Preamble to the discovery of Raman Effect

Today is India’s National Science Day. It celebrates the discovery of Raman effect on 28th February, 1928.

For more details on the discovery of the effect, and various human aspects related to it : you can see my past blogs here, here, here and here.

In this blog, I will briefly discuss about some of the work that directly influenced Raman’s thinking that further led to a remarkable discovery that we know by his name.

All creative pursuits are motivated by ideas from the past. No one gets their ideas in vacuum. All of us are influenced by the information which we perceive and receive. This means consciously or subconsciously the world that we are creating, both in our minds and in reality, is fundamentally influenced by the information in the world.

The discovery behind the Raman effect is no exception to this particular principle. In his formative years, C V Raman was heavily influenced by the research of Rayleigh and Helmholtz, and some classical thinkers including Euclid. Raman was also closely following the development of quantum mechanics in the early 1920s, and he was keenly studying the theoretical and experimental developments in this field.

Two aspects which played a crucial role in motivating Raman’s (Nobel prize winning) work was Compton scattering and Kramers-Heisenberg formula.

Compton scattering was as outstanding experimental achievement that revealed two aspects of light-matter interaction. First, it demonstrated inelastic scattering of electromagnetic radiation interacting with a quantum object (in this case free electrons) in the laboratory frame. Second is that it laid a foundation to revisit the wave-particle duality of light from an experimental viewpoint. Raman and Krishnan’s main paper on light scattering starts by explicitly referring to Compton effect, and motivates observation for optical analogue of Compton scattering.

To quote from Raman’s Nobel lecture :

“In interpreting the observed phenomena, the analogy with the Compton effect was adopted as the guiding principle. The work of Compton had gained general acceptance for the idea that the scattering of radiation is a unitary process in which the conservation principles hold good.”

Next is the Kramers-Heisenberg formula. This mathematical description gives the scattering cross section of a photon interacting with a quantum object (in this case electron). This formula uses second-order perturbation theory, and evokes the famous ‘sum of all the intermediate states’ for non-resonant optical interaction. PAM Dirac played a vital role in deriving this formula from a quantum mechanical framework of radiation. An important and logical consequence of this formula is the emergence of stimulated emission of radiation, and this has had deep implications in understanding LASERs. Raman was keenly studying the formula and made a brilliant conceptual connection between laboratory observation and this formula that revealed the scattering cross-section.

Again to quote from Raman’s Nobel lecture:

“The work of Kramers and Heisenberg, and the newer developments in quantum mechanics which have their root in Bohr’s correspondence principle seem to offer a promising way of approach towards an understanding of the experimental results.”

The above two concepts were important ideas that motivated Raman scattering experiments. Importantly it highlights the jugalbandi between theoretical intuition with concrete experimental observations, which forms the bedrock of modern physics.

Newton famously mentioned about the discoveries he made by ‘standing on the shoulders of the giants’. Various people involved in creative pursuits including scientists acknowledge the fact that new ideas emerge from convergence/mutation of old ideas. The harder part of creativity in science, or for that matter any art form, is to choose the right ideas to combine so that the ’emergent’ new idea has greater value compared to the individual parts. In that sense, science is a great form of creative activity that not only combines old ideas to create new valuable ideas, but also transforms the perspective of the individual seed ideas. Thus ideas combine and evolve.

So let us combine good ideas and evolve. Happy Science Day !

Soft Matter Optics – talk at ACS -India

About 2 years ago (22nd May 2020), when all the academic activities were online, I gave a talk on “Soft-Matter Optics: A Cabinet of Curiosities” organized by American Chemical Society as part of India Science Talks. Below is the embedded video of the online talk.

Link to ACS website can be found here.

In there, I give a broad overview of how interesting optical function can emerge from the complex world of soft matter. In addition to this, I have emphasized how optics can be harnessed to study structure and dynamics of soft-matter systems including colloids, liquid crystal and some biological matter. The target audience are new PhD students and anyone who is entering the field of light-soft matter interaction.

Hot Brownian Colloids – talk

On 19th Jan 2023, I gave a ~40 min talk on “Hot Brownian Colloids in Structured Optical Tweezers” in a very interesting conference on Frontiers in Non-Equilibrium Physics (FNEP) held at Institute of Mathematical Sciences, Chennai.

I mainly spoke about emergent Brownian dynamics of laser-heated colloids under optical confinement. Below is the link to the talk.

I concluded my talk quoting P W Anderson’s essay “More is Different

“The constructionist hypothesis breaks down when confronted with the twin difficulties of scale and complexity.  The behavior of large and complex aggregates of elementary particles, it turns out, is not to be understood in terms of a simple extrapolation of the properties of a few particles.

Instead, at each level of complexity entirely new properties appear, and the understanding of the new behaviors requires research which I think is as fundamental in its nature as any other.”

P.W. Anderson  ‘More is Different’
Science, 177, 4047 (1972)

More is not only different, but also wonderful !

My talk at ICTS

On 1st Dec 2022, I gave a talk on “Structured-Light Scattering : Implications in Momentum Space” as part of a discussion meeting on STRUCTURED LIGHT AND SPIN-ORBIT PHOTONICS held at International Center of Theoretical Sciences, Bangalore.

I mainly spoke about topological light scattering in the frame work of angular momentum of light and absorptive effects in optothermal tweezers created by structured light.

Below is the embedded video link to my talk. The playlist also has many other interesting talks related to the topic.

New paper : Microsphere can narrow emission from a 2D material on a mirror

We have new paper appearing in Applied Physics Letters on how a dielectric microsphere placed on a 2D material deposited on a mirror can act as an optical antenna (see left panel for the schematic of the geometry and an optical image of the realized antenna).

The experimental and simulation efforts were mainly driven by our dynamic PhD student Shailendra Kumar Chaubey, who is very passionate about nanophotonics of 2D materials. He along with Sunny Tiwari and Diptabrata Paul explicitly show how experimental parameters such as sphere size and location of focusing can influence the photoluminescence emission from a WS2 monolayers. The experiments were mainly possible thanks to our collaboration with my colleague Atikur Rahman and his student Gokul, who continue to produce fantastic 2D materials for our nanophotonics study.

Interestingly, the emission from the WS2 monlayers can be as narrow as 4.6 degrees (see right side panel of the figure) which is one of the narrowest angular spread at room temperature. We also capture the energy-momentum photoluminescence spectra from WS2 monolayers, which is convoluted with the beautiful whispering gallery modes of the microsphere (see parts (a) and (d) of the figure).

We envisage such ’emission engineering’ using a simple microsphere can be further harnessed to control emission from quantum and nonlinear photonic 2D materials. Also, it raises new questions on how local photonic density of states can be tailored by altering the local environment around quantum emitters in solid state materials.

Arxiv version of the paper : https://arxiv.org/abs/2110.10387

More surprises in Optical Momentum…

Electromagnetic momentum is a topic with rich history dating back to Maxwell, Poynting, Minkowski, Abraham, Einstein, and many more1.
It has also led to new questions, and an intriguing controversy in electromagnetism2.

An interesting and contemporary question to ask is: what is the behavior of optical momentum in artificial materials ?

One class of artificial materials is the near zero-refractive index (NZI) materials.

What are NZI materials ? The general definition of refractive index from a material view point is that it is proportional to square root of a product: dielectric permittivity (ε) and magnetic permeability (μ) of the given material.

n = (εμ)½ 

 If either of these material values go to zero at a given wavelength of light, then the refractive index goes to zero or close to zero. Such a situation creates new opportunity for enhanced or supressed light-matter interaction. See this popular review on NZI materials3

A recent theoretical paper4 addresses the consequence of evolution of optical momentum in NZI media.
This analysis has thrown a few fundamental surprises that are fascinating such as : absence of interference in Young’s double slit experiments, and some new opportunities in optical cloaking thanks to quantum nature of light. To quote the authors4 :

being inside an NZI materials would lead to an infinite uncertainty on position and zero uncertainty on momentum. Conceptually, this implies that since the resolution is poor and no correct image can be formed, an object of any shape and material can be “hidden” in a NZI material.

There are a few more interesting prospects, and of course, all of them are yet to be verified with experiments.

If you are interested in this topic, I strongly recommend this recent, popular level article5

1.           M. Buchanan, “Minkowski, Abraham and the photon momentum,” 2, Nature Phys 3(2), 73–73, Nature Publishing Group (2007) [doi:10.1038/nphys519].

2.           S. M. Barnett and R. Loudon, “The enigma of optical momentum in a medium,” Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences 368(1914), 927–939, Royal Society (2010) [doi:10.1098/rsta.2009.0207].

3.           “Optics & Photonics News – Zero-Index Platforms: Where Light Defies Geometry,” <https://www.optica-opn.org/home/articles/volume_27/july_august_2016/features/zero-index_platforms_where_light_defies_geometry/> (accessed 5 May 2022).

4.           M. Lobet et al., “Momentum considerations inside near-zero index materials,” 1, Light Sci Appl 11(1), 110, Nature Publishing Group (2022) [doi:10.1038/s41377-022-00790-z].

5.           “Exotic Materials Through Momentum’s Looking-Glass,” <https://www.optica-opn.org/home/newsroom/2022/may/exotic_materials_through_momentum_s_looking-glass/> (accessed 5 May 2022).

57. Single nanoparticle driven thermoplasmonic tweezer : single-molecule SERS

We have a new paper published in Journal of Physical Chemistry Letters on “Single Molecule Surface Enhanced Raman Scattering in a Single Gold Nanoparticle-Driven Thermoplasmonic Tweezer”

Thanks to the fantastic effort by Sunny Tiwari, and excellent support by Utkarsh Khandelwal (former IISER-P undergrad) and Vandana Sharma from my group, we have been able to combine single molecule Raman scattering with a specialized nanoscale optical tweezer.

The uniqueness of this tweezer platform  is that the optical trapping process is driven by the thermo-plasmonic potential created by a SINGLE, 150nm GOLD NANOPARTICLE. Concomitantly, the same field can be used to perform single-molecule Raman spectroscopy. Kind of  “ek teer mae do shikar” strategy Smile

Using this system, not only we push the limits of optothermal trapping of a single nanoparticle (see video) at low laser powers, but also create a platform for deterministic transport of reversible colloidal assembly in a fluid.

We envisage that our nanometric plasmonic tweezer can be harnessed to trap and tweeze biological entities such as single virus and bacteria. Another possible application of our study is to create reconfigurable plasmonic metafluids in physiological and catalytic environments, and to be potentially adapted as an in vivo optothermal tweezer.

All the videos related to this study can be found on our lab’s Youtube channel : https://www.youtube.com/playlist?list=PLVIRTkGrtbrvs7BaNsaH6tjPpzLUizyMI

DoI of the published paper : https://doi.org/10.1021/acs.jpclett.1c03450

preprint version on arxiv : https://arxiv.org/abs/2109.04281

52. Optothermal pulling and trapping..with nanowire plasmons

We have a new paper published in the journal ‘Soft Matter’ titled : Optothermal pulling, trapping, and assembly of colloids using nanowire plasmons

When a silver nanowire is optically illuminated under certain conditions, they propagate surface plasmons. These surface electromagnetic waves not only propagate light at subwavelength scale, but also generate heat along the nanowire.

A question of interest to us: can we use the quasi one-dimensional optothermal potential of a nanowire-plasmon to trap and assemble soft, microscale matter ?

Motivated by this question – Vandana, Sunny and Dipta from my research group, performed optical trapping based experiments to show an interesting pulling and trapping effect on dielectric colloids (see video). Furthermore, by increasing the concentration of the colloids, an emerging two dimensional crystal was observed. Interestingly, the formation of this two dimensional assembly was found to be sensitive to the optical polarization at the excitation point on the nanowire.

Thanks are also due to other co-authors: my colleague Vijayakumar Chikkadi and his student Rathi for helping us to implement the particle tracking code on python.

Optical trapping and tweezing is a fascinating area of research. By adding plasmons to the mix of things, these optical effects become intriguing. Importantly, they facilitate a platform to explore questions in non equilibrium statistical mechanics including optically driven active matter…

Afterall, more is different…

DOI of article : https://doi.org/10.1039/D1SM01365C

Link to arxiv preprint: https://arxiv.org/abs/2109.09557

All videos here :