Patterns of clouds in the sky, wind-sculpted striations
in the desert sand, spots and stripes of animal skin are examples
of patterns that emerge spontaneously in nature. The physical
laws that govern spontaneous pattern formation in these dissimilar
systems are strikingly similar. Any system that is unstable (prone
to change) will spontaneously transform in an attempt to reach
its most stable state (equilibrium). Patterns emerge if during
its evolution towards equilibrium, the system is subjected to
two opposing forces. Our research examines such nonlinear phenomena
when a system simultaneously undergoes optical and chemical changes.
Because the optical and chemical properties of such systems can
be precisely controlled, they provide convenient pathways to examine
complex nonlinear processes. This research, while consistent with
studies of nonlinear light propagation established by optical
physicists and engineers, contribute new chemical perspectives
to this forty-year old field.
Nonlinear phenomena in
photochemical systems
Consider the example of a narrow beam of light.
Regardless of whether it originates from the sun or a laser, the
beam will naturally broaden (diffract) while travelling through
most transparent materials including air, glass and water. In
certain types of materials however, the same beam of light can
trigger a transformation - such as a chemical reaction – that
causes the refractive index along the path of the beam to increase.
A nonlinear situation arises in which the natural tendency of
the beam to diffract is always opposed by refraction, which forces
the beam to focus. Our research in the past four years has revealed
that these conditions elicit a richly diverse suite of nonlinear
phenomena including spontaneous pattern formation.
Our principal findings include
self-trapped beams of light, which travel without broadening in
certain photochemical systems over unexpectedly long distances.
Self-trapping occurs when the beam becomes entrapped within the
narrow channel of increased refractive index inscribed along its
path of propagation. We have established a comprehensive understanding
of the dynamics and properties of self-trapped beams and provided
first experimental confirmation of several theoretical predictions
of their behaviour. We have found self-trapped beams of both laser
and separately, of white light and
learnt that their properties are fundamentally different. Waves
composing a laser beam possess the same wavelength and are strongly
correlated to each other. Exactly the opposite is the case for
white light, which is said to be incoherent because it is composed
of an entire spectrum of wavelengths and has extremely poor correlation.
Once self-trapped, a laser beam exhibits
different and discrete optical modes
– like the vibrational modes of a drum skin or the harmonics of
a violin string. The optical modes of a self-trapped white light
beam however fluctuate so rapidly that only a time-averaged or
smoothed profile of the entire beam can be observed. (It is therefore
particularly remarkable that such a rapidly fluctuating and incoherent
wavepacket collectively self-traps and propagates as a single
entity.) By applying our knowledge of the competition between
diffraction and refraction in self-trapping behaviour, we have
recently been able to demonstrate the spontaneous
formation of patterns in large uniform beams of white light.
Interactions
of self-trapped beams
Scientists have always sought to understand the
interactions between particles – whether they be atoms or planets.
Like these bodies of matter, self-trapped beams of light can also
interact with each other. Under specific conditions, a pair of
self-trapped beams can attract, repel and even appear to orbit
about each other. Because we can now generate self-trapped beams
in photochemical systems, we can also study their interactions.
Our objectives are to establish the basic principles that govern
self-trapped beam interactions through experiments that ask questions
such as (a) is there any exchange of energy between interacting
beams? (b) are there any changes to the fundamental properties
of a self-trapped beam such as its spectrum, coherence and modes?
(c) what type of structures are inscribed in the photochemical
medium as a result of these interactions? (d) are self-trapped
beams restricted to pairwise interactions or do interactions extend
to multiple (> 2) self-trapped beams? (e) how do these interactions
compare with interactions of particles in other systems?
Spontaneous pattern formation:
is coherence important?
Our discovery that a uniform white light beam transforms
spontaneously into an ordered pattern
– although explicable through the mathematics of nonlinear light
propagation – is counterintuitive. Periodic patterns of light
when two or more laser beams, which are mutually coherent, interfere.
Even in his seminal experiment, Young used a pair of slits to
introduce mutual coherence into two beams of sunlight, which in
turn produced an interference pattern and revealed the wave-nature
of light. An understanding of optical pattern formation processes
could bridge the two extremes of periodic interference patterns
and periodic patterns that form spontaneously across a single
broad beam of incoherent white light. Studies are planned to systematically
tune the (spatial) coherence of a beam from excellent to weak
and to monitor the resulting effects on properties of the pattern
such as symmetry, periodicity and degree of order.
Theory development
and modelling
Our experimental research, while confirming several
predictions of light propagation models, also revealed new forms
of nonlinear phenomena (higher order optical modes, white light
phenomena, spontaneous pattern formation). We plan to develop
theoretical models to simulate these phenomena; initial approaches
will seek numerical solutions to problems cast through the nonlinear
Schrödinger equation for nonlinear light propagation.
New materials for nonlinear
light propagation and interactions
Experiments in photopolymers alone have revealed
richly diverse self-trapping phenomena. An even greater variety
of phenomena may be discovered by expanding the search to different
classes of photochemical systems. To this end, we will study self-trapping
phenomena in two different and well known classes of chemical
systems (i) photosensitive liquid crystalline media and (ii) photoisomerizing
azobenzene systems. These systems also exhibit photoinduced index
changes and thus satisfy the basic prerequisite for self-trapping.
Our focus will be on fundamental differences in their photoresponse
relative to photopolymers that could lead to new forms of self-trapped
species; the effects of wavelength of sensitivity, magnitude,
anisotropy and reversibility of refractive index, timescale of
response will be examined in detail. The application in optical
switching, erasable and reconfigurable and birefringent self-induced
waveguides will also be studied.
Spontaneous self-inscription
of complex 3-D optical waveguides and microperiodic structures
Refractive index changes induced during self-trapping
phenomena result in a variety of permanently self-inscribed structures
including 3-D cylindrical waveguides (formed during self-trapping)
and microperiodic structures (during pattern formation). The application
of these structures as self-inscribed passive and active optical
devices will be studied. Particular emphasis will be given to
the development of a new technique “White-light
based Spontaneous Lithography of 3-D Microperiodic Structures”.
Here, pattern formation in multiple beams (maximum of 3) propagating
at different orientations to each other and its potential in spontaneously
forming 3-D ordered microperiodic structures will examined. Unlike
holographic lithography, which relies on the interference of coherent
laser beams, this technique relies on the spontaneous behaviour
of the optical field itself and requires only incoherent (and
cheap) white light from an incandescent source. Resulting structures
can be further modified by introducing active optical components
(metal nanoparticles, chromophores) for further functionality.