Anisotropic Infrared Response of Vanadium Dioxide Microcrystals

TL;DR

This study investigates the anisotropic infrared optical properties of untwinned VO2 microcrystals across its phase transition, combining experimental polarized IR spectroscopy with ab initio calculations for comprehensive understanding.

Contribution

It provides the first detailed measurements of anisotropic phonon and electronic properties of untwinned VO2 microcrystals in both phases, supported by theoretical calculations.

Findings

Good agreement between experimental and theoretical phonon frequencies.

Identification of anisotropic phonon parameters in both phases.

Insights into electronic anisotropy related to the phase transition.

Abstract

Vanadium dioxide (VO2) undergoes a phase transition at a temperature of 340 K between an insulating monoclinic M1 phase and a conducting rutile phase. Accurate measurements of possible anisotropy of the electronic properties and phonon features of VO2 in the insulating monoclinic M1 and metallic rutile phases are a prerequisite for understanding the phase transition in this correlated system. Recently, it has become possible to grow single domain untwinned VO2 microcrystals which makes it possible to investigate the true anisotropy of VO2. We performed polarized transmission infrared micro-spectroscopy on these untwinned microcrystals in the spectral range between 200 cm-1 and 6000 cm-1 and have obtained the anisotropic phonon parameters and low frequency electronic properties in the insulating monoclinic M1 and metallic rutile phases. We have also performed ab initio GGA+U total energy calculations of phonon frequencies for both phases. We find our measurements and calculations to be in good agreement.