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...

http://pubs.acs.org/doi/pdf/10.1021/acsenergylett.6b00396

Pure Cs4PbBr6: Highly Luminescent Zero-Dimensional Perovskite Solids

Zero-dimensional (0D) all-inorganic/organic-inorganic metal halides, as emerging luminescent materials, have attracted unparalleled interest from versatile perspectives due to their unique crystallographic/electronic structures with isolated building units and fascinating optical characteristics. However, significant challenges still exist for 0D metal halides, including their chemical molecular design, photoluminescence (PL) mechanism, PL modification and applications. In this review, we summarize the 0D metal halides through the classification of all-inorganic and organic-inorganic hybrid metal halides, and further emphasize the unique role of B-site cations with different electronic configurations in the PL process. Furthermore, the PL mechanisms focusing on the self-trapped excitons (STEs) model and PL regulation engineering are examined to explore their extraordinary PL properties and further reveal new application prospects. This review aims to provide in-depth insight into the structure-luminescence-application relationship of 0D metal halides and pave the way for the realization of next-generation high-performance luminescent materials.

Recent progress of zero-dimensional luminescent metal halides

Although metal-halide perovskites have recently revolutionized research in optoelectronics through a unique combination of performance and synthetic simplicity, their low-dimensional counterparts can further expand the field with hitherto unknown and practically useful optical functionalities. In this context, we present the strong temperature dependence of the photoluminescence lifetime of low-dimensional, perovskite-like tin-halides and apply this property to thermal imaging. The photoluminescence lifetimes are governed by the heat-assisted de-trapping of self-trapped excitons, and their values can be varied over several orders of magnitude by adjusting the temperature (up to 20 ns °C−1). Typically, this sensitive range spans up to 100 °C, and it is both compound-specific and shown to be compositionally and structurally tunable from −100 to 110 °C going from [C(NH2)3]2SnBr4 to Cs4SnBr6 and (C4N2H14I)4SnI6. Finally, through the implementation of cost-effective hardware for fluorescence lifetime imaging, based on time-of-flight technology, these thermoluminophores have been used to record thermographic videos with high spatial and thermal resolution. Low-dimensional tin-halide perovskites exhibit strong temperature dependence of luminescence decay time that translates into high sensitivity over a wide range of temperatures and as such can be used in high-resolution remote thermography.

High-resolution remote thermometry and thermography using luminescent low-dimensional tin-halide perovskites.

The spatial localization of charge carriers to promote the formation of bound excitons and concomitantly enhance radiative recombination has long been a goal for luminescent semiconductors. Zero-dimensional materials structurally impose carrier localization and result in the formation of localized Frenkel excitons. Now the fully inorganic, perovskite-derived zero-dimensional SnII material Cs4 SnBr6 is presented that exhibits room-temperature broad-band photoluminescence centered at 540 nm with a quantum yield (QY) of 15±5 %. A series of analogous compositions following the general formula Cs4-x Ax Sn(Br1-y Iy )6 (A=Rb, K; x≤1, y≤1) can be prepared. The emission of these materials ranges from 500 nm to 620 nm with the possibility to compositionally tune the Stokes shift and the self-trapped exciton emission bands.

https://onlinelibrary.wiley.com/doi/pdf/10.1002/ange.201806452

Highly Emissive Self‐Trapped Excitons in Fully Inorganic Zero‐Dimensional Tin Halides

Low-dimensional perovskites offer a rare opportunity to investigate lattice dynamics and charge carrier behavior in bulk quantum-confined solids, in addition to them being the leading materials in optoelectronic applications. In particular, zero-dimensional (0D) inorganic perovskites of the Cs4PbX6 (X = Cl, Br, or I) kind have crystal structures with isolated lead halide octahedra [PbX6]4− surrounded by Cs+ cations, allowing the 0D crystals to exhibit the intrinsic properties of an individual octahedron. Using both experimental and theoretical approaches, we studied the electronic and optical properties of the prototypical 0D perovskite Cs4PbBr6. Our results underline that this 0D perovskite behaves akin to a molecule, demonstrating low electrical conductivity and mobility as well as large polaron binding energy. Density functional theory calculations and transient absorption measurements of Cs4PbBr6 perovskite films reveal the polaron band absorption and strong polaron localization features of the material. A short polaron lifetime of ~2 ps is observed in femtosecond transient absorption experiments, which can be attributed to the fast lattice relaxation of the octahedra and the weak interactions among them.

Molecular behavior of zero-dimensional perovskites

The structure of the title compound has been determined by the heavy-atom method from 822 diffractometer reflections and refined by full-matrix least-squares methods to R 0.030. Crystals are orthorhombic, space group P21ab, a= 7.35(1). b= 16.84(2), c= 5.32(1)A, Z= 4. The tin atoms are in distorted square-pyramidal sites. Each maleate ion is bonded through three oxygen atoms to three different tin atoms (Sn–0 2.176, 2.196. 2.440 A), and each tin atom is also bonded to a water molecule (Sn–O 2.312 A).

Crystal structure of tin(II) maleate monohydrate

Crystal structure of tin(ii) maleate monohydrate

Solid‐state properties of materials of the type cs4mx6 (where m = tin or lead and x = chloride or bromide)

Two new compounds Cs4SnBr6 and Cs4SnCl6 have been prepared and the CsBr–SnBr2 phase diagram is described. Phases of the type Cs4Sn1 –nPbnBr6 –xClx(where n= 0–1, x= 0–6) have been examined by X-ray diffraction, electrical conductivity, Mossbauer spectral, and optical reflectance techniques. The electrical conductivity and optical properties of the phases are explained in terms of the population of solid-state bands by the non-bonding electron pairs of the Group 4 atoms. The structures of all the phases are related to that of Cs4PbCl6 which has been redetermined.

Solid-state properties of materials of the type Cs4MX6(where M = Sn or Pb and X = Cl or Br)

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Crystal structure of tin(II) maleate monohydrate

Crystal structure of tin(ii) maleate monohydrate

Solid‐state properties of materials of the type cs4mx6 (where m = tin or lead and x = chloride or bromide)

Solid-state properties of materials of the type Cs4MX6(where M = Sn or Pb and X = Cl or Br)