Electric-field-resolved detection of localized surface plasmons at petahertz-scale frequencies

We present a novel electric-field-resolved approach for probing ultrafast dynamics of localized surface plasmons in metallic nanoparticles. The electric field of the broadband carrier-envelope-phase stable few-cycle light pulse employed in the experiment provides access to time-domain signatures of plasmonic dynamics that are imprinted on the pulse waveform. The simultaneous access to absolute spectral amplitudes and phases of the interacting light allows us obtaining a complex spectral response associated with localized surface plasmons. We benchmark our findings against the absorbance spectrum obtained with a spectrometer as well as the extinction cross-section modeled by a classical Mie scattering theory

Single crystals of caesium formamidinium lead halide perovskites: solution growth and gamma dosimetry

Formamidinium (FA)-based hybrid lead halide perovskites (FAPbX3, X=I or Br/I) have recently led to significant improvements in the performance of perovskite photovoltaics. The remaining major pitfall is the instability of α-FAPbI3, causing the phase transition from the desired three-dimensional cubic perovskite phase to a non-perovskite one-dimensional hexagonal lattice. In this work, we report the facile, inexpensive, solution-phase growth of cm-scale single crystals (SCs) of variable composition CsxFA1−xPbI3−yBry (x=0–0.1, y=0–0.6) which exhibit improved phase stability compared to the parent α-FAPbI3 compound. These SCs possess outstanding electronic quality, manifested by a high-carrier mobility–lifetime product of up to 1.2 × 10−1 cm2 V−1 and a low dark carrier density that, combined with the high absorptivity of high-energy photons by Pb and I, allows the sensitive detection of gamma radiation. With stable operation up to 30 V, these novel SCs have been used in a prototype of a gamma-counting dosimeter

Manganese(II) in Tetrahedral Halide Environment: Factors Governing Bright Green Luminescence

Finding narrow-band light emitters for the visible spectral region remains an immense challenge. Such phosphors are in great demand for solid-state lighting and display application. In this context, green luminescence from tetrahedrally coordinated Mn(II) is an attractive research direction. While the oxide–ligand environment had been studied for decades, much less systematic efforts have been undertaken with regard to halide coordination, especially in the form of fully inorganic halide matrixes. In this study, we synthesized a series of hybrid organic–inorganic Mn(II) halides as well as a range of fully inorganic Zn halide hosts (chlorides, bromides, iodides) doped with Mn(II). In the latter, tetrahedral coordination is attained via substitutional doping owing to the tetrahedral symmetry of Zn sites. We find that the choice of the halide as well as subtle details of the crystal structure profoundly govern the photoluminescence peak positions (500–550 nm range) and emission line widths (40–60 nm) as well as radiative lifetimes (shorter for iodides) through the altered ligand-field effects and degrees of spin–orbit coupling. The photoluminescence quantum yields were as high as 70–90%. The major hurdle for the practical use of these compounds lies in their low absorption coefficients in the blue spectral regions.ISSN:0897-475

Solution-Grown CsPbBr₃ Perovskite Single Crystals for Photon Detection

Solution-Grown CsPbBr₃ Perovskite Single Crystals for Photon Detectio

Perovskite-type superlattices from lead halide perovskite nanocubes

Atomically defined assemblies of dye molecules (such as H and J aggregates) have been of interest for more than 80 years because of the emergence of collective phenomena in their optical spectra1,2,3, their coherent long-range energy transport, their conceptual similarity to natural light-harvesting complexes4,5, and their potential use as light sources and in photovoltaics. Another way of creating versatile and controlled aggregates that exhibit collective phenomena involves the organization of colloidal semiconductor nanocrystals into long-range-ordered superlattices6. Caesium lead halide perovskite nanocrystals7,8,9 are promising building blocks for such superlattices, owing to the high oscillator strength of bright triplet excitons10, slow dephasing (coherence times of up to 80 picoseconds) and minimal inhomogeneous broadening of emission lines11,12. So far, only single-component superlattices with simple cubic packing have been devised from these nanocrystals13. Here we present perovskite-type (ABO3) binary and ternary nanocrystal superlattices, created via the shape-directed co-assembly of steric-stabilized, highly luminescent cubic CsPbBr3 nanocrystals (which occupy the B and/or O lattice sites), spherical Fe3O4 or NaGdF4 nanocrystals (A sites) and truncated-cuboid PbS nanocrystals (B sites). These ABO3 superlattices, as well as the binary NaCl and AlB2 superlattice structures that we demonstrate, exhibit a high degree of orientational ordering of the CsPbBr3 nanocubes. They also exhibit superfluorescence—a collective emission that results in a burst of photons with ultrafast radiative decay (22 picoseconds) that could be tailored for use in ultrabright (quantum) light sources. Our work paves the way for further exploration of complex, ordered and functionally useful perovskite mesostructures.ISSN:0028-0836ISSN:1476-468

Size‐ and Temperature‐Dependent Lattice Anisotropy and Structural Distortion in CsPbBr3 Quantum Dots by Reciprocal Space X‐ray Total Scattering Analysis

Lead halide perovskite nanocrystals (NCs) have emerged as next‐generation semiconductors capable of unifying superior photoemission properties, facile and inexpensive preparation, compositional and structural versatility. Among them, CsPbBr3 is a model system in theoretical and experimental studies owing to its intrinsic chemical stability. Nonetheless, knowledge of the precise magnitude and the size‐ and temperature‐dependent lattice and structural distortions is lacking, and the static/dynamic nature of disorder in NCs remains an open question. Herein, robust reciprocal space X‐ray total scattering analysis is applied and accurate lattice distortions, PbBr bond distances, and PbBrPb angles versus NCs size are extracted. The lattice anisotropy increases upon expansion on downsizing while, upon contraction on cooling, the lattice distortion behaves differently at intermediate (9 nm) and ultrasmall (5 nm) sizes and from the bulk. Bond distances (stretched by ≈1%) do not show any size dependence, whereas equatorial and axial angles denote more symmetric octahedral arrangements in the smallest sizes, where they differ by ≈2° compared to ≈8° in the bulk. Anomalously high atomic displacement parameters of axial bromine ions persisting down to cryogenic temperatures suggest statically disordered octahedral tilts. These results provide insights having important implications on size‐dependent emission properties and the exciton fine structure

Room-Temperature, Highly Pure Single-Photon Sources from All-Inorganic Lead Halide Perovskite Quantum Dots

Attaining pure single-photon emission is key for many quantum technologies, from optical quantum computing to quantum key distribution and quantum imaging. The past 20 years have seen the development of several solid-state quantum emitters, but most of them require highly sophisticated techniques (e.g., ultrahigh vacuum growth methods and cryostats for low-temperature operation). The system complexity may be significantly reduced by employing quantum emitters capable of working at room temperature. Here, we present a systematic study across ∼170 photostable single CsPbX3 (X: Br and I) colloidal quantum dots (QDs) of different sizes and compositions, unveiling that increasing quantum confinement is an effective strategy for maximizing single-photon purity due to the suppressed biexciton quantum yield. Leveraging the latter, we achieve 98% single-photon purity (g(2)(0) as low as 2%) from a cavity-free, nonresonantly excited single 6.6 nm CsPbI3 QDs, showcasing the great potential of CsPbX3 QDs as room-temperature highly pure single-photon sources for quantum technologies.ISSN:1530-6984ISSN:1530-699

Intrinsic formamidinium tin iodide nanocrystals by suppressing the Sn(IV) impurities

International audienceLead halide perovskites successfully advance towards applications in solar cells, light-emitting devices, and high-energy radiation detectors. Recent progress in understanding their uniqueness highlights the role of optoelectronic tolerance to intrinsic defects, particularly long diffusion lengths of carriers, and highly dynamic 3d inorganic framework. This picture indicates that finding an analogous material among non-group-14 metal halides can be very challenging, if possible at all. On the other hand, Sn (II) iodide perovskites exhibit comparably good performance in photovoltaics when synthesized with a low number of trap states. The main challenge with this material originates from the easiness of the trap states generation, which are typically ascribed to the oxidation of Sn(II) to Sn(IV). In this work, we describe the synthesis of colloidal monodisperse FASnI3 NCs, wherein thorough care on the purity of precursors and redox chemistry reduces the concentration of Sn(IV) to an insignificant level, to probe the intrinsic structural and optical properties of these NCs

Size- and Temperature-Dependent Lattice Anisotropy and Structural Distortion in CsPbBr₃ Quantum Dots by Reciprocal Space X-ray Total Scattering Analysis

Lead halide perovskite nanocrystals (NCs) have emerged as next-generation semiconductors capable of unifying superior photoemission properties, facile and inexpensive preparation, compositional and structural versatility. Among them, CsPbBr₃ is a model system in theoretical and experimental studies owing to its intrinsic chemical stability. Nonetheless, knowledge of the precise magnitude and the size- and temperature-dependent lattice and structural distortions is lacking, and the static/dynamic nature of disorder in NCs remains an open question. Herein, robust reciprocal space X-ray total scattering analysis is applied and accurate lattice distortions, Pb-Br bond distances, and Pb-Br-Pb angles versus NCs size are extracted. The lattice anisotropy increases upon expansion on downsizing while, upon contraction on cooling, the lattice distortion behaves differently at intermediate (9 nm) and ultrasmall (5 nm) sizes and from the bulk. Bond distances (stretched by ≈1%) do not show any size dependence, whereas equatorial and axial angles denote more symmetric octahedral arrangements in the smallest sizes, where they differ by ≈2° compared to ≈8° in the bulk. Anomalously high atomic displacement parameters of axial bromine ions persisting down to cryogenic temperatures suggest statically disordered octahedral tilts. These results provide insights having important implications on size-dependent emission properties and the exciton fine structure.ISSN:2688-406