In this work we employ ab initio electronic structure theory at a very high level to resolve a long standing experimental controversy; the interaction between helium and the MgO (100) surface has been studied extensively by other groups, employing diverse experimental approaches. Nevertheless, the binding energy of the lowest bound state is still unclear: the existence of a state at around−5.5 meV is well established but a state at−10 meV has also been reported. The MgO (100)-He system captures the fundamental physics involved in many adsorption problems; the weak binding is governed by long-range electronic correlation for which a fully predictive theory applicable to the solid state has been elusive. The above-mentioned experimental controversy can now be resolved on the basis of the calculations presented in this work. We performed three-dimensional vibrational dynamics calculations on a highly accurate potential-energy surface. The latter was constructed using a method which systematically approaches the exact limit in its treatment of electronic correlation. The outcome is clear: our calculations do not support the existence of a bound state around −10 meV.

Approaching an exact treatment of electronic correlations at solid surfaces: The binding energy of the lowest bound state of helium adsorbed on MgO(100)

MASCHIO, LORENZO;CASASSA, Silvia Maria;
2014

Abstract

In this work we employ ab initio electronic structure theory at a very high level to resolve a long standing experimental controversy; the interaction between helium and the MgO (100) surface has been studied extensively by other groups, employing diverse experimental approaches. Nevertheless, the binding energy of the lowest bound state is still unclear: the existence of a state at around−5.5 meV is well established but a state at−10 meV has also been reported. The MgO (100)-He system captures the fundamental physics involved in many adsorption problems; the weak binding is governed by long-range electronic correlation for which a fully predictive theory applicable to the solid state has been elusive. The above-mentioned experimental controversy can now be resolved on the basis of the calculations presented in this work. We performed three-dimensional vibrational dynamics calculations on a highly accurate potential-energy surface. The latter was constructed using a method which systematically approaches the exact limit in its treatment of electronic correlation. The outcome is clear: our calculations do not support the existence of a bound state around −10 meV.
89
205138
-
http://journals.aps.org/prb/abstract/10.1103/PhysRevB.89.205138
R. Martinez-Casado; D. Usvyat; L. Maschio; G. Mallia; S. Casassa; J. Ellis; M. Schütz; N. M. Harrison
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Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/2318/147121
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