LAPW vs. LMTO full-potential simulations and anharmonic dynamics of KNbO3

TL;DR

This study compares FP-LMTO and LAPW methods for simulating KNbO3, demonstrating that high-precision charge density descriptions reconcile previous discrepancies and introducing a scheme for analyzing anharmonic vibrational dynamics.

Contribution

It provides a detailed comparison of two computational methods for KNbO3 and proposes a new approach to analyze anharmonic vibrational effects beyond the harmonic approximation.

Findings

High-precision charge density description aligns FP-LMTO and LAPW results.

Discrepancies in earlier studies were due to technical limitations in charge density accuracy.

A new scheme for solving the multidimensional vibrational Schrödinger equation is introduced.

Abstract

With the aim to get an insight in the origin of differences in the earlier reported calculation results for KNbO3 and to test the recently proposed implementation of the FP-LMTO method by Methfessel and van Schilfgaarde, we perform a comparative study of the ferroelectric instability in KNbO3 by FP-LMTO and LAPW methods. It is shown that a high precision in the description of the charge density variations over the interstitial region in perovskite materials is essential; the technical limitations of the accuracy of charge-density description apparently accounted for previously reported slight disagreement with the LAPW results. With more accurate description of the charge density by sufficiently fine real-space grid, the results obtained by both methods became almost identical. In order to extract additional information (beyond the harmonic approximation) from the total energy fit obtainable in total-energy calculations, a scheme is proposed to solve the multidimensional vibrational Schroedinger equation in the model of non-interacting anharmonic oscillators via the expansion in hyperspherical harmonics.