Related papers: Ab initio thermodynamics of liquid and solid water
Machine learning models are rapidly becoming widely used to simulate complex physicochemical phenomena with ab initio accuracy. Here, we use one such model as well as direct density functional theory (DFT) calculations to investigate the…
Hexagonal ice ($\rm{I_h}$), the most common structure of ice, displays a variety of fascinating properties. Despite major efforts, a theoretical description of all its properties is still lacking. In particular, correctly accounting for its…
Water is one of the most abundant substances on Earth, and ice, i.e., solid water, has more than 18 known phases. Normally ice in nature exists only as Ice Ih, Ice Ic, or a stacking disordered mixture of both. Although many theoretical…
We have applied path integral simulations, in combination with new ab initio based water potentials, to investigate nuclear quantum effects in liquid water. Because direct ab initio path integral simulations are computationally expensive, a…
Liquid water exhibits several important anomalous properties in the vicinity of the melting temperature ($T_{\mathrm{m}}$) of ice Ih, including a higher density than ice and a density maximum at 4~$^{\circ}$C. Experimentally, an isotope…
The electronic properties and optical response of ice and water are intricately shaped by their molecular structure, including the quantum mechanical nature of hydrogen atoms. In spite of numerous studies appeared over decades, a…
Water is of the utmost importance for life and technology. However, a genuinely predictive ab initio model of water has eluded scientists. We demonstrate that a fully ab initio approach, relying on the strongly constrained and appropriately…
Several thermodynamic properties of ice Ih, II, and III are studied by a quasi-harmonic approximation and compared to results of quantum path integral and classical simulations. This approximation allows to obtain thermodynamic information…
The phase diagram of water harbours many mysteries: some of the phase boundaries are fuzzy, and the set of known stable phases may not be complete. Starting from liquid water and a comprehensive set of 50 ice structures, we compute the…
Various condensed phases of water, spanning from the liquid state to multiple ice phases, have been systematically investigated under extreme conditions of pressure and temperature to delineate their stability boundaries. This study focuses…
Although liquid water is ubiquitous in chemical reactions at roots of life and climate on the earth, the prediction of its properties by high-level ab initio molecular dynamics simulations still represents a formidable task for quantum…
Proton ordering in water ice is a paradigmatic order-disorder transition in a locally constrained system. The ice rules require exactly two hydrogens close to each oxygen, restricting the disorder to an exponentially large yet strongly…
Ice nucleation is a process of great relevance in physics, chemistry, technology and environmental sciences, much theoretical and experimental efforts have been devoted to its understanding, but still it remains a topic of intense research.…
Molecular simulations have provided valuable insight into the microscopic mechanisms underlying homogeneous ice nucleation. While empirical models have been used extensively to study this phenomenon, simulations based on first-principles…
The thermal properties of ice, liquid water and steam are at odds with statistical theories applied to many-body systems. Here, these properties are quantitatively explained with a bulk-scale matter field emerging from the indefinite status…
We examine the influence of the main approximations employed in density-functional theory descriptions of the solid phase of molecular hydrogen near dissociation. We consider the importance of nuclear quantum effects on equilibrium…
Most water in the universe may be superionic, and its thermodynamic and transport properties are crucial for planetary science but difficult to probe experimentally or theoretically. We use machine learning and free energy methods to…
We consider general theoretical models of water and in particular the nature of the motions of the hydrogen nuclei. If the motion of hydrogen nuclei is classical, then the thermodynamic pressure equation of state for heavy water wherein the…
Owing to their small mass, hydrogen atoms exhibit strong quantum behavior even at room temperature. Including these effects in first principles calculations is challenging, because of the huge computational effort required by conventional…
Water adopts many different crystal structures in its solid form. These provide insight into potential structures of water even in its liquid phase, and they can be used to calibrate pair potentials used for simulation of water. In crowded…