Orbital-energy-based atomistic properties#

The orbital-energy-based properties are computed based on the orbital energies of the system. A localization of the orbitals is performed to obtain the atomic properties. The following properties are available:

Orbital-energy-based properties#

Dictionary Key

Description

Equation

response

response function

\(\chi_A = \sum_{i=1}^{n_{\text{occ.}}} \sum_{a=1}^{n_{\text{virt.}}} \chi_A^{ia}\) \(\chi_A^{ia} = \frac{p_{i,A} p_{a,A}}{\Delta\varepsilon^2_{ai}+\Delta^2} \text{ with: } i \in \text{occ. orbital}, a \in \text{virt. orbital}\)

gap

atomistic HL-gap in eV

\(\epsilon_{A,\text{HL-gap}} = \frac{1}{\sum_{i=1}^{n_{\text{occ.}}} \sum_{a=1}^{n_{\text{virt.}}} \lambda_A^{ia}\frac{1}{\Delta\varepsilon_{ia}+\Delta}}-\Delta \text{ with: } \lambda_A^{ia}=\frac{\chi_A^{ia}}{\sum_{j,b}\chi_A^{jb}}\)

chem_pot

chemical potential of an atom

\(\epsilon_{A,F} = \sum_{i=1}^{n_{\text{occ.}}} \sum_{a=1}^{n_{\text{virt.}}} \lambda_A \frac{\varepsilon_a+\varepsilon_i}{2}\)

HOAO

highest occupied atomic orbital

\(\epsilon_{A,\text{HOAO}} = \epsilon_{A,F} - \frac{\epsilon_{A,\text{HL-gap}}}{2}\)

LUAO

lowest unoccupied atomic orbital

\(\epsilon_{A,\text{LUAO}} = \epsilon_{A,F} + \frac{\epsilon_{A,\text{HL-gap}}}{2}\)

where \(\Delta = 0.5 \text{ eV}\) is a damping factor to avoid division by zero.

Note

For calculations with unpaired electrons, the properties are available for the alpha and beta spin channel separately. Without spin polarization, tblite does not provide two sets of density matrices and occupation vectors. In that case, we define occupation vectors that match the number of unpaired electrons using integer occupations. When using spin-polarized Hamiltonians, we use the occupation vectors and orbital energies from solving the UHF equations. In both cases the properties are computed for the alpha and beta spin channel separately. In this case all properties are available with the suffix _alpha and _beta for the alpha and beta spin channel, respectively.

Extended orbital-energy-based atomistic properties#

The extended orbital-energy-based properties are computed based on the atomic properties seen above. The convolution kernel \(f_{\text{log}}(R_A,R_B)\) has been defined in the xtbml section. The following properties are available:

Extended orbital-energy-based properties#

Dictionary Key

Description

Equation

ext_gap

ext. atomistic HL-gap in eV

\(\epsilon_{A,\text{HL-gap, ext}} = \sum_B \epsilon_{B,\text{HL-gap}} \cdot \beta(A,B)\) with: \(\beta(A,B) = \frac{1}{f_{\text{log}}(R_A,R_B) \cdot(\text{CN}_A+1)}\)

ext_chem_pot

ext. chemical potential of an atom

\(\epsilon_{A,F,\text{ext}} = \sum_{B} \mu_{B,F} \cdot \beta(A,B)\)

ext_HOAO

ext. highest occupied atomic orbital

\(\epsilon_{A,\text{HOAO}} = \epsilon_{A,F,\text{ext}} - \frac{\epsilon_{A,\text{HL-gap, ext}}}{2}\)

ext_LUAO

ext. lowest unoccupied atomic orbital

\(\epsilon_{A,\text{LUAO}} = \epsilon_{A,F,\text{ext}} + \frac{\epsilon_{A,\text{HL-gap, ext}}}{2}\)