Anisotropy of the Pressure Effect in the Ti<sub>3</sub>O<sub>5</sub> Phase Transition Process Resolved by Direction-Dependent Interface Propagation

Jütten, Stefan; Bredow, Thomas

doi:10.1021/acs.jpcc.3c04986

Cited by 5 publications

(3 citation statements)

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“…3 c). The easy propagation along the c axis arises from the lower energy barrier as compared to other two ( a and b ) directions, as recently revealed by Jütten and Bredow 27 . The deformation involving the Ti3-Ti3 dimers and associated O atoms does not propagate to the neighboring layers until the present layer completes the transition to the λ -Ti 3 O 5 -like structural motifs.…”

Section: Resultsmentioning

confidence: 52%

“…It might be worthwhile to study the influence of vibrational contributions on phase transitions in other materials that are broadly considered to be strongly correlated. We note in passing that very recently an MLP was also developed by Jütten and Bredow 27 to study the pressure effect on the phase transition of Ti 3 O 5 . However, their developed MLP was mainly used to optimize the interface models with mixed phases, while the kinetic phase transition details have not been explored.…”

Section: Discussionmentioning

confidence: 99%

“…Due to the anisotropy of the strain associated with the phase transition, the photoinduced phase transition in a single crystal of Ti 3 O 5 occurs only when the pump pulse is applied on the a b plane 17 . This process has been recently resolved by direction-dependent interface propagation using interface models optimized by machine-learned force field method 27 . A recent study on doping reveals that it primarily alters the relative energy of both phases, but not the activation barrier 28 .…”

Section: Introductionmentioning

confidence: 99%

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Layer-by-layer phase transformation in Ti3O5 revealed by machine-learning molecular dynamics simulations

Liu,

Wang,

et al. 2024

Nat Commun

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Reconstructive phase transitions involving breaking and reconstruction of primary chemical bonds are ubiquitous and important for many technological applications. In contrast to displacive phase transitions, the dynamics of reconstructive phase transitions are usually slow due to the large energy barrier. Nevertheless, the reconstructive phase transformation from β- to λ-Ti3O5 exhibits an ultrafast and reversible behavior. Despite extensive studies, the underlying microscopic mechanism remains unclear. Here, we discover a kinetically favorable in-plane nucleated layer-by-layer transformation mechanism through metadynamics and large-scale molecular dynamics simulations. This is enabled by developing an efficient machine learning potential with near first-principles accuracy through an on-the-fly active learning method and an advanced sampling technique. Our results reveal that the β−λ phase transformation initiates with the formation of two-dimensional nuclei in the ab-plane and then proceeds layer-by-layer through a multistep barrier-lowering kinetic process via intermediate metastable phases. Our work not only provides important insight into the ultrafast and reversible nature of the β−λ transition, but also presents useful strategies and methods for tackling other complex structural phase transitions.

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Section: Resultsmentioning

confidence: 52%

Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Layer-by-layer phase transformation in Ti3O5 revealed by machine-learning molecular dynamics simulations

Liu,

Wang,

et al. 2024

Nat Commun

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Pressure-induced structural and electronic transformations of energetic ionic salt hydroxylammonium 3,3′-dinitro-bis-(1,2,4-triazole)-1,1′-diolate

Zhao,

Yang

2024

Materials Today Communications

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Effect of Surface Free Energies and Particle Diameter on the Ti₃O₅ β → λ Phase Transition Temperature: A Theoretical Study

Jütten,

Bredow

2024

J. Phys. Chem. C

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The solid−solid heat-storage material Ti 3 O 5 is experimentally known to store thermal energy for long time periods and to release the accumulated energy on demand. During the heat-storage process the lower-energy β-phase is transformed into the higher-energy λ-phase, which is retained at ambient conditions, unless external pressure is applied. Therefore, the metastability of the λ-phase is a crucial aspect of the heat-storage system. In previous theoretical studies it was shown that the hysteresis cannot be explained by conventional bulk models. Here, we present a comprehensive theoretical study of the surfaces of both Ti 3 O 5 phases in order to demonstrate the effect of the surface energy on the relative phase stability. We apply the r 2 SCAN-D3 method to the calculation of surface free energies and show that most λ-phase facets are more stable than the corresponding β-phase surfaces. On the basis of calculated surface free energies we predict the temperature dependency of the crystallite morphology and estimate the size-dependent relative free energy of βand λ-particles. We show that for particles in the experimentally synthesized diameter range the inclusion of surface effects has a substantial effect on the theoretical prediction of phase transition temperatures.

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Anisotropy of the Pressure Effect in the Ti₃O₅ Phase Transition Process Resolved by Direction-Dependent Interface Propagation

Cited by 5 publications

References 51 publications

Layer-by-layer phase transformation in Ti3O5 revealed by machine-learning molecular dynamics simulations

Layer-by-layer phase transformation in Ti3O5 revealed by machine-learning molecular dynamics simulations

Pressure-induced structural and electronic transformations of energetic ionic salt hydroxylammonium 3,3′-dinitro-bis-(1,2,4-triazole)-1,1′-diolate

Effect of Surface Free Energies and Particle Diameter on the Ti₃O₅ β → λ Phase Transition Temperature: A Theoretical Study

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Anisotropy of the Pressure Effect in the Ti3O5 Phase Transition Process Resolved by Direction-Dependent Interface Propagation

Cited by 5 publications

References 51 publications

Layer-by-layer phase transformation in Ti3O5 revealed by machine-learning molecular dynamics simulations

Layer-by-layer phase transformation in Ti3O5 revealed by machine-learning molecular dynamics simulations

Pressure-induced structural and electronic transformations of energetic ionic salt hydroxylammonium 3,3′-dinitro-bis-(1,2,4-triazole)-1,1′-diolate

Effect of Surface Free Energies and Particle Diameter on the Ti3O5 β → λ Phase Transition Temperature: A Theoretical Study

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Anisotropy of the Pressure Effect in the Ti₃O₅ Phase Transition Process Resolved by Direction-Dependent Interface Propagation

Effect of Surface Free Energies and Particle Diameter on the Ti₃O₅ β → λ Phase Transition Temperature: A Theoretical Study