Ph.D. Thesis
Title Hydrogen-bonded Synthetic Molecular Machines
Adviser Prof. David A. Leigh, Forbes Chair of
Organic Chemistry, University of Edinburgh, UK.
Thesis Committee Dr. Hon Wai Lam, Lecturer,
School of Chemistry, University of Edinburgh, UK; Prof. A. Prasanna
de Silva, Chair of Organic Chemistry, Queens University, Belfast,
UK.
Essay
From myosin to F1-ATPase, Nature is full of examples
of molecular devices and it is no exaggeration to say that life itself
ultimately depends upon them. Constructing artificial molecular-level
machines would help us understand their biological counterparts. Furthermore,
molecular-size devices are the next logical step forward (or downwards)
in the race for miniaturization.
Initially, the term molecular machine was
(and sometimes still is) used in a purely iconic manner: the structures
looked like pieces of machinery or they carried out a function
that in the macroscopic world would require a machine to perform it.
Whilst these early reports were unquestionably the key to popularising
the field, we are now in the position to give ourselves a more ambitious
definition. Accordingly, we can describe molecular machines as a
subset of molecular devices (functional molecular systems) in which
some stimulus triggers the controlled, large amplitude mechanical
motion of one component relative to another (or of a substrate relative
to the machine) which results in a net task being performed.
With the objectives outlined in that definition in mind,
my thesis addressed: the search for new methods to achieve controlled
submolecular motion in stimuli-responsive molecular shuttles; the
development of a general design to exploit this controlled motion
to produce a potentially useful response; and, remarkably, the extension
of the work in solution to polymer films and surfaces....[more;
pdf file - 2.89MB]