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Structural Diversity in Multicomponent Nanocrystal Superlattices Comprising Lead Halide Perovskite Nanocubes.

ABSTRACT: Nanocrystal (NC) self-assembly is a versatile platform for materials engineering at the mesoscale. The NC shape anisotropy leads to structures not observed with spherical NCs. This work presents a broad structural diversity in multicomponent, long-range ordered superlattices (SLs) comprising highly luminescent cubic CsPbBr₃ NCs (and FAPbBr₃ NCs) coassembled with the spherical, truncated cuboid, and disk-shaped NC building blocks. CsPbBr₃ nanocubes combined with Fe₃O₄ or NaGdF₄ spheres and truncated cuboid PbS NCs form binary SLs of six structure types with high packing density; namely, AB₂, quasi-ternary ABO₃, and ABO₆ types as well as previously known NaCl, AlB₂, and CuAu types. In these structures, nanocubes preserve orientational coherence. Combining nanocubes with large and thick NaGdF₄ nanodisks results in the orthorhombic SL resembling CaC₂ structure with pairs of CsPbBr₃ NCs on one lattice site. Also, we implement two substrate-free methods of SL formation. Oil-in-oil templated assembly results in the formation of binary supraparticles. Self-assembly at the liquid-air interface from the drying solution cast over the glyceryl triacetate as subphase yields extended thin films of SLs. Collective electronic states arise at low temperatures from the dense, periodic packing of NCs, observed as sharp red-shifted bands at 6 K in the photoluminescence and absorption spectra and persisting up to 200 K.

SUBMITTER: Cherniukh I

PROVIDER: S-EPMC9134504 | biostudies-literature | 2022 May

REPOSITORIES: biostudies-literature

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Structural Diversity in Multicomponent Nanocrystal Superlattices Comprising Lead Halide Perovskite Nanocubes.

Cherniukh Ihor I Sekh Taras V TV Rainò Gabriele G Ashton Olivia J OJ Burian Max M Travesset Alex A Athanasiou Modestos M Manoli Andreas A John Rohit Abraham RA Svyrydenko Mariia M Morad Viktoriia V Shynkarenko Yevhen Y Montanarella Federico F Naumenko Denys D Amenitsch Heinz H Itskos Grigorios G Mahrt Rainer F RF Stöferle Thilo T Erni Rolf R Kovalenko Maksym V MV Bodnarchuk Maryna I MI

ACS nano 20220406 5

Nanocrystal (NC) self-assembly is a versatile platform for materials engineering at the mesoscale. The NC shape anisotropy leads to structures not observed with spherical NCs. This work presents a broad structural diversity in multicomponent, long-range ordered superlattices (SLs) comprising highly luminescent cubic CsPbBr3 NCs (and FAPbBr3 NCs) coassembled with the spherical, truncated cuboid, and disk-shaped NC building blocks. CsPbBr3 nanocubes combined with F ...[more]

PMID: 35385663

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Project description:ConspectusFor almost a decade now, lead halide perovskite nanocrystals have been the subject of a steadily growing number of publications, most of them regarding CsPbBr3 nanocubes. Many of these works report X-ray diffraction patterns where the first Bragg peak has an unusual shape, as if it was composed of two or more overlapping peaks. However, these peaks are too narrow to stem from a nanoparticle, and the perovskite crystal structure does not account for their formation. What is the origin of such an unusual profile, and why has it been overlooked so far? Our attempts to answer these questions led us to revisit an intriguing collective diffraction phenomenon, known for multilayer epitaxial thin films but not reported for colloidal nanocrystals before. By analogy, we call it the multilayer diffraction effect.Multilayer diffraction can be observed when a diffraction experiment is performed on nanocrystals packed with a periodic arrangement. Owing to the periodicity of the packing, the X-rays scattered by each particle interfere with those diffracted by its neighbors, creating fringes of constructive interference. Since the interfering radiation comes from nanoparticles, fringes are visible only where the particles themselves produce a signal in their diffraction pattern: for nanocrystals, this means at their Bragg peaks. Being a collective interference phenomenon, multilayer diffraction is strongly affected by the degree of order in the nanocrystal aggregate. For it to be observed, the majority of nanocrystals within the sample must abide to the stacking periodicity with minimal misplacements, a condition that is typically satisfied in self-assembled nanocrystal superlattices or stacks of colloidal nanoplatelets.A qualitative understanding of multilayer diffraction might explain why the first Bragg peak of CsPbBr3 nanocubes sometimes appears split, but leaves many other questions unanswered. For example, why is the split observed only at the first Bragg peak but not at the second? Why is it observed routinely in a variety of CsPbBr3 nanocrystals samples and not just in highly ordered superlattices? How does the morphology of particles (i.e., nanocrystals vs nanoplatelets) affect the appearance of multilayer diffraction effects? Finally, why is multilayer diffraction not observed in other popular nanocrystals such as Au and CdSe, despite the extensive investigations of their superlattices?Answering these questions requires a deeper understanding of multilayer diffraction. In what follows, we summarize our progress in rationalizing the origin of this phenomenon, at first through empirical observation and then by adapting the diffraction theory developed in the past for multilayer thin films, until we achieved a quantitative fitting of experimental diffraction patterns over extended angular ranges. By introducing the reader to the key advancements in our research, we provide answers to the questions above, we discuss what information can be extracted from patterns exhibiting collective interference effects, and we show how multilayer diffraction can provide insights into colloidal nanomaterials where other techniques struggle. Finally, with the help of literature patterns showing multilayer diffraction and simulations performed by us, we demonstrate that this collective diffraction effect is within reach for many appealing nanomaterials other than halide perovskites.

Dataset Information

Structural Diversity in Multicomponent Nanocrystal Superlattices Comprising Lead Halide Perovskite Nanocubes.

Publications

Structural Diversity in Multicomponent Nanocrystal Superlattices Comprising Lead Halide Perovskite Nanocubes.

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