Does the LCAO Method Create Basis Sets for Tight-Binding and Quantum Dots?

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Discussion Overview

The discussion revolves around the applicability of the Linear Combination of Atomic Orbitals (LCAO) method in creating basis sets for tight-binding models and quantum dots. Participants explore the implications of orbital overlap, orthogonality, and the relationship between LCAO and Bloch's Theorem in different contexts, including density functional theory (DFT) and nanostructures.

Discussion Character

  • Exploratory
  • Technical explanation
  • Debate/contested
  • Homework-related

Main Points Raised

  • Some participants question whether the LCAO method implies tight-binding, particularly in cases of appreciable overlap between atomic orbitals, suggesting that orthogonality may not be maintained.
  • Others argue that if there is significant overlap, perturbation theory may not be applicable for obtaining eigenstates, referencing texts that assume no overlap.
  • One participant mentions using the LCAO approach for metals in DFT simulations with a double-zeta polarized (DZP) basis set, noting that these orbitals are not true quantum mechanical atomic orbitals but rather parametrized forms.
  • There is inquiry into whether DZP basis sets can be applied to tight-binding schemes, despite not being atomic orbitals.
  • Participants discuss the implications of limited periodicity in quantum dots, questioning whether the wave function of an electron would conform to Bloch's Theorem and whether LCAOs must obey this theorem in tight-binding calculations.
  • One response indicates that Bloch's Theorem remains valid under certain crystal symmetries, even in small materials, and mentions its application in interface simulations.
  • Concerns are raised about the limitations of DFT simulations, particularly regarding the maximum number of atoms that can be included in input cells.

Areas of Agreement / Disagreement

Participants express differing views on the implications of orbital overlap and the applicability of Bloch's Theorem in the context of quantum dots and tight-binding models. The discussion remains unresolved regarding the extent to which LCAO can be applied under these conditions.

Contextual Notes

Limitations include the dependence on definitions of overlap and orthogonality, as well as the unresolved nature of how LCAO interacts with Bloch's Theorem in non-periodic systems.

Modey3
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Hello,

Haven't been here in a while. Does the Linear Combination of Atomic Orbitals (LCAO) method of developing a basis set imply tight-binding ? Is there a way of using this basis set for not so tigtly bound (there is appreciable overlap) atomic orbitals and still maintain orthagonality between the atomic orbitals, which is required for a basis set representing the lattice wavefuntion ? I'm leaning towards no, but maybe somebody else has other information.

Best Regards

Modey3
 
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I'd lean to no aswell. If you have appreciative overlap you can't really use perturbation theory to get the eigenstates. A couple of texts I checked also assumed that there's no overlap at all.
 
Modey3 said:
Is there a way of using this basis set for not so tigtly bound (there is appreciable overlap) atomic orbitals and still maintain orthagonality between the atomic orbitals, which is required for a basis set representing the lattice wavefuntion ?
Modey3

One can even use the LCAO approach to study metals like Ta. I am currently doing such DFT simulations where i use a DZP basis set to describe the electronic wavefunctions. Keep in mind that these orbitals are NOT really the QM atomic orbitals. They contain parametrisations that arise from the DFT formalism. Check the Vanderbilt website for more info.

marlon
 
Thanks Marlon,

DZP basis sets are new to me (I just started learning about Ab Initio modeling). Are they only used to provide the basis sets for DFT , or can they be applied to tight-binding schemes even though they arn't atomic orbitals.

This is a little off topic. When studying quantum dots that have limited periodicity. Is it true that the wave function of an electron will not have the form dictated by Blochs Theorem? When one does tight binding calculations for quantum dots do we throw out the requirement that the LCAOs for each orbital (s,p etc..) obey Blochs Theorem? I'm still trying to learn the subtle difference in doing bulk and nanostructure calculations.

Regards

Modey3
 
Modey3 said:
Thanks Marlon,

DZP basis sets are new to me (I just started learning about Ab Initio modeling). Are they only used to provide the basis sets for DFT , or can they be applied to tight-binding schemes even though they arn't atomic orbitals.

Yes ofcourse. These basis sets contain parameters that you can change. By changing them you acquire wavefunctions that resemble the atomic orbitals at hand while keeping the computational effort "low".

This is a little off topic. When studying quantum dots that have limited periodicity. Is it true that the wave function of an electron will not have the form dictated by Blochs Theorem? When one does tight binding calculations for quantum dots do we throw out the requirement that the LCAOs for each orbital (s,p etc..) obey Blochs Theorem? I'm still trying to learn the subtle difference in doing bulk and nanostructure calculations.

Regards

Modey3

The Bloch Theorem is valid due to the atomic/crystal structure of the material at hand. Even if the material is very small, Blochwaves can still be used as long as there is certain crystal symmetry.

For example, Bloch waves are used in interface simulations of a metal gate and a high k material. The magnitude of such a system is in the nanometer range (ie the thickness). Keep in mind that with DFT, one can only simulate input cells containing 200 atoms at maximum !

regards
marlon
 

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