ACS Award in Theoretical Chemistry presented to Frank H. Stillinger

For pioneering computer simulations of water; developing inherent structure theory of liquids and glasses; and profound theoretical insights on water, fluid interfaces, and particle packings

Sponsored by Dell Incorporated

Lecture given at the American Chemical Society Award Meeting April 9, 2013

"Chiral Symmetry Breaking Models for Pre-biotic Environments"

Journal of Physical    Chemistry B    Frank H. Stillinger    Festschrift    [Table of Contents]      Frank's autobiography    "The factors that capture attention and create long-term interests in young children have been, and will remain, subjects of speculation and debate." (more) Tributes

Linear tunnel composed of stacked equilateral trivacancies in a hexagonal close-packed crystal of hard spheres.

His past research activity has involved the molecular theory of water and aqueous solutions, the physical chemistry of solid and liquid surfaces, and atomic and molecular quantum theory. His discoveries include:

• Critical point confluence phenomena (2018)
• The perfect glass paradigm (2016)
• Existence of maximally-disordered jammed packings of monodisperse hard disks (2014).
• Microscopic model for chiral symmetry breaking (2010).
• Diamond and wurtzite structures self-assemble with isotropic pair potentials (2007).
• Statistical mechanical model for inverse melting (2003).
• Kinetically diverse energy landscapes with identical thermodynamics (2002).
• Convergence-limiting singularities in atomic and molecular quantum theory (2000).
• Connection between spinodal curves and mechanical strength of glasses (1997)
• Long-range broken symmetry in impurity-perturbed disk crystals (1995)
• Resolution of the translation-rotation paradox in fragile glass formers (1993)
• Planck's constant expansion for quantum mechanical bound states (1991)
• Impossibility of "ideal" glass transitions in molecular liquids (1988)
• Stillinger-Weber potential for silicon (1986)
• Inverse Lindemann criterion for freezing of liquids (1985)
• Inherent structure theory for liquids (1981)
• Axiomatic basis for spaces with fractional dimension (1977)
• Semiconductor heterostructures supporting bound states in the continuum (1977)
• "Fast sound" in water (1974)
• The Stillinger-Lovett second moment identity for electrolytes (1968)
• Capillary wave theory for liquid interfaces (1965).

What is the "energy landscape" formalism?

Dr. Stillinger has created and exploited the novel approach to condensed-matter phenomena that has become widely known as the "energy landscape" formalism, a colloquial phrase that alludes to the vastly complicated multidimensional potential energy function for many-body systems. This general formalism encompasses equilibrium thermodynamics, irreversible processes, solid and fluid states of matter, and both quantum and classical dynamical systems. Its unconventional strategy has revealed many surprising results. One of the first was the fact that all liquids possess an underlying average "inherent structure" that exhibits enhanced short-range order. Furthermore the energy landscape formalism automatically supplies a novel freezing criterion for liquids that is a conceptual twin to the well-known Lindemann melting criterion for crystals. The natural division of the landscape space into geometrically precise "basins of attraction", each containing its own "inherent structure" minimum, leads to correspondingly precise definitions of metastable states of matter. In application to supercooled liquids and the glasses they form, the Stillinger approach has identified for the first time that the relevant portion of the potential energy landscape exhibits an anomalously rugged topography containing large "metabasin" features. The existence of these metabasins explains the appearance of distinct "alpha" and "beta" relaxation modes in strongly supercooled glass formers. Another important conclusion provided by the Stillinger formalism is that the popular hypothesis of an "ideal glass transition" at positive temperature is not possible for chemically or physically realistic interactions between atoms or molecules. The energy landscape representation and its emphasis on mechanically stable inherent structures leads to a clean identification of an intrinsic profile for liquid-vapor interfaces; this intrinsic profile construction for the first time excludes capillary wave fluctuations without artificial reliance on arbitrary parameters not present in the potential energy function. Subsequent to its introduction the landscape/inherent structure approach has been applied by many others to reveal new insights for gas-phase clusters, for thin films of a wide range of substances, and for the folding landscapes of polypeptides and proteins.

A permanent archival copy of this website is preserved at

- Internet Archive
https://https://archive.org/details/@frank_stillinger

- Zenodo
DOI 10.5281/zenodo.18211425 (this is the universal DOI)
https://zenodo.org/records/18211425