Strong Closed-Shell Interactions in Inorganic Chemistry.

Lighting accounts for one-fifth of global electricity consumption1. Single materials with efficient and stable white-light emission are ideal for lighting applications, but photon emission covering the entire visible spectrum is difficult to achieve using a single material. Metal halide perovskites have outstanding emission properties2,3; however, the best-performing materials of this type contain lead and have unsatisfactory stability. Here we report a lead-free double perovskite that exhibits efficient and stable white-light emission via self-trapped excitons that originate from the Jahn–Teller distortion of the AgCl6 octahedron in the excited state. By alloying sodium cations into Cs2AgInCl6, we break the dark transition (the inversion-symmetry-induced parity-forbidden transition) by manipulating the parity of the wavefunction of the self-trapped exciton and reduce the electronic dimensionality of the semiconductor4. This leads to an increase in photoluminescence efficiency by three orders of magnitude compared to pure Cs2AgInCl6. The optimally alloyed Cs2(Ag0.60Na0.40)InCl6 with 0.04 per cent bismuth doping emits warm-white light with 86 ± 5 per cent quantum efficiency and works for over 1,000 hours. We anticipate that these results will stimulate research on single-emitter-based white-light-emitting phosphors and diodes for next-generation lighting and display technologies. After alloying with metal cations, a lead-free halide double perovskite shows stable performance and remarkably efficient white-light emission, with possible applications in lighting and display technologies.

Efficient and stable emission of warm-white light from lead-free halide double perovskites

The determination of the elastic properties of composite materials (multiphase aggregates, polycrystals, and porous or cracked solids) from the elastic properties of the components may be approached in several ways. The problem may be treated statistically, via scattering theory, through variational principles, or by the assumption of specific geometries for the material under consideration. Each of these methods is reviewed in turn. The widely used Voigt-Reuss-Hill average can be a poor approximation for both two-phase composites and polycrystals, and its replacement by the two Hashin-Shtrikman bounds is recommended. For pore-containing or crack-containing media, specific geometry models must be considered if useful results are to be obtained. If aggregate theory is used to estimate the moduli of individual components of a composite whose bulk properties are known, the shear moduli of the component phases must be matched (within a factor of 2 or 3) for the method to be useful. Results for nonlinear composites (which allow calculation of the pressure variation of aggregate moduli) have been obtained for only a few special cases.

The Elastic Properties of Composite Materials

Since approximately 1950 an increasing portion of experimental solid state physics research has been concerned with studying defects in crystals. This trend might appear to be a rather belated recognition that most of the materials we come into contact with have a random structure. In fact the theoretical understanding and controlled preparation of compounds with defects or random structure has been very slow in developing. The present paper examines and reviews our knowledge of the lattice vibrations associated with defects. The coverage is extremely broad, as shown by the table of contents. It includes localized and resonant modes of isolated defects as well as the modes in highly disordered mixed crystals and glasses. It is primarily a review of experimental work but theoretical results are included where the latter explain or predict significant features. In order to be self-contained several sections of the paper deal entirely with theoretical matters. There is a chapter on explicit solutions of the linear chain vibration problem and a short chapter on Green's function methods. The review emphasizes the infrared absorption and Raman scattering of defects. This is simply because other techniques have not yielded nearly so much information. Neutron scattering and electron tunneling are referred to only where they have shed light on certain systems. Extensive tables of defects and mode frequencies are included for each type of solid. The major solids which are reviewed include semiconductors, ionic compounds, organic compounds, and amorphous insulators.

Optical studies of the vibrational properties of disordered solids

The authors review the physics of ultrafast dynamics in semiconductors and their heterostructures, including both the observed experimental phenomena and the theoretical description of the processes. These are probed by ultrafast optical excitation, generating nonequilibrium states that can be monitored by time-resolved spectroscopy. Light pulses create coherent superpositions of states, and the dynamics of the associated phase relationships can be directly investigated by means of many-pulse experiments. The commonly used experimental techniques are briefly reviewed. A variety of different phenomena can be described within a common theoretical framework based on the density-matrix formalism. The important interactions of the carriers included in the theoretical description are the phonon interactions, the interactions with classical and quantum light fields, and the Coulomb interaction among the carriers themselves. These interactions give rise to a strong interplay between phase coherence and relaxation, which strongly affects the non equilibrium dynamics. Based on the general theory, the authors review the physical phenomena in various semiconductor structures including superlattices, quantum wells, quantum wires, and bulk media. Particular results which have played a central role in understanding the microscopic origins of the relaxation processes are discussed in detail.

Theory of ultrafast phenomena in photoexcited semiconductors

Coherent propagation of quadrupole polaritons in ${\mathrm{Cu}}_{2}$O is demonstrated by time-resolved spectroscopy. This manifests itself in a strong distortion of the temporal shape of a picosecond optical pulse which is in resonance with the 1S exciton polariton. Oscillations with time-dependent period in the transmitted light intensity are quantitatively explained as resulting from quantum beats between the two branches of the exciton polariton. The analysis yields the homogeneous linewidth and oscillator strength.

Coherent propagation and quantum beats of quadrupole polaritons in Cu2O.

Phonon dispersion in AgBr and exchange of the transverse mode Eigenvectors at L

Mise en evidence de l'apparition de battements quantiques pour un etat excitonique dans un solide. Ils sont observes en tant qu'oscillations du declin de la fluorescence assistee par le mode de phonon 2TO(L), pour les etats d'exciton libre indirects de AgBr, dans un champ magnetique apres excitation par un laser pulse a 1 picoseconde. Possibilite de determination de la decomposition des niveaux excitoniques

Observation of quantum beats in the resonance fluorescence of free excitons.

We report the first observation of quantum beats in the resonance fluorescence of a bound exciton in a semiconductor, the ionized-donor exciton complex in CdS. Measurements of the polarization behavior and magnetic-field dependence or the beats permitted a detailed investigation or strain effects and magneto-optical parameters of the states. From the damping of the beats, coherence times of the order of several hundreds of picoseconds are deduced. For the neutral-donor and -acceptor bound exciton states, very rapid dephasing with coherence times of the order or 20 ps is found

W. von der Osten

Papers

Coherent propagation and quantum beats of quadrupole polaritons in Cu2O.

Phonon dispersion in AgBr and exchange of the transverse mode Eigenvectors at L

Observation of quantum beats in the resonance fluorescence of free excitons.

Picosecond quantum-beat spectroscopy of bound excitons in CdS.

Exciton recombination in silver bromide