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Ilya Prigogine (1917 2003): Structure Formation Far from Equilibrium

Ilya Prigogine, winner of the Nobel Prize for Chemistry in 1977, died on 28 May 2003 in Brussels. He was one of the founders of modern theory of irreversibility and a leading figure in science throughout the last 50 years. Prigogine was born in Moscow on 25 January 1917. His family left Russia in 1921 and, after a stay in Germany, settled in Belgium in 1929. Prigogine Ilya Prigogine graduated in chemistry and physics from the Universite Libre de Bruxelles, carried out his PhD in chemistry there, and completed his habilitation thesis in 1945. He became a full Professor in the Faculty of Sciences at the same university in 1951 and held this position until his retirement in 1987. From 1959 to 2003 he was Director of the International Solvay Institutes of Physics and Chemistry, founded by the famous Belgian industrialist Ernest Solvay. From 1967 he was a Professor in the Physics Department of the University of Texas at Austin, where he founded the Ilya Prigogine Center for Studies in Statistical Mechanics, Thermodynamics, and Complex Systems. Prigogines research touched on an extraordinary variety of subjects, yet throughout his career he consistently worked to bring the constructive role of irreversibility into focus in the understanding of natural phenomena. His driving force was the conviction that irreversibility and the arrow of time are fundamental properties of evolution and complexification, which are ubiquitous in the natural world. He realized that he had to break with prevailing ideas to implement this conviction. At times he also felt that his work touched upon matters that extended beyond the traditional realm of the physical sciences. He then had the courage to draw epistemological, philosophical, and cultural conclusions that were in his view appropriate. Because of this continuity of ideas and this humanistic dimension, Prigogines impact on science goes further than his individual technical contributions and his well-known books. analysis of prototypical nonlinear kinetic models such as the reversible Lotka Volterra model and the Brusselator (see Figure 1). This work gradually gave rise to the concept of dissipative structure, which was formulated in 1966 1967 by Prigogine and his colleagues as a state that reflects the ability of a system to utilize energy dissipated out of equilibrium to generate novel phenomena, which arises from the thermodynamic branch of equilibrium-like states through an instability. By identifying the universal role of the distance from equilibrium as a source of order, this result provided a unifying framework for the understanding of a host of selforganization phenomena. It also introduced a type of biological thinking, which acted as a source of inspiration for many and redefined the relationship between the physical and the life sciences. A very important development that illustrates this synergy between biology, irreversibility, thermodynamics, and nonlinear kinetics is the seminal work of Manfred Eigen and his colleagues on hypercycles[2] and the evolution of biological information carriers, initiated in the late 1960s to early 1970s.

Dissipative Structures
Prigogines investigations into irreversibility started with macroscopic-level approaches. His work contributed to a renaissance of the entire field of thermodynamics. In this regard, he was lucky to have been a student in the 1940s of Theophile De Donder, one of the rare scientists of his time to believe that one could set up a consistent thermodynamic theory that extended beyond the range of equilibrium phenomena and incorporated irreversibility in an explicit manner. Prigogine built on De Donders results and in 1945 1949 worked out a general macroscopic theory of systems that operate under constraints that move them away from equilibrium. His work, along with that of Lars Onsager and Josef Meixner, led to a local formulation that culminated in the derivation of an entropy-balance equation, which featured the famous bilinear structure of entropy production. The application of this formalism to the linear range of irreversible processes led him to derive his minimum-entropyproduction theorem, in which he asserted that systems under weak nonequilibrium constraint eventually attain a stable state of minimum dissipation. Following this initial success, he and his Brussels colleague Paul Glansdorff tried for almost two decades to extend the result to the entire range of nonequilibrium phenomena, but made no substantial progress. They eventually realized that this lack of success was not of a technical nature, but rather reflected the lack of universal trends in the ways natural systems evolve away from equilibrium. Interestingly, at about the same time, the groups of Benno Hess[1] in Germany and of Anatol Zhabotinski in Russia were reporting exciting results on oscillatory behavior in biochemical and chemical systems, and provided experimental support of this idea as well as additional motivation for two novel developments: a thermodynamic-stability theory based on the excess entropy generated by the perturbations, and the www.angewandte.org

Foundations of Irreversibility
From the very early stages of his career, Prigogine recognized the need to address the microscopic foundations of irreversible phenomena. In a seminal paper published in 1949, he showed by using Boltzmanns kinetic equation that the local formalism of irreversible thermodynamics was valid only if the particles position velocity probability distribution deviated slightly from local equilibrium. This work was subsequently extended to include chemically reacting systems and still serves as a reference in understanding the origin of the phenomenological rate laws used in chemical kinetics. It also led to the prediction that deviations from these laws (associated with the appearance of a non-Maxwellian velocity distribution of the particles) are possible under certain conditions, for example, when strongly exothermic steps are present in a reaction sequence. By the mid-1950s, the need to go beyond the assumptions upon which the Boltzmann equation is
Angew. Chem. Int. Ed. 2003, 42, 3324 3325


 2003 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

grated fundamental properties of microscopic-level dynamics from the work of and Andrei KolmogorHenri Poincare ov, such as nonintegrability and resonance. This allowed him to specify the types of initial configuration that can evolve thermodynamically and to obtain formal but exact probabilistic equations for these configurations. The fundamental role of probability in the understanding of irreversibility as a time-symmetrybreaking phenomenon was thereby identified. Prigogines insatiable curiosity pushed him to become involved in an extraordinary variety of activities. He was passionate about literature, philosophy, and art, and one of his favorite pastimes was playing the piano. He attracted a large number of students and associates from all over the world. He also became actively involved in science policy, and made a decisive impact on the development of a coherent European Research Program in the mid-1980s. He insisted on the need to establish flexible mechanisms that would enable the rapid recognition and encouragement of innovative ideas from the scientific community, for which he coined the term hopeful fluctuations. Prigogine was one of the most honored scientists of our time. He was a member of the Belgian Royal Academy, the National Academy of Sciences of the USA, and the USSR Academy of Sciences, held honorary degrees from over 40 universities, and received many prestigious scientific awards in addition to the Nobel Prize,[3] such as the Francqui Prize in 1955, the Solvay Prize in 1965, the Cothenius Gold Medal of the Akademie Leopoldina in 1975, the Rumford Gold Medal of the Royal Society in 1976, and the Honda Prize in 1983. Prigogine never really retired. He was working on several projects until the very last days of his life. He authored or co-authored 16 books[4] and a huge number of specialized and review papers as well as articles addressed to the general public. He is survived by his second wife Marina Prokopowicz and his two sons Yves and Pascal. goire Nicolis Gre Libre de Bruxelles Universite Brussels (Belgium)


Figure 1. The Brusselator: In the reaction of compounds A and B to give the products D and E by the mechanism A ! X, 2X Y ! 3X, B X ! Y D, and X ! E, the same periodic trajectory for the concentrations of X and Y is always observed irrespective of the initial conditions (S: unstable stationary state).

based became Prigogines central preoccupation. In the late 1950s to early 1960s, by using a systematic perturbative approach to the solution of the Liouville equation, he and his colleagues derived irreversible-transport equations that encompassed large classes of systems, from dense fluids to anharmonic solids and plasmas. In parallel, in collaboration with Robert Herman, Prigogine developed a kinetic theory of traffic flow in which he managed to incorporate terms related to the behavioral trends of the driver. Following the advent of the concept of dissipative structure in the late 1960s, Prigogine felt that the microscopic basis of irreversibility had to be reassessed. He initiated a new approach that inte-

[1] M. Engelhardt, S. C. Mller, Angew. Chem. 2003, 115, 2432; Angew. Chem. Int. Ed. 2003, 42, 2330. [2] M. Eigen, Int. J. Quantum Chem. 1978, 219. [3] I. Prigogine, Angew. Chem. 1978, 90, 704. [4] For example, a) I. Prigogine, From Being to Becoming, W. H. Freeman, San Francisco, 1980, b) G. Nicolis, I. Prigogine, Self-Organization in Nonequilibrium Systems: From Dissipative Structures to Order through Fluctuations, John Wiley and Sons, New York, 1977; I. Prigogine, I. Stengers, ternite , Fayard, Paris, Entre le temps et le 1988.

Angew. Chem. Int. Ed. 2003, 42, 3324 3325


 2003 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim