Simulations of bulk solids and liquids at an accurate ab initio theoretical level treating all electrons quantum mechanically have long been unthinkable. We present just such simulations for a whole range of structural, dynamical, thermodynamic and response properties of ice (phase Ih), high-pressure ice (phase VIII), dry ice (solid CO2 phase I), high-pressure dry ice (solid CO2 phase III) and liquid water. They are made possible by combining an algorithmic breakthrough (the embedded-fragmentation technique) with the massive computational power of Blue Waters. The calculated properties include structures, equation of state, bulk modulus, thermal expansion, heat capacities, pressure tuning of Fermi resonance, infrared, Raman, and inelastic neutron scattering spectra, solid-solid phase transition, self-diffusion coefficients, Raman noncoincidence, hydrogen-bond lifetime and reorganization in the liquid, some of which accessible only by predictive high-performance computing.
