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Efficient and improved prediction of the band offsets at semiconductor heterojunctions from meta-GGA density functionals: a benchmark study

A. Ghosh, S. Jana, T. Rauch, F. Tran, M. Marques, S. Botti, L. A. Constantin, M. K. Niranjan, P. Samal

The Journal of Chemical Physics, 157, 124108, (2022)

DOI: 10.1063/5.0111693

Download: BibTEX

Accurate theoretical prediction of the band offsets at interfaces of semiconductor heterostructures can often be quite challenging. Although density functional theory has been reasonably successful to carry out such calculations, efficient, accurate semilocal functionals are desirable to reduce the computational cost. In general, the semilocal functionals based on the generalized gradient approximation (GGA) significantly underestimate the bulk bandgaps. This, in turn, results in inaccurate estimates of the band offsets at the heterointerfaces. In this paper, we investigate the performance of several advanced meta-GGA functionals in the computational prediction of band offsets at semiconductor heterojunctions. In particular, we investigate the performance of r2SCAN (two times revised strongly constrained and appropriately normed functional), rMGGAC (revised semilocal functional based on cuspless hydrogen model and Pauli kinetic energy density functional), mTASK (modified Aschebrock and Kümmel meta-GGA functional), and local modified Becke–Johnson exchange-correlation functionals. Our results strongly suggest that these meta-GGA functionals for supercell calculations perform quite well, especially, when compared to computationally more demanding GW calculations. We also present band offsets calculated using ionization potentials and electron affinities, as well as band alignment via the branch point energies. Overall, our study shows that the aforementioned meta-GGA functionals can be used within the density functional theory framework to estimate the band offsets in semiconductor heterostructures with predictive accuracy.

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{"type":"article", "name":"a.ghosh20229", "author":"A. Ghosh and S. Jana and T. Rauch and F. Tran and M. Marques and S. Botti and L. A. Constantin and M. K. Niranjan and P. Samal", "title":"Efficient and improved prediction of the band offsets at semiconductor heterojunctions from metaGGA density functionals: a benchmark study", "journal":"The Journal of Chemical Physics", "volume":"157", "OPTnumber":"12", "OPTmonth":"9", "year":"2022", "OPTpages":"124108", "OPTnote":"", "OPTkey":"density functional theory; exchange correlation functionals; electronic band structure; semiconductor heterostructures; electrostatics; generalized gradient approximations; complex analysis; Ions and properties; heterointerfaces; GW-approximation", "DOI":"10.1063/5.0111693"}
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