Publishers Note

Sir John A. Pople, 19252004

It is with great sadness that we note the passing of Sir John A.

Pople, one of the founding figures of computational chemistry. Dr.
Pople died of cancer on March 15, 2004 at the age of 78.
The following are reflections on the life and work of
John Pople, from the Editors of the Journal of Computational
Chemistry.

ohn Pople was a towering figure in the field of Theoretical and Computational Chemistry. Trained as a
mathematician, his interests developed towards theoretical
chemistry through the influence of his Ph.D. advisor Sir
John Lennard-Jones at the University of Cambridge, where
Pople began his academic career. After becoming a Lecturer
in the Mathematics faculty, in 1958 he was named head of
the Basics Physics Division at the National Physical Laboratory near London. In 1964, he moved to the USA as
Professor for Physical Chemistry at Carnegie-Mellon University. Following his retirement from CMU in 1993, Pople
became Board of Trustees Professor at Northwestern University and continued his very active career. Poples early
papers in statistical mechanics attracted attention, but he
became well known for his theoretical work in NMR spectroscopy and his seminal contributions to and valence
electron theory. Pople developed the PPP (Pariser-ParrPople) and the CNDO/INDO/NDDO set of approximate
methods. His important NMR (with Bernstein and Schneider, 1959) and semi-empirical MO (with Beveridge, 1970)
monographs remained standard references for many years.
John Pople recognized very early that ab initio methods
were the future of molecular quantum chemistry, but was
discouraged by the primitive computational capabilities and
the cumbersome programs of the day. In the late 1960s,
after his experience with the semi-empirical methods, he
began the development of a simple-to-use ab initio program
package, which could be employed by non-theoreticians.

This truly pioneering endeavor culminated with the release

of the first version, Gaussian70, of a continuing series in
1970. As Pople had planned, the very user-friendly input
system and its versatility, untypical for other early quantum
chemical programs, attracted and enabled many non-specialists to use quantum chemistry in their research. For more
than 30 years Gaussian has been the standard program in
computational quantum chemistry, and its development
continues vigorously in the hands of Poples former students.
John Pople also was at the forefront of theoretical
method development, which he then made available to the
community by distributing the Gaussian source code at
moderate cost. Meticulous evaluation of the performance of
various theoretical levels against the best available data, the
use of comparison equations designed to cancel errors, and
the systematic assessment and improvement of theoretical
methods, are very important legacies of Poples approach to
computational chemistry.
Poples classic book, Ab Initio Molecular Orbital Theory (with Hehre, Radom, and Schleyer, Wiley, 1985),
retains its usefulness even today. Pople, a founding member
of the Editorial Board of the Journal of Computational
Chemistry, was a leading promulgator of the application of
computational methods to chemistry. His efforts popularized quantum chemistry and influenced chemists, physicists,
and biochemists alike. His collaborations with chemists
solved difficult problems with quantum chemical methods.
Knighted by Queen Elizabeth II in 2003, Sir John A. Pople
as a forerunner in method advances, program development,
and application to chemical problems. In 1998, the Nobel
Prize in Chemistry was awarded to him for his development of computational methods in quantum chemistry.
Gernot Frenking, Paul von R. Schleyer

2004 Wiley Periodicals, Inc.

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Journal of Computational Chemistry

I knew John from the days of the PPP (Pariser-ParrPople) methods in quantum chemistry, which we utilized in
the early 1960s in studying the electronic spectra of aromatic molecules. In the late 1960s and early 70s, John and
I talked about the ways computational chemistry might
reasonably progress. I remember several discussions concerning the fact that the subject was having such a large
impact outside of university science, and was moving into
the commercial world. His decision was to push ab initio
methods, which he felt would be very important eventually.
Ab initio calculations were still in a rather primitive state
then, and it was Johns development of the idea of using a
series of Gaussian orbitals to represent a Slater orbital
which really made all the difference. Eventually arrived
much sooner than most of us had expected. At that time,
there was no general appreciation of the fact that such large
basis sets would be required, to do most of the calculations
chemists were interested in doing. And the importance of
electron correlation, although a nagging worry, was not of
major concern. John had a handle on all of this, he knew
what to do, and more importantly, he did it. He also had the
foresight to keep developing the methods in a way that was
consistent with the parallel development occurring in the
computers themselves. And it was simultaneous development of computers and computational methods that got
computational chemistry to where it is today. And I think
that most people in the field would agree that John Pople
was the single most important driving force in moving
computational chemistry from where it was a generation
ago to where it is today.
In 1978 1979 I had extensive discussions with Alan
Whitman, a publisher at John Wiley, regarding the possible
establishment of a Journal of Computational Chemistry. He
wanted me to be the editor. By that time, computational
chemistry had become a field of its own, rather than just a
sub-branch of theoretical chemistry. Clearly being the editor
of a new journal in this field would require a great deal of
time and effort, and while I quickly agreed that it would be
a good idea to have such a journal, I was reluctant to
become the editor. I discussed the matter at some length
with John, as I wanted him to play a key role in the startup
phase of the journal by being an effective member of the
Editorial Advisory Board. He too thought that it was time to
found a Journal of Computational Chemistry, and he was
willing to serve on the Advisory Board. Had he not agreed,
the Journal may not have been founded. We published the
first issue in the Spring, 1980. Norman L. Allinger
John Pople changed my life. His influence not only
altered my major research direction, but also led to my
move to Germany primarily in order to have access to more
computer time. I first met John during the unsuccessful
Princeton University Bell Laboratories attempt to woo

him in the early 1960s, but my series of 1968 NSF Center

of Excellence lectures on carbocations at Carnegie-Mellon
initiated our 15-year collaboration. My research group had
been devising a molecular mechanics program and applying
it to rings and strained bridgehead carbocations. We also
had some experience with semi-empirical and ab initio
computations, in collaboration with my Princeton colleague,
L. C. Allen. However, computer time at Princeton was very
limited and the Gaussian program Pople and his group were
developing was much faster. As nonclassical carbocations
afforded good computational opportunities, I first became
Johns consultant, then (after learning some rudiments of
theory) his guinea pig, and very soon his missionary
spreading the ab initio gospel to the disbelieving and resisting chemical masses.
Johns goal was to devise an ab initio computer program
which chemists, without a deep theoretical background,
might employ as a tool in their research. As the semiempirical approach, which Pople had invented, was not
accurate enough, he turned to ab initio methods, which
could be improved systematically. It was widely feared in
the theoretical community that black box users would
make a mess of things and defeat the purpose. In effect, my
research group and I were employed to test these misgivings. Evidently, we passed. John declined to co-author only
one paper (on protonated ozone); in all, we published over
70 together.
Perforce, Johns coworkers at CMU carried out almost
all the computations on joint projects until my sabbatical
leave in Munich in 1974 1975. Rolf Huisgen enabled the
small research group who had come with me to use the
facilities of both the computer center and the education and
cultural ministry. This opportunity to explore ones ideas
hooked me completely. I decided then and there to accept
the Institute Chair and the large fraction of computer time
offered by the University of Erlangen-Nuremberg.
My frequent visits with John at CMU during trips back to
the US, were augmented by his award of a Senior von
Humbolt Fellowship (1980). By dividing the months
granted into several stints, John became a regular summer
visitor to Erlangen and our houseguest in the Wagner
Villa. My stays with Joy and John in Pittsburgh underscored the devotion John had for his wife and children. I
was thrilled to be Johns guest at the Nobel Prize festivities
in Stockholm in 1998. In 2003, he achieved his life-long
ambition of Knighthood.
So many reminiscences flash through my mind. John was
a private person, but he liked to relate vignettes of his life
and career (see his brief autobiography on the Nobel website). As John felt he could not make a profound mark as a
mathematician, he chose chemistry because it was easier.
His initial application from CMU to join the American
Chemical Society was rejected, since he had not taken the

Publishers Note

required number of chemistry courses. While a student in

Cambridge, he inadvertently tormented the renowned philosopher, Ludwig Wittgenstein, by practicing learning the
piano in the dormitory garret they shared.
John was noted for the brevity of his scientific explanations. The sophistication of his answers, always pithy, depended on his perception of the level of knowledge of his
questioner, but always seemed understandable. He advised,
Let the data speak for itself; you dont need detailed
interpretations in the text. John enjoyed our many sightseeing trips in Germany, the first to Rothenburg-ob-derTauber shortly after my arrival. Yitzhak Apeloig took us to
Gamla, one of the last Zealot strongholds in Israel. We
shared the excitement of discovering one weird organolithium molecule after another and breaking the bounds of
conventional structures. John gamely tried to ride my bicycle to the Organic Institute in bicycle-friendly Erlangen, but
gave up after a few wobbles. I wish Johns presentations at
my birthday symposia had been recorded; at the 65th he
revealed his feelings about our collaboration candidly.
Sadly, John did not, as he expected, extend his family
history of longevity. Paul von R. Schleyer
As everyone has noted, John Pople will be remembered
as one of the greatest theoretical chemists of the last century. He made fundamental contributions to the understanding of NMR spectroscopy and to the development of ab
initio and semi-empirical quantum mechanics. In 1970 my
first publication as an undergraduate dealt with applications
of the then new CNDO and NDDO methods, which were
developed by John Pople. The computer program that was
used came from the Pople lab via the Quantum Chemistry
Program Exchange. This small deck of punch cards, which
I subsequently modified for the stream of semi-empirical
methods from the Dewar group, and the availability of
Gaussian70 from the Pople lab had a huge impact on many
careers, including mine. I will always be grateful to John
Pople for this open sharing of code and for developing it in
a readily usable manner. John Pople brought quantum
chemistry to the masses. Also among the long list of his
inspirational activities were his dedication to excellence,
systematic approach, and personal efforts at writing and
testing software. John Pople was a great scholar and role
model for the present and future generations of theoretical
chemists. William L. Jorgensen
John Pople was a colleague, early career mentor and
friend, who demonstrated throughout his life the focus,
drive and enthusiasm for mathematical and scientific discovery that exemplifies scholarly endeavor.
I first met John Pople during a job interview, in February
1984, for an assistant professorship at Carnegie Mellon, a
position I ultimately accepted. John was already a giant in

vii

the area of quantum chemistry and I recall clearly how,

during that first evening encounter and dinner together, John
shared with me his clear vision to develop the theories and
computational methods of model chemistries that would
permit chemists in all discipline areas to explore the conceptual and quantitative principles that control chemical
structure and reactivity. Over the next nine years I had the
privilege of calling John my colleague and the pleasure of
numerous scientific and social discussions with him.
Johns vision regarding the development of methods and
techniques of quantum chemistry also extended to the infrastructure necessary to enable these developments. He was
resolute regarding the importance of evolving computer
technology. When the MicroVax was introduced by the
computer company, Digital Equipment Corporation (DEC),
I remember John commenting on how this sort of development was the start of a revolution for computational chemistry that would bring its techniques to every chemist on his
or her own desktop. Of course he was right, recognizing the
importance of such developments. John worked with his
group to bring these tools to chemists. I benefited from
Johns vision here by being at the forefront of computation
in chemistry by association. John had already made pioneering efforts in this area by being involved with the
purchase of the first DEC Vax 11/780 for computational
chemistry at Carnegie Mellon.
The rapid growth of computational machinery during this
period also fueled a vibrant and creative group of students and
postdoctoral scholars in Johns group to develop new and
imaginative methods and algorithms to extend the scope of
quantum chemistry to larger and chemically more diverse
molecular structures. I benefited significantly through my relationship with John at this time through very fruitful and
highly interactive exchanges between John, his coworkers, my
students, postdocs and myself. We shared joint group meetings
on many occasions at a time during which the evolution of
many new methods, e.g., rapid two-electron integral technology, unfolded through the work of very talented coworkers
such as Martin Head-Gordon, Peter Gill and Benny Johnson.
John was, of course, at the center of this development. I was
always impressed, and learned from this example that when
John was in residence at CMU he spent much of his day in
front of the terminal testing methods, exploring ideas and
writing code. As these methods matured, and I became more
knowledgeable of the power of the methods being developed,
I was keen to begin using quantum chemistry to explore the
energy surfaces of biologically interesting and important molecules and phenomena. The juxtaposition of our groups in this
instance brought about early studies of the phi/psi energy
surface of key models for the peptide backbone in proteins
the alanine and glycine peptides with Teresa and Martin
Head-Gordon and Mike Frisch. Also emerging from similar
interactions were early studies on the effects of polarizability in

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Journal of Computational Chemistry

intermolecular interactions with former Pople student Jim

Foresman. These studies exemplify the impact John had not
only on me and my personal development, but also on the area
of molecular interactions in biological systems.
On a few occasions John also shared his private personality with us, and I retain fond recollections of these interactions. As John approached retirement from CMU, he
formally moved to Chicago, keeping only an apartment
that was just a few blocks from our home in Forest Hills, a
Pittsburgh suburb. The proximity allowed me the opportunity to ask John to join us for an evening meal at home. I
have often recalled to my eldest daughter Alison, now a
sophomore in college but then about three, my fond memories from one of these visits of John on hands and knees on
the floor of our living room playing games endlessly with
her. John clearly had a soft spot for his own grandchildren,
and we were pleased to be able to serve as a surrogate
family on such occasions.
That John Poples impact was significant on the field of
chemistry, and computational chemistry in particular, is
evident from his many accolades, culminating with recognition by Swedens Nobel Committee and Britains Monarchy. However, John also influenced the lives of many
individual through their association and encounters with
him. I was privileged to have been one of those individuals.
Charles L. Brooks III
Professor John Pople was a giant in the field of computational chemistry. He virtually established this field with

PPP and CNDO series of semi-empirical theories followed

with Gaussian70 and many related ab initio theories. These
contributions opened the door to general organic, inorganic
and biological chemists towards a fertile field of computational quantum chemistry. The Journal of Computational
Chemistry contributes to further international development
of this field. Hiroshi Nakatsuji
As a scientist of the younger generation one is typically
intimidated in one way or the other by towering seniors of
the stature of John Pople. Understandably, I was shaken
before I had to give my first large-audience international
public lecture at my alma mater in Erlangen in 1995 on the
occasion of Paul Schleyers birthday, when not only George
Olah (who had won the Nobel Prize in 1994) but also John
Pople were present. Just before my talk I was introduced to
John and, by virtue of his professional down-to-earth manners, he managed to make me feel absolutely comfortable. I
walked away with the feeling that he was truly interested in
what I might have to say. I realize now that without his
foresight in designing easily accessible computational
chemistry software, I would not have had anything to talk
about! Hence, John Poples spirit continues to stay alive
through the many creative ideas and practical applications
he has left for us to apply to new and exciting chemical
problems. Peter R. Schreiner