Shubham Chandel

Quantitative fluorescence and elastic scattering tissue polarimetry using an Eigenvalue calibrated spectroscopic Mueller matrix system

A novel spectroscopic Mueller matrix system has been developed and explored for both fluorescence and elastic scattering polarimetric measurements from biological tissues. The 4 × 4 Mueller matrix measurement strategy is based on sixteen spectrally resolved (λ = 400 - 800 nm) measurements performed by sequentially generating and analyzing four elliptical polarization states. Eigenvalue calibration of the system ensured high accuracy of Mueller matrix measurement over a broad wavelength range, either for forward or backscattering geometry. The system was explored for quantitative fluorescence and elastic scattering spectroscopic polarimetric studies on normal and precancerous tissue sections from human uterine cervix. The fluorescence spectroscopic Mueller matrices yielded an interesting diattenuation parameter, exhibiting differences between normal and precancerous tissues.

Quantitative Mueller matrix fluorescence spectroscopy for precancer detection

Quantitative fluorescence spectroscopic Mueller matrix measurements from the connective tissue regions of human cervical tissue reveal intriguing fluorescence diattenuation and polarizance effects. Interestingly, the estimated fluorescence linear diattenuation and polarizance parameters were considerably reduced in the precancerous tissues as compared to the normal ones. These polarimetry effects of the autofluorescence were found to originate from anisotropically organized collagen molecular structures present in the connective tissues. Consequently, the reduction of the magnitude of these polarimetric parameters at higher grades of precancer was attributed to the loss of anisotropic organization of collagen, which was also confirmed by control experiments. These results indicate that fluorescence spectral diattenuation and polarizance parameters may serve as potentially useful diagnostic metrics.

Complete polarization characterization of single plasmonic nanoparticle enabled by a novel Dark-field Mueller matrix spectroscopy system

Information on the polarization properties of scattered light from plasmonic systems are of paramount importance due to fundamental interest and potential applications. However, such studies are severely compromised due to the experimental difficulties in recording full polarization response of plasmonic nanostructures. Here, we report on a novel Mueller matrix spectroscopic system capable of acquiring complete polarization information from single isolated plasmonic nanoparticle/nanostructure. The outstanding issues pertaining to reliable measurements of full 4 × 4 spectroscopic scattering Mueller matrices from single nanoparticle/nanostructures are overcome by integrating an efficient Mueller matrix measurement scheme and a robust eigenvalue calibration method with a dark-field microscopic spectroscopy arrangement. Feasibility of quantitative Mueller matrix polarimetry and its potential utility is illustrated on a simple plasmonic system, that of gold nanorods. The demonstrated ability to record full polarization information over a broad wavelength range and to quantify the intrinsic plasmon polarimetry characteristics via Mueller matrix inverse analysis should lead to a novel route towards quantitative understanding, analysis/interpretation of a number of intricate plasmonic effects and may also prove useful towards development of polarization-controlled novel sensing schemes.

Development and eigenvalue calibration of an automated spectral Mueller matrix system for biomedical polarimetry

We present a novel spectral Mueller matrix measurement system for both elastic and inelastic scattering (fluorescence) polarimetric measurements. The system comprises of a Xenon lamp as excitation source, a polarization state generator (PSG) and a polarization state analyzer (PSA) unit to generate and analyze polarization states required for 4 x 4 sample Mueller matrix measurements, coupled to a spectrometer for spectrally resolved (λ ~ 400 - 800 nm) signal detection. The PSG unit comprises of a fixed linear polarizer (polarization axis oriented at horizontal position) followed by a rotatable broadband quarter wave plate. The sample-scattered light is collected and collimated using an assembly of lenses, then passes through the PSA unit, and is finally recorded using the spectrometer. The PSA unit essentially consists of a similar arrangement as that of the PSG, but positioned in reverse order, and with the axis of the linear polarizer oriented at vertical position. A sequence of sixteen measurements are performed by changing the orientation of the fast axis of the quarter wave plates of the PSG unit (for generating the four required elliptical polarization states) and that of the PSA unit (for analyzing the corresponding polarization states). The orientation angles (35°, 70°, 105° and 140°) were chosen based on optimization of the PSG and PSA matrices to yield most stable system Mueller matrices. The performance of the polarimeter was calibrated using Eigenvalue calibration method which also yielded the actual values of the system PSG and PSA matrices at each wavelength. The system has been automated and is capable of Mueller matrix measurement with high accuracy over the entire spectral range 400 - 800 nm (elemental error < 0.01). For recording the elastic scattering Mueller matrix of sample, the PSG and PSA matrices for each wavelength are used, while for fluorescence Mueller matrix measurements, the PSG for the excitation wavelength (chosen to be 405 nm) and PSA for varying emission wavelengths (450 - 800 nm) are used. The developed spectral Mueller matrix system has been initially used to record both elastic scattering and fluorescence Mueller matrices from normal and cancerous cervical tissues.

Probing intrinsic anisotropies of fluorescence: Mueller matrix approach

Abstract. We demonstrate that information on “intrinsic” anisotropies of fluorescence originating from preferential orientation/organization of fluorophore molecules can be probed using a Mueller matrix of fluorescence. For this purpose, we have developed a simplified model to decouple and separately quantify the depolarization property and the intrinsic anisotropy properties of fluorescence from the experimentally measured fluorescence Mueller matrix. Unlike the traditionally defined fluorescence anisotropy parameter, the Mueller matrix-derived fluorescence polarization metrics, namely, fluorescence diattenuation and polarizance parameters, exclusively deal with the intrinsic anisotropies of fluorescence. The utility of these newly derived fluorescence polarimetry parameters is demonstrated on model systems exhibiting multiple polarimetry effects, and an interesting example is illustrated on biomedically important fluorophores, collagen.

Polarization-Tailored Fano Interference in Plasmonic Crystals: A Mueller Matrix Model of Anisotropic Fano Resonance

Fano resonance is observed in a wide range of micro- and nano-optical systems and has been a subject of intensive investigations due to its numerous potential applications. Methods that can control or modulate Fano resonance by tuning some experimentally accessible parameters are highly desirable for realistic applications. Here we present a simple yet elegant approach using the Mueller matrix formalism for controlling the Fano interference effect and engineering the resulting asymmetric spectral line shape in an anisotropic optical system. The approach is founded on a generalized model of anisotropic Fano resonance, which relates the spectral asymmetry to physically meaningful and experimentally accessible parameters of interference, namely, the Fano phase shift and the relative amplitudes of the interfering modes. The differences in these parameters between orthogonal linear polarizations in an anisotropic system are exploited to desirably tune the Fano spectral asymmetry using pre- and postselection of optimized polarization states. The concept is demonstrated on waveguided plasmonic crystals using Mueller matrix-based polarization analysis. The approach enabled tailoring of several exotic regimes of Fano resonance in a single device, including the complete reversal of the spectral asymmetry, and shows potential for applications involving control and manipulation of electromagnetic waves at the nanoscale.

Mueller matrix polarimetry in fluorescence scattering from biological tissues

Mueller matrix polarimetric investigation of normal and diseased human cervical tissue samples in fluorescence scattering yields the possibility of early detection of the disease and a novel probe to monitor morphological changes during disease progression.

Tunable Spin dependent beam shift by simultaneously tailoring geometric and dynamical phases of light in inhomogeneous anisotropic medium

Spin orbit interaction and the resulting Spin Hall effect of light are under recent intensive investigations because of their fundamental nature and potential applications. Here, we report an interesting manifestation of spin Hall effect of light and demonstrate its tunability in an inhomogeneous anisotropic medium exhibiting spatially varying retardance level. In our system, the beam shift occurs only for one circular polarization mode keeping the other orthogonal mode unaffected, which is shown to arise due to the combined spatial gradients of the geometric phase and the dynamical phase of light. The constituent two orthogonal circular polarization modes of an input linearly polarized light evolve in different trajectories, eventually manifesting as a large and tunable spin separation. The spin dependent beam shift and the demonstrated principle of simultaneously tailoring space-varying geometric and dynamical phase of light for achieving its tunability (of both magnitude and direction), may provide an attractive route towards development of spin-optical devices.

Giant spin hall effect of light in an exotic optical system

We report a giant enhancement of Spin Hall (SH) shift even for normal incidence in an exotic optical system, an inhomogeneous anisotropic medium having complex spatially varying birefringent structure. The spatial variation of birefringence is obtained by changing the three dimensional orientation of liquid crystal by modulating the pixels with user-controlled greyscale value. This polarization dependent spatial variation (in a plane transverse to the direction of propagation of light) of the transmitted light beam (for incident fundamental Gaussian beam lacking any intrinsic angular momentum) through such inhomogeneous anisotropic medium was recorded using an Eigenvalue calibrated Stokes- Mueller imaging system. Giant SH shift was manifested as distinctly different spatial distribution of the recorded output Stokes vector elements for two orthogonal (left and right) input circular polarization states. We unravel the reason for such large enhancement of SH shift by performing rigorous three dimensional analysis of polarization evolution in such complex anisotropic medium. The theoretical analysis revealed that generation of large magnitude of transverse energy flow (quantified via the Poynting vector evolution inside the medium) originating from Spin Orbit Interaction (SOI) in the inhomogeneous birefringent medium leads to the observation of such a large spin dependent deflection of the trajectory of light beam.

Mueller matrix spectroscopy of fano resonance in plasmonic oligomers

Abstract Fano resonance in plasmonic oligomers originating from the interference of a spectrally broad superradiant mode and a discrete subradiant mode is under intensive recent investigations due to numerous potential applications. In this regard, development of experimental means to understand and control the complex Fano interference process and to modulate the resulting asymmetric Fano spectral line shape is highly sought after. Here we present a polarization Mueller matrix measurement and inverse analysis approach for quantitative understanding and interpretation of the complex interference process that lead to Fano resonance in symmetry broken plasmonic oligomers. The spectral Mueller matrices of the plasmonic oligomers were recorded using a custom designed dark-field Mueller matrix spectroscopy system. These were subsequently analyzed using differential Mueller matrix decomposition technique to yield the quantitative sample polarimetry characteristics, namely, polarization diattenuation (d) and linear retardance ( δ ) parameters. The unique signature of the interference of the superradiant dipolar plasmon mode and the subradiant quadrupolar mode of the symmetry broken plasmonic oligomers manifested as rapid spectral variation of the diattenuation and the linear retardance parameters across the Fano spectral dip. The polarization information contained in the Mueller matrix was further utilized to desirably control the Fano spectral line shape. The experimental Mueller matrix analysis was complemented with finite element based numerical simulations, which enabled quantitative understanding of the interference of the superradiant and the subradiant plasmon modes and its link with the polarization diattenuation and retardance parameters preparation.