Bulletin of the American Physical Society
APS March Meeting 2017
Volume 62, Number 4
Monday–Friday, March 13–17, 2017; New Orleans, Louisiana
Session P1: Van der Waals Bonding in Advanced Materials IIIFocus
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Sponsoring Units: DMP DCOMP Chair: Timo Thonhauser, Wake Forest University Room: 260 |
Wednesday, March 15, 2017 2:30PM - 3:06PM |
P1.00001: Long-Range van der Waals Correction to a Semilocal Density Functional: The Tail Need Not Wag the Dog Invited Speaker: John P. Perdew The SCAN [1] (strongly constrained and appropriately normed) meta-generalized gradient approximation satisfies all 17 exact constraints that a semilocal functional can. Without being fitted to any bonded system, it correctly describes most kinds of bonding [2], including intermediate-range van der Waals (vdW) interaction. It can be supplemented [3.4] with a long-range vdW correction such as D3 or rVV10, which have the flexibility to exclude any intermediate-range contribution. Accurate results are found for free molecules [3], for molecules weakly bound to metal surfaces [4], and for interlayer binding energies of layered materials [4]. Despite being a pair-interaction model, the rVV10 correction to SCAN also gives a random-phase-approximation-like long-range contribution to the binding energy curve for graphene on a nickel surface [4]. [1] J. Sun, A. Ruzsinszky, and J.P. Perdew, Phys. Rev. Lett. \textbf{115}, 036402 (2015). [2] J. Sun \textit{et al}., Nature Chem. \textbf{8}, 831 (2016). [3[ J.G. Brandenburg, J.E. Bates, J. Sun, and J.P. Perdew, Phys. Rev. B \textbf{94,} 115144 (2016). [4] H. Peng, Z. Yang, J.P. Perdew, and J. Sun, Phys. Rev. X \textbf{6}, 041005 (2016). [Preview Abstract] |
Wednesday, March 15, 2017 3:06PM - 3:18PM |
P1.00002: Improved metallic surface properties using a new van der Waals density functional Abhirup Patra, Jianwei Sun, Jefferson Bates, John P. Perdew An incorrect description of van der Waals (vdW) interactions for different problems using popular density functional theory (DFT) is found in many cases, especially where long-range van der Waals interactions are present. Metallic surfaces are such systems. Physical properties of surfaces such as surface energy and work function can be affected by the long-range van der Waals interaction present at the surface barrier. In this work we explore the performance of the new vdW-corrected non-local density functional SCAN$+$rVV10$^{\mathrm{1}}$ for such surfaces. We find that, when the new meta-GGA functional SCAN is combined with the non-local rVV10 method, it can not only give a better description of the van der Waals interaction in molecules and layered materials, but can be equally used as a more versatile competitor of LDA for metal surfaces. 1.Versatile van der Waals Density Functional Based on a Meta-Generalized Gradient Approximation, H. Peng, Z. Yang, J. P. Perdew, J. Sun, Phys. Rev. X~6, 041005 (2016). Acknowledgments: NSF under DMR-1305135, CNS-09-5884, and by DOE under DE-SC0012575, DE-AC02-05CH11231 [Preview Abstract] |
Wednesday, March 15, 2017 3:18PM - 3:30PM |
P1.00003: A hybrid version of the SCAN functional including long-range dispersion interactions Hsin-Yu Ko, Marcos F. Calegari Andrade, Biswajit Santra, Annabella Selloni, Roberto Car The recently developed meta-GGA density functional, called SCAN (strongly constrained and appropriately normed) [1], provides an accurate description of the electronic structure in a broad class of systems characterized by different bonding interactions, including intermediate range van-der-Waals (vdW) bonding [2]. Here we consider a hybrid version of the SCAN functional [3] with inclusion of long-range vdW interactions via a re-parameterized Tkatchenko-Scheffler scheme [4]. Calculations for the S22 molecular database, ice hexamer clusters, and bulk ice Ih indicate that this functional further improves the description of vdW and hydrogen bonding interactions. [1] J Sun, A Ruzsinszky, and J P Perdew, PRL 115, 036402 [2] J Sun et al, Nat Chem 8, 831 [3] K Hui and J-D Chai, JCP 144, 044114 [4] A Tkatchenko and M Scheffler, PRL 102, 073005 [Preview Abstract] |
Wednesday, March 15, 2017 3:30PM - 3:42PM |
P1.00004: Extending the applicability of Many-Body Dispersion (MBD) to large-scale systems: DFTB+MBD Martin St\"{o}hr, Reinhard J. Maurer, Alexandre Tkatchenko The inclusion of van der Waals (vdW) dispersion interactions in electronic-structure calculations has significantly extended the applicability of DFT. However, the accessible system sizes with DFT+vdW remain small for many practically relevant applications. On the other hand, Density-Functional Tight-Binding (DFTB) is an electronic-structure method of choice for systems with several 1000s of atoms. A severe drawback of DFTB and other semi-empirical methods, however, is the missing direct access to atomic polarizabilities, required for most common \textit{ab initio} vdW models. Here, we present a novel approach to derive accurate effective polarizabilities directly from the atom-centered basis set representation of the density-matrix [1]. This enables the use of sophisticated dispersion models such as the Many-Body Dispersion (MBD) scheme [2] in conjunction with most electronic-structure methods including both DFT and DFTB, thus allowing the investigation of many-body effects in large-scale systems. We exemplify the viability of such a combined approach by adressing the impact of many-body dispersion on the solvation effect in biomolecular systems with DFTB+MBD. [1] M. St\"{o}hr et al., J. Chem. Phys. 144, 151101, 2016; [2] A. Tkatchenko et al., Phys. Rev. Lett. 108, 236402, 2012. [Preview Abstract] |
Wednesday, March 15, 2017 3:42PM - 3:54PM |
P1.00005: (De)stabilizing dispersion interactions via external electric charges Andrii Kleshchonok, Alexandre Tkatchenko Van der Waals (vdW) or dispersion interactions play a central role in the structure, stability, and reaction mechanisms in large variety of molecules and materials. However, in many situations of interest in material science and biophysics, vdW interactions should account for the coupling with external (in)homogeneous electric fields. In this work we address the effect of external static charge field on long-range electron correlations. By using the quantum Drude oscillator model, we derive analytical expressions of the charge induced dipole-quadrupole dispersion energy, that is accounted neither in standard DFT methods, nor in popular vdW correction schemes. Analysing the scaling laws of this dispersion term, we conclude that positive charge stabilizes dispersion interactions, while a negative charge has an opposite effect. Benchmark over S22 molecular dataset estimates the induced dispersion to be in the range of 20-300 \% of conventional electrostatic energy. Our findings could have broad potential implications, including exfoliation of 2D materials, chemical reaction rates in charged droplets, and biological membranes. [Preview Abstract] |
Wednesday, March 15, 2017 3:54PM - 4:06PM |
P1.00006: Unifying microscopic and continuum treatments of van der Waals and Casimir interactions Prashanth Venkataram, Jan Hermann, Alexandre Tkatchenko, Alejandro Rodriguez We present an approach for computing long-range, dispersive van der Waals (vdW) interactions between complex molecular systems and arbitrarily shaped macroscopic bodies, melding atomistic treatments of electronic fluctuations based on density functional theory (DFT) in the former, with continuum descriptions of strongly shape-dependent electromagnetic fields in the latter, thus capturing many-body and multiple scattering effects to all orders. Such a theory is especially important when considering vdW interactions at mesoscopic scales, i.e. between molecules and structured surfaces with features on the scale of molecular sizes, in which case the finite sizes, complex shapes, and resulting non-local electronic excitations of molecules are strongly influenced by electromagnetic retardation and wave effects that depend crucially on the shapes of surrounding macroscopic bodies. We show that these effects together can modify vdW interactions by orders of magnitude compared to previous treatments based on Casimir-Polder [1] or nonretarded [2] approximations, which are valid only at macroscopically large or atomic-scale separations, respectively. [1] J. F. Babb, J. Phys: Conf. Ser. 19, 1 (2005) [2] J. F. Dobson and T. Gould, J. Phys: Condensed Matter 24, 073201 (2012) [Preview Abstract] |
Wednesday, March 15, 2017 4:06PM - 4:18PM |
P1.00007: Unified many-body approach to van der Waals interactions based on semi-local polarizability functional Jan Hermann, Matthias Scheffler, Alexandre Tkatchenko Electromagnetic coupling of charge fluctuations leads to van der Waals (vdW) attraction in systems ranging from metal nanoparticles to dielectric materials. In this regard, broadly applicable and accurate description of vdW interactions in complex materials is an elusive and unsolved puzzle. Many promising approaches model various subsets of this general problem, but are limited in scope by the underlying parametrization (atomic models), in accuracy due to missing many-body interactions (nonlocal density functionals), or in efficiency by working with virtual orbital space (e.g., random-phase approximation). Here, we present a unifying method that combines key elements from different theories and accurately describes vdW interactions in covalent, ionic, and metallic systems. In particular, we employ a semi-local polarizability functional of the electron density and its gradient to parametrize material response and its coupling within the many-body dispersion framework, and demonstrate the generality of the method on binding in molecular dimers and crystals, carbon-based nanomaterials, oxides, and salts, as well as on adsorption of molecules on metal surfaces. Our approach allows consistent modelling of a wide spectrum of materials as well as hybrid materials with mixed bond types. [Preview Abstract] |
Wednesday, March 15, 2017 4:18PM - 4:30PM |
P1.00008: vdW-DF $+U$ description of solid oxygen at low pressure Shusuke Kasamatsu, Takeo Kato, Osamu Sugino Oxygen is known to solidify at low temperature into the paramagnetic cubic $\gamma$ phase under 54 K, rhombohedral frustrated magnet $\beta$ phase under 44 K, and the monoclinic antiferromagnetic $\alpha$ phase under 24 K [1]. The structures of these phases result from a subtle balance of the van der Waals and spin-spin interactions between O$_2$ molecules, and their description using conventional semilocal density functional approximations have proved to be quite unsatisfactory. Recently developed vdW-DF functionals solve the problem partially, but due to inaccruate description of the exchange interaction, the predicted lattice parameters of the $\alpha$ phase are still off by as large as 15\% compared to experiment [1]. Semiempirical tuning of spin-spin interaction in the vdW-DF energy functional (vdW-DF-SGC [1]) have also yielded sub-par results. In this work, we report that the DFT$+U$ approach used in combination with certain vdW-DF functionals performs surprisingly well in this regard [2]. This is explained by the correction of overbinding between antiferromagnetic O$_2$ pairs due to the on-site $U$ interaction applied on the O p orbitals. [1] M. Obata et al.: Phys. Procedia 75, 771 (2015). [2] S. Kasamatsu, T. Kato, and O. Sugino, arXiv:1606.08568 [cond-mat.mtrl-sci] [Preview Abstract] |
Wednesday, March 15, 2017 4:30PM - 4:42PM |
P1.00009: The Dipole Polarizability of a Condensed-Phase Water Molecule Ka Un Lao, Jaclyn Lunger, Junteng Jia, Robert DiStasio The dipole polarizability, $\alpha$, provides a measure of the tendency of a molecule or material to deform (or polarize) in the presence of an electric field and is a critical component of the induction and dispersion interactions. Within the framework of density functional theory (DFT), we present a hierarchy of first principles based approaches for computing the dipole polarizability of a molecule located in the condensed phase. This hierarchy includes a successive treatment of both short-range (hybridization, Pauli exchange-repulsion, etc.) and long-range (Coulomb) electrodynamical response screening in the computation of $\alpha$, while simultaneously accounting for the surrounding condensed-phase environment. Utilizing highly accurate liquid water configurations generated from van der Waals inclusive hybrid DFT based ab initio molecular dynamics, we computed $\alpha$ for this ensemble of liquid water molecules as a first application of this approach. In addition, we introduce a practical yet highly accurate scheme for assigning the polarizability of a water molecule on-the-fly during liquid water simulations that is straightforward to use in current polarizable force fields when computing the induction and dispersion interactions in large-scale aqueous environments. [Preview Abstract] |
Wednesday, March 15, 2017 4:42PM - 4:54PM |
P1.00010: Parameterization of Nonbonded Interactions between Molybdenum Disul?de and Water Mohammad Heiranian, Yanbin Wu, Narayana Aluru Recently, single-layer nanoporous molybdenum disulfide (MoS$_{\mathrm{2}})$ membranes have been found to be a promising material in various applications such as DNA sequencing, water purification and power generation. To understand the physics taking place in such nanofluidics systems, an accurate forcefield is needed to describe the van der Waals and coulombic interactions between MoS$_{\mathrm{2}}$ and water. In this work, the high-accuracy adiabatic-connection fluctuation-dissipation based random phase approximation (RPA) method is used to implement water-MoS$_{\mathrm{2}}$ parameters for use in molecular dynamics simulations. The accuracy of the developed parameters is validated by comparing the resulting water-MoS$_{\mathrm{2}}$ contact angle, an interface property, from MD with that of experiments. The accurate description of water-MoS$_{\mathrm{2}}$ interface, studied here, will facilitate the future studies of the above-mentioned applications. [Preview Abstract] |
Wednesday, March 15, 2017 4:54PM - 5:06PM |
P1.00011: Plasmons in quasi-two-dimensional metals Felipe H. da Jornada, Lede Xian, H. Sener Sen, Angel Rubio, Steven G. Louie We employ ab initio density-functional theory (DFT) and GW calculations to understand and predict the plasmon dispersion in quasi-two-dimensional (quasi-2D) metals. We show that, unlike what is found in idealized 2D electron gases, plasmons are virtually dispersionless in real quasi-2D metals for a wide range of excitation wave vectors that are experimentally accessible. We further develop a simpler model that captures this plasmon dispersion in quasi-2D metals and which depends on a single parameter: the characteristic screening length due to interband transitions. Our ab initio calculations further predict that monolayer metallic transition metal dichalcogenides are excellent candidates to explore these dispersionless (flat) plasmons: having large excitation energy that is away from the Landau damping regions makes them ideal systems to support long-lived, spatially-localized 2D plasmons which are highly tunable with substrate. This work is supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division; the National Science Foundation; the European Research Council project (ERC-2015-AdG-694097), and the AFOSR Grant No. FA2386-15-1-0006 AOARD 144088. [Preview Abstract] |
Wednesday, March 15, 2017 5:06PM - 5:18PM |
P1.00012: Topological phase transition from trigonal warping in van der Waals multilayers Junjie Zeng, Yafei Ren, Zhenhua Qiao We investigate theoretically in Bernal-stacked bilayer graphene system the effect of the trigonal warping, which stems from the interlayer hopping, upon distinctive topological phases, such as the quantum anomalous Hall effect as well as the quantum valley Hall effect. We find that the trigonal warping plays a vital part in the formation of topological phases in large exchange field and/or interlayer potential difference by changing Chern numbers. The presence of the trigonal warping terms shrinks the phase space of quantum anomalous/valley Hall effect and leads to the emergence of the valley-polarized quantum anomalous Hall effect with high Chern numbers ranging from C $=$ -7 to 7. Inspired by those findings, we believe that, in a larger sense, it is auspicious for other van der Waals layer-structured materials to possess similar constructive effect under the considerations alike. [Preview Abstract] |
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