arXiv subjects

Jiawang Hong

Publications and source records attributed to Jiawang Hong.

At least 37 records · Page 2Linked to original sources

arXiv2020

Orbital-Energy Splitting in Anion Ordered Ruddlesden-Popper Halide Perovskites for Tunable Optoelectronic Applications

The electronic orbital characteristics at the band edges plays an important role in determining the electrical, optical and defect properties of perovskite photovoltaic materials. It is highly desirable to establish the relationship between the underlying atomic orbitals and the optoelectronic properties as a guide to maximize the photovoltaic performance. Here, using first-principles calculations and taking anion ordered Ruddlesden-Popper (RP) phase halide perovskites Cs$_{n+1}$Ge$_n$I$_{n+1}$Cl$_{2n}$ as an example, we demonstrate how to rationally optimize the optoelectronic properties (e.g., band gap, transition dipole matrix elements, carrier effective masses, band width) through a simple band structure parameter. Our results show that reducing the splitting energy $|Δc|$ of p orbitals of B-site atom can effectively reduce the band gap and carrier effective masses while greatly improving the optical absorption in the visible region. Thereby, the orbital-property relationship with $Δc$ is well established through biaxial compressive strain. Finally, it is shown that this approach can be reasonably extended to several other non-cubic halide perovskites with similar p orbitals characteristics at the conduction band edges. Therefore, we believe that our proposed orbital engineering approach provides atomic-level guidance for understanding and optimizing the device performance of layered perovskite solar cells.

cond-mat.mtrl-sci↗

arXiv2020

Conductive Domain Walls in Non-Oxide Ferroelectrics Sn2P2S6

The conductive domain wall (CDW) is extensively investigated in ferroelectrics, which can be considered as a quasi-two-dimensional reconfigurable conducting channel embedded into an insulating material. Therefore, it is highly important for the application of ferroelectric nanoelectronics. Hitherto, most CDW investigations are restricted in oxides, and limited work has been reported in non-oxides to the contrary. Here, by successfully synthesizing the non-oxide ferroelectric Sn2P2S6 single crystal, we observed and confirmed the domain wall conductivity by using different scanning probe techniques which origins from the nature of inclined domain walls. Moreover, the domains separated by CDW also exhibit distinguishable electrical conductivity due to the interfacial polarization charge with opposite signs. The result provides a novel platform for understanding electrical conductivity behavior of the domains and domain walls in non-oxide ferroelectrics.

cond-mat.mtrl-sci↗

arXiv2020

Domain evolution in bended freestanding BaTiO3 ultrathin films: a phase-field simulation

Perovskite ferroelectric oxides are usually considered to be brittle materials, however, recent work [Dong et al., Science 366, 475 (2019)] demonstrated the super-elasticity in the freestanding BaTiO3 thin films. This property may originate from the ferroelectric domain evolution during the bending, which is difficult to observe in experiments. Therefore, understanding the relation among the bending deformation, thickness of the films, and the domain dynamics is critical for their potential applications in flexible ferroelectric devices. Here, we reported the dynamics of ferroelectric polarization in the freestanding BaTiO3 ultrathin films in the presence of large bending deformation up to 40° using phase-field simulation. The ferroelectric domain evolution reveals the transition from the flux-closure to a/c domains with "vortex-like" structures, which caused by the increase of out-of-plane ferroelectric polarization. Additionally, by varying the film thickness in the identical bending situation, we found the a/c phase with "vortex-like" structure emerges only as the film thickness reached 12 nm or higher. Results from our investigations provide instructive information for the microstructure evolution of bending ferroelectric perovskite oxide films, which could serve as guide for the future application of ferroelectric films on flexible electronic devices.

cond-mat.mtrl-sci↗

arXiv2020

Screening piezoelectricity in determination of flexoelectric coefficient at nanoscale

Piezoelectricity usually accompanies with flexoelectricity in polar materials which is the linear response of polarization to a strain gradient. Therefore, it is hard to eliminate piezoelectric effect in determination of pure flexoelectric response. In this work, we propose an analytical method to characterize the flexoelectric coefficient quantitatively at nanoscale in piezoelectric materials by screening piezoelectricity. Our results show that the flexoelectricity reduces the nanopillar stiffness while the piezoelectricity enhances it. With careful design of the shape of the nanopillars and measuring their stiffness difference, the flexoelectric coefficient can be obtained with the piezoelectric contribution eliminated completely. This approach avoids the measurement of electrical properties with dynamic load, which helps to reduce the challenge of flexoelectric measurement at nanoscale. Our work will be beneficial to quantitative characterization of flexoelectric properties and design of flexoelectric devices at nanoscale.

cond-mat.mtrl-sci↗

arXiv2020

Ferroelastic switching with van der Waals direction transformation in layered PdSe2 driven by uniaxial and shear strain

Uniaxial and biaxial strain approaches are usually implemented to switch the ferroelastic states, which play a key role in the application of the ferroics and shape memory materials. In this work, by using the first-principles calculations, we found not only uniaxial strain, but also shear strain can induce a novel ferroelastic switching, in which the van der Waals (vdW) layered direction rotates with the ferroelastic transition in layered bulk PdSe2. The shear strain induces ferroelastic switching with three times amplitude smaller than uniaxial strain. The novel three-states ferroelastic switching in layered PdSe2 also occurs under shear strain. Our result shows that the shear strain could be used as an effective approach for manipulating the functionalities of layered materials in potential device applications.

cond-mat.mtrl-sci↗

arXiv2020

Flexo-diffusion effect: the strong influence on lithium diffusion induced by strain gradient

Lithium ion batteries (LIBs) work under sophisticated external force field and its electrochemical properties could be modulated by strain. Owing to the electro-mechanical coupling, the change of micro-local-structures can greatly affect lithium (Li) diffusion rate in solid state electrolytes and electrode materials of LIBs. In this study, we find that strain gradient in bilayer graphene (BLG) significantly affects Li diffusion barrier, which is termed as the flexo-diffusion effect, through first-principles calculations. The Li diffusion barrier substantially decreases/increases under the positive/negative strain gradient, leading to the change of Li diffusion coefficient in several orders of magnitude at 300 K. Interestingly, the regulation effect of strain gradient is much more significant than that of uniform strain field, which can have a remarkable effect on the rate performance of batteries, with a considerable increase in the ionic conductivity and a slight change of the original material structure. Moreover, our ab initio molecular dynamics simulations (AIMD) show that the asymmetric distorted lattice structure provides a driving force for Li diffusion, resulting in oriented diffusion along the positive strain gradient direction. These findings could extend present LIBs technologies by introducing the novel strain gradient engineering.

cond-mat.mtrl-sci↗

arXiv2020

Strain gradient drives lithium dendrite growth from the atomic-scale simulations

Dendrite formation is a major obstacle, such as capacity loss and short circuit, to the next-generation high-energy-density lithium (Li) metal batteries. The development of successful Li dendrite mitigation strategies is impeded by an insufficient understanding of Li dendrite growth mechanisms. Li-plating-induced internal stress in Li metal and its effect on dendrite growth have been studied in previous models and experiments, while the underlying microcosmic mechanism is elusive. Here, we analyze the role of plating-induced stress in dendrite formation through first-principles calculations and ab initio molecular dynamics simulations. We show that the deposited Li forms a stable atomic nanofilm structure on copper (Cu) substrate. It is found that the adsorption energy of Li atoms increases from the Li-Cu interface to deposited Li surface, leading to more aggregated Li atoms at the interface. Compared to the pristine Li metal, the deposited Li in the early stage becomes compacted and suffers in-plane compressive stress. Interestingly, we find that there is a giant strain gradient distribution from the Li-Cu interface to deposited Li surface, which makes the deposited atoms adjacent to the Cu surface tend to press upwards with perturbation, causing the dendrite growth. This understanding provides an insight to the atomic-scale origin of Li dendrite growth and may be useful for suppressing the Li dendrite in the Li-metal-based rechargeable batteries.

cond-mat.mtrl-sci↗

arXiv2020

Structural Stability and Optoelectronic Properties of Tetragonal MAPbI3 under Strain

In recent years, organic-inorganic hybrid perovskites have attracted wide attention due to their excellent optoelectronic properties in the application of optoelectronic devices. In the manufacturing process of perovskite solar cells, perovskite films inevitably have residual stress caused by non-stoichiometry components and the external load. However, their effects on the structural stability and photovoltaic performance of perovskite solar cells are still not clear. In this work, we investigated the effects of external strain on the structural stability and optoelectronic properties of tetragonal MAPbI3 by using the first-principles calculations. We found that the migration barrier of I- ion increases in the presence of compressive strain and decreases with tensile strain, indicating that the compressive strain can enhance the structural stability of halide perovskites. In addition, the light absorption and electronic properties of MAPbI3 under compressive strain are also improved. The variations of the band gap under triaxial and biaxial strains are consistent within a certain range of strain, resulting from the fact that the band edge positions are mainly influenced by the Pb-I bond in the equatorial plane. Our results provide useful guidance for realizing the commercial applications of MAPbI3-based perovskite solar cells.

cond-mat.mtrl-sci↗

arXiv2019

Thickness-dependent in-plane polarization and structural phase transition in van der Waals Ferroelectric CuInP2S6

Van der Waals (vdW) layered materials have rather weaker interlayer bonding than the intra-layer bonding, therefore the exfoliation along the stacking direction enables the achievement of monolayer or few layers vdW materials with emerging novel physical properties and functionalities. The ferroelectricity in vdW materials recently attracts renewed interest for the potential use in high-density storage devices. As the thickness going thinner, the competition between the surface energy, depolarization field and interfacial chemical bonds may give rise to the modification of ferroelectricity and crystalline structure, which has limited investigations. In this work, combining the piezoresponse force microscope scanning, contact resonance imaging, we report the existence of the intrinsic in-plane polarization in vdW ferroelectrics CuInP2S6 (CIPS) single crystals, whereas below a critical thickness between 90-100 nm, the in-plane polarization disappears. The Young's modulus also shows an abrupt stiffness at the critical thickness. Based on the density functional theory calculations, we ascribe these behaviors to a structural phase transition from monoclinic to trigonal structure, which is further verified by transmission electron microscope technique. Taken together, these findings demonstrate the foundational importance of structural phase transition for enhancing the rich functionality and broad utility of vdW ferroelectrics.

cond-mat.mtrl-sci↗

arXiv2019

Anomalous lattice thermal conductivity in layered materials MNCl (M=Zr, Hf) driven by the lanthanide contraction

High performance thermoelectric devices requires materials with low lattice thermal conductivities. Many strategies, such as phonon engineering, have been made to reduce lattice thermal conductivity without simultaneously decrease of the charge transport performance. It is a simple and effective approach to use materials with heavy element to reduce the lattice thermal conductivity. Here, based on the first-principles calculations and phonon Boltzmann transport equations, we find the replacement of Zr with heavy element Hf in ZrNCl doesn't reduce the lattice thermal conductivity, instead, it surprisingly increases by about 4 times at 300K. This unusual lattice thermal conductivity is mainly attributed to the dramatic enhancement in phonon lifetimes in Hf compound, originating from the strong interatomic bonding due to lanthanide contraction. Our findings unveil the microscopic mechanisms of high thermal transport properties in materials with heavy element, providing an alternative strategy in materials design with low lattice thermal conductivity for thermoelectric applications such as power restoration and generation.

cond-mat.mtrl-sci↗

arXiv2019

Spontaneous photo-generated carrier separation of SnO/BiOX (X=Cl, Br, I) bilayer under visible light irradiation for water splitting

Alloying in 2D materials plays a more and more important role due to wide range bandgap tunability and integrating the advantages of HER and OER. Here, the novel bilayers of SnO/BiOX (X= Cl, Br and I) bilayer are constructed to integrate the advantages of narrow bandgap and separating photo-generated carriers. The bandgap of the bilayers can be tuned from 1.09 to 1.84 eV, remarkably improving the utilization of solar energy. The large difference in effective masses and built-in electric field effectively hamper the fast recombination of photo-generated carries, which highly enhances the photocatalytic efficiency. Besides that, the type-II band alignment guarantee the two half reactions could occur at different surfaces. Moreover, the optical absorption (the strong transition between band edges and high joint density of states) and band-edge level further confirm the SnO/BiOX (X= Cl and Br) bilayer is a promising candidate for overall water-splitting.

cond-mat.mtrl-sci↗

arXiv2019

Mechanical Properties of Formamidinium Halide Perovskites FABX3 (FA = CH(NH2)2; B = Pb, Sn; X = Br, I) From First-Principles

The mechanical properties of formamidinium halide perovskite FABX3(FA = CH(NH2)2; B = Pb, Sn; X = Br, I) were systematically investigated by using the first-principles calculations. Our results reveal that FABX3 perovskites possess excellent mechanical flexibility, ductility and strong anisotropy. It shows that the planar organic cation FA+ has an important effect on the mechanical properties of FABX3 perovskites. In addition, our results indicate that: (i) the moduli (bulk modulus B, Young's modulus E, and shear modulus G) of FABBr3 are larger than those of FABI3 for the same B atom and (ii) the moduli of FAPbX3 are larger than those of FASnX3 for the same halide atom. The reason of the two trends was demonstrated by carefully analyzing the bond strength between B and X atom based on the projected crystal orbital Hamilton population method.

cond-mat.mtrl-sci↗

arXiv2019

Lithium intercalation drives remarkable mechanical properties deterioration in bulk and single-layered phosphorus: A first-principles study

It is of critical importance to understand the mechanical properties change of electrode materials during lithium intercalation in the mechanical design of Li-ion batteries, for the purpose of the high reliability and safety in their applications. Here, we investigated the mechanical properties of both bulk and single layer phosphorus during the lithium intercalation process by using the first-principles calculations. Our results show that the Young's modulus of bulk and layered phosphorus strongly depends on the lithium intercalation. The mechanical bearing capacities, such as critical strain and stress, are significantly reduced by several times after lithium intercalation in both bulk and single layer phosphorus, which may reduce the reliability of Li-ion batteries. Our findings suggest that this remarkable mechanical properties deterioration during Li intercalation should be considered carefully in the mechanical design of Li-ion batteries, in order to keep they working reliably and safely in the charge-discharge process.

cond-mat.mtrl-sci↗

arXiv2019

Orbital Engineering in Three Dimensional Halide Perovskites towards Two Dimensional Properties with Strong Anisotropy

The discovery of double perovskites A2B(I)B(III)X6 (A=monovalent cation; B(I)/B(III) = metal cation; X = halogen) as Pb(II)-free alternatives has attracted widespread attention, making it possible to introduce d-block metal cations (e.g., d0 and d10) into halide perovskites. However, at present, there are quite limited insights into the underlying bonding orbitals for d-block metal cation-based halide perovskites. Here, we present an orbital engineering strategy to construct two-dimensional (2D) electronic structures in three-dimensional (3D) halide perovskites by rationally controlling the d orbitals of the metal cations to hybridize with the halide p orbitals. Taking Cs2Au(I)Au(III)I6 as an example, we demonstrate that the flat conduction band and valence band at the band edges can be achieved simultaneously by combining two metal cations with different d orbital configurations using the first-principles calculations. The predicted carrier mobilities show huge anisotropy along the in-plane and out-of-plane directions in Cs2Au(I)Au(III)I6, further confirming the 2D electronic properties. In addition, the anisotropic static dielectronic constants and Young's modulus are also observed. More importantly, it is found that Cs2Au(I)Au(III)I6 has excellent mechanical flexible and an ultra-small shear modulus among halide perovskites. Our work provides valuable guidance for achieving low-dimensional electronic characteristic in three-dimensional halide perovskites for novel electronic applications.

cond-mat.mtrl-sci↗

arXiv2019

The coexistence of magnetism and ferroelectricity in 3d transition metal doped SnTe monolayer

The realization of multiferroicity in 2D nanomaterials is crucially important for designing advanced nanoelectronic devices such as non-volatile multistate data storage. In this work, the coexistence of ferromagnetism and ferroelectricity is reported in monolayer SnTe system by transition metal (TM) doping. Based on first-principles calculations, the spontaneous spin polarization could be realized by TM doping in ferroelectric SnTe monolayer. In addition to in-plane ferroelectric polarization, the out-of-plane ferroelectric polarization emerges in Mn (Fe)-doped SnTe monolayer due to the internal displacement of TM from the surface. Interestingly, the crystalline field centered on TM and interaction between the dopant and Te gradually enhanced with the increment of atomic number of doping elements, which explains why the formation energy decreases. The realization of multiferroics in SnTe monolayer could provide theoretical guidance for experimental preparation of low-dimensional multiferroic materials.

cond-mat.mtrl-sci↗

arXiv2019

First-principles study of the structural, electronic, magnetic and ferroelectric properties of a charge ordered Iron(II)- Iron(III) formate framework

Density functional theory calculations have been performed for the structural, electronic, magnetic and ferroelectric properties of a mixed-valence Fe(II)-Fe(III) formate framework [NH$_2$(CH$_3$)$_2$][Fe$^{\rm III}$Fe$^{\rm II}$(HCOO)$_6$] (DMAFeFe). Recent experiments report a spontaneous electric polarization and our calculations are in agreement with the reported experimental value. Furthermore, we shed light into the microscopic mechanism leading to the observed value and as well how to possibly enhanced the polarization. The interplay between charge ordering, dipolar ordering of DMA$^+$ cations and the induced structural distortions suggest new interesting directions to explore in these complex multifunctional hybrid perovskites.

cond-mat.mtrl-sci↗

arXiv2019

Frustrated Magnetism in Mott Insulating (V$_{1-x}$Cr$_x$)$_2$O$_3$

V2O3 famously features all four combinations of paramagnetic vs antiferromagnetic, and metallic vs insulating states of matter in response to %-level doping, pressure in the GPa range, and temperature below 300 K. Using time-of-flight neutron spectroscopy combined with density functional theory calculations of magnetic interactions, we have mapped and analyzed the inelastic magnetic neutron scattering cross section over a wide range of energy and momentum transfer in the chromium stabilized antiferromagnetic and paramagnetic insulating phases (AFI & PI). Our results reveal an important magnetic frustration and degeneracy of the PI phase which is relieved by the rhombohedral to monoclinic transition at $T_N=185$ K due to a significant magneto-elastic coupling. This leads to the recognition that magnetic frustration is an inherent property of the paramagnetic phase in $\rm (V_{1-x}Cr_x)_2O_3$ and plays a key role in suppressing the magnetic long range ordering temperature and exposing a large phase space for the paramagnetic Mott metal-insulator transition to occur.

cond-mat.str-el↗

arXiv2018

High Curie temperature half metallic 2D M2Se3 (M = Co, Ni, and Pd) monolayers with superior mechanical flexibility

Pursuing two-dimensional (2D) intrinsic ferromagnetism with high Curie temperature and great mechanical flexibility has attracted great interest in flexible spintronics. In the present work, we carried out a density functional theory (DFT) investigation on the 2D M2Se3 (M=Co, Ni and Pd) monolayers to understand their structural stabilities, electronic, magnetic and mechanical properties. Our results show that the Co2Se3 monolayer exhibits a fascinating half-metallic ferromagnetism with high Curie temperature (>700K). In addition, due to their unique buckling hinge-like structure, M2Se3 monolayers possess the large out-of-plane negative Poisson's ratio (NPR) and superior mechanical flexibility evidenced by their unusual critical strain two times greater than the well-known 2D materials. These findings imply that 2D M2Se3 family is the promising materials for the applications in the flexible and high-density spintronic nanodevices.

cond-mat.mtrl-sci↗