High-Throughput Design of Peierls and Charge Density Wave Phases in Q1D Organometallic Materials

TL;DR

This study introduces a first-principles approach to predict symmetry-lowering phases in Q1D organometallic materials using soft-phonon modes, validated on a large materials dataset, and provides an accessible data platform.

Contribution

It validates the 1/q*-criterion for designing low-dimensional materials and identifies various stable phases, including novel gap-closing transitions, with a publicly available data platform.

Findings

Validated the 1/q*-criterion for phase prediction

Identified stable phases in 1199 Q1D materials

Discovered materials with gap-opening and gap-closing transitions

Abstract

Soft-phonon modes of an undistorted phase encode a material's preference for symmetry lowering. However, the evidence is sparse for the relationship between an unstable phonon wavevector's reciprocal and the number of formula units in the stable distorted phase. This "1/q*-criterion" holds great potential for the first-principles design of materials, especially in low-dimension. We validate the approach on the Q1D materials space containing 1199 ring-metal units and identify candidates that are stable in undistorted (1 unit), Peierls (2 units), charge density wave (3-5 units), or long wave (>5 units) phases. We highlight materials exhibiting gap-opening as well as an uncommon gap-closing Peierls transition, and discuss an example case stabilized as a charge density wave insulator. We present the data generated for this study through an interactive publicly accessible Big Data analytics platform (http://moldis.tifrh.res.in/data/rmq1d) facilitating limitless and seamless data-mining explorations.