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RUDOLPH A. MARCUS
My first encounters with McGill University came when I
was still in a baby carriage. My mother used to wheel me about the campus when we lived in
that neighborhood and, as she recounted years later, she would tell me that I would go to
McGill. There was some precedent for my going there, since two of my father's brothers
received their M.D.'s at McGill.
I have always loved going to school. Since neither of my parents had a higher education,
my academic "idols" were these two paternal uncles and one of their uncles, my
great-uncle, Henrik Steen (né Markus). My admiration for him, living in faraway Sweden,
was not because of a teol.dr. (which he received from the University of Uppsala in 1915)
nor because of the many books he wrote - I knew nothing of that - but rather because he
was reputed to speak 13 languages. I learned decades later that the number was only 9!
Growing up, mostly in Montreal, I was an only child of loving parents. I admired my
father's athletic prowess - he excelled in several sports - and my mother's expressive
singing and piano playing.
My interest in the sciences started with mathematics in the very beginning, and later with
chemistry in early high school and the proverbial home chemistry set. My education at
Baron Byng High School was excellent, with dedicated masters (boys and girls were
separate). I spent the next years at McGill University, for both undergraduate and, as was
the custom of the time, graduate study. Our graduate supervisor, Carl A. Winkler,
specialized in rates of chemical reactions. He himself had received his Ph.D. as a student
of Cyril Hinshelwood at Oxford. Hinshelwood was later the recipient of the Nobel Prize for
his work on chemical kinetics. Winkler brought to his laboratory an enthusiastic
joyousness in research and was much loved by his students.
During my McGill years, I took a number of math courses, more than other students in
chemistry. Upon receiving a Ph.D. from McGill University in 1946, I joined the new
post-doctoral program at the National Research Council of Canada in Ottawa. This program
at NRC later became famous, but at the time it was still in its infancy and our titles
were Junior Research Officers. The photochemistry group was headed by E.W.R. Steacie, an
international figure in the study of free-radical reactions and a major force in the
development of the basic research program at NRC. I benefitted from the quality of his
research on gas phase reaction rates. Like my research on chemical reaction rates in
solution at McGill (kinetics of nitration), it was experimental in nature. There were no
theoretical chemists in Canada at the time, and as students I don't think we ever
considered how or where theories were conceived.
About 1948 a fellow post-doctoral at NRC, Walter Trost, and I formed a two-man seminar to
study theoretical papers related to our experimental work. This adventure led me to
explore the possibility of going on a second post-doctoral, but in theoretical work, which
seemed like a radical step at the time. I had a tendency to break the glass vacuum
apparatus, due to a still present impetuous haste, with time-consuming consequences.
Nevertheless, the realization that breaking a pencil point would have far less disastrous
consequences played little or no role, I believe, in this decision to explore theory!
I applied in 1948 to six well-known theoreticians in the U.S. for a postdoctoral research
fellowship. The possibility that one of them might take on an untested applicant, an
applicant hardly qualified for theoretical research, was probably too much to hope for.
Oscar K. Rice at the University of North Carolina alone responded favorably, subject to
the success of an application he would make to the Office of Naval Research for this
purpose. It was, and in February 1949 I took the train south, heading for the University
of North Carolina in Chapel Hill. I was impressed on arrival there by the red clay, the
sandy walks, and the graciousness of the people.
After that, I never looked back. Being exposed to theory, stimulated by a basic love of
concepts and mathematics, was a marvelous experience. During the first three months I read
everything I could lay my hands on regarding reaction rate theory, including Marcelin's
classic 1915 theory which came within one small step of the Transition State Theory of
1935. I read numerous theoretical papers in German, a primary language for the
"chemical dynamics" field in the 1920s and 1930s, attended my first formal
course in quantum mechanics, given by Nathan n in the Physics Department, and was
guided by Oscar in a two-man weekly seminar in which I described a paper I had read and he
pointed out assumptions in it that I had overlooked. My life as a working theorist began
three months after this preliminary study and background reading, when Oscar gently nudged
me toward working on a particular problem.
Fortunately for me, Oscar's gamble paid off. Some three months later, I had formulated a
particular case of what was later entitled by B. Seymour Rabinovitch, RRKM theory
("Rice-Ramsperger-Kassel-Marcus"). In it, I blended statistical ideas from the
RRK theory of the 1920s with those of the transition state theory of the mid-1930s. The
work was published in 1951. In 1952 I wrote the generalization of it for other reactions.
In addition, six months after arrival in Chapel Hill, I was also blessed by marriage to
Laura Hearne, an attractive graduate student in sociology at UNC. She is here with me at
this ceremony. Our three sons, Alan, Kenneth and Raymond, and two daughters-in-law are
also present today.
In 1951, I attempted to secure a faculty position. This effort met with little success (35
letters did not yield 35 no's, since not everyone replied!). Very fortunately, that spring
I met Dean Raymond Kirk of the Polytechnic Institute of Brooklyn at an American Chemical
Society meeting in Cleveland, which I was attending primarily to seek a faculty position.
This meeting with Dean Kirk, so vital for my subsequent career, was arranged by Seymour
Yolles, a graduate student at UNC in a course I taught during Rice's illness. Seymour had
been a student at Brooklyn Poly and learned, upon accidentally encountering Dr. Kirk, that
Kirk was seeking new faculty. After a subsequent interview at Brooklyn Poly, I was hired,
and life as a fully independent researcher began.
I undertook an experimental research program on both gas phase and solution reaction
rates, wrote the 1952 RRKM papers, and wondered what to do next in theoretical research. I
felt at the time that it was pointless to continue with RRKM since few experimental data
were available. Some of our experiments were intended to produce more.
After some minor pieces of theoretical study that I worked on, a student in my statistical
mechanics class brought to my attention a problem in polyelectrolytes. Reading everything
I could about electrostatics, I wrote two papers on that topic in 1954/55. This
electrostatics background made me fully ready in 1955 to treat a problem I had just read
about on electron transfers. I comment on this next period on electron transfer research
in my Nobel Lecture. About 1960, it became clear that it was best for me to bring the
experimental part of my research program to a close - there was too much to do on the
theoretical aspects - and I began the process of winding down the experiments. I spent a
year and a half during 1960-61 at the Courant Mathematical Institute at New York
University, auditing many courses which were, in part, beyond me, but which were,
nevertheless, highly instructive.
In 1964, I joined the faculty of the University of Illinois in Urbana-Champaign and I
never undertook any further experiments there. At Illinois, my interests in electron
transfer continued, together with interests in other aspects of reaction dynamics,
including designing "natural collision coordinates", learning about action-angle
variables, introducing the latter into molecular collisions, reaction dynamics, and later
into semiclassical theories of collisions and of bound states, and spending much of my
free time in the astronomy library learning more about classical mechanics, celestial
mechanics, quasiperiodic motion, and chaos. I spent the academic year of 1975-76 in
Europe, first as Visiting Professor at the University of Oxford and later as a Humboldt
Awardee at the Technical University of Munich, where I was first exposed to the problem of
electron transfer in photosynthesis.
In 1978, I accepted an offer from the California Institute of Technology to come there as
the Arthur Amos Noyes Professor of Chemistry. My semiclassical interlude of 1970-80 was
intellectually a very stimulating one, but it involved for me less interaction with
experiments than had my earlier work on unimolecular reaction rates or on electron
transfers. Accordingly, prompted by the extensive experimental work of my colleagues at
Caltech in these fields of unimolecular reactions, intramolecular dynamics and of electron
transfer processes, as well as by the rapidly growing experimental work in both broad
areas world-wide, I turned once again to those particu
lar topics and to the many new types of studies that were being made. Their scope and
challenge continues to grow to this day in both fields. Life would be indeed easier if the
experimentalists would only pause for a little while!
There was a time when I had wondered about how much time and energy had been lost doing
experiments during most of my stay at Brooklyn Poly- experiments on gas phase reactions,
flash photolysis, isotopic exchange electron transfer, bipolar electrolytes, nitration,
and photoelectrochemistry, among others-and during all of my stay at NRC and at McGill. In
retrospect, I realized that this experimental background heavily flavored my attitude and
interests in theoretical research. In the latter I drew, in most but not all cases, upon
experimental findings or puzzles for theoretical problems to study. The growth of
experiments in these fields has served as a continually rejuvenating influence. This
interaction of experiment and theory, each stimulating the other, has been and continues
to be one of the joys of my experience.
Honors received for the theoretical work include the Irving Langmair and the Peter Debye
Awards of the American Chemical Society (1978, 1988), the Willard Gibbs, Theodore William
Richards, and Pauling Medals, and the Remsen and Edgar Fahs Smith Awards, from various
sections of the ACS, (1988, 1990, 1991, 1991, 1991), the Robinson and the Centenary Medals
of the Faraday Division of the Royal Society of Chemistry (1982, 1988), Columbia
University's Chandler Medal (1983) and Ohio State's William Lloyd Evans Award (1990), a
Professorial Fellowship at University College, Oxford (1975 to 1976) and a Visiting
Professorship in Theoretical Chemistry at Oxford during that period, the Wolf Prize in
Chemistry (1985), the National Medal of Science (1989), the Hirschfelder Prize in
Chemistry (1993), election to the National Academy of Sciences (1970), the American
Academy of Arts and Sciences (1973), the American Philosophical Society (1990), honorary
membership in the Royal Society of Chemistry (1991), and foreign membership in the Royal
Society (London) (1987) and in the Royal Society of Canada (1993). Honorary degrees were
conferred by the University of Chicago and by Goteborg, Polytechnic, McGill, and Queen's
Universities and by the University of New Brunswick (1983, 1986, 1987, 1988, 1993, 1993).
A commemorative issue of the Journal of Physical Chemistry was published in 1986.
