Quantum Monte Carlo study of one-dimensional transition-metal organometallic cluster systems and their suitability as spin filters

Horvathova, Lucia; Derian, René; Mitáš, Luboš; Štich, Ivan

doi:10.1103/physrevb.90.115414

Cited by 13 publications

(4 citation statements)

References 32 publications

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“…Our modeling of surface spin polarization on bare ceria surface is also applicable in the fields of band gap opening, spintronics and thermoelectricity of 2D magnetic materials [38][39][40]. Particularly, electronic structure of surface spin polarized CeO 2 is akin to 2D ferromagnetic insulator [41,42], where doping can allow spin-polarized current [43][44][45]. We found the surface spin polarization is only stabilized in DFT simulation with a Gaussian type orbital basis.…”

Section: Introductionmentioning

confidence: 84%

Modeling surface spin polarization on ceria-supported Pt nanoparticles

Kang¹,

Vincent²,

Lee³

et al. 2022

J. Phys.: Condens. Matter

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In this work, we employ density functional theory simulations to investigate possible spin polarization of CeO$_2$-(111) surface and its impact on the interactions between a ceria support and Pt nanoparticles. With a Gaussian type orbital basis, our simulations suggest that the CeO$_2$-(111) surface exhibits a robust surface spin polarization due to the internal charge transfer between atomic Ce and O layers. In turn, it can lower the surface oxygen vacancy formation energy and enhance the oxide reducibility. We show that the inclusion of spin polarization can significantly reduce the major activation barrier in the proposed reaction pathway of CO oxidation on ceria-supported Pt nanoparticles. For metal-support interactions, surface spin polarization enhances the bonding between Pt nanoparticles and ceria surface oxygen, while CO adsorption on Pt nanoparticles weakens the interfacial interaction regardless of spin polarization. However, the stable surface spin polarization can only be found in the simulations based on the Gaussian type orbital basis. Given the potential importance in the design of future high-performance catalysts, our present study suggests a pressing need to examine the surface ferromagnetism of transition metal oxides in both experiment and theory.

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Section: Introductionmentioning

confidence: 84%

Modeling surface spin polarization on ceria-supported Pt nanoparticles

Kang¹,

Vincent²,

Lee³

et al. 2022

J. Phys.: Condens. Matter

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“…A recent application to C 20 [48] demonstrated the importance of using multi-determinant trial wavefunctions in DMC, to properly capture differences in electron correlation effects between different isomers. Clusters with potential technologically important applications have been studied, including metal hydride clusters for hydrogen storage applications [49], and possible half-metallic pi-bonded transition metal organometallic sandwiches for spintronics [50,51].…”

Section: Applications 221 Clustersmentioning

confidence: 99%

Roadmap on post-DFT methods for nanoscience

Per

Cleland

2020

Nano Futures

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Computational electronic-structure calculations of nanoscale systems are powerful tools which provide fundamental insight, help interpret experiment results, and ultimately aid the development of new materials. Density functional theory (DFT) dominates this field, and has had an enormously beneficial impact on nanoscience. However, there are still many situations in which present DFT fails to provide accurate quantitative predictions. The development of methods which provide more reliable predictive power is a growing field, and these approaches are becoming practical alternatives to DFT for nanoscience applications. In this article, we review four promising alternatives: Diffusion Monte Carlo, domain-based local pair natural orbital coupled cluster, the time-dependent formulation of DFT, and the GW method. We provide descriptive overviews of each method, accompanied by examples of where they have been applied to problems relevant to nanoscience, and discuss the major challenges they currently face as well as the outlook for the future. Between them these methods comprise a flexible toolkit whose continued development will be a big step towards the reliable computational design of new materials.

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“…The difference would be partly attributed to the dynamical correlation effect, which becomes more important at shorter binding length as well as exchange repulsions. Even under the fixed-node approximation, the dynamical correlation is expected to be well described, [17,18,[23][24][25][26][27][28][29][30][31] and hence the present DMC curve is regarded as the best description of the binding of CHS.…”

Section: Calibration Of Dftmentioning

confidence: 99%

“…Such severe scalabilities obstruct the applications to larger molecules being likely in the practical cases. In contrast, DMC (diffusion Monte Carlo) method is quite promising, and its applicability to more practical issues gets rapidly extended. − This framework is regarded in principle as the most reliable that can achieve “numerically exact solutions” in some cases, , and there has been so far several applications to noncovalent systems, − to calibrate even over accurate molecular orbital methods such as CCSD(T). DMC scales at worst to ∼ N 3 , making it possible to be applied further to larger molecules including molecular crystals. − …”

Section: Introductionmentioning

confidence: 99%

A Computational Scheme To Evaluate Hamaker Constants of Molecules with Practical Size and Anisotropy

Hongo

2017

J. Chem. Theory Comput.

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We propose a computational scheme to evaluate Hamaker constants, A, of molecules with practical sizes and anisotropies. Upon the increasing feasibility of diffusion Monte Carlo (DMC) methods to evaluate binding curves for such molecules to extract the constants, we discussed how to treat the averaging over anisotropy and how to correct the bias due to the nonadditivity. We have developed a computational procedure for dealing with the anisotropy and reducing statistical errors and biases in DMC evaluations, based on possible validations on predicted A. We applied the scheme to cyclohexasilane molecule, SiH, used in "printed electronics" fabrications, getting A ≈ 105 ± 2 zJ, being in plausible range supported even by other possible extrapolations. The scheme provided here would open a way to use handy ab initio evaluations to predict wettabilities as in the form of materials informatics over broader molecules.

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Quantum Monte Carlo study of one-dimensional transition-metal organometallic cluster systems and their suitability as spin filters

Cited by 13 publications

References 32 publications

Modeling surface spin polarization on ceria-supported Pt nanoparticles

Modeling surface spin polarization on ceria-supported Pt nanoparticles

Roadmap on post-DFT methods for nanoscience

A Computational Scheme To Evaluate Hamaker Constants of Molecules with Practical Size and Anisotropy

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