{
  "id": "1207.3427",
  "version": "v1",
  "published": "2012-07-14T14:36:43.000Z",
  "updated": "2012-07-14T14:36:43.000Z",
  "title": "Towards a microscopic description of the free-energy landscape of water",
  "authors": [
    "Diego Prada-Gracia",
    "Roman Shevchuk",
    "Peter Hamm",
    "Francesco Rao"
  ],
  "categories": [
    "cond-mat.stat-mech",
    "physics.chem-ph"
  ],
  "abstract": "Free-energy landscape theory is often used to describe complex molecular systems. Here, a microscopic description of water structure and dynamics based on configuration-space-networks and molecular dynamics simulations of the TIP4P/2005 model is applied to investigate the free-energy landscape of water. The latter is built on top of a large set of water microstates describing the kinetic stability of local hydrogen-bond arrangements up to the second solvation shell. In temperature space, the landscape displays three regions with an overall different organization. At ambient conditions, the free-energy surface is characterized by structural inhomogeneities with multiple, structurally well defined, short-lived basins of attraction. Below around ambient temperature, the liquid rapidly becomes homogeneous. In this regime, the landscape is funneled-like, with fully-coordinated water arrangements at the bottom of the funnel. Finally, a third region develops below the temperature of maximal compressibility (Widom line) where the funnel becomes steeper with few interconversions between microstates other than the fully coordinated ones. Our results present a viable a way to manage the complexity of water structure and dynamics, connecting microscopic properties to its ensemble behavior.",
  "revisions": [
    {
      "version": "v1",
      "updated": "2012-07-14T14:36:43.000Z"
    }
  ],
  "analyses": {
    "subjects": [
      "65.20.Jk",
      "61.20.Ja",
      "61.20.Ne",
      "62.10.+s",
      "82.30.Rs"
    ],
    "keywords": [
      "microscopic description",
      "water structure",
      "second solvation shell",
      "local hydrogen-bond arrangements",
      "molecular dynamics simulations"
    ],
    "tags": [
      "journal article"
    ],
    "publication": {
      "doi": "10.1063/1.4755746",
      "journal": "Journal of Chemical Physics",
      "year": 2012,
      "month": "Oct",
      "volume": 137,
      "number": 14,
      "pages": 4504
    },
    "note": {
      "typesetting": "TeX",
      "pages": 0,
      "language": "en",
      "license": "arXiv",
      "status": "editable",
      "adsabs": "2012JChPh.137n4504P"
    }
  }
}