Long Range Interactions In Nanoscale Science
Roger H. French,a,b,* V. Adrian Parsegian,c Rudolf Podgornik,c,d Rick F. Rajter,e Anand Jagota,f
Jian Luo,g Dilip Asthagiri,h Manoj K. Chaudhury,i Yet-ming Chiang,j Steve Granick,k Sergei
Kalinin,l Mehran Kardar,m Roland Kjellander,n David C. Langreth,o Jennifer Lewis,p Steve
Lustig,q David Wesolowski,r John Wettlaufer,s Wai-Yim Ching,t Mike Finnis,u Frank Houlihan,v
O. Anatole von Lilienfeld,w Carel Jan van Oss,x Thomas Zemby
a. DuPont Co. Central Research, E400-5207 Experimental Station, Wilmington, DE 19880, USA
b. Department of Materials Science and Engineering, University of Pennsylvania, Philadelphia, PA19104
c. Laboratory of Physical and Structural Biology, NICHD, National Institutes of Health, Bethesda, Maryland
20892-0924, USA
d. Faculty of Mathematics and Physics, University of Ljubljana, Ljubljana SI-1000, Slovenia and Department
of Theoretical Physics, J. Stefan Institute, Ljubljana 1000, Slovenia
e. Department of Materials Science and Engineering, MIT, Cambridge, Massachusetts 02139-4307, USA
f. Department of Chemical Engineering, Lehigh University, Bethlehem, Pennsylvania, USA
g. School of Materials Science and Engineering, Clemson University, 201 Olin Hall, Clemson, SC 29634
h. Department Of Chemical & Biomolecular Engineering, Johns Hopkins University, Baltimore, MD 21218
i. Department of Chemical Engineering, Lehigh University, Bethlehem, Pennsylvania, USA
j. Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA
02139 (USA)
k. Materials Research Laboratory, University of Illinois, Urbana, Illinois 61801, USA
l. Materials Science and Technology Division and The Center for Nanophase Materials Science, Oak Ridge
National Laboratory, Oak Ridge, Tennessee 37831, USA
m. Department of Physics, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
n. Department of Chemistry, Göteborg University, SE-412 96 Göteborg, Sweden
o. Center for Materials Theory, Department of Physics and Astronomy, Rutgers University, Piscataway, New
Jersey 08854-8019
p. Frederick Seitz Materials Research Laboratory, Materials Science and Engineering, Department, University
of Illinois, Urbana, Illinois 61801
q. DuPont Co. Central Research, E400-5472 Experimental Station, Wilmington, DE 19880, USA
r. Oak Ridge National Laboratory, Chemical Sciences Division, P.O. Box 2008, Oak Ridge, TN 37831-6110,
USA
s. Department Of Geophysics and Physics, Yale University, New Haven, CT 06520-8109
t. Department of Physics, University of Missouri–Kansas City, Kansas City, Missouri 64110, USA
u. Department of Materials and Department of Physics, Imperial College London, Exhibition Road, London
SW7 2AZ, United Kingdom
v. AZ Electronic Materials Corp USA, 70 Meister Avenue, Somerville, NJ 08876
w. Multiscale Dynamic Material Modeling Department, Sandia National Laboratories, Albuquerque, NM
87185, USA
x. Department of Microbiology, 2Department of Chemical Engineering, and Department of Geology,
University at Buffalo, Buffalo, New York, USA
y. CEA/SACLAY, LIONS at Service de Chimie Moléculaire, 91191-Gif-sur-Yvette Cedex, France
* corresponding author: roger.h.french@usa.dupont.com
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Section – Page: 1
Abstract
Focusing on the electrodynamic, electrostatic and acid-base interactions that dominate the
organization of small objects at separations of a few nanometers, we first review the strengths
and weaknesses in our understanding of these interactions. With this perspective, we describe a
large number of potentially instructive systems from which we can learn about organizing forces
and the means to modulate them. We then survey the many practical systems whose design is
guided by intuition and by systematic manipulation made to harness these nanoscale forces. Our
survey of these ingenious systems reveals not only the promise of new devices and materials but
also the need to be able to design them using better knowledge of the operative forces. Having
identified areas where basic research is now needed, we can discern how this research can
contribute to nascent and ongoing applications of nano-devices.
Table Of Contents
Long Range Interactions In Nanoscale Science..............................................................................1
Abstract ..........................................................................................................................................2
Table Of Contents...........................................................................................................................2
Introduction.....................................................................................................................................2
Conclusions.....................................................................................................................................5
Acknowledgements.........................................................................................................................6
2 References.....................................................................................................................................8
Introduction
R.P. Feynman in his by now famous musings on the possibility of nanotechnology
(Feynman, 1959) noted that “...as we go down in size, there are a number of interesting
problems that arise. All things do not simply scale down in proportion. There is the problem that
materials stick together by the molecular (Van der Waals) attractions. It would be like this: After
you have made a part and you unscrew the nut from a bolt, it isn't going to fall down because the
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gravity isn't appreciable; it would even be hard to get it off the bolt. It would be like those old
movies of a man with his hands full of molasses, trying to get rid of a glass of water. There will
be several problems of this nature that we will have to be ready to design for”. The importance of
long-range interactions (LRIs) - which according to the background and preferences are also
referred to as van der Waals,
Casimir, Lifshitz, electrodynamic fluctuation or dispersion
interactions - in the synthesis, design and manipulation of materials at a nanometer scale was
thus recognized from the very beginning of nanosciences. Nevertheless it was only quite recently
that all the intricacies of not just van der Waals, as alluded to by Feynman, but all LRIs on the
nanoscale came to the front of scientific endeavors, in research areas as varied as quantum field
theory, quantum and classical density functional theories, various mean-field and strong coupling
statistical mechanical formulations, liquid state integral equation – closure approximations,
computer simulations as well as novel experimental designs and methods, not to say anything
about the exciting new developments and prospects in technological applications. The
role
of
LRIs in self-assembling active devices from heterogeneous components appears to be
fundamental, since they govern the stability of component clusters on the nanoscale and for
better or for worse can not be ignored in the design of nanodevices and nanoactuators. The new
technological paradigms that might be developed as a consequences of these fundamental studies
and ensuing technological breakthroughs on the nanoscale will no doubt contribute to solving
some pressing societal problems on the macroscale and introduce new ways of thinking and
paradigm shifts necessary in order to make some old problems closer to a solution.
The present review is the outcome of a workshop panel entitled Long Range Interactions
In Nanoscale Science, convened under the auspices of the United States Department Of Energy,
Council for the Division of Materials Sciences and Engineering, Basic Energy Sciences, set to
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survey, identify, report and assess basic research challenges, needs and opportunities in the area
of LRIs at the nanoscale. It assessed recent advances in the theory, computation, and
measurement of the primary LRIs: electrodynamic, electrostatic, and polar, as well as secondary
LRIs, closely based upon but distinct from the primary variety: hydrogen bonding,
hydrophobic/hydrophilic/hydration, steric, structural and entropic interactions.
It set out to
create a comprehensive framework and language of LRIs in nano-sciences as well as to identify
strategies to harness these forces for the design of new materials and devices.
This endeavor requires spanning a vast range of scientific landscapes from field theory all
the way to colloid science, from physical sciences to chemistry and biology, from theory to
experiment and computation, coupling the tenets of basic science fundamentals of LRIs to
tractable experimentally accessible systems that are manipulable on the nanoscale and can in the
not too distant future launch sophisticated technological applications. The review focuses on the
fundamental aspects of electrodynamic, electrostatic and polar acid/base foundations of LRIs, by
invoking various instructive systems that accentuate different aspects of LRIs, such as atoms,
molecules, nano-, meso- and macro-scopic interfaces, surfaces and defects, as well as chemical
equilibria in liquids, suspensions and colloidal aggregates. The aim being all the time to
understand and harness the properties of LRIs in nanoscale systems such as e.g. surfaces and
interfaces that are enabled by the LRIs, colloidal macro and nanoscale self-assembly, and the
design and chemical construction of electronic, optical and sensing properties of devices
constructed from nanomaterials. This review sets out to map and assess this vast space of
scientific endevor in as comprehensive and simple terms as possible, but not simpler. Hopefully
it meets at least a part of these goals and requirements.
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Conclusions
Evidence gathered for this report reveals not only abundant creativity in the design of
devices but also inspiring research on physical forces governing organization on the nanometer
scale. Careful consideration of this research also shows clearly an unevenness in our grasp of the
basic organizing forces. Perhaps the greatest surprise is the inadequacy of theories of polar and
electrostatic interactions compared with the present-day sophistication in formulating and
computing charge-fluctuation forces. We cannot avoid these areas of ignorance. Electrostatics
and polar interactions need conceptual advances. There is still no good algorithm to handle the
strong electric fields near ions nor any language to include the powerful solvation forces
surrounding even the simplest molecules.
Realizing that few systems operate by only one kind of interaction, we are faced with the
paradox that the most sophisticated and accurate theory about one kind of force is vitiated when
combined with less reliably formulated interactions. The panel was unanimous in its ardent plea
that attention and significant research support be devoted to fundamentals. With better force
measurement, theoretical formulation, and potentials for computer simulation, design of
materials will accelerate and likely move faster than is possible with trial-and-error approaches.
A second fundamental need is in education. Bluntly put, don't duck the areas of
ignorance. The emphasis must shift to learning-to-learn: better modes of teaching about forces as
the need to learn them is recognized; better preparation in the basics of several sciences so as to
remove the daunting fear of new learning after graduation. The possibilities – by supplementary
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coursework, by computer facilities, by specialized texts that are written at a friendly level – can
then be realized in many ways.
Then, third and greatest, the heavy work of designing and making materials, testing them,
and creating synthetic pathways to provide needed supply. While theory and computation still
fall short, the creation of materials is simultaneously a source of testing design ideas and of
providing samples with systematically varied properties for systematic construction. It would
qualitatively improve this iteration if material synthesis were made more accessible. With the
magnificent facilities now being developed in national centers, even DoE nanoscience centers,
people will have new possibilities for design and application of design ideas. Training and
linking programs that facilitate use of existing facilities is an economically practical strategy.
A neglected source of creativity was seen in the act of the meeting itself. At all times
during exchanges, during presentations of recent work, during discussions of what people needed
to learn, there was an ardor in the learning being experienced by the participants themselves.
One person, from a major DoE national lab, told the organizers, "I couldn't figure out why you
even invited me. Now, I'm learning more than I could have expected, and I find people eager to
talk. Thanks for asking me. This meeting has created new collaborations for me and has changed
the way I will work." Perhaps meetings that force people to focus on a problem they are not
studying, but still a problem needing solution, will bring out creative spirits of the kind that were
so happily evident at our workshop.
Acknowledgements
The authors would like to acknowledge Harriet Kung of the Division of Materials
Sciences and Engineering, one of the research divisions in the Office of Basic Energy Sciences
of the U.S. Department of Energy and Frances Hellman, chairperson of the Council for the
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Division of Materials Sciences and Engineering for sponsoring the LRI in NS workshop. Christie
Ashton and Sophia Kitts for organizational assistance and Barbara French for assistance in edting
the manuscript. And to all of the participants who provided their time and energy and most
importantly their intellectual insights with out which this would not have been possible.
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