| 1. |
- Gambino, Davide, et al.
(författare)
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Nonequilibrium ab initio molecular dynamics determination of Ti monovacancy migration rates in B1 TiN
- 2017
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Ingår i: Physical Review B. - : AMER PHYSICAL SOC. - 2469-9950 .- 2469-9969. ; 96:10
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Tidskriftsartikel (refereegranskat)abstract
- We use the color diffusion (CD) algorithm in nonequilibrium (accelerated) ab initio molecular dynamics simulations to determine Ti monovacancy jump frequencies in NaCl-structure titanium nitride (TiN), at temperatures ranging from 2200 to 3000 K. Our results showthat theCDmethod extended beyond the linear-fitting rate-versus-force regime [Sangiovanni et al., Phys. Rev. B 93, 094305 (2016)] can efficiently determine metal vacancy migration rates in TiN, despite the low mobilities of lattice defects in this type of ceramic compound. We propose a computational method based on gamma-distribution statistics, which provides unambiguous definition of nonequilibrium and equilibrium (extrapolated) vacancy jump rates with corresponding statistical uncertainties. The acceleration-factor achieved in our implementation of nonequilibrium molecular dynamics increases dramatically for decreasing temperatures from 500 for T close to the melting point T-m, up to 33 000 for T approximate to 0.7 T-m
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| 2. |
- Mosyagin, Igor, et al.
(författare)
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Effect of dispersion corrections on ab initio predictions of graphite and diamond properties under pressure
- 2018
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Ingår i: Physical Review B. - : AMER PHYSICAL SOC. - 2469-9950 .- 2469-9969. ; 98:17
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Tidskriftsartikel (refereegranskat)abstract
- There are several approaches to the description of van der Waals (vdW) forces within density functional theory. While they are generally found to improve the structural and energetic properties of those materials dominated by weak dispersion forces, it is not known how they behave when the material is subject to an external pressure. This could be an issue when considering the pressure-induced structural phase transitions, which are currently attracting great attention following the discovery of an ultrahard phase formed by the compression of graphite at room temperature. In order to model this transition, the functional must be capable of simultaneously describing both strong covalent bonds and weak dispersion interactions as an isotropic pressure is applied. Here, we report on the ability of several dispersion-correction functionals to describe the energetic, structural, and elastic properties of graphite and diamond, when subjected to an isotropic pressure. Almost all of the tested vdW corrections provide an improved description of both graphite and diamond compared to the local density approximation. The relative error does not change significantly as pressure is applied, and in some cases even decreases. We therefore conclude that the use of dispersion-corrected exchange-correlation functionals, which have been neglected to date, will improve the accuracy and reliability of theoretical investigations into the pressure-induced phase transition of graphite.
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| 3. |
- Sangiovanni, Davide, et al.
(författare)
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Superioniclike Diffusion in an Elemental Crystal: bcc Titanium
- 2019
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Ingår i: Physical Review Letters. - : AMER PHYSICAL SOC. - 0031-9007 .- 1079-7114. ; 123:10
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 4. |
- Brännvall, Marian, et al.
(författare)
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Machine learning approach for longitudinal spin fluctuation effects in bcc Fe at Tc and under Earth-core conditions
- 2022
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Ingår i: Physical Review B. - : AMER PHYSICAL SOC. - 2469-9950 .- 2469-9969. ; 105:14
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Tidskriftsartikel (refereegranskat)abstract
- We propose a machine learning approach to predict the shapes of the longitudinal spin fluctuation (LSF) energy landscapes for each local magnetic moment. This approach allows the inclusion of the effects of LSFs in, e.g., the simulation of a magnetic material with ab initio molecular dynamics in an effective way. This type of simulation requires knowledge of the reciprocal interaction between atoms and moments, which, in principle, would entail calculating the energy landscape of each atom at every instant in time. The machine learning approach is based on the kernel ridge regression method and developed using bcc Fe at the Curie temperature and ambient pressure as a test case. We apply the trained machine learning models in a combined atomistic spin dynamics and ab initio molecular dynamics (ASD-AIMD) simulation, where they are used to determine the sizes of the magnetic moments of every atom at each time step. In addition to running an ASD-AIMD simulation with the LSF machine learning approach for bcc Fe at the Curie temperature, we also simulate Fe at temperature and pressure comparable to the conditions at the Earth's inner solid core. The latter simulation serves as a critical test of the generality of the method and demonstrates the importance of the magnetic effects in Fe in the Earth's core despite its extreme temperature and pressure.
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| 5. |
- Casillas Trujillo, Luis, et al.
(författare)
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Screw dislocation core structure in the paramagnetic state of bcc iron from first-principles calculations
- 2020
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Ingår i: Physical Review B. - : AMER PHYSICAL SOC. - 2469-9950 .- 2469-9969. ; 102:9
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Tidskriftsartikel (refereegranskat)abstract
- Iron-based alloys are widely used as structural components in engineering applications. This calls for a fundamental understanding of their mechanical properties, including those of pure iron. Under operational temperatures the mechanical and magnetic properties will differ from those of ferromagnetic body-centered-cubic iron at 0 K. In this theoretical work we study the effect of disordered magnetism on the screw dislocation core structure and compare with results for the ordered ferromagnetic case. Dislocation cores control some local properties such as the choice of glide plane and the associated dislocation mobility. Changes in the magnetic state can lead to modifications in the structure of the core and affect dislocation mobility. In particular, we focus on the core properties of the 1/2 < 111 > screw dislocation in the paramagnetic state. Using the noncollinear disordered local moment approximation to address paramagnetism, we perform structural relaxations within density functional theory. We obtain the dislocation core structure for the easy and hard cores in the paramagnetic state, and compare them with their ferromagnetic counterparts. By averaging the energy of several disordered magnetic configurations, we obtain an energy difference between the easy- and hard-core configurations, with a lower, but statistically close, value than the one reported for the ferromagnetic case. The magnetic moment and atomic volume at the dislocation core differ between paramagnetic and ferromagnetic states, with possible consequences on the temperature dependence of defect-dislocation interactions.
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| 6. |
- Ekholm, Marcus, et al.
(författare)
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Assessing the SCAN functional for itinerant electron ferromagnets
- 2018
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Ingår i: Physical Review B. - : AMER PHYSICAL SOC. - 2469-9950 .- 2469-9969. ; 98:9
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Tidskriftsartikel (refereegranskat)abstract
- Density functional theory is a standard model for condensed-matter theory and computational material science. The accuracy of density functional theory is limited by the accuracy of the employed approximation to the exchange-correlation functional. Recently, the so-called strongly constrained appropriately normed (SCAN) [Sun, Ruzsinszky, and Perdew, Phys. Rev. Lett. 115, 036402 (2015)] functional has received a lot of attention due to promising results for covalent, metallic, ionic, as well as hydrogen- and van der Waals-bonded systems alike. In this work, we focus on assessing the performance of the SCAN functional for itinerant magnets by calculating basic structural and magnetic properties of the transition metals Fe, Co, and Ni. We find that although structural properties of bcc-Fe seem to be in good agreement with experiment, SCAN performs worse than standard local and semilocal functionals for fcc-Ni and hcp-Co. In all three cases, the magnetic moment is significantly overestimated by SCAN, and the 3d states are shifted to lower energies, as compared to experiments.
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| 7. |
- Ferrantino, Luca, et al.
(författare)
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Aesthetic Outcomes of Non-functional Immediately Restored Single Post-extraction Implants with and without Connective Tissue Graft: A Multicenter Randomized Controlled Trial.
- 2021
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Ingår i: Clinical oral implants research. - : Wiley. - 1600-0501 .- 0905-7161. ; 32:6, s. 684-694
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Tidskriftsartikel (refereegranskat)abstract
- To compare the one-year aesthetic results of flapless single implants, placed in fresh extraction sockets with bone replacement and immediate provisional restoration with or without a connective tissue graft (CGT).The present study proposes a partially blinded multicenter parallel randomized controlled trial, where computer-generated tables were used for central randomization to allocate treatments. 59 out of the 60 patients screened by eight private practices in Northern Italy fulfilled the inclusion criteria. Immediate implants was placed in a fresh extraction socket with a non-functional immediate provisional restoration with (Test group) or without (Control group) a CGT. The primary outcome variable was the implant Crown Aesthetic Index (ICAI) at the 1-year follow-up.ICAI for the 59 randomized patients (Test group = 31, Control group = 28) at the 1-year follow-up was 4.69 (95% CI = 3.16 - 6.22) for the Test group and 3.45 (95%CI = 1.83-5.08) for the Control group, without statistically significant difference between the two groups (p=0.086). One implant failure was recorded in each group, resulting in an implant survival rate of 96.8% [95%CI = 83.3 - 99.9] for the Test group and 96.4% [95%CI = 81.7 -99.9] for the Control group. Other secondary outcome variables and complication rates were comparable across the two groups.Within the limitations of the present clinical trial, the results suggested that the adjunct use of CTG is not mandatory to achieve successful aesthetic outcomes for a well-planned immediate implant placement with immediate non-functional provisional restoration in a fresh extraction socket.
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| 8. |
- Gambino, Davide, 1991-
(författare)
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Ab Initio Modeling of Magnetic Materials in the High-Temperature Paramagnetic Phase
- 2021
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The modeling of magnetic materials at finite temperatures is an ongoing challenge in the field of theoretical physics. This field has strongly benefited from the development of computational methods, which allow to predict material’s properties and explain physical effects on the atomic scale, and are now employed to direct the design of new materials. However, simulations need to be as accurate as possible to give reliable insights into solid-state phenomena, which means that, most desirably, all competing effects occurring in a system at realistic conditions should be included. This task is particularly difficult in the modeling of magnetic materials from first principles, due to the quantum nature of magnetism and its interplay with other phenomena related to the atomic degrees of freedom. The aim of this thesis is therefore to develop methods that enable the inclusion of magnetic effects in finite temperature simulations based on density functional theory (DFT), while considering on the same footing vibrational and structural degrees of freedom,with a particular focus on the high-temperature paramagnetic phase. The type of couplings investigated in this thesis can be separated in two big categories: interplay between magnetism and structure, and between magnetism and vibrations.Regarding the former category, I have tried to shine some light on the effect of the paramagnetic state on atomic positions in a crystal in the presence of defects or for complicated systems, as opposed to the ordered magnetic state. To model the high-temperature paramagnetic phase of magnetic materials, the disordered local moment (DLM) approach is employed in the whole work. In this framework, I have developed a method to perform local lattice relaxations in the disordered magnetic state, which consists of a step-wise partial relaxation of the atomic positions, while changing the configuration of the magnetic moments at each step of the procedure. This method has been tested on point defects in paramagnetic bcc Fe, namely the single vacancy and, separately, the C interstitial in octahedral position, and on Fe1-xCrx alloys, finding non-negligible effects on formation energies. In addition, the feasibility of investigating extended defects like dislocations in the paramagnetic state with this method has also been proven by studying the screw dislocation in bcc Fe. The DLM-relaxation method has then been used to investigate intrinsic and extrinsic defects in CrN, an antiferromagnetic semiconductor studied for thermoelectric applications, found in the paramagnetic state at operating temperature, and a newly synthesized compound, Fe3CO7, which features a complicated crystal structure and unusual electronic properties, with possible important implications for the chemistry of Earth’s mantle.The other focus of this thesis is the coupling between magnetism and lattice vibrations. As a pre-step to perform fully coupled atomistic spin dynamics-ab initio molecular dynamics (ASD-AIMD) simulations, I have first investigated the effect of vibrations on the so called longitudinal spin fluctuations, a mechanism occurring at finite temperatures and important for itinerant electron magnetic systems. I have developed a framework to investigate the dependence of the local moment’s energy landscapes on the instantaneous positions of the atoms, testing it on Fe at different temperature and pressure conditions. This study has laid the foundation to apply machine learning techniques to the prediction of the energy landscapes during an ASD-AIMD simulation. Finally, I have investigated the phase stability of Fe at ambient pressure from the theoretical Curie temperature up to its melting point with ASD-AIMD. This task is carried out by applying a pool of thermodynamic techniques to calculate free energy differences, and therefore I have defined a strategy to discern the thermodynamic equilibrium structure in magnetic materials in the high temperature paramagnetic phase based on first principles dynamical simulations. The methodologies developed and applied in this work constitute an improvement towards the simulation of magnetic materials accounting for the coupling of all effects, and the hope is to bridge a gap between theory and experiments.
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| 9. |
- Gambino, Davide, et al.
(författare)
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Density functional description of spin, lattice, and spin-lattice dynamics in antiferromagnetic and paramagnetic phases at finite temperatures
- 2022
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Ingår i: Physical Review B. - : American Physical Society. - 2469-9950 .- 2469-9969. ; 106:13
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Tidskriftsartikel (refereegranskat)abstract
- Describing the (a) electronic and magnetic properties (EMPs) of compounds generally requires the specification of (b) the type of spin configurations one is considering [e.g., antiferromagnetic (AFM) or paramagnetic (PM) phases, with or without spin short-range order (SRO)] and lattice structure (e.g., atomic displacements, possible symmetry breaking) of such phases at a given temperature. Indeed, studying the interplay between the spin configuration and lattice structure (SCLS) and the ensuing EMPs has been an outstanding challenge in the theory of matter. The traditional approach of electronic phases of matter has generally focused on the interelectronic interactions, regarding the lattice structure as a spectator degree of freedom (DOF), often fixed from an external source (experiment or model assumptions). However, one expects that the EMPs of a compound can generally respond self-consistently to changes in SCLS (including symmetry), and at the same time, the SCLS can change in response to different electron and spin distributions visited during the calculation of the EMPs. This ping-pong-like interplay where structure affects electronic properties and the latter affect structure is indeed a cornerstone of much of the intricacy of understanding quantum materials. However, there is a limited understanding of the theory required to determine the SCLS at finite temperature in a way that can affect the EMPs and vice versa. We use here a practical, density functional theory (DFT)-based approach that provides the SCLS as a function of temperature, involving the description of spin, lattice, and spin-lattice dynamics of AFM and PM phases, thus providing the required ping-pong partners to the description of the EMPs of different phases. We distinguish three levels of dynamics: (I) dynamics of the spin DOFs treated via noncollinear Heisenberg Monte Carlo solved with exchange energies obtained from first-principles DFT cluster expansion, (II) dynamics of the lattice DOFs treated by ab initio molecular dynamics (AIMD) employing a fixed, representative spin configuration from Level I at the simulated temperature, and (III) coupling of spin and lattice dynamics via Landau-Lifshitz-Gilbert spin dynamics combined with AIMD. Such SCLSs at each of the three levels are used as inputs to DFT supercell calculations, providing the EMPs at each temperature. The results of this sequence include electronic band structures, bandgaps, density of states, as well as the statistical distribution of local moments and the SRO parameters, each as a function of temperature. Herein, we define a path to include temperature in magnetic insulators at different levels of spin dynamics by intercommunication between electronic structure theory and statistical mechanics. Using NiO as a test case, we address the separability of the DOFs in magnetic insulators for a minimal description of EMPs, demonstrating that inclusion of spin dynamics and, to some level, lattice dynamics is enough to explain the EMPs.
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| 10. |
- Gambino, Davide, 1991-, et al.
(författare)
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Lattice relaxations in disordered Fe-based materials in the paramagnetic state from first principles
- 2018
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Ingår i: Physical Review B. - : AMER PHYSICAL SOC. - 2469-9950 .- 2469-9969. ; 98:6
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Tidskriftsartikel (refereegranskat)abstract
- The first-principles calculation of many material properties, in particular related to defects and disorder, starts with the relaxation of the atomic positions of the system under investigation. This procedure is routine for nonmagnetic and magnetically ordered materials. However, when it comes to magnetically disordered systems, in particular the paramagnetic phase of magnetic materials, it is not clear how the relaxation procedure should be performed or which geometry should be used. Here we propose a method for the structural relaxation of magnetic materials in the paramagnetic regime, in an adiabatic fast-magnetism approximation within the disordered local moment (DLM) picture in the framework of density functional theory. The method is straightforward to implement using any ab initio code that allows for structural relaxations. We illustrate the importance of considering the disordered magnetic state during lattice relaxations by calculating formation energies and geometries for an Fe vacancy and C insterstitial atom in body-centered cubic (bcc) Fe as well as bcc Fe1-xCrx random alloys in the paramagnetic state. In the vacancy case, the nearest neighbors to the vacancy relax toward the vacancy of 0.14 angstrom (-5% of the ideal bcc nearest-neighbor distance), which is twice as large as the relaxation in the ferromagnetic case. The vacancy formation energy calculated in the DLM state on these positions is 1.60 eV, which corresponds to a reduction of about 0.1 eV compared to the formation energy calculated using DLM but on ferromagnetic-relaxed positions. The carbon interstitial formation energy is found to be 0.41 eV when the DLM relaxed positions are used, as compared to 0.59 eV when the FM-relaxed positions are employed. For bcc Fe0.5Cr0.5 alloys, the mixing enthalpy is reduced by 5 meV/atom, or about 10%, when the DLM state relaxation is considered, as compared to positions relaxed in the ferromagnetic state.
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