Identification of sub-angstrom many-body localization in quantum materials by Bragg scattering phase breaking and ultrafast structural dynamics

TL;DR

This paper introduces a novel ultrafast structural response method using Bragg scattering phase breaking to identify sub-angstrom local correlated structures in quantum materials, revealing many-body localization and topological order.

Contribution

It proposes a new approach to directly detect atomic-scale local correlated structures driven by many-body interactions in quantum materials.

Findings

Identification of static off-center Ag displacements in AgCrSe2

Observation of transition from static to dynamic local structures with temperature

Reproduction of local structures through density functional theory simulations

Abstract

Defects, fluctuations, degenerate states and correlated interactions facilitate the emergence of exotic properties in condensed matter systems while also inducing atomic-scale local correlated structures that deviate from the average long-range order. Establishing the structure-property relationship from the perspective of these atomic-scale local correlated structures remains ambiguous and controversial due to the lack of direct methods for identifying such local correlated structures. In this work, based on the photoexcited ultrafast structural response, we propose a Bragg scattering phase breaking regime to identify the sub-angstrom local correlated structures in quantum materials. With this regime, we unambiguously identify the many-body-interaction driven local correlated structures with static off-center Ag displacements of 0 to 0.5 angstrom in the low temperature ground state of AgCrSe2. As temperature rising, these static local correlated structures transform to a dynamic state where the thermal fluctuations overwhelm the multiple localized quantum states, signifying the strong anharmonicity of the local structures. The state-of-the-art density functional theory simulation well reproduces the intrinsic many-body-interaction driven local correlated structures. These unique local correlated structures evidence the first many-body localization with topological order characteristic in real material systems and provide a unified scenario for the versatile quantum properties in single crystalline AgCrSe2. Our work not only offers a universal approach to characterize sub-angstrom local correlated structures across a wide range of quantum materials but also deepens our understanding of the fundamental mechanism behind exotic properties from the perspective of atomic-scale local correlated structures.