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Haifeng Song

Publications and source records attributed to Haifeng Song.

29 records · Page 2Linked to original sources
arXiv2016

Three-dimensional bulk electronic structure of the Kondo lattice CeIn3 revealed by photoemission

We show the three-dimensional electronic structure of the Kondo lattice CeIn3 using soft x-ray angle resolved photoemission spectroscopy in the paramagnetic state. For the first time, we have directly observed the three-dimensional topology of the Fermi surface of CeIn3 by photoemission. The Fermi surface has a complicated hole pocket centred at the Γ-Z line and an elliptical electron pocket centred at the R point of the Brillouin zone. Polarization and photon-energy dependent photoemission results both indicate the nearly localized nature of the 4f electrons in CeIn3, consistent with the theoretical prediction by means of the combination of density functional theory and single-site dynamical meanfield theory. Those results illustrate that the f electrons of CeIn3, which is the parent material of CeMIn5 compounds, are closer to the localized description than the layered CeMIn5 compounds.

cond-mat.str-el↗
arXiv2016

Effect of vacancies on the mechanical properties of zirconium: An ab initio investigation

It is well known that the irradiation-induced defects strongly influence the mechanical properties of zirconium (Zr) or its alloys in nuclear reactors. However, how the point defect changes the mechanical properties has been rarely studied. Here, we systematically investigated the effect of vacancies on the mechanical properties of alpha-Zr based on density functional theory (DFT). Both uniformly distributed vacancies and vacancy clusters were considered. Our results reveal that the existence of vacancy will reduce the bulk modulus, while enhance the shear and Young's moduli. Based on these moduli, the ductility and hardness were further calculated. With the introduction of vacancy, the ductility decreases, but the hardness increases. However, when the vacancy concentration is larger than a critical value, a rise in the ductility and a reduction in the hardness occur, which indicates the degeneration of the material. Moreover, it was found that the vacancies lead to a more isotropic distribution of Young's modulus in 3D space. To further investigate how the clustering of vacancies influences the mechanical properties, the most stable configurations of di- and trivacancy clusters have been predicted, which correspond to the most compact distribution of vacancies. Compared with the uniform distribution of vacancies, clustering of vacancies will strengthen the above changes of elastic moduli, ductility and hardness. Our results indicate that the increase of the vacancy concentration may be the basic cause for the changes of the mechanical properties under irradiation, while the formation of vacancy clusters intensifies these changes.

cond-mat.mtrl-sci↗
arXiv2016

On the existence of the optimal order for wavefunction extrapolation in Born-Oppenheimer molecular dynamics

Wavefunction extrapolation greatly reduces the number of self-consistent field (SCF) iterations and thus the overall computational cost of Born-Oppenheimer molecular dynamics (BOMD) that is based on the Kohn-Sham density functional theory. Going against the intuition that the higher order of extrapolation possesses a better accuracy, we demonstrate, from both theoretical and numerical perspectives, that the extrapolation accuracy firstly increases and then decreases with respect to the order, and an optimal extrapolation order in terms of minimal number of SCF iterations always exists. We also prove that the optimal order tends to be larger when using larger MD time steps or more strict SCF convergence criteria. By example BOMD simulations of a solid copper system, we show that the optimal extrapolation order covers a broad range when varying the MD time step or the SCF convergence criterion. Therefore, we suggest the necessity for BOMD simulation packages to open the user interface and to provide more choices on the extrapolation order. Another factor that may influence the extrapolation accuracy is the alignment scheme that eliminates the discontinuity in the wavefunctions with respect to the atomic or cell variables. We prove the equivalence between the two existing schemes, thus the implementation of either of them does not lead to essential difference in the extrapolation accuracy.

physics.comp-ph↗
arXiv2015

Multiscale dynamics of open three-level quantum systems with two quasi-degenerate levels

We consider a three-level quantum system interacting with a bosonic thermal reservoir. Two energy levels of the system are nearly degenerate but well separated from the third one. The system-reservoir interaction constant is larger than the energy difference of the degenerate levels, but it is smaller than the separation between the latter and the remaining level. We show that the quasi-degeneracy of energy levels leads to the existence of a manifold of quasi-stationary states, and the dynamics exhibits two characteristic time scales. On the first, shorter one, initial states approach the quasi-stationary manifold. Then, on the much longer second time scale, the final unique equilibrium is reached.

quant-ph↗
arXiv2014

Overlapping Resonances in Open Quantum Systems

An $N$-level quantum system is coupled to a bosonic heat reservoir at positive temperature. We analyze the system-reservoir dynamics in the following regime: The strength $λ$ of the system-reservoir coupling is fixed and small, but larger than the spacing $σ$ of system energy levels. For vanishing $σ$ there is a manifold of invariant system-reservoir states and for $σ>0$ the only invariant state is the joint equilibrium. The manifold is invariant for $σ=0$ but becomes quasi-invariant for $σ>0$. Namely, on a first time-scale of the order $1/λ^2$, initial states approach the manifold. Then they converge to the joint equilibrium state on a much larger time-scale of the order $λ^2/σ^2$. We give a detailed expansion of the system-reservoir evolution showing the above scenario.

math-ph↗
arXiv2014

The different roles of Pu-oxide overlayers in the hydrogenation of Pu-metal: An ab initio molecular dynamics study based on vdW-DFT+U

Based on the van der Waals density functional theory (vdW-DFT)+U scheme, we carry out the ab initio molecular dynamics (AIMD) study of the interaction dynamics for H$_{2}$ impingement against the stoichiometric PuO$_{2}$(111), the reduced PuO$_{2}$(111), and the stoichiometric $α$-Pu$_{2}$O$_{3}$(111) surfaces. The hydrogen molecular physisorption states, which can not be captured by pure DFT+\textit{U} method, are obtained by employing the vdW-DFT+\textit{U} scheme. We show that except for the weak physisorption, PuO$_{2}$(111) surfaces are so difficult of access that almost all of the H$_{2}$ molecules will bounce back to the vacuum when their initial kinetic energies are not sufficient. Although the dissociative adsorption of H$_{2}$ on PuO$_{2}$(111) surfaces is found to be very exothermic, the collision-induced dissociation barriers of H$_{2}$ are calculated to be as high as $3.2$ eV and $2.0$ eV for stoichiometric and reduced PuO$_{2}$ surfaces, respectively. Unlike PuO$_{2}$, our AIMD study directly reveals that the hydrogen molecules can penetrate into $α$-Pu$_{2}$O$_{3}$(111) surface and diffuse easily due to the $25$\ native O vacancies located along the $\langle $111$\rangle $ diagonals of $α$-Pu$_{2}$O$_{3}$ matrix. By examining the temperature effect and the internal vibrational excitations of H$_{2}$, we provide a detailed insight into the interaction dynamics of H$_{2}$ in $α$-Pu$_{2}$O$_{3}$. The optimum pathways for hydrogen penetration and diffusion, the corresponding energy barriers ($1.0$ eV and $0.53$ eV, respectively) and rate constants are systematically calculated. Overall, our study fairly reveals the different interaction mechanisms between H$_{2}$ and Pu-oxide surfaces, which have strong implications to the interpretation of experimental observations.

cond-mat.mtrl-sci↗
arXiv2012

A rigorous derivation of the transition rate for the dissipative two-state system

The transition rate for a two-state system interacting with a bosonic heat bath, from the initial state `up' at time t=0 to `down' at time t>0, was derived formally in the seminal paper [12] by Leggett, Chakravarty, Dorsey, Fisher, Garg and Zwerger. The expression was obtained for small tunneling parameter of the two-level system using time-dependent perturbation theory to second order. It contains all orders in the parameter of coupling between the system and the bath. We give a rigorous derivation of the transition rate, using a quantum resonance approach.

math-ph↗
arXiv2012

First-principles study of surface properties of PuO2: Effects of thickness and O-vacancy on surface stability and chemical activity

The (111), (110), and (001) surfaces properties of PuO2 are studied by using density-functional theory+U method. The total-energy static calculations determine the relative order of stability for low-index PuO2 surfaces, namely, O-terminated (111) > (110) > defective (001) > polar (001). The effect of thickness is shown to modestly modulate the surface stability and chemical activity of the (110) surface. The high work function of 6.19 eV indicates the chemical inertia of the most stable (111) surface, and the surface O-vacancy with concentration C_V=25% can efficiently lower the work function to 4.35 eV, which is a crucial indicator of the difference in the surface chemical activities between PuO2 and α-Pu2O3. For the polar (001) surface, 50% on-surface O-vacancy can effectively quench the dipole moment and stabilize the surface structure, where the residual surface oxygen atoms are arranged in a zigzag manner along the <100> direction. We also investigate the relative stability of PuO2 surfaces in an oxygen environment. Under oxygen-rich conditions, the stoichiometric O-terminated (111) is found to be the most stable surface. Whereas under O-reducing conditions, the on-surface O-vacancy of C_V = 1/9 is stable, and for high reducing conditions, the (111) surface with nearly one monolayer subsurface oxygen removed (C_V = 8/9) becomes most stable.

cond-mat.mtrl-sci↗
arXiv2012

The environmental dependence of redox energetics of PuO2 and α-Pu2O3: A quantitative solution from DFT+U calculations

We report a comprehensive density functional theory (DFT) + $U$ study of the energetics of charged and neutral oxygen defects in both PuO$_{2}$ and $α$-Pu$_{2}$O$_{3}$, and present a quantitative determination of the equilibrium compositions of reduced PuO$_{2}$ (PuO$_{2-x}$) as functions of environmental temperature and partial pressure of oxygen, which shows fairly agreement with corresponding high-temperature experiments. Under ambient conditions, the endothermic reduction of PuO$_{2}$ to $α$-Pu$_{2}$O$_{3} $ is found to be facilitated by accompanying volume expansion of PuO$_{2-x}$ and the possible migration of O-vacancy, whereas further reduction of $α$-Pu$_{2}$O$_{3}$ is predicted to be much more difficult. In contrast to the endothermic oxidation of PuO$_{2}$,\ the oxidation of $α$-Pu$_{2} $O$_{3}$ is a stable exothermic process.

cond-mat.mtrl-sci↗
arXiv2007

Mean-field potential calculations of high-pressure equation of state for shock-compressed BeO

A systematic study of the Hugoniot equation of state, phase transition, and the other thermodynamic properties including the Hugoniot temperature, the electronic and ionic heat capacities, and the Grüneisen parameter for shock-compressed BeO, is presented by calculating the total free energy. The method of calculations combines first-principles treatment for 0-K and finite-T electronic contribution and the mean-field-potential approach for the vibrational contribution of the lattice ion to the total energy. Our calculated Hugoniot shows good agreement with the experimental data.

cond-mat.mtrl-sci↗