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  • 1.
    Filippov, Stanislav
    et al.
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten. Stockholm Univ, Sweden.
    Grinderslev, Jakob B.
    Aarhus Univ, Denmark.
    Andersson, Mikael S.
    Chalmers Univ Technol, Sweden.
    Armstrong, Jeff
    Rutherford Appleton Lab, England.
    Karlsson, Maths
    Chalmers Univ Technol, Sweden.
    Jensen, Torben R.
    Aarhus Univ, Denmark.
    Klarbring, Johan
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Simak, Sergey
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Haussermann, Ulrich
    Stockholm Univ, Sweden.
    Analysis of Dihydrogen Bonding in Ammonium Borohydride2019Ingår i: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 123, nr 47, s. 28631-28639Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    The structural and vibrational properties of ammonium borohydride, NH4BH4, have been examined by first-principles density functional theory (DFT) calculations and inelastic neutron scattering (INS). The H disordered crystal structure of NH4BH4 is composed of the tetrahedral complex ions NH4+ and BH4-, which are arranged as in the fcc NaCl structure and linked by intermolecular dihydrogen bonding. Upon cooling, the INS spectra revealed a structural transition between 45 and 40 K. The reversible transition occurs upon heating between 46 and 49 K. In the low-temperature form reorientational dynamics are frozen. The libration modes for BH4- and NH4+ are near 300 and 200 cm(-1), respectively. Upon entering the fcc high-temperature form, NH4+ ions attain fast reorientational dynamics, as indicated in the disappearance of the NH4+ libration band, whereas BH4- ions become significantly mobile only at temperatures above 100 K. The vibrational behavior of BH4- ions in NH4BH4 compares well to the heavier alkali metal borohydrides, NaBH4-CsBH4. DFT calculations revealed a nondirectional nature of the dihydrogen bonding in NH4BH4 with only weak tendency for long-range order. Different rotational configurations of complex ions appear quasi-degenerate, which is reminiscent of glasses.

  • 2.
    Filippov, Stanislav
    et al.
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten. Stockholm Univ, Sweden.
    Klarbring, Johan
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Haussermann, Ulrich
    Stockholm Univ, Sweden.
    Simak, Sergey
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Temperature-induced phase transition and Li self-diffusion in Li2C2: A first-principles study2019Ingår i: PHYSICAL REVIEW MATERIALS, ISSN 2475-9953, Vol. 3, nr 2, artikel-id 023602Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Lithium carbide, Li2C2, is a fascinating material that combines strong covalent and weak ionic bonding resulting in a wide range of unusual properties. The mechanism of its phase transition from the ground-state orthorhombic (Immm) to the high-temperature cubic (Fm (3) over barm) crystal structure is not well understood and here we elucidate it with help of first-principles calculations. We show that stabilization of the cubic phase is a result of a temperature-induced disorientation of the C-C dumbbells and their further thermal rotations. Due to these rotations rather large deviatoric stress, which is associated with the dumbbell alignment along one of the crystallographic axes, averages out making the cubic structure mechanically stable. At high temperature we observe a type-II superionic transition to a state of high Li self-diffusion involving collective ionic motion mediated by the formation of Frenkel pairs.

  • 3.
    Klarbring, Johan
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Low-energy paths for octahedral tilting in inorganic halide perovskites2019Ingår i: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 99, nr 10, artikel-id 104105Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Instabilities relating to cooperative octahedral tilting is common in materials with perovskite structures, in particular in the subclass of halide perovskites. In this work the energetics of octahedral tilting in the inorganic metal halide perovskites CsPbI3 and CsSnI3 are investigated using first-principles density functional theory calculations. Several low-energy paths between symmetry equivalent variants of the stable orthorhombic (Pnma) perovskite variant are identified and investigated. The results are in favor of the presence of dynamic disorder in the octahedral tilting phase transitions of inorganic halide perovskites. In particular, one specific type of path, corresponding to an out-of-phase "tilt switch," is found to have significantly lower energy barrier than the others, which indicates the existence of a temperature range where the dynamic fluctuations of the octahedra follow only this type of path. This could produce a time averaged structure corresponding to the intermediate tetragonal (P4/mbm) structure observed in experiments. Deficiencies of the commonly employed simple one-dimensional "double-well" potentials in describing the dynamics of the octahedra are pointed out and discussed.

  • 4.
    Klarbring, Johan
    et al.
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Simak, Sergey
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Nature of the octahedral tilting phase transitions in perovskites: A case study of CaMnO32018Ingår i: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 97, nr 2, artikel-id 024108Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    The temperature-induced antiferrodistortive (AFD) structural phase transitions in CaMnO3, a typical perovskite oxide, are studied using first-principles density functional theory calculations. These transitions are caused by tilting of the MnO6 octahedra that are related to unstable phonon modes in the high-symmetry cubic perovskite phase. Transitions due to octahedral tilting in perovskites normally are believed to fit into the standard soft-mode picture of displacive phase transitions. We calculate phonon-dispersion relations and potential-energy landscapes as functions of the unstable phonon modes and argue based on the results that the phase transitions are better described as being of order-disorder type. This means that the cubic phase emerges as a dynamical average when the system hops between local minima on the potential-energy surface. We then perform ab initio molecular dynamics simulations and find explicit evidence of the order-disorder dynamics in the system. Our conclusions are expected to be valid for other perovskite oxides, and we finally suggest how to predict the nature (displacive or order-disorder) of the AFD phase transitions in any perovskite system.

  • 5.
    Klarbring, Johan
    et al.
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Simak, Sergey
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Phase Stability of Dynamically Disordered Solids from First Principles2018Ingår i: Physical Review Letters, ISSN 0031-9007, E-ISSN 1079-7114, Vol. 121, nr 22, artikel-id 225702Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Theoretical studies of phase stability in solid materials with dynamic disorder are challenging due to the failure of the standard picture of atoms vibrating around fixed equilibrium positions. Dynamically disordered solid materials show immense potential in applications. In particular, superionic conductors, where the disorder results in exceptionally high ionic conductivity, are very promising as solid state electrolytes in batteries and fuel cells. The biggest obstacle in living up to this potential is the limited stability of the dynamically disordered phases. Here, we outline a method to obtain the free energy of a dynamically disordered solid. It is based on a stress-strain thermodynamic integration on a deformation path between a mechanically stable ordered variant of the disordered phase, and the dynamically disordered phase itself. We show that the large entropy contribution associated with the dynamic disorder is captured in the behavior of the stress along the deformation path. We apply the method to Bi2O3, whose superionic delta phase is the fastest known solid oxide ion conductor. We accurately reproduce the experimental transition enthalpy and the critical temperature of the phase transition from the low temperature ground state a phase to the superionic d phase. The method can be used for a first-principles description of the phase stability of superionic conductors and other materials with dynamic disorder, when the disordered phase can be connected to a stable phase through a continuous deformation path.

  • 6.
    Klarbring, Johan
    et al.
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Skorodumova, Natalia V.
    KTH Royal Inst Technol, Sweden; Uppsala Univ, Sweden.
    Simak, Sergey
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Finite-temperature lattice dynamics and superionic transition in ceria from first principles2018Ingår i: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 97, nr 10, artikel-id 104309Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Ab initio molecular dynamics (AIMD) in combination with the temperature dependent effective potential (TDEP) method has been used to go beyond the quasiharmonic approximation and study the lattice dynamics in ceria, CeO2, at finite temperature. The results indicate that the previously proposed connection between the B-1u phonon mode turning imaginary and the transition to the superionic phase in fluorite structured materials is an artifact of the failure of the quasiharmonic approximation in describing the lattice dynamics at elevated temperatures. We instead show that, in the TDEP picture, a phonon mode coupling to the E-u mode prevents the B-1u mode from becoming imaginary. We directly observe the superionic transition at high temperatures in our AIMD simulations and find that it is initiated by the formation of oxygen Frenkel pairs (FP). These FP are found to form in a collective process involving simultaneous motion of two oxygen ions.

  • 7.
    Klarbring, Johan
    et al.
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Vekilova, Olga Yu.
    KTH Royal Institute Technology, Sweden; Uppsala University, Sweden.
    Nilsson, Johan O.
    KTH Royal Institute Technology, Sweden.
    Skorodumova, Natalia V.
    KTH Royal Institute Technology, Sweden; Uppsala University, Sweden.
    Simak, Sergey
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Ionic conductivity in Sm-doped ceria from first-principles non-equilibrium molecular dynamics2016Ingår i: Solid State Ionics, ISSN 0167-2738, E-ISSN 1872-7689, Vol. 296, s. 47-53Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Sm-doped ceria is a prospective electrolyte material for intermediate-temperature solid-oxide fuel cells (IT-SOFC). Equilibrium ab initio molecular dynamics (AIMD) studies of oxygen ion diffusion in this material are currently impractical due to the rareness of diffusive events on the accessible timescale. To overcome this issue we have performed ab initio non-equilibrium molecular dynamics calculations of Sm-doped ceria using the color diffusion algorithm. Applying an external force field we have been able to increase the frequency of diffusive events over the simulation time, while keeping the physical mechanism of diffusion intact. We have investigated the temperature dependence of the maximum strength of the applied external field that could be used while maintaining the response of the system in a linear regime. This allows one to obtain the diffusivity at zero field. The bulk ionic conductivity has been calculated and found to match the experimental data well. We have also compared the description of the diffusion process by our method to previous findings and show that the migration mechanism and site preference of oxygen vacancies with respect to the Sm dopants is well reproduced. (C) 2016 Elsevier B.V. All rights reserved.

  • 8.
    Nilsson, Johan O.
    et al.
    KTH Royal Institute Technology, Sweden.
    Yu Vekilova, Olga
    KTH Royal Institute Technology, Sweden.
    Hellman, Olle
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Klarbring, Johan
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Simak, Sergey
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Skorodumova, Natalia V.
    KTH Royal Institute Technology, Sweden; Uppsala University, Sweden.
    Ionic conductivity in Gd-doped CeO2: Ab initio color-diffusion nonequilibrium molecular dynamics study2016Ingår i: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 93, nr 2, s. 024102-Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    A first-principles nonequilibrium molecular dynamics (NEMD) study employing the color-diffusion algorithm has been conducted to obtain the bulk ionic conductivity and the diffusion constant of gadolinium-doped cerium oxide (GDC) in the 850-1150 K temperature range. Being a slow process, ionic diffusion in solids usually requires simulation times that are prohibitively long for ab initio equilibrium molecular dynamics. The use of the color-diffusion algorithm allowed us to substantially speed up the oxygen-ion diffusion. The key parameters of the method, such as field direction and strength as well as color-charge distribution, have been investigated and their optimized values for the considered system have been determined. The calculated ionic conductivity and diffusion constants are in good agreement with available experimental data.

  • 9.
    Ning, Weihua
    et al.
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Biomolekylär och Organisk Elektronik. Linköpings universitet, Tekniska fakulteten. Nanjing Tech Univ, Peoples R China.
    Zhao, Xin-Gang
    Jilin Univ, Peoples R China.
    Klarbring, Johan
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Bai, Sai
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Biomolekylär och Organisk Elektronik. Linköpings universitet, Tekniska fakulteten.
    Ji, Fuxiang
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Biomolekylär och Organisk Elektronik. Linköpings universitet, Tekniska fakulteten.
    Wang, Feng
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Biomolekylär och Organisk Elektronik. Linköpings universitet, Tekniska fakulteten.
    Simak, Sergey
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Tao, Youtian
    Nanjing Tech Univ, Peoples R China.
    Ren, Xiao-Ming
    Nanjing Tech Univ, Peoples R China.
    Zhang, Lijun
    Jilin Univ, Peoples R China.
    Huang, Wei
    Nanjing Tech Univ, Peoples R China.
    Abrikosov, Igor
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten. Natl Univ Sci and Technol MISIS, Russia.
    Gao, Feng
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Biomolekylär och Organisk Elektronik. Linköpings universitet, Tekniska fakulteten.
    Thermochromic Lead-Free Halide Double Perovskites2019Ingår i: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 29, nr 10, artikel-id 1807375Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Lead-free halide double perovskites with diverse electronic structures and optical responses, as well as superior material stability show great promise for a range of optoelectronic applications. However, their large bandgaps limit their applications in the visible light range such as solar cells. In this work, an efficient temperature-derived bandgap modulation, that is, an exotic fully reversible thermochromism in both single crystals and thin films of Cs2AgBiBr6 double perovskites is demonstrated. Along with the thermochromism, temperature-dependent changes in the bond lengths of Ag Symbol of the Klingon Empire Br (R-Ag Symbol of the Klingon Empire Br) and Bi Symbol of the Klingon Empire Br (R-Bi Symbol of the Klingon Empire Br) are observed. The first-principle molecular dynamics simulations reveal substantial anharmonic fluctuations of the R-Ag Symbol of the Klingon Empire Br and R-Bi Symbol of the Klingon Empire Br at high temperatures. The synergy of anharmonic fluctuations and associated electron-phonon coupling, and the peculiar spin-orbit coupling effect, is responsible for the thermochromism. In addition, the intrinsic bandgap of Cs2AgBiBr6 shows negligible changes after repeated heating/cooling cycles under ambient conditions, indicating excellent thermal and environmental stability. This work demonstrates a stable thermochromic lead-free double perovskite that has great potential in the applications of smart windows and temperature sensors. Moreover, the findings on the structure modulation-induced bandgap narrowing of Cs2AgBiBr6 provide new insights for the further development of optoelectronic devices based on the lead-free halide double perovskites.

  • 10.
    Sangiovanni, Davide
    et al.
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten. Ruhr Univ Bochum, Germany.
    Klarbring, Johan
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Smirnova, D.
    Ruhr Univ Bochum, Germany; Russian Acad Sci, Russia.
    Skripnyak, Natalia
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Gambino, Davide
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Mrovec, M.
    Ruhr Univ Bochum, Germany.
    Simak, Sergey
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Abrikosov, Igor
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Superioniclike Diffusion in an Elemental Crystal: bcc Titanium2019Ingår i: Physical Review Letters, ISSN 0031-9007, E-ISSN 1079-7114, Vol. 123, nr 10, artikel-id 105501Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Recent theoretical investigations [A. B. Belonoshko et aL Nat. Geosci. 10, 312 (2017)] revealed the occurrence of the concerted migration of several atoms in bcc Fe at inner-core temperatures and pressures. Here, we combine first-principles and semiempirical atomistic simulations to show that a diffusion mechanism analogous to the one predicted for bcc iron at extreme conditions is also operative and of relevance for the high-temperature bcc phase of pure Ti at ambient pressure. The mechanism entails a rapid collective movement of numerous (from two to dozens) neighbors along tangled closed-loop paths in defect-free crystal regions. We argue that this phenomenon closely resembles the diffusion behavior of superionics and liquid metals. Furthermore, we suggest that concerted migration is the atomistic manifestation of vanishingly small co-mode phonon frequencies previously detected via neutron scattering and the mechanism underlying anomalously large and markedly non-Arrhenius self-diffusivities characteristic of bcc Ti.

  • 11.
    Spektor, Kristina
    et al.
    ESRF, France.
    Crichton, Wilson A.
    ESRF, France.
    Konar, Sumit
    Univ Edinburgh, Scotland; Univ Edinburgh, Scotland.
    Filippov, Stanislav
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Klarbring, Johan
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Simak, Sergey
    Linköpings universitet, Institutionen för fysik, kemi och biologi, Teoretisk Fysik. Linköpings universitet, Tekniska fakulteten.
    Haussermann, Ulrich
    Stockholm Univ, Sweden.
    Unraveling Hidden Mg-Mn-H Phase Relations at High Pressures and Temperatures by in Situ Synchrotron Diffraction2018Ingår i: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 57, nr 3, s. 1614-1622Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    The MgMnH system was investigated by in situ high pressure studies of reaction mixtures MgH2MnH2. The formation conditions of two complex hydrides with composition Mg3MnH7 were established. Previously known hexagonal Mg3MnH7 (h-Mg3MnH7) formed at pressures 1.52 GPa and temperatures between 480 and 500 degrees C, whereas an orthorhombic form (o-Mg3MnH7) was obtained at pressures above 5 GPa and temperatures above 600 degrees C. The crystal structures of the polymorphs feature octahedral [Mn(I)H-6](5) complexes and interstitial H-. Interstitial H- is located in trigonal bipyramidal and square pyramidal interstices formed by Mg2+ ions in h- and o-Mg3MnH7, respectively. The hexagonal form can be retained at ambient pressure, whereas the orthorhombic form upon decompression undergoes a distortion to monoclinic Mg3MnH7 (m-Mg3MnH7). The structure elucidation of o- and m-Mg3MnH7 was aided by first-principles density functional theory (DFT) calculations. Calculated enthalpy versus pressure relations predict m- and o-Mg3MnH7 to be more stable than h-Mg3MnH7 above 4.3 GPa. Phonon calculations revealed o-Mg3MnH7 to be dynamically unstable at pressures below 5 GPa, which explains its phase transition to m-Mg3MnH7 on decompression. The electronic structure of the quenchable polymorphs h- and m-Mg3MnH7 is very similar. The stable 18-electron complex [MnH6](5-) is mirrored in the occupied states, and calculated band gaps are around 1.5 eV. The study underlines the significance of in situ investigations for mapping reaction conditions and understanding phase relations for hydrogen-rich complex transition metal hydrides.

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