Showing papers by "S. Shahab Naghavi published in 2018"
TL;DR: In this article, the authors show that the anharmonicity and soft phonon modes associated with covalently bonded [Se2]2− dimers lead to ultralow lattice thermal conductivities in Pd2Se3 monolayers (1.5 and 2.9 W m−1 K−1 along the a- and b-axes at 300 K, respectively), which are comparable to those of high performance bulk thermoelectric materials such as PbTe.
Abstract: A high power factor and low lattice thermal conductivity are two essential ingredients of highly efficient thermoelectric materials. Although monolayers of transition-metal dichalcogenides possess high power factors, high lattice thermal conductivities significantly impede their practical applications. Our first-principles calculations show that these two ingredients are well fulfilled in the recently synthesized Pd2Se3 monolayer, whose crystal structure is composed of [Se2]2– dimers, Se2– anions, and Pd2+ cations coordinated in a square-planar manner. Our detailed analysis of third-order interatomic force constants reveals that the anharmonicity and soft phonon modes associated with covalently bonded [Se2]2– dimers lead to ultralow lattice thermal conductivities in Pd2Se3 monolayers (1.5 and 2.9 W m–1 K–1 along the a- and b-axes at 300 K, respectively), which are comparable to those of high-performance bulk thermoelectric materials such as PbTe. Moreover, the “pudding-mold” type band structure, caused by...
100 citations
TL;DR: LiMgSnPd (F43m, No. 216) is a quaternary Heusler semiconductor with band gaps in the range of 0.3 to 2.5 eV as discussed by the authors.
Abstract: Intermetallic compounds with sizable band gaps are attractive for their unusual properties but rare. Here, we present a new family of stable semiconducting quaternary Heusler compounds, designed based on the 18-electron rule and discovered by means of high-throughput ab initio calculations based on the 18-electron rule. The 99 new semiconductors reported here adopt the ordered quaternary Heusler structure with the prototype of LiMgSnPd (F43m, No. 216) and contain 18 valence electrons per formula unit. They are realized by filling the void in the half Heusler structure with a small and electropositive atom, i.e., lithium. These new stable quaternary Heusler semiconductors possess band gaps in the range of 0.3 to 2.5 eV, and exhibit some unusual properties different from conventional semiconductors, such as strong optical absorption, giant dielectric screening, and high Seebeck coefficient, which suggest these semiconductors have potential applications as photovoltaic and thermoelectric materials. While th...
58 citations
TL;DR: Two high-performance full-Heusler thermoelectric compounds with high intrinsic band degeneracy are identified, Li2TlBi and Li2InBi, which have exceptionally high power factors and low lattice thermal conductivities at room temperature.
Abstract: Improving the figure of merit $zT$ of thermoelectric materials requires simultaneously a high power factor and low thermal conductivity. An effective approach for increasing the power factor is to align the band extremum and achieve high band degeneracy ($\geq$ 12) near the Fermi level as realized in PbTe [\textcolor{blue}{Pei et. al. \textit{Nature} 473, 66 (2010)}], which usually relies on band structure engineering, e.g., chemical doping and strain. However, very few materials could achieve such a high band degeneracy without heavy doping or suffering impractical strain. By employing state-of-the-art first-principles methods with direct computation of phonon and carrier lifetime, we demonstrate that two new full-Heusler compounds Li$_2$TlBi and Li$_2$InBi, possessing a PbTe-like electronic structure, show exceptionally high power factors ($\sim$ 20 mWm$^{-1}$K$^{-2}$ at 300 K) and low lattice thermal conductivities (2.36 and 1.55 Wm$^{-1}$K$^{-1}$) at room temperature. The Tl$^{+}$Bi$^{3-}$ (In$^{+}$Bi$^{3-}$) sublattice forms a rock-salt structure, and the additional two valence electrons from Li atoms essentially make these compounds isovalent with Pb$^{2+}$Te$^{2-}$. The larger rock-salt sublattice of TlBi (InBi) shifts the valence band maximum from L point to the middle of the $\Sigma$ line, increasing the band degeneracy from fourfold to twelvefold. On the other hand, resonance bond in the PbTe-like sublattice and soft Tl-Bi (In-Bi) bonding interaction is responsible for intrinsic low lattice thermal conductivities. Our results present a novel strategy of designing high-performance thermoelectric materials.
40 citations
TL;DR: Changing the π-conjugated linker at the acceptor site from ethylene linker to acetylene linkers further improves the light-harvesting ability of meso-β-porphyrin dyes, making them promising candidates for dye-sensitized solar cell application.
Abstract: Over the past decade, tremendous effort has been made to improve the light-harvesting ability of push–pull porphyrin dyes. Despite notable success achieved in this direction, push–pull porphyrin dyes still suffer from a poor light-harvesting efficiency owing to the lack of absorption between the Soret and Q-bands. To tackle this issue, here we design a series of push–pull porphyrin dyes with anchoring groups either at meso- or β-position using calculations based on first-principles time-dependent density functional theory. In contrast to the common perception, we find that porphyrin dyes bearing an electron-donor at the meso-position and an electron-acceptor at the β-position produce an additional extended band between the Soret and Q-bands appearing at around 500 nm due to S0 → S3 excitation, leading to a much higher light-harvesting performances compared to meso- and β-disubstituted ones. In addition, changing the π-conjugated linker at the acceptor site from ethylene linker (C═C) to acetylene linker (C...
23 citations
TL;DR: In this paper, the elastic constants and derived properties of tetragonal Heusler compounds were calculated using the high accuracy of the full-potential linearized augmented plane wave (FPLAPW) method.
Abstract: In the present work, the elastic constants and derived properties of tetragonal Heusler compounds were calculated using the high accuracy of the full-potential linearized augmented plane wave (FPLAPW) method. To find the criteria required for an accurate calculation, the consequences of increasing the numbers of k-points and plane waves on the convergence of the calculated elastic constants were explored. Once accurate elastic constants were calculated, elastic anisotropies, sound velocities, Debye temperatures, malleability, and other measurable physical properties were determined for the studied systems. The elastic properties suggested metallic bonding with intermediate malleability, between brittle and ductile, for the studied Heusler compounds. To address the effect of off-stoichiometry on the mechanical properties, the virtual crystal approximation (VCA) was used to calculate the elastic constants. The results indicated that an extreme correlation exists between the anisotropy ratio and the stoichiometry of the Heusler compounds, especially in the case of Ni2MnGa. Metastable cubic Ni2MnGa exhibits a very high anisotropy (≈28) and hypothetical cubic Rh2FeSn violates the Born-Huang stability criteria in the L21 structure. The bulk moduli of the investigated tetragonal compounds do not vary much (≈130 ...190 GPa). The averaged values of the other elastic moduli are also rather similar, however, rather large differences are found for the elastic anisotropies of the compounds. These are reflected in very different spatial distributions of Young’s moduli when comparing the different compounds. The slowness surfaces of the compounds also differ considerably even though the average sound velocities are in the same order of magnitude (3.2 ... 3.6 km/s). The results demonstrate the importance of the elastic properties not only for purely tetragonal Heusler compounds but also for phase change materials that exhibit magnetic shape memory or magnetocaloric effects.
23 citations
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TL;DR: LiMgSnPd (F$\bar{\mathbf{4}}$3m, No. as mentioned in this paper ) is a stable quaternary Heusler semiconductor with band gaps from 0.3 to 2.5
Abstract: Intermetallic compounds with sizable band gaps are attractive for their unusual properties but rare. Here, we present a new family of stable semiconducting quaternary Heusler compounds, designed and discovered by means of high-throughput \textit{ab initio} calculations based on the 18-electron rule. The 99 new semiconductors reported here adopt the ordered quaternary Heusler structure with the prototype of LiMgSnPd (F$\bar{\mathbf{4}}$3m, No.\,216) and contain 18 valence electrons per formula unit. They are realized by filling the void in the half Heusler structure with a small and electropositive atom, i.e., lithium. These new stable quaternary Heusler semiconductors possess a range of band gaps from 0.3 to 2.5\,eV, and exhibit some unusual properties different from conventional semiconductors, such as strong optical absorption, giant dielectric screening, and high Seebeck coefficient, which suggest these semiconductors have potential applications as photovoltaic and thermoelectric materials. While this study opens up avenues for further exploration of this novel class of semiconducting quaternary Heuslers, the design strategy used herein is broadly applicable across a potentially wide array of chemistries to discover new stable materials.
2 citations