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İbrahim Dursun

Cornell University

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Osman M. Bakr

King Abdullah University of Science and Technology

Omar F. Mohammed

King Abdullah University of Science and Technology

Makhsud I. Saidaminov

University of Victoria

Ayan A. Zhumekenov

King Abdullah University of Science and Technology

Tom Wu

Hong Kong Polytechnic University

Michele De Bastiani

King Abdullah University of Science and Technology

Bekir Türedi

King Abdullah University of Science and Technology

Md Azimul Haque

National Renewable Energy Laboratory

Jun Yin

Hong Kong Polytechnic University

Ahmed L. Abdelhady

Khalifa University of Science and Technology

Cooperative Institutions

King Abdullah University of Science and Technology

University of Toronto

University of Science and Technology

Kootenay Association for Science & Technology

Italian Institute of Technology

Physical Sciences (United States)

The University of Texas at Dallas

Korea University of Science and Technology

Xi'an Jiaotong University

Nanyang Technological University

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The Role of Surface Tension in the Crystallization of Metal Halide Perovskites

ACS Energy Letters (2017)

Ayan A. Zhumekenov V. M. Burlakov Makhsud I. Saidaminov Abdulilah Alofi Md Azimul Haque

The exciting intrinsic properties discovered in single crystals of metal halide perovskites still await their translation into optoelectronic devices. The poor understanding and control of the crystallization process of these materials are current bottlenecks retarding the shift toward single-crystal-based optoelectronics. Here we theoretically and experimentally elucidate the role of surface tension in the rapid synthesis of perovskite single crystals by inverse temperature crystallization. Understanding the nucleation and growth mechanisms enabled us to exploit surface tension to direct the growth of monocrystalline films of perovskites (AMX3, where A = CH3NH3 + or MA; M = Pb2+, Sn2+; X = Br–, I–) on the solution surface. We achieve up to 1 cm2-sized monocrystalline films with thickness on the order of the charge carrier diffusion length (∼5–10 μm). Our work paves the way to control the crystallization process of perovskites, including thin-film deposition, which is essential to advance the performance benchmarks of perovskite optoelectronics.

Crystal (programming language)

10.1021/acsenergylett.7b00468

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Citations (181)

Why are Hot Holes Easier to Extract than Hot Electrons from Methylammonium Lead Iodide Perovskite?

Advanced Energy Materials (2019)

İbrahim Dursun Partha Maity Jun Yin Bekir Türedi Ayan A. Zhumekenov

Abstract Charge‐carriers photoexcited above a semiconductor's bandgap rapidly thermalize to the band‐edge. The cooling of these difficult to collect “hot” carriers caps the available photon energy that solar cells–including efficient perovskite solar cells–may utilize. Here, the dynamics and efficiency of hot carrier extraction from MAPbI 3 (MA = methylammonium) perovskite by spiro‐OMeTAD (a hole‐transporting layer) and TiO 2 (an electron‐transporting layer) are investigated and explained using both ultrafast electronic spectroscopy and theoretical modeling. Time‐resolved spectroscopy reveals a quasi‐equilibrium distribution of hot carriers forming upon excess‐energy excitation of the perovskite–a distribution largely unaffected by the presence of TiO 2 . In contrast, the quasi‐equilibrium distribution of hot carriers is virtually nonexistent when spiro‐OMeTAD is present, which is indicative of efficient hot hole extraction at the interface of MAPbI 3 . Density functional theory calculations predict that deep energy‐levels of MAPbI 3 exhibit electronically delocalized character, with significant overlap with the localized valence band charge of the spiro‐OMeTAD molecules lying on the surface of MAPbI 3 . Consequently, hot holes are easily extracted from the deep energy‐levels of MAPbI 3 by spiro‐OMeTAD. These findings uncover the origins of efficient hot hole extraction in perovskites and offer a practical blueprint for optimizing solar cell interlayers to enable hot carrier utilization.

Thermalisation

Charge carrier

Perovskite solar cell

10.1002/aenm.201900084

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Citations (76)

Molecular behavior of zero-dimensional perovskites

Science Advances (2017)

Jun Yin Partha Maity Michele De Bastiani İbrahim Dursun Osman M. Bakr

Researchers provide new insights into the formation of small polarons in zero-dimensional perovskites.

Zero (linguistics)

Zero temperature

10.1126/sciadv.1701793

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Citations (212)

Efficient Photon Recycling and Radiation Trapping in Cesium Lead Halide Perovskite Waveguides

ACS Energy Letters (2018)

İbrahim Dursun Yangzi Zheng Tianle Guo Michele De Bastiani Bekir Türedi

Cesium lead halide perovskite materials have attracted considerable attention for potential applications in lasers, light-emitting diodes, and photodetectors. Here, we provide the experimental and theoretical evidence for photon recycling in CsPbBr3 perovskite microwires. Using two-photon excitation, we recorded photoluminescence (PL) lifetimes and emission spectra as a function of the lateral distance between PL excitation and collection positions along the microwire, with separations exceeding 100 μm. At longer separations, the PL spectrum develops a red-shifted emission peak accompanied by an appearance of well-resolved rise times in the PL kinetics. We developed quantitative modeling that accounts for bimolecular recombination and photon recycling within the microwire waveguide and is sufficient to account for the observed decay modifications. It relies on a high radiative efficiency in CsPbBr3 perovskite microwires and provides crucial information about the potential impact of photon recycling and waveguide trapping on optoelectronic properties of cesium lead halide perovskite materials.

Caesium

Waveguide

10.1021/acsenergylett.8b00758

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Citations (71)

High-quality bulk hybrid perovskite single crystals within minutes by inverse temperature crystallization

Nature Communications (2015)

Makhsud I. Saidaminov Ahmed L. Abdelhady Banavoth Murali Erkki Alarousu V. M. Burlakov

Abstract Single crystals of methylammonium lead trihalide perovskites (MAPbX 3 ; MA=CH 3 NH 3 + , X=Br − or I − ) have shown remarkably low trap density and charge transport properties; however, growth of such high-quality semiconductors is a time-consuming process. Here we present a rapid crystal growth process to obtain MAPbX 3 single crystals, an order of magnitude faster than previous reports. The process is based on our observation of the substantial decrease of MAPbX 3 solubility, in certain solvents, at elevated temperatures. The crystals can be both size- and shape-controlled by manipulating the different crystallization parameters. Despite the rapidity of the method, the grown crystals exhibit transport properties and trap densities comparable to the highest quality MAPbX 3 reported to date. The phenomenon of inverse or retrograde solubility and its correlated inverse temperature crystallization strategy present a major step forward for advancing the field on perovskite crystallization.

Trihalide

Crystal (programming language)

Protein crystallization

10.1038/ncomms8586

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Citations (1,696)

CsPb₂Br₅ Single Crystals: Synthesis and Characterization

ChemSusChem (2017)

İbrahim Dursun Michele De Bastiani Bekir Türedi Badriah Alamer Aleksander Shkurenko

Abstract CsPb 2 Br 5 is a ternary halogen‐plumbate material with close characteristics to the well‐reported halide perovskites. Owing to its unconventional two‐dimensional structure, CsPb 2 Br 5 is being looked at broadly for potential applications in optoelectronics. CsPb 2 Br 5 investigations are currently limited to nanostructures and powder forms of the material, which present unclear and conflicting optical properties. In this study, we present the synthesis and characterization of CsPb 2 Br 5 bulk single crystals, which enabled us to finally clarify the material's optical features. Our CsPb 2 Br 5 crystal has a two‐dimensional structure with Pb 2 Br 5 − layers spaced by Cs + cations, and exhibits approximately 3.1 eV indirect band gap with no emission in the visible spectrum.

Characterization

10.1002/cssc.201701131

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Citations (148)

Planar-integrated single-crystalline perovskite photodetectors

Nature Communications (2015)

Makhsud I. Saidaminov Valerio Adinolfi Riccardo Comin Ahmed L. Abdelhady Wei Peng

Abstract Hybrid perovskites are promising semiconductors for optoelectronic applications. However, they suffer from morphological disorder that limits their optoelectronic properties and, ultimately, device performance. Recently, perovskite single crystals have been shown to overcome this problem and exhibit impressive improvements: low trap density, low intrinsic carrier concentration, high mobility, and long diffusion length that outperform perovskite-based thin films. These characteristics make the material ideal for realizing photodetection that is simultaneously fast and sensitive; unfortunately, these macroscopic single crystals cannot be grown on a planar substrate, curtailing their potential for optoelectronic integration. Here we produce large-area planar-integrated films made up of large perovskite single crystals. These crystalline films exhibit mobility and diffusion length comparable with those of single crystals. Using this technique, we produced a high-performance light detector showing high gain (above 10 4 electrons per photon) and high gain-bandwidth product (above 10 8 Hz) relative to other perovskite-based optical sensors.

Photodetection

Electron Mobility

10.1038/ncomms9724

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Citations (677)

Pure Cs₄PbBr₆: Highly Luminescent Zero-Dimensional Perovskite Solids

ACS Energy Letters (2016)

Makhsud I. Saidaminov Jawaher Almutlaq Smritakshi P. Sarmah İbrahim Dursun Ayan A. Zhumekenov

So-called zero-dimensional perovskites, such as Cs4PbBr6, promise outstanding emissive properties. However, Cs4PbBr6 is mostly prepared by melting of precursors that usually leads to a coformation of undesired phases. Here, we report a simple low-temperature solution-processed synthesis of pure Cs4PbBr6 with remarkable emission properties. We found that pure Cs4PbBr6 in solid form exhibits a 45% photoluminescence quantum yield (PLQY), in contrast to its three-dimensional counterpart, CsPbBr3, which exhibits more than 2 orders of magnitude lower PLQY. Such a PLQY of Cs4PbBr6 is significantly higher than that of other solid forms of lower-dimensional metal halide perovskite derivatives and perovskite nanocrystals. We attribute this dramatic increase in PL to the high exciton binding energy, which we estimate to be ∼353 meV, likely induced by the unique Bergerhoff–Schmitz–Dumont-type crystal structure of Cs4PbBr6, in which metal-halide-comprised octahedra are spatially confined. Our findings bring this class of perovskite derivatives to the forefront of color-converting and light-emitting applications.

Quantum yield

Crystal (programming language)

10.1021/acsenergylett.6b00396

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Citations (529)

Formamidinium Lead Halide Perovskite Crystals with Unprecedented Long Carrier Dynamics and Diffusion Length

ACS Energy Letters (2016)

Ayan A. Zhumekenov Makhsud I. Saidaminov Md Azimul Haque Erkki Alarousu Smritakshi P. Sarmah

State-of-the-art perovskite solar cells with record efficiencies were achieved by replacing methylammonium (MA) with formamidinium (FA) in perovskite polycrystalline films. However, these films suffer from severe structural disorder and high density of traps; thus, the intrinsic properties of FA-based perovskites remain obscured. Here we report the detailed optical and electrical properties of FAPbX3 (where X = Br– and I–) single crystals. FAPbX3 crystals exhibited markedly enhanced transport compared not just to FAPbX3 polycrystalline films but also, surprisingly, to MAPbX3 single crystals. Particularly, FAPbBr3 crystals displayed a 5-fold longer carrier lifetime and 10-fold lower dark carrier concentration than those of MAPbBr3 single crystals. We report long carrier diffusion lengths—much longer than previously thought—of 6.6 μm for FAPbI3 and 19.0 μm for FAPbBr3 crystals, the latter being one of the longest reported values in perovskite materials. These findings are of great importance for future integrated applications of these perovskites.

Formamidinium

Carrier lifetime

10.1021/acsenergylett.6b00002

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Citations (823)