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1. Ultrafast photoinduced band splitting and carrier dynamics in chiral tellurium nanosheets

   https://doi.org/10.1038/s41467-020-17766-5  

   Jnawali, Giriraj ; Xiang, Yuan ; Linser, Samuel M. ; Shojaei, Iraj Abbasian ; Wang, Ruoxing ; Qiu, Gang ; Lian, Chao ; Wong, Bryan M. ; Wu, Wenzhuo ; Ye, Peide D. ; et al ( August 2020 , Nature Communications)

   Trigonal tellurium (Te) is a chiral semiconductor that lacks both mirror and inversion symmetries, resulting in complex band structures with Weyl crossings and unique spin textures. Detailed time-resolved polarized reflectance spectroscopy is used to investigate its band structure and carrier dynamics. The polarized transient spectra reveal optical transitions between the uppermost spin-splitH₄andH₅and the degenerateH₆valence bands (VB) and the lowest degenerateH₆conduction band (CB) as well as a higher energy transition at the L-point. Surprisingly, the degeneracy of theH₆CB (a proposed Weyl node) is lifted and the spin-split VB gap is reduced upon photoexcitation before relaxing to equilibrium as the carriers decay. Using ab initio density functional theory (DFT) calculations, we conclude that the dynamic band structure is caused by a photoinduced shear strain in the Te film that breaks the screw symmetry of the crystal. The band-edge anisotropy is also reflected in the hot carrier decay rate, which is a factor of two slower along the c-axis than perpendicular to it. The majority of photoexcited carriers near the band-edge are seen to recombine within 30 ps while higher lying transitions observed near 1.2 eV appear to have substantially longer lifetimes, potentially due to contributions of intervalley processes in the recombination rate. These newmore »findings shed light on the strong correlation between photoinduced carriers and electronic structure in anisotropic crystals, which opens a potential pathway for designing novel Te-based devices that take advantage of the topological structures as well as strong spin-related properties.

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2. Mixed phononic and non-phononic transport in hybrid lead halide perovskites: glass-crystal duality, dynamical disorder, and anharmonicity

   https://doi.org/10.1039/C8EE02820F  

   Zhu, Taishan ; Ertekin, Elif ( January 2019 , Energy & Environmental Science)

   In hybrid materials, a high-symmetry lattice is decorated by low-symmetry building blocks. The result is an aperiodic solid that hosts many nearly-degenerate disordered configurations. Using the perovskite methylammonium lead iodide (MAPbI 3 ) as a prototype hybrid material, we show that the inherent disorder renders the conventional phonon picture of transport insufficient. Ab initio molecular dynamics and analysis of the spectral energy density reveal that vibrational carriers simultaneously exhibit features of both classical phonons and of carriers typically found in glasses. The low frequency modes retain elements of acoustic waves but exhibit extremely short lifetimes of only a few tens of picoseconds. For higher frequency modes, strong scattering due to rapid motion and reconfiguration of the organic cation molecules induces a loss of definition of the wave vector. Lattice dynamics shows that these carriers are more akin to diffusons – the nonwave carriers in vitreous materials – and are the dominant contributors to thermal conduction near room temperature. To unify the framework of glassy diffusons with that of phonons scattered at the ultimate limit, three-phonon interactions resolved from first-principles expose anharmonic effects two orders of magnitude higher than in silicon. The dominant anharmonic interactions occur within modes of the PbImore »6 octahedral framework itself, as well as between modes of the octahedral framework and modes localized to the MA molecules. The former arises from long-range interactions due to resonant bonding, and the latter from polar rotor scattering of the MA molecules. This establishes a clear microscopic connection between symmetry-breaking, dynamical disorder, anharmonicity, and the loss of wave nature in MAPbI 3 .« less
3. Shell model results for nuclear β−-decay properties of sd-shell nuclei

   https://doi.org/10.1093/ptep/ptaa012  

   Kumar, Anil ; Srivastava, Praveen C ; Suzuki, Toshio ( March 2020 , Progress of Theoretical and Experimental Physics)

   Abstract We evaluate the allowed $\beta^-$-decay properties of nuclei with $Z = 8$–$15$ systematically under the framework of the nuclear shell model using the valence space Hamiltonians derived from modern ab initio methods, such as in-medium similarity renormalization group and coupled-cluster theory. For comparison we also show results obtained with fitted interaction derived from chiral effective field theory and phenomenological universal $sd$-shell Hamiltonian version B interaction. We have performed calculations for O $\rightarrow$ F, F $\rightarrow$ Ne, Ne $\rightarrow$ Na, Na $\rightarrow$ Mg, Mg $\rightarrow$ Al, Al $\rightarrow$ Si, Si $\rightarrow$ P, and P $\rightarrow$ S transitions. Theoretical results for $B(GT)$, $\log ft$ values, and half-lives are discussed and compared with the available experimental data.
4. Pressure dependence of direct optical transitions in ReS2 and ReSe2

   https://doi.org/10.1038/s41699-019-0102-x  

   Oliva, Robert ; Laurien, Magdalena ; Dybala, Filip ; Kopaczek, Jan ; Qin, Ying ; Tongay, Sefaattin ; Rubel, Oleg ; Kudrawiec, Robert ( May 2019 , npj 2D Materials and Applications)

   The ReX₂system (X = S, Se) exhibits unique properties that differ from other transition metal dichalcogenides. Remarkably, its reduced crystal symmetry results in a complex electronic band structure that confers this material in-plane anisotropic properties. In addition, multilayered ReX₂presents a strong 2D character even in its bulk form. To fully understand the interlayer interaction in this system, it is necessary to obtain an accurate picture of the electronic band structure. Here, we present an experimental and theoretical study of the electronic band structure of ReS₂and ReSe₂at high-hydrostatic pressures. The experiments are performed by photoreflectance spectroscopy and are analyzed in terms of ab initio calculations within the density functional theory. Experimental pressure coefficients for the two most dominant excitonic transitions are obtained and compared with those predicted by the calculations. We assign the transitions to the Zk-point of the Brillouin zone and otherk-points located away from high-symmetry points. The origin of the pressure coefficients of the measured direct transitions is discussed in terms of orbital analysis of the electronic structure and van der Waals interlayer interaction. The anisotropic optical properties are studied at high pressure by means of polarization-resolved photoreflectance measurements.
5. Molecular Dynamics Simulations on Relaxed Reduced-DimensionalPotential Energy Surfaces

   Lui, C. ( April 2019 , The journal of physical chemistry. A.)

   Molecular dynamics (MD) simulations with full-dimensional potential energy surfaces (PESs) obtained from high-level ab initio calculations are frequently used to model reaction dynamics of small molecules (i.e., molecules with up to 10 atoms). Construction of full-dimensional PESs for larger molecules is, however, not feasible since the number of ab initio calculations required grows rapidly with the increase of dimension. Only a small number of coordinates are often essential for describing the reactivity of even very large systems, and reduced-dimensional PESs with these coordinates can be built for reaction dynamics studies. While analytical methods based on transition-state theory framework are well established for analyzing the reduced-dimensionalPESs, MD simulation algorithms capable of generating trajectories on such surfaces are more rare. In this work, we present a new MD implementation that utilizes the relaxed reduced-dimensional PES for standard micro canonical (NVE) and canonical (NVT) MD simulations.The method is applied to the pyramidal inversion of a NH3molecule. The results from the MD simulations on a reduced, three-dimensional PES are validated against the ab initio MD simulations, as well as MD simulations on full-dimensional PES and experimental data.