Large-scale atomistic simulation of quantum effects in SrTiO3 from first principles

Quantum effects of lattice vibration play a major role in many physical properties of condensed-matter systems, including thermal properties, such as specific heat, structural phase transition, as well as phenomena, such as quantum crystal and quantum paraelectricity that are closely related to zero-point fluctuations. However, realizing atomistic simulations for realistic materials with a fully quantum-mechanical description remains a great challenge. Here, we propose a first-principles strategy for large-scale molecular dynamics simulation, where a high-accuracy force field obtained by deep-potential (DP) is combined with quantum thermal bath (QTB) method to account for quantum effects. We demonstrate the power of this DP+QTB method using the archetypal example SrTiO3, which exhibits several phenomena induced by quantum fluctuations, such as the suppressed structure phase-transition temperature, the quantum paraelectric ground state at low temperatures and the quantum critical behavior 1/T2 law of dielectric constant. Our DP+QTB strategy is efficient in simulating large-scale system and is first principles. More importantly, quantum effects of other systems could also be investigated as long as the corresponding DP model is trained. This strategy would greatly enrich our vision and means to study quantum behavior of condensed-matter physics.

Automated summary

Quantum effects of lattice vibration have a significant impact on the physical properties of condensed-matter systems. However, simulating realistic materials with a fully quantum-mechanical description remains challenging. In this study, a first-principles strategy combining a high-accuracy force field and quantum thermal bath method is proposed to account for quantum effects in molecular dynamics simulations. The efficiency and applicability of this strategy are demonstrated using the example of SrTiO3, highlighting its potential for studying quantum behavior in condensed-matter physics.