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Nanocrystals of Cesium Lead Halide Perovskites (CsPbX3, X = Cl, Br, and I): Novel Optoelectronic Materials Showing Bright Emission with Wide Color Gamut
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† Institute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir Prelog Weg 1, CH-8093 Zürich, Switzerland
‡ Laboratory for Thin Films and Photovoltaics, Empa − Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, CH-8600 Dübendorf, Switzerland
§ Centre for Sustainable Chemical Technologies and Department of Chemistry, University of Bath, Bath BA2 7AY, United Kingdom
*E-mail: [email protected]
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Nano Letters

Cite this: Nano Lett. 2015, 15, 6, 3692–3696
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https://doi.org/10.1021/nl5048779
Published January 29, 2015

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Abstract

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Metal halides perovskites, such as hybrid organic–inorganic CH3NH3PbI3, are newcomer optoelectronic materials that have attracted enormous attention as solution-deposited absorbing layers in solar cells with power conversion efficiencies reaching 20%. Herein we demonstrate a new avenue for halide perovskites by designing highly luminescent perovskite-based colloidal quantum dot materials. We have synthesized monodisperse colloidal nanocubes (4–15 nm edge lengths) of fully inorganic cesium lead halide perovskites (CsPbX3, X = Cl, Br, and I or mixed halide systems Cl/Br and Br/I) using inexpensive commercial precursors. Through compositional modulations and quantum size-effects, the bandgap energies and emission spectra are readily tunable over the entire visible spectral region of 410–700 nm. The photoluminescence of CsPbX3 nanocrystals is characterized by narrow emission line-widths of 12–42 nm, wide color gamut covering up to 140% of the NTSC color standard, high quantum yields of up to 90%, and radiative lifetimes in the range of 1–29 ns. The compelling combination of enhanced optical properties and chemical robustness makes CsPbX3 nanocrystals appealing for optoelectronic applications, particularly for blue and green spectral regions (410–530 nm), where typical metal chalcogenide-based quantum dots suffer from photodegradation.

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This paper was published on the Web on February 2, 2015. The discussion of the preparation of Cs-oleate and synthesis of CsPbX3 NCs in the Supporting Information has been corrected, and the paper was reposted on April 14, 2015.

Colloidal semiconductor nanocrystals (NCs, typically 2–20 nm large), also known as nanocrystal quantum dots (QDs), are being studied intensively as future optoelectronic materials. (1-4) These QD materials feature a very favorable combination of quantum-size effects, enhancing their optical properties with respect to their bulk counterparts, versatile surface chemistry, and a “free” colloidal state, allowing their dispersion into a variety of solvents and matrices and eventual incorporation into various devices. To date, the best developed optoelectronic NCs in terms of size, shape, and composition are binary and multinary (ternary, quaternary) metal chalcogenide NCs. (1, 5-9) In contrast, the potential of semiconducting metal halides in the form of colloidal NCs remains rather unexplored. In this regard, recent reports on highly efficient photovoltaic devices with certified power conversion efficiencies approaching 20% using hybrid organic–inorganic lead halides MAPbX3 (MA = CH3NH3, X = Cl, Br, and I) as semiconducting absorber layers are highly encouraging. (10-14)
In this study, we turn readers’ attention to a closely related family of materials: all-inorganic cesium lead halide perovskites (CsPbX3, X = Cl, Br, I, and mixed Cl/Br and Br/I systems; isostructural to perovskite CaTiO3 and related oxides). These ternary compounds are far less soluble in common solvents (contrary to MAPbX3), which is a shortcoming for direct solution processing but a necessary attribute for obtaining these compounds in the form of colloidal NCs. Although the synthesis, crystallography, and photoconductivity of direct bandgap CsPbX3 have been reported more than 50 years ago, (15) they have never been explored in the form of colloidal nanomaterials.
Here we report a facile colloidal synthesis of monodisperse, 4–15 nm CsPbX3 NCs with cubic shape and cubic perovskite crystal structure. CsPbX3 NCs exhibit not only compositional bandgap engineering, but owing to the exciton Bohr diameter of up to 12 nm, also exhibit size-tunability of their bandgap energies through the entire visible spectral region of 410–700 nm. Photoluminescence (PL) of CsPbX3 NCs is characterized by narrow emission line widths of 12–42 nm, high quantum yields of 50–90%, and short radiative lifetimes of 1–29 ns.

Figure 1

Figure 1. Monodisperse CsPbX3 NCs and their structural characterization. (a) Schematic of the cubic perovskite lattice; (b,c) typical transmission electron microscopy (TEM) images of CsPbBr3 NCs; (d) X-ray diffraction patterns for typical ternary and mixed-halide NCs.

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Synthesis of Monodisperse CsPbX3 NCs

Our solution-phase synthesis of monodisperse CsPbX3 NCs (Figure 1) takes advantage of the ionic nature of the chemical bonding in these compounds. Controlled arrested precipitation of Cs+, Pb2+, and X– ions into CsPbX3 NCs is obtained by reacting Cs-oleate with a Pb(II)-halide in a high boiling solvent (octadecene) at 140–200 °C (for details, see the Supporting Information). A 1:1 mixture of oleylamine and oleic acid are added into octadecene to solubilize PbX2 and to colloidally stabilize the NCs. As one would expect for an ionic metathesis reaction, the nucleation and growth kinetics are very fast. In situ PL measurements with a CCD-array detector (Supporting Information Figure S1) indicate that the majority of growth occurs within the first 1–3 s (faster for heavier halides). Consequently, the size of CsPbX3 NCs can be most conveniently tuned in the range of 4–15 nm by the reaction temperature (140–200 °C) rather than by the growth time. Mixed-halide perovskites, that is, CsPb(Cl/Br)3 and CsPb(Br/I)3, can be readily produced by combining appropriate ratios of PbX2 salts. Note that Cl/I perovskites cannot be obtained due to the large difference in ionic radii, which is in good agreement with the phase diagram for bulk materials. (16) Elemental analyses by energy dispersive X-ray (EDX) spectroscopy and by Ratherford backscattering spectrometry (RBS) confirmed the 1:1:3 atomic ratio for all samples of CsPbX3 NCs, including mixed-halide systems.
CsPbX3 are known to crystallize in orthorhombic, tetragonal, and cubic polymorphs of the perovskite lattice with the cubic phase being the high-temperature state for all compounds. (16-18) Interestingly, we find that all CsPbX3 NCs crystallize in the cubic phase (Figure 1d), which can be attributed to the combined effect of the high synthesis temperature and contributions from the surface energy. For CsPbI3 NCs, this is very much a metastable state, because bulk material converts into cubic polymorph only above 315 °C. At room temperature, an exclusively PL-inactive orthorhombic phase has been reported for bulk CsPbI3 (a yellow phase). (16-19) Our first-principles total energy calculations (density functional theory, Figure S2, Table S1 in Supporting Information) confirm the bulk cubic CsPbI3 phase to have 17 kJ/mol higher internal energy than the orthorhombic polymorph (7 kJ/mol difference for CsPbBr3). Weak emission centered at ∼710 nm has been observed from melt-spun bulk CsPbI3, shortly before recrystallization into the yellow phase. (18) Similarly, our solution synthesis of CsPbI3 at 305 °C yields cubic-phase 100–200 nm NCs with weak, short-lived emission at 714 nm (1.74 eV), highlighting the importance of size reduction for stabilizing the cubic phase and indicating that all CsPbI3 NCs in Figure 2b (5–15 nm in size) exhibit quantum-size effects (i.e., higher band gap energies due to quantum confinement, as discussed below). Cubic 4–15 nm CsPbI3 NCs recrystallize into the yellow phase only upon extended storage (months), whereas all other compositions of CsPbX3 NCs appear fully stable in a cubic phase.

Figure 2

Figure 2. Colloidal perovskite CsPbX3 NCs (X = Cl, Br, I) exhibit size- and composition-tunable bandgap energies covering the entire visible spectral region with narrow and bright emission: (a) colloidal solutions in toluene under UV lamp (λ = 365 nm); (b) representative PL spectra (λexc = 400 nm for all but 350 nm for CsPbCl3 samples); (c) typical optical absorption and PL spectra; (d) time-resolved PL decays for all samples shown in (c) except CsPbCl3.

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Optical Properties of Colloidal CsPbX3 NCs

Optical absorption and emission spectra of colloidal CsPbX3 NCs (Figure 2b,c) can be tuned over the entire visible spectral region by adjusting their composition (ratio of halides in mixed halide NCs) and particle size (quantum-size effects). Remarkably bright PL of all NCs is characterized by high QY of 50–90% and narrow emission line widths of 12–42 nm. The combination of these two characteristics had been previously achieved only for core–shell chalcogenide-based QDs such as CdSe/CdS due to the narrow size distributions of the luminescent CdSe cores, combined with an epitaxially grown, electronically passivating CdS shell. (5, 20) Time-resolved photoluminescence decays of CsPbX3 NCs (Figure 2d) indicate radiative lifetimes in the range of 1–29 ns with faster emission for wider-gap NCs. For comparison, decay times of several 100 ns are typically observed in MAPbI3 (PL peak at 765 nm, fwhm = 50 nm) (21) and 40–400 ns for MAPbBr3–xClx (x = 0.6–2). (22)
Very bright emission of CsPbX3 NCs indicates that contrary to uncoated chalcogenide NCs surface dangling bonds do not impart severe midgap trap states. This observation is also in good agreement with the high photophysical quality of hybrid organic–inorganic perovskites (MAPbX3), despite their low-temperature solution-processing, which is generally considered to cause a high density of structural defects and trap states. In particular, thin-films of MAPbX3 exhibit relatively high PL QYs of 20–40% at room temperature (23, 24) and afford inexpensive photovoltaic devices approaching 20% in power conversion efficiency (10-12) and also electrically driven light-emitting devices. (25)
Ternary CsPbX3 NCs compare favorably to common multinary chalcogenide NCs: both ternary (CuInS2, CuInSe2, AgInS2, and AgInSe2) and quaternary (CuZnSnS2 and similar) compounds. CsPbX3 materials are highly ionic and thus are rather stoichiometric and ordered due to the distinct size and charge of the Cs and Pb ions. This is different from multinary chalcogenide materials that exhibit significant disorder and inhomogeneity in the distribution of cations and anions owing to little difference between the different cationic and anionic sites (all are essentially tetrahedral). In addition, considerable stoichiometric deviations lead to a large density of donor–acceptor states due to various point defects (vacancies, interstitials, etc.) within the band gap, both shallow and deep. These effects eventually lead to absent or weak and broad emission spectra and long multiexponent lifetimes. (7, 26-29)

Figure 3

Figure 3. (a) Quantum-size effects in the absorption and emission spectra of 5–12 nm CsPbBr3 NCs. (b) Experimental versus theoretical (effective mass approximation, EMA) size dependence of the band gap energy.

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For a colloidal semiconductor NC to exhibit quantum-dot-like properties (shown in Figures 2b and 3), the NC diameter must be comparable or smaller than that of the natural delocalization lengths of an exciton in a bulk semiconductor (i.e., the exciton Bohr diameter, a0). The electronic structure of CsPbX3 (X = Cl, Br, and I), including scalar relativistic and spin–orbit interactions, was calculated using VASP code (30) and confirms that the upper valence band is formed predominately by the halide p-orbitals and the lower conduction band is formed by the overlap of the Pb p-orbitals (Figures S3 and S4 and Tables S2 and S3 in Supporting Information). Effective masses of the electrons and holes were estimated from the band dispersion, while the high-frequency dielectric constants were calculated by using density functional perturbation theory. (31) Within the effective mass approximation (EMA), (32) we have estimated the effective Bohr diameters of Wannier–Mott excitons and the binding energies for CsPbCl3 (5 nm, 75 meV), CsPbBr3 (7 nm, 40 meV), and CsPbI3 (12 nm, 20 meV). Similarly, in closely related hybrid perovskite MAPbI3 small exciton binding energies of ≤25 meV have been suggested computationally (33-35) and found experimentally. (36) For comparison, the typical exciton binding energies in organic semiconductors are above 100 meV. The confinement energy (ΔE = ℏ2π2/2m*r2, where r is the particle radius and m* is the reduced mass of the exciton) provides an estimate for the blue shift of the emission peak and absorption edge and is in good agreement with the experimental observations (Figure 3b).

Figure 4

Figure 4. (a) Emission from CsPbX3 NCs (black data points) plotted on CEI chromaticity coordinates and compared to most common color standards (LCD TV, dashed white triangle, and NTSC TV, solid white triangle). Radiant Imaging Color Calculator software from Radiant Zemax (http://www.radiantzemax.com) was used to map the colors. (b) Photograph (λexc = 365 nm) of highly luminescent CsPbX3 NCs-PMMA polymer monoliths obtained with Irgacure 819 as photoinitiator for polymerization.

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Recently, highly luminescent semiconductor NCs based on Cd-chalcogenides have inspired innovative optoelectronic applications such as color-conversion LEDs, color-enhancers in backlight applications (e.g., Sony’s 2013 Triluminos LCD displays), and solid-state lighting. (4, 37, 38) Compared to conventional rare-earth phosphors or organic polymers and dyes, NCs often show superior quantum efficiency and narrower PL spectra with fine-size tuning of the emission peaks and hence can produce saturated colors. A CIE chromaticity diagram (introduced by the Commision Internationale de l’Eclairage) (39) allows the comparison of the quality of colors by mapping colors visible to the human eye in terms of hue and saturation. For instance, well-optimized core–shell CdSe-based NCs cover ≥100% of the NTSC TV color standard (introduced in 1951 by the National Television System Committee). (39) Figure 4a shows that CsPbX3 NCs allow a wide gamut of pure colors as well. Namely, a selected triangle of red, green, and blue emitting CsPbX3 NCs encompasses 140% of the NTSC standard, extending mainly into red and green regions.
Light-emission applications, discussed above, and also luminescent solar concentrators (40, 41) require solution-processability and miscibility of NC-emitters with organic and inorganic matrix materials. To demonstrate such robustness for CsPbX3 NCs, we embedded them into poly(methylmetacrylate) (PMMA), yielding composites of excellent optical clarity and with bright emission (Figure 4b). To accomplish this, CsPbX3 NCs were first dispersed in a liquid monomer (methylmetacrylate, MMA) as a solvent. Besides using known heat-induced polymerization with radical initiators, (41) we also performed polymerization already at room-temperature by adding a photoinitiator Irgacure 819 (bis(2,4,6-trimethylbenzoyl)-phenylphosphineoxide), (42) followed by 1h of UV-curing. We find that the presence of CsPbX3 NCs increases the rate of photopolymerization, compared to a control experiment with pure MMA. This can be explained by the fact that the luminescence from CsPbX3 NCs may be reabsorbed by the photoinitiator that has a strong absorption band in the visible spectral region, increasing the rate of polymerization.

Conclusions

In summary, we have presented highly luminescent colloidal CsPbX3 NCs (X = Cl, Br, I, and mixed Cl/Br and Br/I systems) with bright (QY = 50–90%), stable, spectrally narrow, and broadly tunable photoluminescence. Particularly appealing are highly stable blue and green emitting CsPbX3 NCs (410–530 nm), because the corresponding metal-chalcogenide QDs show reduced chemical and photostability at these wavelengths. In our ongoing experiments, we find that this simple synthesis methodology is also applicable to other metal halides with related crystal structures (e.g., CsGeI3, Cs3Bi2I9, and Cs2SnI6, to be published elsewhere). Future studies with these novel QD-materials will concentrate on optoelectronic applications such as lasing, light-emitting diodes, photovoltaics, and photon detection.

Supporting Information

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Synthesis details, calculations, and additional figures. This material is available free of charge via the Internet at http://pubs.acs.org.

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Author Information

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  • Corresponding Author
    • Maksym V. Kovalenko - Institute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir Prelog Weg 1, CH-8093 Zürich, Switzerland;  Laboratory for Thin Films and Photovoltaics, Empa − Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, CH-8600 Dübendorf, Switzerland;  Email: [email protected]
  • Authors
    • Loredana Protesescu - Institute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir Prelog Weg 1, CH-8093 Zürich, Switzerland;  Laboratory for Thin Films and Photovoltaics, Empa − Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, CH-8600 Dübendorf, Switzerland
    • Sergii Yakunin - Institute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir Prelog Weg 1, CH-8093 Zürich, Switzerland;  Laboratory for Thin Films and Photovoltaics, Empa − Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, CH-8600 Dübendorf, Switzerland
    • Maryna I. Bodnarchuk - Institute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir Prelog Weg 1, CH-8093 Zürich, Switzerland;  Laboratory for Thin Films and Photovoltaics, Empa − Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, CH-8600 Dübendorf, Switzerland
    • Franziska Krieg - Institute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir Prelog Weg 1, CH-8093 Zürich, Switzerland;  Laboratory for Thin Films and Photovoltaics, Empa − Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, CH-8600 Dübendorf, Switzerland
    • Riccarda Caputo - Institute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir Prelog Weg 1, CH-8093 Zürich, Switzerland
    • Christopher H. Hendon - Centre for Sustainable Chemical Technologies and Department of Chemistry, University of Bath, Bath BA2 7AY, United Kingdom
    • Ruo Xi Yang - Centre for Sustainable Chemical Technologies and Department of Chemistry, University of Bath, Bath BA2 7AY, United Kingdom
    • Aron Walsh - Centre for Sustainable Chemical Technologies and Department of Chemistry, University of Bath, Bath BA2 7AY, United Kingdom
  • Author Contributions

    The manuscript was prepared through the contribution of all coauthors. All authors have given approval to the final version of the manuscript.

  • Notes
    The authors declare no competing financial interest.

Acknowledgment

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This work was financially supported by the European Research Council (ERC) via Starting Grant (306733). The work at Bath was supported by the ERC Starting Grant (277757) and by the EPSRC (Grants EP/M009580/1 and EP/K016288/1). Calculations at Bath were performed on ARCHER via the U.K.’s HPC Materials Chemistry Consortium (Grant EP/L000202). Calculations at ETH Zürich were performed on the central HPC cluster BRUTUS. We thank Nadia Schwitz for a help with photography, Professor Dr. H. Grützmacher and Dr. G. Müller for a sample of Irgacure 819 photoinitiator, Dr. F. Krumeich for EDX measurements, Dr. M. Döbeli for RBS measurements (ETH Laboratory of Ion Beam Physics), and Dr. N. Stadie for reading the manuscript. We gratefully acknowledge the support of the Electron Microscopy Center at Empa and the Scientific Center for Optical and Electron Microscopy (ScopeM) at ETH Zürich.

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    Organometal Perovskite Light Absorbers Toward a 20% Efficiency Low-Cost Solid-State Mesoscopic Solar Cell
    Park, Nam-Gyu
    Journal of Physical Chemistry Letters (2013), 4 (15), 2423-2429CODEN: JPCLCD; ISSN:1948-7185. (American Chemical Society)
    A review of recent progress in perovskite-sensitized solid-state mesoscopic solar cells. Recently, perovskite CH3NH3PbI3 sensitizer has attracted great attention due to its superb light-harvesting characteristics. Organometallic or org. materials were mostly used as sensitizers for solid-state dye-sensitized solar cells at early stages. Inorg. nanocrystals have lately received attention as light harvesters due to their high light-absorbing properties. Metal chalcogenides have been investigated with solid-state dye-sensitized solar cells; however, the best power conversion efficiency was reported to be around 6%. CH3NH3PbX3 (X = Cl, Br, or I) perovskite sensitizer made a breakthrough in solid-state mescoscopic solar cells, where the first record efficiency of ∼10% was reported in 2012 using submicrometer-thick TiO2 film sensitized with CH3NH3PbI3. A rapid increase in efficiency approaching 14% followed shortly. On the basis of the recent achievements, a power conversion efficiency as high as 20% is expected based on optimized perovskite-based solid-state solar cells.
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    Zhou, H.; Chen, Q.; Li, G.; Luo, S.; Song, T.-b.; Duan, H.-S.; Hong, Z.; You, J.; Liu, Y.; Yang, Y. Science 2014, 345, 542– 546
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    Interface engineering of highly efficient perovskite solar cells
    Zhou, Huanping; Chen, Qi; Li, Gang; Luo, Song; Song, Tze-bing; Duan, Hsin-Sheng; Hong, Ziruo; You, Jingbi; Liu, Yongsheng; Yang, Yang
    Science (Washington, DC, United States) (2014), 345 (6196), 542-546CODEN: SCIEAS; ISSN:0036-8075. (American Association for the Advancement of Science)
    Advancing perovskite solar cell technologies toward their theor. power conversion efficiency (PCE) requires delicate control over the carrier dynamics throughout the entire device. By controlling the formation of the perovskite layer and careful choices of other materials, the authors suppressed carrier recombination in the absorber, facilitated carrier injection into the carrier transport layers, and maintained good carrier extn. at the electrodes. When measured via reverse bias scan, cell PCE is typically boosted to 16.6% on av., with the highest efficiency of ~19.3% in a planar geometry without antireflective coating. The fabrication of the perovskite solar cells was conducted in air and from soln. at low temps., which should simplify manufg. of large-area perovskite devices that are inexpensive and perform at high levels.
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    High-temperature structural evolution of caesium and rubidium triiodoplumbates
    Trots, D. M.; Myagkota, S. V.
    Journal of Physics and Chemistry of Solids (2008), 69 (10), 2520-2526CODEN: JPCSAW; ISSN:0022-3697. (Elsevier Ltd.)
    CsPbI3 and RbPbI3 were investigated by in situ powder diffraction within temp. ranges of 298-687 K and 298-714 K, resp. Both compds. crystallize in orthorhombic Pnma symmetry and expand isotropically upon a heating, revealing almost the same relative change of the lattice parameters. A pronounced difference in the structural evolution close to 600 K was obsd., namely, CsPbI3 undergoes 1st-order reversible phase transformation Pnma 563 K↔ Pnma + Pm‾3m 602 ↔ K Pm‾3m, whereas no transitions (except of the sample's melting) in RbPbI3 were detected. An attempt to clarify the relation between the existence/absence of a phase transition and bulging out of the I environment around alk. ions was undertaken.
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    Semiconducting Tin and Lead Iodide Perovskites with Organic Cations: Phase Transitions, High Mobilities, and Near-Infrared Photoluminescent Properties
    Stoumpos, Constantinos C.; Malliakas, Christos D.; Kanatzidis, Mercouri G.
    Inorganic Chemistry (2013), 52 (15), 9019-9038CODEN: INOCAJ; ISSN:0020-1669. (American Chemical Society)
    A broad org.-inorg. series of hybrid metal iodide perovskites AMI3, where A is the methylammonium (MeNH3+) or formamidinium (HC(NH2)2+) cation and M is Sn (1 and 2) or Pb (3 and 4) are reported. The compds. were prepd. through a variety of synthetic approaches, and the nature of the resulting materials is discussed in terms of their thermal stability and optical and electronic properties. The chem. and phys. properties of these materials strongly depend on the prepn. method. Single crystal x-ray diffraction anal. of 1-4 classifies the compds. in the perovskite structural family. Structural phase transitions were obsd. and studied by temp.-dependent single crystal x-ray diffraction in the 100-400 K range. The charge transport properties of the materials are discussed in conjunction with diffuse reflectance studies in the mid-IR region that display characteristic absorption features. Temp.-dependent studies show a strong dependence of the resistivity as a function of the crystal structure. Optical absorption measurements indicate that 1-4 behave as direct-gap semiconductors with energy band gaps distributed at 1.25-1.75 eV. The compds. exhibit an intense near-IR luminescence (PL) emission in the 700-1000 nm range (1.1-1.7 eV) at room temp. Solid solns. between the Sn and Pb compds. are readily accessible throughout the compn. range. The optical properties such as energy band gap, emission intensity, and wavelength can be readily controlled for the isostructural series of solid solns. MeNH3Sn1-xPbxI3 (5). The charge transport type in these materials was characterized by Seebeck coeff. and Hall-effect measurements. The compds. behave as p- or n-type semiconductors depending on the prepn. method. The samples with the lowest carrier concn. are prepd. from soln. and are n-type; p-type samples can be obtained through solid state reactions exposed in air in a controllable manner. In the case of Sn compds., there is a facile tendency toward oxidn. which causes the materials to be doped with Sn4+ and thus behave as p-type semiconductors displaying metal-like cond. The compds. appear to possess very high estd. electron and hole mobilities that exceed 2000 cm2/(V s) and 300 cm2/(V s), resp., as shown in the case of MeNH3SnI3 (1). The authors also compare the properties of the title hybrid materials with those of the all-inorg. CsSnI3 and CsPbI3 prepd. using identical synthetic methods.
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    Babin, V.; Fabeni, P.; Nikl, M.; Nitsch, K.; Pazzi, G. P.; Zazubovich, S. Phys. Status Solidi B 2001, 226, 419– 428
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    Christodoulou, S.; Vaccaro, G.; Pinchetti, V.; De Donato, F.; Grim, J. Q.; Casu, A.; Genovese, A.; Vicidomini, G.; Diaspro, A.; Brovelli, S.; Manna, L.; Moreels, I. J. Mater. Chem. C 2014, 2, 3439– 3447
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    Synthesis of highly luminescent wurtzite CdSe/CdS giant-shell nanocrystals using a fast continuous injection route
    Christodoulou, S.; Vaccaro, G.; Pinchetti, V.; De Donato, F.; Grim, J. Q.; Casu, A.; Genovese, A.; Vicidomini, G.; Diaspro, A.; Brovelli, S.; Manna, L.; Moreels, I.
    Journal of Materials Chemistry C: Materials for Optical and Electronic Devices (2014), 2 (17), 3439-3447CODEN: JMCCCX; ISSN:2050-7534. (Royal Society of Chemistry)
    We synthesized CdSe/CdS giant-shell nanocrystals, with a CdSe core diam. between 2.8 nm and 5.5 nm, and a CdS shell thickness of up to 7-8 nm (equiv. to about 20 monolayers of CdS). Both the core and shell have a wurtzite crystal structure, yielding epitaxial growth of the shell and nearly defect-free crystals. As a result, the photoluminescence (PL) quantum efficiency (QE) is as high as 90%. Quant. PL measurements at various excitation wavelengths allow us to sep. the nonradiative decay into contributions from interface and surface trapping, giving us pathways for future optimization of the structure. In addn., the NCs do not blink, and the giant shell and concurring strong electron delocalization efficiently suppress Auger recombination, yielding a biexciton lifetime of about 15 ns. The corresponding biexciton PL QE equals 11% in 5.5/18.1 nm CdSe/CdS. Variable-temp. time-resolved PL and PL under magnetic fields further reveal that the emission at cryogenic temp. originates from a neg. trion-state, in agreement with other CdSe/CdS giant-shell systems reported in the literature.
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    Wehrenfennig, C.; Liu, M.; Snaith, H. J.; Johnston, M. B.; Herz, L. M. J. Phys. Chem. Lett. 2014, 5, 1300– 1306
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    Homogeneous Emission Line Broadening in the Organo Lead Halide Perovskite CH3NH3PbI3-xClx
    Wehrenfennig, Christian; Liu, Mingzhen; Snaith, Henry J.; Johnston, Michael B.; Herz, Laura M.
    Journal of Physical Chemistry Letters (2014), 5 (8), 1300-1306CODEN: JPCLCD; ISSN:1948-7185. (American Chemical Society)
    The org.-inorg. hybrid perovskites methylammonium lead iodide (CH3NH3PbI3) and the partially Cl-substituted mixed halide CH3NH3PbI3-xClx emit strong and broad photoluminescence (PL) around their band gap energy of ∼1.6 eV. However, the nature of the radiative decay channels behind the obsd. emission and, in particular, the spectral broadening mechanisms are still unclear. Here the authors study these processes for high-quality vapor-deposited films of CH3NH3PbI3-xClx using time- and excitation-energy dependent photoluminescence spectroscopy. The PL spectrum is homogeneously broadened with a line width of 103 meV most likely as a consequence of phonon coupling effects. Further anal. reveals that defects or trap states play a minor role in radiative decay channels. In terms of possible lasing applications, the emission spectrum of the perovskite is sufficiently broad to have potential for amplification of light pulses < 100 fs pulse duration.
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    Zhang, M.; Yu, H.; Lyu, M.; Wang, Q.; Yun, J.-H.; Wang, L. Chem. Commun. 2014, 50, 11727– 11730
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    Xing, G.; Mathews, N.; Lim, S. S.; Yantara, N.; Liu, X.; Sabba, D.; Grätzel, M.; Mhaisalkar, S.; Sum, T. C. Nat. Mater. 2014, 13, 476– 480
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    Low-temperature solution-processed wavelength-tunable perovskites for lasing
    Xing, Guichuan; Mathews, Nripan; Lim, Swee Sien; Yantara, Natalia; Liu, Xinfeng; Sabba, Dharani; Graetzel, Michael; Mhaisalkar, Subodh; Sum, Tze Chien
    Nature Materials (2014), 13 (5), 476-480CODEN: NMAACR; ISSN:1476-1122. (Nature Publishing Group)
    Low-temp. soln.-processed materials that show optical gain and can be embedded into a wide range of cavity resonators are attractive for the realization of on-chip coherent light sources. Org. semiconductors and colloidal quantum dots are considered the main candidates for this application. However, stumbling blocks in org. lasing include intrinsic losses from bimol. annihilation and the conflicting requirements of high charge carrier mobility and large stimulated emission; whereas challenges pertaining to Auger losses and charge transport in quantum dots still remain. Herein, the authors reveal that soln.-processed org.-inorg. halide perovskites (CH3NH3PbX3 where X = Cl, Br, I), which demonstrated huge potential in photovoltaics, also have promising optical gain. Their ultra-stable amplified spontaneous emission at strikingly low thresholds stems from their large absorption coeffs., ultralow bulk defect densities and slow Auger recombination. Straightforward visible spectral tunability (390-790 nm) is demonstrated. Importantly, in view of their balanced ambipolar charge transport characteristics, these materials may show elec. driven lasing.
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    Deschler, F.; Price, M.; Pathak, S.; Klintberg, L. E.; Jarausch, D.-D.; Higler, R.; Hüttner, S.; Leijtens, T.; Stranks, S. D.; Snaith, H. J.; Atatüre, M.; Phillips, R. T.; Friend, R. H. J. Phys. Chem. Lett. 2014, 5, 1421– 1426
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    High Photoluminescence Efficiency and Optically Pumped Lasing in Solution-Processed Mixed Halide Perovskite Semiconductors
    Deschler, Felix; Price, Michael; Pathak, Sandeep; Klintberg, Lina E.; Jarausch, David-Dominik; Higler, Ruben; Huttner, Sven; Leijtens, Tomas; Stranks, Samuel D.; Snaith, Henry J.; Atature, Mete; Phillips, Richard T.; Friend, Richard H.
    Journal of Physical Chemistry Letters (2014), 5 (8), 1421-1426CODEN: JPCLCD; ISSN:1948-7185. (American Chemical Society)
    The study of the photophys. properties of org.-metallic lead halide perovskites, which demonstrate excellent photovoltaic performance in devices with electron- and hole-accepting layers, helps to understand their charge photogeneration and recombination mechanism and unravels their potential for other optoelectronic applications. The authors report surprisingly high luminescence (PL) quantum efficiencies, ≤70%, in these soln.-processed cryst. films. Photoexcitation in the pristine MeNH3PbI3-xClx perovskite results in free charge carrier formation within 1 ps and these free charge carriers undergo bimol. recombination on time scales of 10s to 100s of ns. To exemplify the high luminescence yield of the MeNH3PbI3-xClx perovskite, the authors construct and demonstrate the operation of an optically pumped vertical cavity laser comprising a layer of perovskite between a dielec. mirror and evapd. Au top mirrors. These long carrier lifetimes together with exceptionally high luminescence yield are unprecedented in such simply prepd. inorg. semiconductors, and these properties are ideally suited for photovoltaic diode operation.
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    Tan, Z.-K.; Moghaddam, R. S.; Lai, M. L.; Docampo, P.; Higler, R.; Deschler, F.; Price, M.; Sadhanala, A.; Pazos, L. M.; Credgington, D.; Hanusch, F.; Bein, T.; Snaith, H. J.; Friend, R. H. Nat. Nanotechnol. 2014, 9, 687– 692
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    Bright light-emitting diodes based on organometal halide perovskite
    Tan, Zhi-Kuang; Moghaddam, Reza Saberi; Lai, May Ling; Docampo, Pablo; Higler, Ruben; Deschler, Felix; Price, Michael; Sadhanala, Aditya; Pazos, Luis M.; Credgington, Dan; Hanusch, Fabian; Bein, Thomas; Snaith, Henry J.; Friend, Richard H.
    Nature Nanotechnology (2014), 9 (9), 687-692CODEN: NNAABX; ISSN:1748-3387. (Nature Publishing Group)
    Solid-state light-emitting devices based on direct-bandgap semiconductors have, over the past two decades, been utilized as energy-efficient sources of lighting. However, fabrication of these devices typically relies on expensive high-temp. and high-vacuum processes, rendering them uneconomical for use in large-area displays. Here, we report high-brightness light-emitting diodes based on soln.-processed organometal halide perovskites. We demonstrate electroluminescence in the near-IR, green and red by tuning the halide compns. in the perovskite. In our IR device, a thin 15 nm layer of CH3NH3PbI3-xClx perovskite emitter is sandwiched between larger-bandgap titanium dioxide (TiO2) and poly(9,9'-dioctylfluorene) (F8) layers, effectively confining electrons and holes in the perovskite layer for radiative recombination. We report an IR radiance of 13.2 W sr-1 m-2 at a c.d. of 363 mA cm-2, with highest external and internal quantum efficiencies of 0.76% and 3.4%, resp. In our green light-emitting device with an ITO/PEDOT:PSS/CH3NH3PbBr3/F8/Ca/Ag structure, we achieved a luminance of 364 cd m-2 at a c.d. of 123 mA cm-2, giving external and internal quantum efficiencies of 0.1% and 0.4%, resp. We show, using photoluminescence studies, that radiative bimol. recombination is dominant at higher excitation densities. Hence, the quantum efficiencies of the perovskite light-emitting diodes increase at higher current densities. This demonstration of effective perovskite electroluminescence offers scope for developing this unique class of materials into efficient and color-tunable light emitters for low-cost display, lighting and optical communication applications.
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    The defect structure of undoped CuInS2 was studied by elec., photoluminescence, and stoichiometric analyses. For a multilevel system such as CuInS2, the ionization energies were detd. to be 0.038, 0.068 and 0.145 eV for the S vacancy, In interstitial and In occupying the Cu vacancy, resp. A defect model based on deviation from the ideal chem. formula was developed to illustrate the self-compensation effects, in which quant. investigations of the structural defects in undoped CuInS2 crystals are provided.
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    Huang, L.; Zhu, X.; Publicover, N. G.; Hunter, K. W.; Ahmadiantehrani, M.; de Bettencourt-Dias, A.; Bell, T. W. J. Nanopart. Res. 2013, 15, 2056
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    Cadmium (Cd)- and zinc (Zn)-alloyed copper-indium-sulfide (Cu-In-S or CIS) nanocrystals (NCs) several nanometers in diam. were prepd. using thermal decompn. methods, and the effects of Cd and Zn on optical properties, including the tuning of NC photoluminescence (PL) wavelength and quantum yield (QY), were investigated. It was found that incorporation of Cd into CIS enhances the peak QY of NCs whereas Zn alloying diminishes the peak. In contrast with Zn alloying, Cd alloying does not result in a pronounced luminescence blue shift. The further PL decay study suggests that Cd alloying reduces surface or intrinsic defects whereas alloying with Zn increases the overall no. of defects.
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    The formal relationship between ultrasoft (US) Vanderbilt-type pseudopotentials and Blochl's projector augmented wave (PAW) method is derived. The total energy functional for US pseudopotentials can be obtained by linearization of two terms in a slightly modified PAW total energy functional. The Hamilton operator, the forces, and the stress tensor are derived for this modified PAW functional. A simple way to implement the PAW method in existing plane-wave codes supporting US pseudopotentials is pointed out. In addn., crit. tests are presented to compare the accuracy and efficiency of the PAW and the US pseudopotential method with relaxed-core all-electron methods. These tests include small mols. (H2, H2O, Li2, N2, F2, BF3, SiF4) and several bulk systems (diamond, Si, V, Li, Ca, CaF2, Fe, Co, Ni). Particular attention is paid to the bulk properties and magnetic energies of Fe, Co, and Ni.
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    This article reviews with many refs. the current status of lattice-dynamical calcns. in crystals, using d.-functional perturbation theory, with emphasis on the plane-wave pseudopotential method. Several specialized topics are treated, including the implementation for metals, the calcn. of the response to macroscopic elec. fields and their relevance to long-wavelength vibrations in polar materials, the response to strain deformations, and higher-order responses. The success of this methodol. is demonstrated with a no. of applications existing in the literature.
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    Atomistic Origins of High-Performance in Hybrid Halide Perovskite Solar Cells
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    Nano Letters (2014), 14 (5), 2584-2590CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
    The performance of organometallic perovskite solar cells has rapidly surpassed that of both conventional dye-sensitized and org. photovoltaics. High-power conversion efficiency can be realized in both mesoporous and thin-film device architectures. The authors address the origin of this success in the context of the materials chem. and physics of the bulk perovskite as described by electronic structure calcns. In addn. to the basic optoelectronic properties essential for an efficient photovoltaic device (spectrally suitable band gap, high optical absorption, low carrier effective masses), the materials are structurally and compositionally flexible. As the authors show, hybrid perovskites exhibit spontaneous elec. polarization; the authors also suggest ways in which this can be tuned through judicious choice of the org. cation. The presence of ferroelec. domains will result in internal junctions that may aid sepn. of photoexcited electron and hole pairs, and redn. of recombination through segregation of charge carriers. The combination of high dielec. const. and low effective mass promotes both Wannier-Mott exciton sepn. and effective ionization of donor and acceptor defects. The photoferroic effect could be exploited in nanostructured films to generate a higher open circuit voltage and may contribute to the current-voltage hysteresis obsd. in perovskite solar cells.
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    Org.-inorg. perovskites are a class of soln.-processed semiconductors holding promise for the realization of low-cost efficient solar cells and on-chip lasers. Despite the recent attention they have attracted, fundamental aspects of the photophysics underlying device operation still remain elusive. Here we use photoluminescence and transmission spectroscopy to show that photoexcitations give rise to a conducting plasma of unbound but Coulomb-correlated electron-hole pairs at all excitations of interest for light-energy conversion and stimulated optical amplification. The conductive nature of the photoexcited plasma has crucial consequences for perovskite-based devices: in solar cells, it ensures efficient charge sepn. and ambipolar transport while, concerning lasing, it provides a low threshold for light amplification and justifies a favorable outlook for the demonstration of an elec. driven laser. We find a significant trap d., whose cross-section for carrier capture is however low, yielding a minor impact on device performance.
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    Phosphors in phosphor-converted white light-emitting diodes: Recent advances in materials, techniques and properties
    Ye, S.; Xiao, F.; Pan, Y. X.; Ma, Y. Y.; Zhang, Q. Y.
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    A review. Phosphor-converted white light-emitting diodes (pc-WLEDs) are emerging as an indispensable solid-state light source for the next generation lighting industry and display systems due to their unique properties including but not limited to energy savings, environment-friendliness, small vol., and long persistence. Until now, major challenges in pc-WLEDs have been to achieve high luminous efficacy, high chromatic stability, brilliant color-rending properties, and price competitiveness against fluorescent lamps, which rely critically on the phosphor properties. A comprehensive understanding of the nature and limitations of phosphors and the factors dominating the general trends in pc-WLEDs is of fundamental importance for advancing technol. applications. This report aims to provide the most recent advances in the synthesis and application of phosphors for pc-WLEDs with emphasis specifically on: (a) principles to tune the excitation and emission spectra of phosphors: prediction according to crystal field theory, and structural chem. characteristics (e.g. covalence of chem. bonds, electronegativity, and polarization effects of element); (b) pc-WLEDs with phosphors excited by blue-LED chips: phosphor characteristics, structure, and activated ions (i.e. Ce3+ and Eu2+), including YAG:Ce, other garnets, non-garnets, sulfides, and (oxy)nitrides; (c) pc-WLEDs with phosphors excited by near UV LED chips: single-phased white-emitting phosphors (e.g. Eu2+-Mn2+ activated phosphors), red-green-blue phosphors, energy transfer, and mechanisms involved; and (d) new clues for designing novel high-performance phosphors for pc-WLEDs based on available LED chips. Emphasis shall also be placed on the relationships among crystal structure, luminescence properties, and device performances. In addn., applications, challenges and future advances of pc-WLEDs will be discussed.
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    Bomm, J.; Buechtemann, A.; Chatten, A. J.; Bose, R.; Farrell, D. J.; Chan, N. L. A.; Xiao, Y.; Slooff, L. H.; Meyer, T.; Meyer, A.; van Sark, W. G. J. H. M.; Koole, R. Sol. Energy Mater. Sol. Cells 2011, 95, 2087– 2094
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Cite this: Nano Lett. 2015, 15, 6, 3692–3696
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https://doi.org/10.1021/nl5048779
Published January 29, 2015

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  • Abstract

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    Figure 1

    Figure 1. Monodisperse CsPbX3 NCs and their structural characterization. (a) Schematic of the cubic perovskite lattice; (b,c) typical transmission electron microscopy (TEM) images of CsPbBr3 NCs; (d) X-ray diffraction patterns for typical ternary and mixed-halide NCs.

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    Figure 2

    Figure 2. Colloidal perovskite CsPbX3 NCs (X = Cl, Br, I) exhibit size- and composition-tunable bandgap energies covering the entire visible spectral region with narrow and bright emission: (a) colloidal solutions in toluene under UV lamp (λ = 365 nm); (b) representative PL spectra (λexc = 400 nm for all but 350 nm for CsPbCl3 samples); (c) typical optical absorption and PL spectra; (d) time-resolved PL decays for all samples shown in (c) except CsPbCl3.

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    Figure 3

    Figure 3. (a) Quantum-size effects in the absorption and emission spectra of 5–12 nm CsPbBr3 NCs. (b) Experimental versus theoretical (effective mass approximation, EMA) size dependence of the band gap energy.

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    Figure 4

    Figure 4. (a) Emission from CsPbX3 NCs (black data points) plotted on CEI chromaticity coordinates and compared to most common color standards (LCD TV, dashed white triangle, and NTSC TV, solid white triangle). Radiant Imaging Color Calculator software from Radiant Zemax (http://www.radiantzemax.com) was used to map the colors. (b) Photograph (λexc = 365 nm) of highly luminescent CsPbX3 NCs-PMMA polymer monoliths obtained with Irgacure 819 as photoinitiator for polymerization.

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      There is no corresponding record for this reference.
    15. 15
      Moller, C. K. Nature 1958, 182, 1436– 1436
      There is no corresponding record for this reference.
    16. 16
      Sharma, S.; Weiden, N.; Weiss, A. Z. Phys. Chem. 1992, 175, 63– 80
      There is no corresponding record for this reference.
    17. 17
      Trots, D. M.; Myagkota, S. V. J. Phys. Chem. Solids 2008, 69, 2520– 2526
      17
      High-temperature structural evolution of caesium and rubidium triiodoplumbates
      Trots, D. M.; Myagkota, S. V.
      Journal of Physics and Chemistry of Solids (2008), 69 (10), 2520-2526CODEN: JPCSAW; ISSN:0022-3697. (Elsevier Ltd.)
      CsPbI3 and RbPbI3 were investigated by in situ powder diffraction within temp. ranges of 298-687 K and 298-714 K, resp. Both compds. crystallize in orthorhombic Pnma symmetry and expand isotropically upon a heating, revealing almost the same relative change of the lattice parameters. A pronounced difference in the structural evolution close to 600 K was obsd., namely, CsPbI3 undergoes 1st-order reversible phase transformation Pnma 563 K↔ Pnma + Pm‾3m 602 ↔ K Pm‾3m, whereas no transitions (except of the sample's melting) in RbPbI3 were detected. An attempt to clarify the relation between the existence/absence of a phase transition and bulging out of the I environment around alk. ions was undertaken.
    18. 18
      Stoumpos, C. C.; Malliakas, C. D.; Kanatzidis, M. G. Inorg. Chem. 2013, 52, 9019– 9038
      18
      Semiconducting Tin and Lead Iodide Perovskites with Organic Cations: Phase Transitions, High Mobilities, and Near-Infrared Photoluminescent Properties
      Stoumpos, Constantinos C.; Malliakas, Christos D.; Kanatzidis, Mercouri G.
      Inorganic Chemistry (2013), 52 (15), 9019-9038CODEN: INOCAJ; ISSN:0020-1669. (American Chemical Society)
      A broad org.-inorg. series of hybrid metal iodide perovskites AMI3, where A is the methylammonium (MeNH3+) or formamidinium (HC(NH2)2+) cation and M is Sn (1 and 2) or Pb (3 and 4) are reported. The compds. were prepd. through a variety of synthetic approaches, and the nature of the resulting materials is discussed in terms of their thermal stability and optical and electronic properties. The chem. and phys. properties of these materials strongly depend on the prepn. method. Single crystal x-ray diffraction anal. of 1-4 classifies the compds. in the perovskite structural family. Structural phase transitions were obsd. and studied by temp.-dependent single crystal x-ray diffraction in the 100-400 K range. The charge transport properties of the materials are discussed in conjunction with diffuse reflectance studies in the mid-IR region that display characteristic absorption features. Temp.-dependent studies show a strong dependence of the resistivity as a function of the crystal structure. Optical absorption measurements indicate that 1-4 behave as direct-gap semiconductors with energy band gaps distributed at 1.25-1.75 eV. The compds. exhibit an intense near-IR luminescence (PL) emission in the 700-1000 nm range (1.1-1.7 eV) at room temp. Solid solns. between the Sn and Pb compds. are readily accessible throughout the compn. range. The optical properties such as energy band gap, emission intensity, and wavelength can be readily controlled for the isostructural series of solid solns. MeNH3Sn1-xPbxI3 (5). The charge transport type in these materials was characterized by Seebeck coeff. and Hall-effect measurements. The compds. behave as p- or n-type semiconductors depending on the prepn. method. The samples with the lowest carrier concn. are prepd. from soln. and are n-type; p-type samples can be obtained through solid state reactions exposed in air in a controllable manner. In the case of Sn compds., there is a facile tendency toward oxidn. which causes the materials to be doped with Sn4+ and thus behave as p-type semiconductors displaying metal-like cond. The compds. appear to possess very high estd. electron and hole mobilities that exceed 2000 cm2/(V s) and 300 cm2/(V s), resp., as shown in the case of MeNH3SnI3 (1). The authors also compare the properties of the title hybrid materials with those of the all-inorg. CsSnI3 and CsPbI3 prepd. using identical synthetic methods.
    19. 19
      Babin, V.; Fabeni, P.; Nikl, M.; Nitsch, K.; Pazzi, G. P.; Zazubovich, S. Phys. Status Solidi B 2001, 226, 419– 428
      There is no corresponding record for this reference.
    20. 20
      Christodoulou, S.; Vaccaro, G.; Pinchetti, V.; De Donato, F.; Grim, J. Q.; Casu, A.; Genovese, A.; Vicidomini, G.; Diaspro, A.; Brovelli, S.; Manna, L.; Moreels, I. J. Mater. Chem. C 2014, 2, 3439– 3447
      20
      Synthesis of highly luminescent wurtzite CdSe/CdS giant-shell nanocrystals using a fast continuous injection route
      Christodoulou, S.; Vaccaro, G.; Pinchetti, V.; De Donato, F.; Grim, J. Q.; Casu, A.; Genovese, A.; Vicidomini, G.; Diaspro, A.; Brovelli, S.; Manna, L.; Moreels, I.
      Journal of Materials Chemistry C: Materials for Optical and Electronic Devices (2014), 2 (17), 3439-3447CODEN: JMCCCX; ISSN:2050-7534. (Royal Society of Chemistry)
      We synthesized CdSe/CdS giant-shell nanocrystals, with a CdSe core diam. between 2.8 nm and 5.5 nm, and a CdS shell thickness of up to 7-8 nm (equiv. to about 20 monolayers of CdS). Both the core and shell have a wurtzite crystal structure, yielding epitaxial growth of the shell and nearly defect-free crystals. As a result, the photoluminescence (PL) quantum efficiency (QE) is as high as 90%. Quant. PL measurements at various excitation wavelengths allow us to sep. the nonradiative decay into contributions from interface and surface trapping, giving us pathways for future optimization of the structure. In addn., the NCs do not blink, and the giant shell and concurring strong electron delocalization efficiently suppress Auger recombination, yielding a biexciton lifetime of about 15 ns. The corresponding biexciton PL QE equals 11% in 5.5/18.1 nm CdSe/CdS. Variable-temp. time-resolved PL and PL under magnetic fields further reveal that the emission at cryogenic temp. originates from a neg. trion-state, in agreement with other CdSe/CdS giant-shell systems reported in the literature.
    21. 21
      Wehrenfennig, C.; Liu, M.; Snaith, H. J.; Johnston, M. B.; Herz, L. M. J. Phys. Chem. Lett. 2014, 5, 1300– 1306
      21
      Homogeneous Emission Line Broadening in the Organo Lead Halide Perovskite CH3NH3PbI3-xClx
      Wehrenfennig, Christian; Liu, Mingzhen; Snaith, Henry J.; Johnston, Michael B.; Herz, Laura M.
      Journal of Physical Chemistry Letters (2014), 5 (8), 1300-1306CODEN: JPCLCD; ISSN:1948-7185. (American Chemical Society)
      The org.-inorg. hybrid perovskites methylammonium lead iodide (CH3NH3PbI3) and the partially Cl-substituted mixed halide CH3NH3PbI3-xClx emit strong and broad photoluminescence (PL) around their band gap energy of ∼1.6 eV. However, the nature of the radiative decay channels behind the obsd. emission and, in particular, the spectral broadening mechanisms are still unclear. Here the authors study these processes for high-quality vapor-deposited films of CH3NH3PbI3-xClx using time- and excitation-energy dependent photoluminescence spectroscopy. The PL spectrum is homogeneously broadened with a line width of 103 meV most likely as a consequence of phonon coupling effects. Further anal. reveals that defects or trap states play a minor role in radiative decay channels. In terms of possible lasing applications, the emission spectrum of the perovskite is sufficiently broad to have potential for amplification of light pulses < 100 fs pulse duration.
    22. 22
      Zhang, M.; Yu, H.; Lyu, M.; Wang, Q.; Yun, J.-H.; Wang, L. Chem. Commun. 2014, 50, 11727– 11730
      There is no corresponding record for this reference.
    23. 23
      Xing, G.; Mathews, N.; Lim, S. S.; Yantara, N.; Liu, X.; Sabba, D.; Grätzel, M.; Mhaisalkar, S.; Sum, T. C. Nat. Mater. 2014, 13, 476– 480
      23
      Low-temperature solution-processed wavelength-tunable perovskites for lasing
      Xing, Guichuan; Mathews, Nripan; Lim, Swee Sien; Yantara, Natalia; Liu, Xinfeng; Sabba, Dharani; Graetzel, Michael; Mhaisalkar, Subodh; Sum, Tze Chien
      Nature Materials (2014), 13 (5), 476-480CODEN: NMAACR; ISSN:1476-1122. (Nature Publishing Group)
      Low-temp. soln.-processed materials that show optical gain and can be embedded into a wide range of cavity resonators are attractive for the realization of on-chip coherent light sources. Org. semiconductors and colloidal quantum dots are considered the main candidates for this application. However, stumbling blocks in org. lasing include intrinsic losses from bimol. annihilation and the conflicting requirements of high charge carrier mobility and large stimulated emission; whereas challenges pertaining to Auger losses and charge transport in quantum dots still remain. Herein, the authors reveal that soln.-processed org.-inorg. halide perovskites (CH3NH3PbX3 where X = Cl, Br, I), which demonstrated huge potential in photovoltaics, also have promising optical gain. Their ultra-stable amplified spontaneous emission at strikingly low thresholds stems from their large absorption coeffs., ultralow bulk defect densities and slow Auger recombination. Straightforward visible spectral tunability (390-790 nm) is demonstrated. Importantly, in view of their balanced ambipolar charge transport characteristics, these materials may show elec. driven lasing.
    24. 24
      Deschler, F.; Price, M.; Pathak, S.; Klintberg, L. E.; Jarausch, D.-D.; Higler, R.; Hüttner, S.; Leijtens, T.; Stranks, S. D.; Snaith, H. J.; Atatüre, M.; Phillips, R. T.; Friend, R. H. J. Phys. Chem. Lett. 2014, 5, 1421– 1426
      24
      High Photoluminescence Efficiency and Optically Pumped Lasing in Solution-Processed Mixed Halide Perovskite Semiconductors
      Deschler, Felix; Price, Michael; Pathak, Sandeep; Klintberg, Lina E.; Jarausch, David-Dominik; Higler, Ruben; Huttner, Sven; Leijtens, Tomas; Stranks, Samuel D.; Snaith, Henry J.; Atature, Mete; Phillips, Richard T.; Friend, Richard H.
      Journal of Physical Chemistry Letters (2014), 5 (8), 1421-1426CODEN: JPCLCD; ISSN:1948-7185. (American Chemical Society)
      The study of the photophys. properties of org.-metallic lead halide perovskites, which demonstrate excellent photovoltaic performance in devices with electron- and hole-accepting layers, helps to understand their charge photogeneration and recombination mechanism and unravels their potential for other optoelectronic applications. The authors report surprisingly high luminescence (PL) quantum efficiencies, ≤70%, in these soln.-processed cryst. films. Photoexcitation in the pristine MeNH3PbI3-xClx perovskite results in free charge carrier formation within 1 ps and these free charge carriers undergo bimol. recombination on time scales of 10s to 100s of ns. To exemplify the high luminescence yield of the MeNH3PbI3-xClx perovskite, the authors construct and demonstrate the operation of an optically pumped vertical cavity laser comprising a layer of perovskite between a dielec. mirror and evapd. Au top mirrors. These long carrier lifetimes together with exceptionally high luminescence yield are unprecedented in such simply prepd. inorg. semiconductors, and these properties are ideally suited for photovoltaic diode operation.
    25. 25
      Tan, Z.-K.; Moghaddam, R. S.; Lai, M. L.; Docampo, P.; Higler, R.; Deschler, F.; Price, M.; Sadhanala, A.; Pazos, L. M.; Credgington, D.; Hanusch, F.; Bein, T.; Snaith, H. J.; Friend, R. H. Nat. Nanotechnol. 2014, 9, 687– 692
      25
      Bright light-emitting diodes based on organometal halide perovskite
      Tan, Zhi-Kuang; Moghaddam, Reza Saberi; Lai, May Ling; Docampo, Pablo; Higler, Ruben; Deschler, Felix; Price, Michael; Sadhanala, Aditya; Pazos, Luis M.; Credgington, Dan; Hanusch, Fabian; Bein, Thomas; Snaith, Henry J.; Friend, Richard H.
      Nature Nanotechnology (2014), 9 (9), 687-692CODEN: NNAABX; ISSN:1748-3387. (Nature Publishing Group)
      Solid-state light-emitting devices based on direct-bandgap semiconductors have, over the past two decades, been utilized as energy-efficient sources of lighting. However, fabrication of these devices typically relies on expensive high-temp. and high-vacuum processes, rendering them uneconomical for use in large-area displays. Here, we report high-brightness light-emitting diodes based on soln.-processed organometal halide perovskites. We demonstrate electroluminescence in the near-IR, green and red by tuning the halide compns. in the perovskite. In our IR device, a thin 15 nm layer of CH3NH3PbI3-xClx perovskite emitter is sandwiched between larger-bandgap titanium dioxide (TiO2) and poly(9,9'-dioctylfluorene) (F8) layers, effectively confining electrons and holes in the perovskite layer for radiative recombination. We report an IR radiance of 13.2 W sr-1 m-2 at a c.d. of 363 mA cm-2, with highest external and internal quantum efficiencies of 0.76% and 3.4%, resp. In our green light-emitting device with an ITO/PEDOT:PSS/CH3NH3PbBr3/F8/Ca/Ag structure, we achieved a luminance of 364 cd m-2 at a c.d. of 123 mA cm-2, giving external and internal quantum efficiencies of 0.1% and 0.4%, resp. We show, using photoluminescence studies, that radiative bimol. recombination is dominant at higher excitation densities. Hence, the quantum efficiencies of the perovskite light-emitting diodes increase at higher current densities. This demonstration of effective perovskite electroluminescence offers scope for developing this unique class of materials into efficient and color-tunable light emitters for low-cost display, lighting and optical communication applications.
    26. 26
      Ueng, H. Y.; Hwang, H. L. J. Phys. Chem. Solids 1989, 50, 1297– 1305
      26
      The defect structure of copper indium sulfide (CuInS2). Part I. Intrinsic defects
      Ueng, H. Y.; Hwang, H. L.
      Journal of Physics and Chemistry of Solids (1989), 50 (12), 1297-305CODEN: JPCSAW; ISSN:0022-3697.
      The defect structure of undoped CuInS2 was studied by elec., photoluminescence, and stoichiometric analyses. For a multilevel system such as CuInS2, the ionization energies were detd. to be 0.038, 0.068 and 0.145 eV for the S vacancy, In interstitial and In occupying the Cu vacancy, resp. A defect model based on deviation from the ideal chem. formula was developed to illustrate the self-compensation effects, in which quant. investigations of the structural defects in undoped CuInS2 crystals are provided.
    27. 27
      Huang, L.; Zhu, X.; Publicover, N. G.; Hunter, K. W.; Ahmadiantehrani, M.; de Bettencourt-Dias, A.; Bell, T. W. J. Nanopart. Res. 2013, 15, 2056
      27
      Cadmium- and zinc-alloyed Cu-In-S nanocrystals and their optical properties
      Huang, Liming; Zhu, Xiaoshan; Publicover, Nelson G.; Hunter, Kenneth W.; Ahmadiantehrani, Mojtaba; de Bettencourt-Dias, Ana; Bell, Thomas W.
      Journal of Nanoparticle Research (2013), 15 (11), 2056/1-2056/10, 10 pp.CODEN: JNARFA; ISSN:1388-0764. (Springer)
      Cadmium (Cd)- and zinc (Zn)-alloyed copper-indium-sulfide (Cu-In-S or CIS) nanocrystals (NCs) several nanometers in diam. were prepd. using thermal decompn. methods, and the effects of Cd and Zn on optical properties, including the tuning of NC photoluminescence (PL) wavelength and quantum yield (QY), were investigated. It was found that incorporation of Cd into CIS enhances the peak QY of NCs whereas Zn alloying diminishes the peak. In contrast with Zn alloying, Cd alloying does not result in a pronounced luminescence blue shift. The further PL decay study suggests that Cd alloying reduces surface or intrinsic defects whereas alloying with Zn increases the overall no. of defects.
    28. 28
      De Trizio, L.; Prato, M.; Genovese, A.; Casu, A.; Povia, M.; Simonutti, R.; Alcocer, M. J. P.; D’Andrea, C.; Tassone, F.; Manna, L. Chem. Mater. 2012, 24, 2400– 2406
      There is no corresponding record for this reference.
    29. 29
      Zhang, W.; Zhong, X. Inorg. Chem. 2011, 50, 4065– 4072
      There is no corresponding record for this reference.
    30. 30
      Kresse, G.; Joubert, D. Phys. Rev. B 1999, 59, 1758
      30
      From ultrasoft pseudopotentials to the projector augmented-wave method
      Kresse, G.; Joubert, D.
      Physical Review B: Condensed Matter and Materials Physics (1999), 59 (3), 1758-1775CODEN: PRBMDO; ISSN:0163-1829. (American Physical Society)
      The formal relationship between ultrasoft (US) Vanderbilt-type pseudopotentials and Blochl's projector augmented wave (PAW) method is derived. The total energy functional for US pseudopotentials can be obtained by linearization of two terms in a slightly modified PAW total energy functional. The Hamilton operator, the forces, and the stress tensor are derived for this modified PAW functional. A simple way to implement the PAW method in existing plane-wave codes supporting US pseudopotentials is pointed out. In addn., crit. tests are presented to compare the accuracy and efficiency of the PAW and the US pseudopotential method with relaxed-core all-electron methods. These tests include small mols. (H2, H2O, Li2, N2, F2, BF3, SiF4) and several bulk systems (diamond, Si, V, Li, Ca, CaF2, Fe, Co, Ni). Particular attention is paid to the bulk properties and magnetic energies of Fe, Co, and Ni.
    31. 31
      Baroni, S.; de Gironcoli, S.; Dal Corso, A.; Giannozzi, P. Rev. Mod. Phys. 2001, 73, 515
      31
      Phonons and related crystal properties from density-functional perturbation theory
      Baroni, Stefano; De Gironcoli, Stefano; Dal Corso, Andrea; Giannozzi, Paolo
      Reviews of Modern Physics (2001), 73 (2), 515-562CODEN: RMPHAT; ISSN:0034-6861. (American Physical Society)
      This article reviews with many refs. the current status of lattice-dynamical calcns. in crystals, using d.-functional perturbation theory, with emphasis on the plane-wave pseudopotential method. Several specialized topics are treated, including the implementation for metals, the calcn. of the response to macroscopic elec. fields and their relevance to long-wavelength vibrations in polar materials, the response to strain deformations, and higher-order responses. The success of this methodol. is demonstrated with a no. of applications existing in the literature.
    32. 32
      Yu, P. Y.; Cardona, M. Fundamentals of Semiconductors; Springer: New York, 1996.
      There is no corresponding record for this reference.
    33. 33
      Even, J.; Pedesseau, L.; Katan, C. J. Phys. Chem. C 2014, 118, 11566– 11572
      There is no corresponding record for this reference.
    34. 34
      Frost, J. M.; Butler, K. T.; Brivio, F.; Hendon, C. H.; van Schilfgaarde, M.; Walsh, A. Nano Lett. 2014, 14, 2584– 2590
      34
      Atomistic Origins of High-Performance in Hybrid Halide Perovskite Solar Cells
      Frost, Jarvist M.; Butler, Keith T.; Brivio, Federico; Hendon, Christopher H.; van Schilfgaarde, Mark; Walsh, Aron
      Nano Letters (2014), 14 (5), 2584-2590CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
      The performance of organometallic perovskite solar cells has rapidly surpassed that of both conventional dye-sensitized and org. photovoltaics. High-power conversion efficiency can be realized in both mesoporous and thin-film device architectures. The authors address the origin of this success in the context of the materials chem. and physics of the bulk perovskite as described by electronic structure calcns. In addn. to the basic optoelectronic properties essential for an efficient photovoltaic device (spectrally suitable band gap, high optical absorption, low carrier effective masses), the materials are structurally and compositionally flexible. As the authors show, hybrid perovskites exhibit spontaneous elec. polarization; the authors also suggest ways in which this can be tuned through judicious choice of the org. cation. The presence of ferroelec. domains will result in internal junctions that may aid sepn. of photoexcited electron and hole pairs, and redn. of recombination through segregation of charge carriers. The combination of high dielec. const. and low effective mass promotes both Wannier-Mott exciton sepn. and effective ionization of donor and acceptor defects. The photoferroic effect could be exploited in nanostructured films to generate a higher open circuit voltage and may contribute to the current-voltage hysteresis obsd. in perovskite solar cells.
    35. 35
      Menéndez-Proupin, E.; Palacios, P.; Wahnón, P.; Conesa, J. Phys. Rev. B 2014, 90, 045207
      There is no corresponding record for this reference.
    36. 36
      Saba, M.; Cadelano, M.; Marongiu, D.; Chen, F.; Sarritzu, V.; Sestu, N.; Figus, C.; Aresti, M.; Piras, R.; Geddo Lehmann, A.; Cannas, C.; Musinu, A.; Quochi, F.; Mura, A.; Bongiovanni, G. Nat. Commun. 2014, 5, 5049
      36
      Correlated electron-hole plasma in organometal perovskites
      Saba, Michele; Cadelano, Michele; Marongiu, Daniela; Chen, Feipeng; Sarritzu, Valerio; Sestu, Nicola; Figus, Cristiana; Aresti, Mauro; Piras, Roberto; Geddo Lehmann, Alessandra; Cannas, Carla; Musinu, Anna; Quochi, Francesco; Mura, Andrea; Bongiovanni, Giovanni
      Nature Communications (2014), 5 (), 5049CODEN: NCAOBW; ISSN:2041-1723. (Nature Publishing Group)
      Org.-inorg. perovskites are a class of soln.-processed semiconductors holding promise for the realization of low-cost efficient solar cells and on-chip lasers. Despite the recent attention they have attracted, fundamental aspects of the photophysics underlying device operation still remain elusive. Here we use photoluminescence and transmission spectroscopy to show that photoexcitations give rise to a conducting plasma of unbound but Coulomb-correlated electron-hole pairs at all excitations of interest for light-energy conversion and stimulated optical amplification. The conductive nature of the photoexcited plasma has crucial consequences for perovskite-based devices: in solar cells, it ensures efficient charge sepn. and ambipolar transport while, concerning lasing, it provides a low threshold for light amplification and justifies a favorable outlook for the demonstration of an elec. driven laser. We find a significant trap d., whose cross-section for carrier capture is however low, yielding a minor impact on device performance.
    37. 37
      Kim, T.-H.; Jun, S.; Cho, K.-S.; Choi, B. L.; Jang, E. MRS Bull. 2013, 38, 712– 720
      There is no corresponding record for this reference.
    38. 38
      Supran, G. J.; Shirasaki, Y.; Song, K. W.; Caruge, J.-M.; Kazlas, P. T.; Coe-Sullivan, S.; Andrew, T. L.; Bawendi, M. G.; Bulović, V. MRS Bull. 2013, 38, 703– 711
      There is no corresponding record for this reference.
    39. 39
      Ye, S.; Xiao, F.; Pan, Y. X.; Ma, Y. Y.; Zhang, Q. Y. Mater. Sci. Eng. R 2010, 71, 1– 34
      39
      Phosphors in phosphor-converted white light-emitting diodes: Recent advances in materials, techniques and properties
      Ye, S.; Xiao, F.; Pan, Y. X.; Ma, Y. Y.; Zhang, Q. Y.
      Materials Science & Engineering, R: Reports (2010), R71 (1), 1-34CODEN: MIGIEA; ISSN:0927-796X. (Elsevier B.V.)
      A review. Phosphor-converted white light-emitting diodes (pc-WLEDs) are emerging as an indispensable solid-state light source for the next generation lighting industry and display systems due to their unique properties including but not limited to energy savings, environment-friendliness, small vol., and long persistence. Until now, major challenges in pc-WLEDs have been to achieve high luminous efficacy, high chromatic stability, brilliant color-rending properties, and price competitiveness against fluorescent lamps, which rely critically on the phosphor properties. A comprehensive understanding of the nature and limitations of phosphors and the factors dominating the general trends in pc-WLEDs is of fundamental importance for advancing technol. applications. This report aims to provide the most recent advances in the synthesis and application of phosphors for pc-WLEDs with emphasis specifically on: (a) principles to tune the excitation and emission spectra of phosphors: prediction according to crystal field theory, and structural chem. characteristics (e.g. covalence of chem. bonds, electronegativity, and polarization effects of element); (b) pc-WLEDs with phosphors excited by blue-LED chips: phosphor characteristics, structure, and activated ions (i.e. Ce3+ and Eu2+), including YAG:Ce, other garnets, non-garnets, sulfides, and (oxy)nitrides; (c) pc-WLEDs with phosphors excited by near UV LED chips: single-phased white-emitting phosphors (e.g. Eu2+-Mn2+ activated phosphors), red-green-blue phosphors, energy transfer, and mechanisms involved; and (d) new clues for designing novel high-performance phosphors for pc-WLEDs based on available LED chips. Emphasis shall also be placed on the relationships among crystal structure, luminescence properties, and device performances. In addn., applications, challenges and future advances of pc-WLEDs will be discussed.
    40. 40
      Bomm, J.; Buechtemann, A.; Chatten, A. J.; Bose, R.; Farrell, D. J.; Chan, N. L. A.; Xiao, Y.; Slooff, L. H.; Meyer, T.; Meyer, A.; van Sark, W. G. J. H. M.; Koole, R. Sol. Energy Mater. Sol. Cells 2011, 95, 2087– 2094
      40
      Fabrication and full characterization of state-of-the-art quantum dot luminescent solar concentrators
      Bomm, Jana; Buechtemann, Andreas; Chatten, Amanda J.; Bose, Rahul; Farrell, Daniel J.; Chan, Ngai L. A.; Xiao, Ye; Slooff, Lenneke H.; Meyer, Toby; Meyer, Andreas; van Sark, Wilfried G. J. H. M.; Koole, Rolf
      Solar Energy Materials & Solar Cells (2011), 95 (8), 2087-2094CODEN: SEMCEQ; ISSN:0927-0248. (Elsevier B.V.)
      The fabrication and full characterization of luminescent solar concentrators (LSCs) comprising CdSe core/multishell quantum dots (QDs) is reported. TEM anal. shows that the QDs are well dispersed in the acrylic medium while maintaining a high quantum yield of 45%, resulting in highly transparent and luminescent polymer plates. A detailed optical anal. of the QD-LSCs including absorption, emission, and time-resolved fluorescence measurements is presented. Both silicon and GaAs solar cells attached to the side of the QD-LSCs are used to measure the external quantum efficiency and power conversion efficiency (2.8%) of the devices. Stability tests show only a minor decrease of 4% in photocurrent upon an equiv. of three months outdoor illumination. The optical data are used as input for a ray-trace model that is shown to describe the properties of the QD-LSCs well. The model was then used to extrapolate the properties of the small test devices to predict the power conversion efficiency of a 50×50 cm2 module with a variety of different solar cells. The work described here gives a detailed insight into the promise of QD-based LSCs.
    41. 41
      Meinardi, F.; Colombo, A.; Velizhanin, K. A.; Simonutti, R.; Lorenzon, M.; Beverina, L.; Viswanatha, R.; Klimov, V. I.; Brovelli, S. Nat. Photonics 2014, 8, 392– 399
      41
      Large-area luminescent solar concentrators based on 'Stokes-shift-engineered' nanocrystals in a mass-polymerized PMMA matrix
      Meinardi, Francesco; Colombo, Annalisa; Velizhanin, Kirill A.; Simonutti, Roberto; Lorenzon, Monica; Beverina, Luca; Viswanatha, Ranjani; Klimov, Victor I.; Brovelli, Sergio
      Nature Photonics (2014), 8 (5), 392-399CODEN: NPAHBY; ISSN:1749-4885. (Nature Publishing Group)
      Luminescent solar concentrators are cost-effective complements to semiconductor photovoltaics that can boost the output of solar cells and allow for the integration of photovoltaic-active architectural elements into buildings (for example, photovoltaic windows). Colloidal quantum dots are attractive for use in luminescent solar concentrators, but their small Stokes shift results in reabsorption losses that hinder the realization of large-area devices. Here, we use 'Stokes-shift-engineered' CdSe/CdS quantum dots with giant shells (giant quantum dots) to realize luminescent solar concentrators without reabsorption losses for device dimensions up to tens of centimeters. Monte-Carlo simulations show a 100-fold increase in efficiency using giant quantum dots compared with core-only nanocrystals. We demonstrate the feasibility of this approach by using high-optical-quality quantum dot-polymethylmethacrylate nanocomposites fabricated using a modified industrial method that preserves the light-emitting properties of giant quantum dots upon incorporation into the polymer. Study of these luminescent solar concentrators yields optical efficiencies >10% and an effective concn. factor of 4.4. These results demonstrate the significant promise of Stokes-shift-engineered quantum dots for large-area luminescent solar concentrators.
    42. 42
      Gruetzmacher, H.; Geier, J.; Stein, D.; Ott, T.; Schoenberg, H.; Sommerlade, R. H.; Boulmaaz, S.; Wolf, J.-P.; Murer, P.; Ulrich, T. Chimia 2008, 62, 18– 22
      There is no corresponding record for this reference.

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