furthermore, to guide the community’s search for new designs of stimuli-responsive halide perovskites, we outline several important criteria for effective switchable materials. Finally, we provide our perspective on the current challenges and future developments of these emerging materials. Halide perovskites have recently shown potential as stimuli-responsive materials (SRMs) for a range of important technologies such as smart windows, memory devices, data storage, and sensors. Here, we overview these emerging SRMs that are based on halide perovskite systems of switchable optical and electrical properties as well as discuss their switching characteristics and practical applications. We summarize the reversible chemical and structural transformations of these materials and categorize them by their switching mechanisms. Furthermore, to guide the community’s search for new designs of stimuli-responsive halide perovskites, we outline several important criteria for effective switchable materials. Finally, we provide our perspective on the current challenges and future developments of these emerging materials. Since the dawn of civilization, nature has been a source of inspiration for humanity’s technological feats: from irrigation and architecture to flight and gene editing. Materials engineering has also drawn on elements of nature to impart desirable functionalities on artificial materials that empower new technologies, a prime embodiment of which are stimuli-responsive materials (SRMs). Chameleon-inspired SRMs that can reversibly switch their colors or other physical properties with exposure to external stimuli—e.g., light, temperature, pressure, electricity, and chemical environment—are valuable for a range of technologies,1Urban M.W. Stimuli-Responsive Materials. The Royal Society of Chemistry, 2016Google Scholar such as smart windows and mirrors,2Wang Y. Runnerstrom E.L. Milliron D.J. Switchable materials for smart windows.Annu. Rev. Chem. Biomol. Eng. 2016; 7: 283-304Crossref PubMed Scopus (206) Google Scholar anti-glare glasses,3Lampert C.M. Chromogenic smart materials.Mater. Today. 2004; 7: 28-35Crossref Scopus (262) Google Scholar memory devices,4Heremans P. Gelinck G.H. Müller R. Baeg K.-J. Kim D.-Y. Noh Y.-Y. Polymer and organic nonvolatile memory devices †.Chem. Mater. 2011; 23: 341-358Crossref Scopus (435) Google Scholar data encryption,5Wang H. Ji X. Page Z.A. Sessler J.L. Fluorescent materials-based information storage.Mater. Chem. Front. 2020; 4: 1024-1039Crossref Google Scholar logic gates,6Erbas-Cakmak S. Kolemen S. Sedgwick A.C. Gunnlaugsson T. James T.D. Yoon J. Akkaya E.U. Molecular logic gates: the past, present and future.Chem. Soc. Rev. 2018; 47: 2228-2248Crossref PubMed Google Scholar and sensors.7Hu L. Zhang Q. Li X. Serpe M.J. Stimuli-responsive polymers for sensing and actuation.Mater. Horiz. 2019; 6: 1774-1793Crossref Google Scholar Prussian Blue (1704) is probably the oldest synthetic SRM; it undergoes discoloration on reduction and turns back to its colored state when oxidized.3Lampert C.M. Chromogenic smart materials.Mater. Today. 2004; 7: 28-35Crossref Scopus (262) Google Scholar The long-known pH indicators also display reversible color change in response to acidity level. More recent developments of SRMs include molecular switches based on spiropyrans, diarylethenes, azobenzenes, stilbenes, and helicenes with photo-, thermo-, and electro-switchable properties.8Irie M. Fukaminato T. Matsuda K. Kobatake S. Photochromism of diarylethene molecules and crystals: memories, switches, and actuators.Chem. Rev. 2014; 114: 12174-12277Crossref PubMed Scopus (1357) Google Scholar, 9Moulin E. Faour L. Carmona-Vargas C.C. Giuseppone N. From molecular machines to stimuli-responsive materials.Adv. Mater. 2020; 32e1906036Crossref PubMed Scopus (29) Google Scholar, 10Feringa B.L. Browne W.R. Molecular Switches. John Wiley & Sons, 2011Crossref Google Scholar Their structural diversity offers vast possibilities for tailoring desired functionalities. Furthermore, there is a broad array of crystalline materials—referred to as dynamic molecular crystals—which display switchable characteristics in solid state.11Sato O. Dynamic molecular crystals with switchable physical properties.Nat. Chem. 2016; 8: 644-656Crossref PubMed Scopus (366) Google Scholar Yet, the widespread applications of these molecular systems are often limited by their inferior charge transport characteristics, broad emission peaks, as well as aggregation-caused quenching effects in some specific cases. Hybrid organic-inorganic crystalline materials present a promising platform to overcome these limitations. Among them, halide perovskites offer a combination of optoelectronic characteristics that makes them uniquely suited for practical applications of SRMs. Specifically, these semiconductors demonstrate long charge-carrier diffusion lengths (more than 1 μm),12Shi D. Adinolfi V. Comin R. Yuan M. Alarousu E. Buin A. Chen Y. Hoogland S. Rothenberger A. Katsiev K. et al.Solar cells. Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals.Science. 2015; 347: 519-522Crossref PubMed Scopus (2826) Google Scholar,13Dong Q. Fang Y. Shao Y. Mulligan P. Qiu J. Cao L. Huang J. Solar cells. Electron-hole diffusion lengths > 175 μm in solution-grown CH3NH3PbI3 single crystals.Science. 2015; 347: 967-970Crossref PubMed Scopus (3114) Google Scholar tunable direct band gaps (1–3 eV),14Kovalenko M.V. Protesescu L. Bodnarchuk M.I. Properties and potential optoelectronic applications of lead halide perovskite nanocrystals.Science. 2017; 358: 745-750Crossref PubMed Scopus (870) Google Scholar large optical absorption coefficients (up to 105 cm−1),15De Wolf S. Holovsky J. Moon S.J. Löper P. Niesen B. Ledinsky M. Haug F.J. Yum J.H. Ballif C. Organometallic halide perovskites: sharp optical absorption edge and its relation to photovoltaic performance.J. Phys. Chem. Lett. 2014; 5: 1035-1039Crossref PubMed Scopus (1466) Google Scholar narrow photoluminescence (PL) emission peaks,16Protesescu L. Yakunin S. Bodnarchuk M.I. Krieg F. Caputo R. Hendon C.H. Yang R.X. Walsh A. Kovalenko M.V. Nanocrystals of cesium lead halide perovskites (CsPbX₃, X = Cl, Br, and I): novel optoelectronic materials showing bright emission with wide color gamut.Nano Lett. 2015; 15: 3692-3696Crossref PubMed Scopus (3931) Google Scholar and high PL quantum yields (up to near-unity).17Dutta A. Behera R.K. Pal P. Baitalik S. Pradhan N. Near-unity photoluminescence quantum efficiency for all CsPbX3 (X=Cl, Br, and I) perovskite nanocrystals: a generic synthesis approach.Angew. Chem. Int. Ed. Engl. 2019; 58: 5552-5556Crossref PubMed Scopus (49) Google Scholar Furthermore, the low formation energies18Moore D.T. Sai H. Tan K.W. Smilgies D.M. Zhang W. Snaith H.J. Wiesner U. Estroff L.A. Crystallization kinetics of organic–inorganic trihalide perovskites and the role of the lead anion in crystal growth.J. Am. Chem. Soc. 2015; 137: 2350-2358Crossref PubMed Scopus (227) Google Scholar, 19Nagabhushana G.P. Shivaramaiah R. Navrotsky A. Direct calorimetric verification of thermodynamic instability of lead halide hybrid perovskites.Proc. Natl. Acad. Sci. USA. 2016; 113: 7717-7721Crossref PubMed Scopus (223) Google Scholar, 20Brunetti B. Cavallo C. Ciccioli A. Gigli G. Latini A. On the thermal and thermodynamic (in)stability of methylammonium lead halide perovskites.Sci. Rep. 2016; 6: 31896Crossref PubMed Scopus (135) Google Scholar and soft crystal nature21Even J. Carignano M. Katan C. Molecular disorder and translation/rotation coupling in the plastic crystal phase of hybrid perovskites.Nanoscale. 2016; 8: 6222-6236Crossref PubMed Google Scholar,22Fabini D.H. Hogan T. Evans H.A. Stoumpos C.C. Kanatzidis M.G. Seshadri R. Dielectric and thermodynamic signatures of low-temperature glassy dynamics in the hybrid perovskites CH3NH3PbI3 and HC(NH2)2PbI3.J. Phys. Chem. Lett. 2016; 7: 376-381Crossref PubMed Scopus (68) Google Scholar of halide perovskites add additional degrees of dynamic structural “switchability.” Herein, we overview the stimuli-responsive halide perovskites, their switchable properties, and applications. We first outline some essential criteria for switchable systems based on these materials and categorize them by their switching mechanisms including their chemical and structural transformations. We then highlight the current applications of stimuli-responsive halide perovskites and provide an assessment of the challenges and future outlooks for their development. One of the major advantages of halide perovskites over traditional inorganic semiconductors is their facile and inexpensive synthesis. Halide perovskites can self-assemble from solution into high-quality crystalline phases at relatively low temperatures (below 150°C) and yet deliver high efficiencies in optoelectronic devices.23Manser J.S. Saidaminov M.I. Christians J.A. Bakr O.M. Kamat P.V. Making and breaking of lead halide perovskites.Acc. Chem. Res. 2016; 49: 330-338Crossref PubMed Scopus (427) Google Scholar The low energy barriers and Gibbs free energies for their crystallization make them easy to synthesize but, as a downside, prone to degradation pathways too.19Nagabhushana G.P. Shivaramaiah R. Navrotsky A. Direct calorimetric verification of thermodynamic instability of lead halide hybrid perovskites.Proc. Natl. Acad. Sci. USA. 2016; 113: 7717-7721Crossref PubMed Scopus (223) Google Scholar,20Brunetti B. Cavallo C. Ciccioli A. Gigli G. Latini A. On the thermal and thermodynamic (in)stability of methylammonium lead halide perovskites.Sci. Rep. 2016; 6: 31896Crossref PubMed Scopus (135) Google Scholar This intrinsic instability of halide perovskites is typically seen as an adverse effect that deteriorates their device performance and requires remediation. In contrast, this instability can be advantageous for designing switchable perovskite systems. To be of practical use, a switchable perovskite system should meet some essential conditions. First, the system should entail a perovskite phase that on being exposed to an external stimulus can reversibly transform into another stable (or metastable) state, not necessarily perovskite, which displays some physical properties distinct from the parent perovskite (Figures 1A–1C). In the absence of an external stimulus, the system should retain one of its states for sufficiently long periods. Second, the transformations between the states should occur readily at high switching rates, preferably on timescales on the order of seconds or minutes, if not shorter. Third, the system should demonstrate excellent durability, maintaining its performance over thousands of switching cycles without significant degradation. Below, we discuss in detail the chemical and structural transformations in both three-dimensional (3D) and two-dimensional (2D) halide perovskites in response to external stimuli such as chemical environment (including humidity), temperature, light, and electric field. We particularly focus on the examples from the perspective of the outlined criteria. Halide perovskites are highly sensitive to their chemical environment due to the intrinsic instability. Moisture is one of the major causes for their degradation. The archetypal MAPbI3 (where MA+ is methylammonium, or CH3NH3+) perovskite irreversibly decomposes into PbI2 when exposed to water. However, under controlled humidity conditions, the reaction proceeds reversibly with the formation of intermediate hydrates24Leguy A.M.A. Hu Y. Campoy-Quiles M. Alonso M.I. Weber O.J. Azarhoosh P. van Schilfgaarde M. Weller M.T. Bein T. Nelson J. et al.Reversible hydration of CH3NH3PbI3 in films, single crystals, and solar cells.Chem. Mater. 2015; 27: 3397-3407Crossref Scopus (770) Google Scholar,25Haque M.A. Syed A. Akhtar F.H. Shevate R. Singh S. Peinemann K.V. Baran D. Wu T. Giant humidity effect on hybrid halide perovskite microstripes: reversibility and sensing mechanism.ACS Appl. Mater. Interfaces. 2019; 11: 29821-29829Crossref PubMed Scopus (22) Google Scholar:MAPbI3 + H2O ⇄ MAPbI3·H2O(Equation 1) 4 MAPbI3 + 2 H2O ⇄ MA4PbI6·2H2O + 3 PbI2(Equation 2) MAPbI3 + 3 MAI + 2 H2O ⇄ MA4PbI6·2H2O(Equation 3) MAPbI3 thin films spontaneously transform into MA4PbI6·2H2O at temperatures below 30°C and relative humidity (RH) ≥40% and recover back by dehydration above 60°C (Figure 2A).26Halder A. Choudhury D. Ghosh S. Subbiah A.S. Sarkar S.K. Exploring thermochromic behavior of hydrated hybrid perovskites in solar cells.J. Phys. Chem. Lett. 2015; 6: 3180-3184Crossref Scopus (60) Google Scholar, 27Zhang Y. Tso C.Y. Iñigo J.S. Liu S. Miyazaki H. Chao C.Y.H. Yu K.M. Perovskite thermochromic smart window: advanced optical properties and low transition temperature.Appl. Energy. 2019; 254: 113690Crossref Scopus (24) Google Scholar, 28Huisman B.A.H. Palazon F. Bolink H.J. Zero-dimensional hybrid organic–inorganic lead halides and their post-synthesis reversible transformation into three-dimensional perovskites.Inorg. Chem. 2021; 60: 5212-5216Crossref PubMed Scopus (0) Google Scholar The switching times for hydration and dehydration reactions vary with RH and temperature, respectively, and are on timescales of few minutes.27Zhang Y. Tso C.Y. Iñigo J.S. Liu S. Miyazaki H. Chao C.Y.H. Yu K.M. Perovskite thermochromic smart window: advanced optical properties and low transition temperature.Appl. Energy. 2019; 254: 113690Crossref Scopus (24) Google Scholar,29Liu S. Du Y.W. Tso C.Y. Lee H.H. Cheng R. Feng S.-P. Yu K.M. Organic hybrid perovskite (MAPbI3−xClx) for thermochromic smart window with strong optical regulation ability, low transition temperature, and narrow hysteresis width.Adv. Funct. Mater. 2021; 31: 2010426Crossref Scopus (1) Google Scholar A similar dynamic equilibrium with completely reversible and instantaneous switching for nearly 40 cycles occurs between MAPbBr3 perovskite and its dihydrate, MA4PbBr6·2H2O.30Sharma S.K. Phadnis C. Das T.K. Kumar A. Kavaipatti B. Chowdhury A. Yella A. Reversible dimensionality tuning of hybrid perovskites with humidity: visualization and application to stable solar cells.Chem. Mater. 2019; 31: 3111-3117Crossref Scopus (11) Google Scholar Noteworthy, both hydrates and other non-perovskite phases discussed below are not only structurally different from their parent perovskites but also display distinct optical properties.24Leguy A.M.A. Hu Y. Campoy-Quiles M. Alonso M.I. Weber O.J. Azarhoosh P. van Schilfgaarde M. Weller M.T. Bein T. Nelson J. et al.Reversible hydration of CH3NH3PbI3 in films, single crystals, and solar cells.Chem. Mater. 2015; 27: 3397-3407Crossref Scopus (770) Google Scholar This, as will be demonstrated in the forthcoming sections, is essential for applications in smart photovoltaic windows. Some nitrogen-containing molecules also reversibly react with halide perovskites. For instance, perovskite thin films bleach on exposure to triethylamine (Et3N),31Kim S.-H. Kirakosyan A. Choi J. Kim J.H. Detection of volatile organic compounds (VOCs), aliphatic amines, using highly fluorescent organic-inorganic hybrid perovskite nanoparticles.Dyes Pigm. 2017; 147: 1-5Crossref Scopus (15) Google Scholar ammonia (NH3),32Zhao Y. Zhu K. Optical bleaching of perovskite (CH3NH3)PbI3 through room-temperature phase transformation induced by ammonia.Chem. Commun. (Camb). 2014; 50: 1605-1607Crossref PubMed Scopus (0) Google Scholar and pyridine (C6H5N)33Jain S.M. Qiu Z. Häggman L. Mirmohades M. Johansson M.B. Edvinsson T. Boschloo G. Frustrated Lewis pair-mediated recrystallization of CH3NH3PbI3 for improved optoelectronic quality and high voltage planar perovskite solar cells.Energy Environ. Sci. 2016; 9: 3770-3782Crossref Google Scholar vapors but immediately recover when the vapor is removed. Yet, such instability at ambient conditions is disadvantageous for on-demand switching, unless the perovskite phase is sealed in the atmosphere of a switching gas as demonstrated recently.34Wheeler L.M. Moore D.T. Ihly R. Stanton N.J. Miller E.M. Tenent R.C. Blackburn J.L. Neale N.R. Switchable photovoltaic windows enabled by reversible photothermal complex dissociation from methylammonium lead iodide.Nat. Commun. 2017; 8: 1722Crossref PubMed Scopus (48) Google Scholar Namely, MAPbI3 thin film can be sealed in the atmosphere of inert gas containing 2% methylamine (CH3NH2) gas.34Wheeler L.M. Moore D.T. Ihly R. Stanton N.J. Miller E.M. Tenent R.C. Blackburn J.L. Neale N.R. Switchable photovoltaic windows enabled by reversible photothermal complex dissociation from methylammonium lead iodide.Nat. Commun. 2017; 8: 1722Crossref PubMed Scopus (48) Google Scholar This system forms a non-perovskite MAPbI3·xCH3NH2 complex (solid, x ≤ 2) at room temperature and dissociates back into initial reactants by solar photothermal heating at >35°C. Importantly, the two phases can reversibly switch between one another for over 20 cycles with transition times of less than 3 min. Interestingly, N,N-dimethylformamide (DMF)—being a good solvent for MAPbI3—also forms a relatively stable MAPbI3·DMF complex, which dissociates back above 60°C.35Guo Y. Shoyama K. Sato W. Matsuo Y. Inoue K. Harano K. Liu C. Tanaka H. Nakamura E. Chemical pathways connecting lead(II) iodide and perovskite via polymeric plumbate(II) fiber.J. Am. Chem. Soc. 2015; 137: 15907-15914Crossref PubMed Scopus (147) Google Scholar,36Hao F. Stoumpos C.C. Liu Z. Chang R.P.H. Kanatzidis M.G. Controllable perovskite crystallization at a gas–solid interface for hole conductor-free solar cells with steady power conversion efficiency over 10%.J. Am. Chem. Soc. 2014; 136: 16411-16419Crossref PubMed Scopus (322) Google Scholar Meanwhile, non-polar solvent such as dichloromethane (CH2Cl2) can induce the reversible transformation of 2D (PEA)2SnBr4 (where PEA+ is phenethylammonium, or C6H5CH2CH2NH3+) perovskite into 0D-networked [(PEA)6Br2]SnBr6·2CH2Cl2 non-perovskite phase in the presence of excess PEABr (Figure 2B).37Xu L.-J. Lin H. Lee S. Zhou C. Worku M. Chaaban M. He Q. Plaviak A. Lin X. Chen B. et al.0D and 2D: the cases of phenylethylammonium tin bromide hybrids.Chem. Mater. 2020; 32: 4692-4698Crossref Scopus (11) Google Scholar Ion exchange is a widely used approach for post-synthetic modification of halide perovskites. Depending on the exchanged ion, these reactions may either or not preserve the perovskite structure. For instance, anion exchange reactions in MAPbX3 and CsPbX3 (where X = Cl−, Br−, I−) perovskite nanocrystals are typically complete yet fully reversible processes that occur on timescales of a few seconds without the destruction of perovskite structure (Figure 3A).38Nedelcu G. Protesescu L. Yakunin S. Bodnarchuk M.I. Grotevent M.J. Kovalenko M.V. Fast anion-exchange in highly luminescent nanocrystals of cesium lead halide perovskites (CsPbX3, X = Cl, Br, I).Nano Lett. 2015; 15: 5635-5640Crossref PubMed Scopus (1261) Google Scholar, 39Akkerman Q.A. D’Innocenzo V. Accornero S. Scarpellini A. Petrozza A. Prato M. Manna L. Tuning the optical properties of cesium lead halide perovskite nanocrystals by anion exchange reactions.J. Am. Chem. Soc. 2015; 137: 10276-10281Crossref PubMed Scopus (1184) Google Scholar, 40Jang D.M. Park K. Kim D.H. Park J. Shojaei F. Kang H.S. Ahn J.P. Lee J.W. Song J.K. Reversible halide exchange reaction of organometal trihalide perovskite colloidal nanocrystals for full-range band gap tuning.Nano Lett. 2015; 15: 5191-5199Crossref PubMed Scopus (301) Google Scholar, 41Yoon Y.J. Lee K.T. Lee T.K. Kim S.H. Shin Y.S. Walker B. Park S.Y. Heo J. Lee J. Kwak S.K. et al.Reversible, full-color luminescence by post-treatment of perovskite nanocrystals.Joule. 2018; 2: 2105-2116Abstract Full Text Full Text PDF Scopus (0) Google Scholar Some cation exchange reactions—such as between MAPbX3 and FAPbX3 (where FA+ is formamidinium, or CH(NH2)2+)—also preserve the perovskite structure.42Eperon G.E. Beck C.E. Snaith H.J. Cation exchange for thin film lead iodide perovskite interconversion.Mater. Horiz. 2016; 3: 63-71Crossref Google Scholar,43Zhou Y. Yang M. Pang S. Zhu K. Padture N.P. Exceptional morphology-preserving evolution of formamidinium lead triiodide perovskite thin films via organic-cation displacement.J. Am. Chem. Soc. 2016; 138: 5535-5538Crossref PubMed Scopus (137) Google Scholar Meanwhile, other reactions—such as the interconversion between MAPbI3 and NH4PbI3—are accompanied by structural changes in the connectivity of the octahedral network.44Huang W. Manser J.S. Sadhu S. Kamat P.V. Ptasinska S. Direct observation of reversible transformation of CH3NH3PbI3 and NH4PbI3 induced by polar gaseous molecules.J. Phys. Chem. Lett. 2016; 7: 5068-5073Crossref PubMed Scopus (38) Google Scholar However, we note that any system based on an ion-exchange reaction generally requires at least two chemical stimuli (one per each direction) to switch between the states, which makes them impracticable. As for chemical transformations without the use of external chemical stimuli, a switchable system based on CsPbBr3 perovskite quantum dots (QDs) embedded in a glass matrix has recently been proposed.45Huang X. Guo Q. Yang D. Xiao X. Liu X. Xia Z. Fan F. Qiu J. Dong G. Reversible 3D laser printing of perovskite quantum dots inside a transparent medium.Nat. Photonics. 2020; 14: 82-88Crossref Scopus (84) Google Scholar The precursor glass containing Cs, Pb, Br, and other elements was successively treated by high-power laser irradiation and thermal annealing to induce the crystallization of CsPbBr3 QDs at the laser focal point. The QDs decompose into CsBr and PbBr2 under low-power laser irradiation and recover back by thermal annealing for at least 10 cycles without significant degradation of properties. The glass matrix plays a crucial role in protecting the QDs from humidity to enable reliable switching even after several months of storing in polar solvents. Later, a laser-induced switching strategy was used for CsPbCl3-xBrx (where 0 < x < 3) perovskite system as well.46Huang X. Guo Q. Kang S. Ouyang T. Chen Q. Liu X. Xia Z. Yang Z. Zhang Q. Qiu J. Dong G. Three-dimensional laser-assisted patterning of blue-emissive metal halide perovskite nanocrystals inside a glass with switchable photoluminescence.ACS Nano. 2020; 14: 3150-3158Crossref PubMed Scopus (22) Google Scholar Although solid-state switching is usually more preferred for practical reasons, halide perovskites can still demonstrate switching behavior in a dissolved state. A thermochromic perovskite ink containing the mixture of MABr, PbBr2, MAI, and PbI2 dispersed in DMF/γ-butyrolactone shows a reversible color evolution from pale yellow to orange, then further to red and black, when gradually heated from 25°C to 120°C.47De Bastiani M. Saidaminov M.I. Dursun I. Sinatra L. Peng W. Buttner U. Mohammed O.F. Bakr O.M. Thermochromic perovskite inks for reversible smart window applications.Chem. Mater. 2017; 29: 3367-3370Crossref Scopus (54) Google Scholar This is accompanied by the precipitation of MAPbI2.7Br0.3, MAPbI2.4Br0.6, and MAPbI1.8Br1.2 perovskites, respectively. Importantly, the initial state can be restored when the ink is cooled down to 25°C, yet the colored states are stable at room temperature up to several hours. 2D Ruddlesden-Popper (RP) and Dion-Jacobson (DJ) perovskites offer a rich platform for post-synthetic chemical modifications with the preservation of their innate “perovskite” structure. Namely, the organic interlayers in their structure can intercalate small guest molecules, react with them, or undergo other chemical changes (e.g., polymerization) in both reversible and irreversible manners.48Smith I.C. Smith M.D. Jaffe A. Lin Y. Karunadasa H.I. Between the sheets: postsynthetic transformations in hybrid perovskites.Chem. Mater. 2017; 29: 1868-1884Crossref Scopus (57) Google Scholar For instance, 1-chloronaphthalene and 1,2-dichlorobenzene solvent molecules can reversibly intercalate into the structure of (C10H21NH3)2CdCl4 perovskite resulting in, respectively, (C10H21NH3)2CdCl4·C10H7Cl and (C10H21NH3)2CdCl4·C6H4Cl2 phases with the increased interlayer distances.49Dolzhenko Y.I. Inabe T. Maruyama Y. In situ x-ray observation on the intercalation of weak interaction molecules into perovskite-type layered crystals (C9H19NH3)2PbI4 and (C10H21NH3)2CdCl4.Bull. Chem. Soc. Jpn. 1986; 59: 563-567Crossref Google Scholar However, these compounds are unstable in the absence of solvent medium, likely due to the weak van der Waals interactions between the host and guest molecules. Meanwhile, more stable intercalation products can be achieved via covalent bonding. As an example, (BEA)2PbBr4 (where BEA+ is butyleneammonium, or CH2=CHC2H4NH3+) perovskite reversibly reacts with I2, forming a relatively stable (BEA-I2)2PbBr4, or (ICH2ICHC2H4NH3)2PbBr4, phase with a half-life of 72 h (Figure 3B).50Solis-Ibarra D. Karunadasa H.I. Reversible and irreversible chemisorption in nonporous-crystalline hybrids.Angew. Chem. Int. Ed. Engl. 2014; 53: 1039-1042Crossref PubMed Scopus (0) Google Scholar We speculate that sealing these perovskites in an iodine atmosphere could, in fact, help stabilize the intercalated states for longer periods, whereas the controlled on-demand release of iodine could be realized by heating. Formamidinium (FA+) forms both 3D and 2D perovskites, including the continuum of intermediate phases. This allows the design of switchable systems based on FAn+1PbnX3n+1 (where n = 1, 2, 3, …∞, X = Br−, I−) perovskites that can reversibly transform across different compositions spanning 2D FA2PbX4 (n = 1) to 3D α-FAPbX3 (n = ∞) perovskites and finally to 1D δ-FAPbX3:51Rosales B.A. Mundt L.E. Allen T.G. Moore D.T. Prince K.J. Wolden C.A. Rumbles G. Schelhas L.T. Wheeler L.M. Reversible multicolor chromism in layered formamidinium metal halide perovskites.Nat. Commun. 2020; 11: 5234Crossref PubMed Scopus (6) Google Scholar(n + 1) FAn+1PbnX3n+1 ⇄ n FAn+2Pbn+1X3n+4 + FAX(Equation 4) This equilibrium shifts toward higher-n phases by exposing the system to solvent vapors (including humidity) and reverses back by mild heating or blowing dry He. The switching is enabled by reversible shuttling of FAX between the perovskite domain and the adjacent FAX reservoir. Over 10 cycles of reversible switching with transitions on timescales of seconds to minutes can be achieved. FAPbI3 and CsPbI3 perovskites are thermodynamically stable only at high temperatures.52Masi S. Gualdrón-Reyes A.F. Mora-Seró I. Stabilization of black perovskite phase in FAPbI3 and CsPbI3.ACS Energy Lett. 2020; 5: 1974-1985Crossref Scopus (13) Google Scholar At ambient conditions, they spontaneously transform into δ-FAPbI3 and δ-CsPbI3 non-perovskite phases. These processes are facilitated in the presence of moisture. Yet, both materials can be kinetically stabilized at room temperature for longer periods by various strategies such as thermal annealing,53Zhumekenov A.A. Saidaminov M.I. Haque M.A. Alarousu E. Sarmah S.P. Murali B. Dursun I. Miao X.-H. Abdelhady A.L. Wu T. et al.Formamidinium lead halide perovskite crystals with unprecedented long carrier dynamics and diffusion length.ACS Energy Lett. 2016; 1: 32-37Crossref Scopus (434) Google Scholar strain engineering,54Steele J.A. Jin H. Dovgaliuk I. Berger R.F. Braeckevelt T. Yuan H. Martin C. Solano E. Lejaeghere K. Rogge S.M.J. et al.Thermal unequilibrium of strained black CsPbI3 thin films.Science. 2019; 365: 679-684Crossref PubMed Scopus (162) Google Scholar sealing in an inert atmosphere,55Straus D.B. Guo S. Cava R.J. Kinetically stable single crystals of perovskite-phase CsPbI3.J. Am. Chem. Soc. 2019; 141: 11435-11439Crossref PubMed Scopus (49) Google Scholar doping,56Alanazi A.Q. Kubicki D.J. Prochowicz D. Alharbi E.A. Bouduban M.E.F. Jahanbakhshi F. Mladenović M. Milić J.V. Giordano F. Ren D. et al.Atomic-level micros" @default.
• W3191194165 created "2021-08-16" @default.
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• W3191194165 date "2021-08-01" @default.
• W3191194165 modified "2023-10-15" @default.
• W3191194165 title "Stimuli-responsive switchable halide perovskites: Taking advantage of instability" @default.
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