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Register a new userVibrational coherent control of localized d-d electronic excitation
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Added by
Alexandre Marciniak
Publication date
2020
fields
Physics
and research's language is
English
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Addressing the role of quantum coherence in the interplay between the different matter constituents (electrons, phonons and spin) is a critical step towards understanding transition metal oxides and design complex materials with new functionalities. Here we use coherent vibrational control of onsite d-d electronic transitions in a model edge-sharing insulating transition metal oxide (CuGeO3) to single-out the effects of vibrational coherence in electron-phonon coupling. By comparing time domain experiments based on high and low frequency ultrashort pumps with a fully quantum description of phonon assisted absorption, we could distinguish the processes associated to incoherent thermal lattice fluctuations from those driven by the coherent motion of the atoms. In particular, while thermal fluctuation of the phonon bath uniformly increases the electronic absorption, the resonant excitation of phonon modes results also in light-induced transparency which is coherently controlled by the vibrational motion.
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We review existing manifestations and prospects for ferroelectricity in electronically and optically active carbon-based materials. The focus point is the proposal for the electronic ferroelectricity in conjugated polymers from the family of substituted polyacetylenes. The attractive feature of synthetic organic ferroelectrics is a very high polarizability coming from redistribution of the electronic density, rather than from conventional displacements of ions. Next fortunate peculiarity is the symmetry determined predictable design of perspective materials. The macroscopic electric polarization follows ultimately from combination of two types of a microscopic symmetry breaking which are ubiquitous to qusi-1D electronic systems. The state supports anomalous quasi-particles - microscopic solitons, carrying non-integer electric charges, which here play the role of nano-scale nucleus of ferroelectric domain walls. Their spectroscopic features in optics can interfere with low-frequency ferroelectric repolarization providing new accesses and applications. In addition to already existing electronic ferroelectricity in organic crystals and donor-acceptor chains, we point to a class of conducting polymers and may be also to nano-ribbons of the graphene where such a state can be found. These proposals may lead to potential applications in modern intensive searches of carbon ferroelectrics.
We have measured the specific heat of zincblende ZnS for several isotopic compositions and over a broad temperature range (3 to 1100 K). We have compared these results with calculations based on ab initio electronic band structures, performed using both LDA and GGA exchange- correlation functionals. We have compared the lattice dynamics obtained in this manner with experimental data and have calculated the one-phonon and two-phonon densities of states. We have also calculated mode Grueneisen parameters at a number of high symmetry points of the Brillouin zone. The electronic part of our calculations has been used to investigate the effect of the 3d core electrons of zinc on the spin-orbit splitting of the top valence bands. The effect of these core electrons on the band structure of the rock salt modification of ZnS is also discussed.
We report ab initio calculations of the electronic band structure and the phonon dispersion relations of the zincblende-type mercury chalcogenides (beta-HgS, HgSe, and HgTe). The latter have been used to evaluate the temperature dependence of the specific heat which has been compared with experimental data. The electronic band structure of these materials has been confirmed to have an inverted direct gap of the alpha-tin type, which makes HgSe and HgTe semimetallic. For beta-HgS, however, our calculations predict a negative spin-orbit splitting which restores semiconducting properties to the material in spite of the inverted gap. We have calculated the spin-orbit induced linear terms in k which appear at the Gamma_8 valence bands. We have also investigated the pressure dependence of the crystal structure and the phonons.
The coherence of collective modes, such as phonons, and their modulation of the electronic states are long sought in complex systems, which is a cross-cutting issue in photovoltaics and quantum electronics. In photovoltaic cells and lasers based on metal halide perovskites, the presence of polaronic coupling, i.e., photocarriers dressed by the macroscopic motion of charged lattice, assisted by terahertz (THz) longitudinal optical (LO) phonons, has been intensely studied yet still debated. This may be key for explaining the remarkable properties of the perovskite materials, e.g., defect tolerance, long charge lifetimes and diffusion length. Here we use the intense single-cycle THz pulse with the peak electric field up to $E_{THz}=$1000,kV/cm to drive coherent band-edge oscillations at room temperature in CH$_3$NH$_3$PbI$_3$. We reveal the oscillatory behavior dominantly to a specific quantized lattice vibration mode at $omega_{mathrm{LO}}sim$4 THz, being both dipole and momentum forbidden. THz-driven coherent dynamics exhibits distinguishing features: the room temperature coherent oscillations at $omega_{mathrm{LO}}$ longer than 1 ps in both single crystals and thin films; the {em mode-selective} modulation of different band edge states assisted by electron-phonon ($e$-$ph$) interaction; {em dynamic mode splitting} controlled by temperature due to entropy and anharmonicity of organic cations. Our results demonstrate intense THz-driven coherent band-edge modulation as a powerful probe of electron-lattice coupling phenomena and provide compelling implications for polaron correlations in perovskites.
We report the synthesis and properties of two new insulating phases of SrFeO3-d with introduction of oxygen deficiencies in metallic SrFeO3 ; one with 0.15 < d < 0.19 (sample A)and the other above d = 0.19 (sample B). Sample A shows large negative magnetoresistance around the charged ordering (CO) temperature with magnetic anomalies seen in the temperature dependent resistivity,magnetization and M-H hysteresis loops. Sample B shows a smooth insulating behavior with no thermal hysteresis in the resistivity and with a small positive magnetoresistance. cac and cdc show multiple features associated with a frustrated magnetic order (helical) due to competing ferro- and antiferromagnetic interactions. The competing effects of ferro- and antiferromagnetic phases extend up to T ~ 230 K revealing a new high temperature scale in this system. These observations are discussed in the context of magnetic interactions associated with the varying Fe4+/Fe3+ ratio.
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