My Metaphoric Oxygen

There is no Frigate like a Book
To take us Lands away
Nor any Coursers like a Page
Of prancing Poetry –
This Traverse may the poorest take
Without oppress of Toll –
How frugal is the Chariot
That bears the Human Soul –

                             BY EMILY DICKINSON

Generally speaking, scientists are natural philosophers: they observe nature, ask questions, hypothesize an answer, test them through experiments and extend this exploration by escaping into the universe of ideas in books and journals. New ideas emerge from this exploration and join the chorus, and the intellectual journey continues. In my own research on light scattering, I have been deeply influenced by ideas of various fellow-explorers. For me, journal papers and books encompass the “metaphorical oxygen” for creativity and knowledge. Below I introduce you to some classic books which keep my research alive.

  1. Absorption and Scattering of Light by Small Particles
    • Author(s): Craig F. Bohren and Donald R. Huffman
      • Comments: There are two kinds of authors who write textbooks. One is the ‘boring kind’ and the other is the ‘Bohren kind’. If you want to fall in love with light scattering (and science in general), read books and articles by Craig Bohren. It will not only deeply influence your thinking, but also will show how a textbook can, and should, evolve a subject systematically. This particular classic has some of the most important ideas related to how light behaves when it interacts with matter comparable to the wavelength of light, and forms the bedrock on which a lot of contemporary research, including nanophotonics and plasmonics, is pursued. This book has wit, humour and a touch of poetry jumbled up together as flowing river of knowledge. To give you a spirit of their writings, let me reproduce the first paragraph of their introduction

Bhoren

  1. Light Scatteing by Small Particles
    • Author(s): H.C. van de Hulst
      • Comments: The first edition of this book was published in 1957, by the author was a legendary astronomer. This book has a beautiful description of single and multiple-scattering phenomenon, and describes specific situations where they apply. Written with an astrophysical viewpoint, it elegantly combines depth and breadth in a lucid way. This book has perhaps served as inspiration to most of the books written on light scattering.
  1. The scattering of light and other electromagnetic radiation
    • Author(s):  Milton Kerker
    • Comments: Some researchers have remarkable ability to choose problems that have far reaching consequences beyond the next research paper. Milton Kerker was one such legend. His research papers and this book has not only influenced the way physics of light scattering is studied, but has had deep impact on utilization of light scattering in various branches of science and technology. This 600 odd page book is indeed a masterpiece, and in a unique way caters to almost all kinds of researchers who are interested in light scattering.
  2. Dynamic Light Scattering with applications to chemistry, biology and physics
    • Author(s): Bruce J. Berne and Robert Pecora
      • Comments: A majority of the matter in biology and chemistry are suspended in a fluid. When an object in a medium undergoes Brownian motion, it influences the way a light beam scatters and traverses through that medium. This book explain the how and why of this fascinating topic. Written by experts in chemical physics, this classic serves as the foundation for light scattering in soft-condensed matter physics.
  1. Molecular Light Scattering and Optical Activity
    • Author(s): Laurence Barron
      • Comments: Historically, light scattering by molecules has been studied by legends such as Rayleigh, Raman and many more. Interestingly, all these legends emphasized the connection between polarization of scattered light and structure of matter. In this book, Barron puts together these ideas in a very elegant way, and motivates and develops the phenomenon of optical activity from a molecular physics viewpoint. Given that a majority of biomolecules are chiral in nature, the insight that one obtains by reading this book has direct implication in understanding the structure and dynamics of biomolecules such as amino acids, proteins and DNA.
  1. Scattering, Absorption, and Emission of Light by Small Particles
    • Author(s): MI Mishchenko, LD Travis, AA Lacis
      • Comments: Mischchenko is a scientist at NASA, and his books on light scattering have had great influence in aerosol science, radar technology and many more. The T-matrix codes based on this book forms a very important tool across the research community that works on weather prediction and pollution monitoring.
  1. Wave Propagation and Scattering in Random Media (Vol 1 and 2)
    • Author(s): Akira Ishimaru
      • Comments: This classic from late 1970s was one of the elaborate attempts to put together wave propagation and scattering in a random media on a rigorous mathematical foundation. This 2 volume book has solutions to various mathematical problems that one encounters in light scattering physics, and makes an important connection to transport theory of light in a medium.
  1. Optical Scattering Measurement and Analysis
    • Author(s): John C. Stover
      • Comments: If you are interested in experimental aspect of light scattering, this is one of the best books. It is essentially a field guide, which tells you how to quantitatively make a light scattering measurement, and what aspects to look-out for. This is a very good book for students who want to get a hands-on experience in light scattering.
  1. LASER LIGHT SCATTERING, Basic Principles and Practice
    • Author(s): Benjamin Chu
      • Comments: Chu’s book develops the topic of laser light scattering in terms of both experimental aspect and theoretical foundations. Importantly, it connects the topics of light scattering to optical spectroscopy, and shows how one can obtain meaningful information about light-matter interaction.
  1. Mesoscopic Physics of Electrons and Photons
    • Author(s): E. Akkermans and G. Montambaux
      • Comments: Quantum mechanical entities such as electrons and photons can be confined in space and time. Depending on the geometry of confinement, very interesting physics such as weak and strong localization can emerge. This book looks at the physics of confined electron and photon from a unified viewpoint. It highlights similarities and difference between the electrons (fermions) and photons (bosons).
  1. The Raman Effect: A Unified Treatment of the Theory of Raman Scattering by Molecules
    • Author(s): Derek A. Long
      • Comments: Written by a pioneer in the field, this book till date remains the most rigorous treatment on Raman scattering of light from a theoretical viewpoint. Based on quantum mechanical arguments, this book relies on perturbation theory, and clearly shows the connection between structure of molecules and how they influence the scattered light.
  1. Principles of Surface Enhanced Raman Spectroscopy and Other Plasmonic Effect
    • Author(s): Eric C Le Ru and Pablo G. Etchegoin
      • Comments: The most definitive book written on surface enhanced Raman scattering by two physicists whom I greatly admire. This book gives unified treatment of plasmonics and surface enhanced inelastic light scattering, and is written in a style catering to physics audience. The book has a lot of details and explanations, and also serves as excellent introduction to plasmonics and vibrational spectroscopy. Given that the authors themselves are pioneers in single-molecule Raman scattering, their insight into single molecule optics in plasmonic field is fascinating. Unfortunately, Etchegoin succumbed to cancer, and I could never meet him. However his great ideas and thoughts stay on…
  1. Introduction to Wave Scattering, Localization and Mesoscopic Phenomena
    • Author(s): Ping Sheng
      • Comments: Random lasing is an emerging topic of research in nanophotonics. The fact that one can have random structures assembled in space and time, and yet achieve spatial and temporal coherence is quite remarkable. This book brings together insights from wave scattering and mesoscopic physics to show how light behaves when confined to small volumes compared to wavelength of light. The insights obtained from this book are heavily used in the literature on random lasers.
  1. Fundamentals of Atmospheric Radiation
    • Author(s): Craig F. Bohren and Eugene E. Clothiaux
      • Comments: Bohren weaves his magic…..again. Although the title of this book indicates atmospheric radiation, the way the authors treat the topic of absorption, emission and scattering of light is fascinating. This book gives a broad viewpoint of interaction of light with matter, and shows one can and should treat the subject coherently. The references and problems are very relevant and interesting, and I have found some gems while reading through this text.

Trapping Questions and Evolving Answers

A voice said, Look me in the stars
And tell me truly, men of earth,
If all the soul-and-body scars
Were not too much to pay for birth.

—- “A Question” By Robert Frost

In research, as in life, humble questions can sometimes lead to profound answers. A curious question flying as a passing thought in the mind of a researcher can equally lead to some important discoveries and inventions. Furthermore, what starts as a simple question, evolves into a creature that the questioners themselves would have not envisaged. This evolution of thought in various directions is fascinating to say the least, and history of science is dotted with such examples.

Take for example Arthur Ashkin of Bell Labs, who in late 1960s, asked the following question:

“is it possible to observe significant motion of small particles using the forces of radiation pressure from laser light?”

 Note- at that point of time, lasers were still a relatively new invention, and people were looking for an application. In that context, it was indeed an interesting question to ask about the effect of laser beam on a small particle which may be immersed in fluid or in vacuum. After all, radiation pressure should have some effect on the motion of particles, as evidenced in the case of comet tails.

With this question, Ashkin embarked on a journey that conceptually and literally pushed and revolutionized a large part of our science and technology based on lasers. Ashkin’s question led to the realization of laser-based optical trap of microscopic objects, which further evolved into a major experimental tool not only in physics but also in biology and chemistry.

Below figure shows the conceptual schematic of Ashkin’s experiment, in which he introduced two counter-propagating laser beam which created an optical potential to stably trap an object in space and time. The physics of optical trapping itself in intriguing, in which, the compelling battle between forces due to in-line pushing and orthogonal pulling will be eventually won by the pulling component.  A stable energy minimum is achieved at the center of the focused laser beam, in which the object of interest happily resides. Of course, parameters such as refractive index of the object and the medium play a critical role, so does the alignment of laser beam and its wavelength.

trap Ash
Optical schematic of the first optical trap created by Arthur Ashkin. Adapted from the original paper [1]*.
 There are two important aspects to Ashkin’s work. One is that he pursued on a simple question that lead to an important observation, which has had far researching consequences not only in physics but also in biology and allied research areas, and the second point is that a few people, in his own lab felt that the discovery was not important. In the first chapter of his book, Ashkin describes a very interesting situation after he had performed this seminal work:

 It may be interesting and instructive to recall the initial reactions of other scientists to paper [1]*, which described the earliest trapping work. At Bell Labs., before a manuscript could be sent out to a journal it had to undergo an internal review to make sure it would not tarnish the laboratory’s excellent reputation in research. Since paper [1]*was intended for Physical Review Letters, it was sent to the theoretical physics department for comment. The Bell Labs, internal reviewer made only four points: (i) there was no new physics here, (ii) the reviewer could not actually find anything wrong with the work (this is a reminiscent of the famous Pauli insult, when he commented on some work he thought worthless that “it is not even wrong!”), (iii) the work could probably be published somewhere, and (iv) but not in Phys. Rev. Lett.This four-point internal referee report from the theoretical group greatly distressed me, and so I went to my boss, Rudi Kompfner, inventor of the traveling wave tube, whom I greatly admired. Rudi, a man usually slow to anger, simply said, “Hell, just send it in!” As it turned out, I had no problem whatever with the Physical Review Letters reviewers. In 1999, paper [1]* had the honor of being selected as one of the 23 seminal papers on atomic physics reprinted in the compilation, “The Physical Review — The First Hundred Years”, edited by Henry Stroke, American Institute of Physics Press and Springer Verlag (1999) on the occasion of the centennial of the American Physical Society.

There are at least two important lessons in this story: a) not always one can instantaneously judge the importance of a research work and b) the notion of “new physics” depends on how you look at a topic and judge its implication. To see how a new result can connect to something else requires a kind of broad view of science well beyond the boundaries of the “known unknowns”.

Going further, Ashkin did not stop his train of questions. He writes that he was intrigued by the observations which further motivated him to explore on the following topics:

Could traps be observed for macroscopic particles in other media such as air or even in a vacuum? Could optical manipulation be used as a practical tool for studying light scattering, for example, and other properties of small macroscopic particles?

Evolution of Ideas

After some resistance, slowly the physics community started taking notice of Ashkin’s experiments, and paid more attention towards the simple yet powerful methods he was developing. What followed was indeed a revolution. The methods he developed immediately caught the attention of two very diverse research communities – one was of atomic physicists and other one was of biologists. Whereas the former were interested in trapping and cooling atoms, the later were in desperate search for non-invasive optical tools that could trap and manipulate cellular and sub-cellular objects. Optical trapping indeed catered enormously towards these research efforts. It not only led to “new and interesting physics”, but also some wonderful experiments in soft-matter and biological sciences. In order to give you a gist of the way Ashkin’s work evolved, below I give a table of interesting research results. As you will see, the papers themselves discuss topics and problems that were not envisaged by Ashkin, but the influence of his ideas percolated deep and wide.

Year Link to the relevant papers and my comments
1982 Electromagnetic mirrors for neutral atomsThis paper theoretically proposed use of evanescent optical fields at dielectric-vaccum interface to reflect neutral atoms. The concept of radiation pressure at an interface was emphasized.
1986 ·       Three-dimensional viscous confinement and cooling of atoms by resonance radiation pressure·       Experimental observation of optically trapped atoms

These were the foundational experiments on laser cooling and trapping of atoms, which went on to win the 1997 Nobel Prize in physics. Note that Ashkin missed out on the prize!

1989 Optical Binding

This introduced a fascinating concept of binding microscopic objects with long range optical forces facilitated by electromagnetic fields. This topic is still of great interest, and still inspires a variety of experiments.

1992 Movement of micrometer-sized particles in the evanescent field of a laser beam
This paper was a pioneering contribution towards movement of particles in fluids using an evanescent wave of laser beam.
1993 Direct observation of kinesin stepping by optical trapping interferometry
The abstract of this paper is worth a read and tells a compelling story :“Do biological motors move with regular steps? To address this question, we constructed instrumentation with the spatial and temporal sensitivity to resolve movement on a molecular scale. We deposited silica beads carrying single molecules of the motor protein kinesin on microtubules using optical tweezers and analysed their motion under controlled loads by interferometry. We find that kinesin moves with 8-nm steps.”
1996 Optical vortex trapping of particles This was one of the first experiments to use vortex beams to trap objects. In conclusion of the paper, the authors envisage trapping application based on holograms, which were created soon after the proposal.
1997 Theory of nanometric tweezerA first significant jump towards extrapolating optical trapping to sub-wavelength scales. The idea of utilizing a metal nano-tip to trap dielectric objects was proposed. This paper laid an excellent foundation for optical manipulation at nanometer scale.
1998 Optical tweezer arrays and optical substrates created with diffractive optics
This literally added new dimensions to optical trapping, where a diffractive optical element, a static hologram in this case, was introduced in the optical scheme. This laid the foundation towards parallel trapping on conventional set-up, and has turned out to be extremely useful for applications in soft-matter physics and biological applications.
2001 Force of surface plasmon-coupled evanescent fields on Mie particles
This theoretical paper compares how evanescently-excited surface plasmon polaritons at metal-dielectric interface can exert more force on Mie particle compared to a dielectric-dielectric interface, thus creating a platform for film-based plasmonic manipulation of micro-objects.
2006 Surface Plasmon Radiation Forces This was the first report that experimentally showed how surface plasmon from a metal interface exerted about 40 times more force on a micron sized particles compared to a dielectric interface. Importantly, this paper measure the trapping potential depths created by surface plasmon on a metal-film.
2007 Parallel and selective trapping in a patterned plasmonic landscape This was perhaps THE BREAKTHROUGH experiment in plasmonic trapping,  that showed how gold nano-disc could create parallel traps  of micron scale object at significantly lower power compared to optical trapping. A majority of plasmon trapping experiments nowadays derive their inspiration from this paper
2009 Self-induced back-action optical trapping of dielectric nanoparticles This experimental paper is one of the first reports which harness the feedback from the trapped 50 nm object to improve the performance of the trap. This significantly reduces the power of laser one needs to use for trapping experiments and represents truly a nanometric optical trap.
2010 Laser Printing Single Gold NanoparticlesOptical trapping forces are harnessed to printing individual gold nanoparticles on glass substrates. This has opened up new opportunities to directly fabricate nanostructure from colloidal phase onto a surface of interest.
2012 Subkelvin Parametric Feedback Cooling of a Laser-Trapped Nanoparticle To quote the authors “Using a single laser beam for both trapping and cooling we demonstrate a temperature compression ratio of four orders of magnitude”. This opens a new avenue to perform optical tests of quantum mechanics using isolated nanoparticles.
2014  Plasmofluidic Single-Molecule Surface Enhanced Raman Scattering from Dynamic Assembly of Plasmonic NanoparticlesThis is an experiment report from my group where we showed that one could not only create a large scale plasmonic trap of multiple nanoparticles, but also one can utilize it to perform single-molecule spectroscopy.
2016 Direct Measurement of Photon Recoil from a Levitated Nanoparticle Another experimental breakthrough where the photon recoil from a single nanoparticle is measured.
2018 Opto-thermoelectric nanotweezers This experimental paper shows how optical, thermo-plasmonic and electric fields can be combined to trap and manipulate nano-object in fluids.

To conclude I will again quote Ashkin, who makes an important observation in an editorial he wrote on the occasion of commemorating 50 years after the discovery of laser:

As we look to the future, what can we anticipate? Certainly much more of the present hot fields such as: single atom studies; properties and behavior of single biological molecules such as mechanoenzymes and nucleic acids; mechanical properties of single molecules and tissue; studies of particle arrays; and particle separation schemes. Of course, we cannot anticipate serendipitous discoveries. We can only hope to recognize them when they occur.

After all, one question leads to another….and the rest is evolution…you see!