Ji Hoon Shim

Peierls distortion as a route to high thermoelectric performance in In4Se3―δ crystals

Thermoelectric energy harvesting—the transformation of waste heat into useful electricity—is of great interest for energy sustainability. The main obstacle is the low thermoelectric efficiency of materials for converting heat to electricity, quantified by the thermoelectric figure of merit, ZT. The best available n-type materials for use in mid-temperature (500–900 K) thermoelectric generators have a relatively low ZT of 1 or less, and so there is much interest in finding avenues for increasing this figure of merit. Here we report a binary crystalline n-type material, In4Se3-δ, which achieves the ZT value of 1.48 at 705 K—very high for a bulk material. Using high-resolution transmission electron microscopy, electron diffraction, and first-principles calculations, we demonstrate that this material supports a charge density wave instability which is responsible for the large anisotropy observed in the electric and thermal transport. The high ZT value is the result of the high Seebeck coefficient and the low thermal conductivity in the plane of the charge density wave. Our results suggest a new direction in the search for high-performance thermoelectric materials, exploiting intrinsic nanostructural bulk properties induced by charge density waves.

Correlated Electronic Structure of LaO1 xFxFeAs

We compute the electronic structure, momentum resolved spectral function and optical conductivity of the new superconductor LaO1-xFxFeAs within the combination of the density functional theory and dynamical mean field theory. We find that the compound in the normal state is a strongly correlated metal and the parent compound is a bad metal at the verge of the metal insulator transition. We argue that the superconductivity is not phonon mediated.

Correlated electronic structure of LaOFeAs

We compute the electronic structure, momentum resolved spectral function and optical conductivity of the new superconductor LaO1-xFxFeAs within the combination of the density functional theory and dynamical mean field theory. We find that the compound in the normal state is a strongly correlated metal and the parent compound is a bad metal at the verge of the metal insulator transition. We argue that the superconductivity is not phonon mediated.

Fluctuating valence in a correlated solid and the anomalous properties of δ-plutonium

Plutonium displays phase transitions with enormous volume differences among its phases and both its Pauli like magnetic susceptibility and resistivity are an order of magnitude larger than those of simple metals. Curium is also highly resistive but its susceptibility is Curie-like at high temperatures and orders antiferromagnetically at low temperatures. The anomalous properties of the late actinides stem from the competition between the itinerancy and localization of its f electrons, which makes the late actinides elemental strongly correlated materials. A central problem in this field is to understand the mechanism by which these materials resolve these conflicting tendencies. In this letter we identify the electronic mechanisms responsible for the anomalous behaviour of late actinides. We revisit the concept of valence using theoretical approach that treats magnetism, Kondo screening, atomic multiplet effects, spin orbit coupling and crystal field splitting on the same footing. Plutonium is found to be in a rare mixed valent state, namely its ground state is a superposition of two distinct valencies. Curium settles in a single valence magnetically ordered state at low temperatures. The f7 atomic configuration of Curium is contrasted with the multiple configuration manifolds present in Plutonium ground state which we characterize by a valence histogram. The balance between the Kondo screening and magnetism is determined by the competition between spin orbit coupling and the strength of atomic multiplets which is in turn regulated by the degree of itinerancy. The approach presented here, highlights the electronic origin of the bonding anomalies in plutonium and can be applied to predict generalized valences and the presence or absence of magnetism in other compounds starting from first principles.Although the nuclear properties of the late actinides (plutonium, americium and curium) are fully understood and widely applied to energy generation, their solid-state properties do not fit within standard models and are the subject of active research. Plutonium displays phases with enormous volume differences, and both its Pauli-like magnetic susceptibility and resistivity are an order of magnitude larger than those of simple metals. Curium is also highly resistive, but its susceptibility is Curie-like at high temperatures and orders antiferromagnetically at low temperatures. The anomalous properties of the late actinides stem from the competition between itinerancy and localization of their f-shell electrons, which makes these elements strongly correlated materials. A central problem in this field is to understand the mechanism by which these conflicting tendencies are resolved in such materials. Here we identify the electronic mechanisms responsible for the anomalous behaviour of late actinides, revisiting the concept of valence using a theoretical approach that treats magnetism, Kondo screening, atomic multiplet effects and crystal field splitting on the same footing. We find that the ground state in plutonium is a quantum superposition of two distinct atomic valences, whereas curium settles into a magnetically ordered single valence state at low temperatures. The f7 configuration of curium is contrasted with the multiple valences of the plutonium ground state, which we characterize by a valence histogram. The balance between the Kondo screening and magnetism is controlled by the competition between spin–orbit coupling, the strength of atomic multiplets and the degree of itinerancy. Our approach highlights the electronic origin of the bonding anomalies in plutonium, and can be applied to predict generalized valences and the presence or absence of magnetism in other compounds starting from first principles.

Anisotropic Dirac fermions in a Bi square net of SrMnBi2.

We report the observation of highly anisotropic Dirac fermions in a Bi square net of SrMnBi(2), based on a first-principles calculation, angle-resolved photoemission spectroscopy, and quantum oscillations for high-quality single crystals. We found that the Dirac dispersion is generally induced in the (SrBi)(+) layer containing a double-sized Bi square net. In contrast to the commonly observed isotropic Dirac cone, the Dirac cone in SrMnBi(2) is highly anisotropic with a large momentum-dependent disparity of Fermi velocities of ~8. These findings demonstrate that a Bi square net, a common building block of various layered pnictides, provides a new platform that hosts highly anisotropic Dirac fermions.

Enhancement of the Thermoelectric Figure-of-Merit in a Wide Temperature Range in In4Se3–xCl0.03 Bulk Crystals

IO N Because of the increasing awareness of renewable energy issues, much attention has been devoted to thermoelectric energy harvesting technology. The dimensionless thermoelectric fi gureof-merit is defi ned by ZT = S 2 σ T/ κ , where S , σ , T , and κ are the Seebeck coeffi cient, electrical conductivity, absolute temperature, and thermal conductivity, respectively. Regarding a high ZT , it has long been sought both by lowering the thermal conductivity by exploiting the phonon-glass and electron-crystal concept [ 1–5 ] and by enhancing the power factor S 2 σ by utilizing the quantum confi nement effect [ 6 , 7 ] in low-dimensional nanostructured materials. Recently, we proposed that the charge density wave represents a new direction for high thermoelectric performance in bulk crystalline materials. [ 8 , 9 ] Low-dimensional electronic transport with strong electron–phonon coupling breaks the translational symmetry of the lattice because of the energy instability in a high-symmetry crystalline lattice. [ 10 ] The lattice dimerization along the electronic transport plane lowers the lattice thermal conductivity as a result of lowering of the phonon energy. Through quasi one-dimensional lattice distortion (Peierls distortion) in In 4 Se 3– x bulk single crystals, we achieved a high ZT of 1.48 at 705 K. [ 9 ] However, two challenges remain for practical applications. Firstly, the reported ZT could be increased further if we could increase the carrier concentration of the In 4 Se 3– x crystals because it is far from the carrier concentration of a heavily doped semiconductor (on the order of 10 19 cm − 3 ) that is generally considered to be optimal for thermoelectric materials. Secondly, ZT decreases signifi cantly as the temperature decreases, which limits the operational temperature range to within 350 –430 ° C. [ 9 ] Here, we report a signifi cant increase in ZT (maximum ZT ( ZT max ) = 1.53) over a wide temperature range in chlorine-doped In 4 Se 3– x Cl 0.03

Modeling the Localized-to-Itinerant Electronic Transition in the Heavy Fermion System CeIrIn5

We address the fundamental question of crossover from the localized to the itinerant state of a paradigmatic heavy fermion material: CeIrIn5. The temperature evolution of the one-electron spectra and the optical conductivity are predicted from first-principles calculation. The buildup of coherence in the form of a dispersive many-body feature is followed in detail, and its effects on the conduction electrons of the material are revealed. We find multiple hybridization gaps and link them to the crystal structure of the material. Our theoretical approach explains the multiple peak structures observed in optical experiments and the sensitivity of CeIrIn5 to substitutions of the transition metal element and may provide a microscopic basis for the more phenomenological descriptions currently used to interpret experiments in heavy fermion systems.

Interlayer orientation-dependent light absorption and emission in monolayer semiconductor stacks

Two-dimensional stacks of dissimilar hexagonal monolayers exhibit unusual electronic, photonic and photovoltaic responses that arise from substantial interlayer excitations. Interband excitation phenomena in individual hexagonal monolayer occur in states at band edges (valleys) in the hexagonal momentum space; therefore, low-energy interlayer excitation in the hexagonal monolayer stacks can be directed by the two-dimensional rotational degree of each monolayer crystal. However, this rotation-dependent excitation is largely unknown, due to lack in control over the relative monolayer rotations, thereby leading to momentum-mismatched interlayer excitations. Here, we report that light absorption and emission in MoS2/WS2 monolayer stacks can be tunable from indirect- to direct-gap transitions in both spectral and dynamic characteristics, when the constituent monolayer crystals are coherently stacked without in-plane rotation misfit. Our study suggests that the interlayer rotational attributes determine tunable interlayer excitation as a new set of basis for investigating optical phenomena in a two-dimensional hexagonal monolayer system.

Density functional calculations of electronic structure and magnetic properties of the hydrocarbon K 3 picene superconductor near the metal-insulator transition

We have investigated the electronic structures and magnetic properties of a newly discovered hydrocarbon superconductor,

Anisotropic Dirac electronic structures of A MnBi 2 ( A = Sr ,Ca)

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