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Accurate thermochemistry of covalent and ionic solids from spin-component-scaled MP2

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arxiv 2208.04865 v1 pith:7RDQYMUR submitted 2022-08-09 cond-mat.mtrl-sci physics.chem-ph

Accurate thermochemistry of covalent and ionic solids from spin-component-scaled MP2

classification cond-mat.mtrl-sci physics.chem-ph
keywords scs-mp2alreadybulkchemistrycohesiveconstantcovalentenergy
verification ladder T0 review T1 audit T2 compute T3 formal T4 reserved
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We study the performance of spin-component-scaled second-order M{\o}ller-Plesset perturbation theory (SCS-MP2) for the prediction of the lattice constant, bulk modulus, and cohesive energy of 12 simple, three-dimensional, covalent and ionic semiconductors and insulators. We find that SCS-MP2 and the simpler scaled opposite-spin MP2 (SOS-MP2) yield predictions that are significantly improved over the already good performance of MP2. Specifically, when compared to experimental values with zero-point vibrational corrections, SCS-MP2 (SOS-MP2) yields mean absolute errors of 0.015 (0.017) {\AA} for the lattice constant, 3.8 (3.7) GPa for the bulk modulus, and 0.06 (0.08) eV for the cohesive energy, which are smaller than those of leading density functionals by about a factor of two or more. We consider a reparameterization of the spin scaling parameters and find that the optimal parameters for these solids are very similar to those already in common use in molecular quantum chemistry, suggesting good transferability and reliable future applications to surface chemistry on insulators.

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