Tailoring between network rigidity and nanosecond transient absorption in a-GexAs35-xSe65 thin films

In this letter, we report the first observation of dramatic decrease in nanosecond (ns) pulsed laser induced transient absorption (TA) in a-GexAs35-xSe65 thin films by tuning the amorphous network from floppy to rigid. Our results provide the direct experimental evidence of a self trapped exciton mechanism, where trapping of the excitons occurs through bond rearrangements. Taken together, a rigid amorphous network with more constraints than degrees of freedom, are unable to undergo any such bond rearrangements and results in weaker TA. However, we also demonstrate that excitation fluence can be effectively utilized as a simple tool to lift up enough constraints to introduce large TA even in rigid networks. Apart from this, we also show that TA is tunable with network rigidity as it blueshift when the mean coordination is increased from 2.35 to 2.6.Comment: 5 pages, 4 figure

Spin-Hall effect in the scattering of structured light from plasmonic nanowire

Spin-orbit interactions are subwavelength phenomena which can potentially lead to numerous device related applications in nanophotonics. Here, we report Spin-Hall effect in the forward scattering of Hermite-Gaussian and Gaussian beams from a plasmonic nanowire. Asymmetric scattered radiation distribution was observed for circularly polarized beams. Asymmetry in the scattered radiation distribution changes the sign when the polarization handedness inverts. We found a significant enhancement in the Spin-Hall effect for Hermite-Gaussian beam as compared to Gaussian beam for constant input power. The difference between scattered powers perpendicular to the long axis of the plasmonic nanowire was used to quantify the enhancement. In addition to it, nodal line of HG beam acts as the marker for the Spin-Hall shift. Numerical calculations corroborate experimental observations and suggest that the Spin flow component of Poynting vector associated with the circular polarization is responsible for the Spin-Hall effect and its enhancement.Comment: Optics Letters (accepted), 201

Role of Ge:As ratio in controlling the light-induced response of a-GexAs35-xSe65 thin films

In this paper, we present interesting results on the quantification of photodarkening (PD), photobleaching (PB) and transient PD (TPD) in a- GexAs35-xSe65 thin films as a function of network rigidity. Composition dependent light-induced responses of these samples indicate that there exist two parallel competing mechanisms of instantaneous PD arising from the As part of the network, and PB arising from the Ge part of the network. Raman spectra of the as-prepared and illuminated samples provide first direct evidence of the light-induced structural changes: an increase in AsSe3/2 pyramidal and GeSe4/2 corner-sharing tetrahedra units together with new Ge-O bond formation and decrease in energetically unstable edge sharing GeSe4/2 tetrahedra. Importantly, for a fixed Se concentration, Ge:As ratio plays the critical role in controlling the net light-induced response rather than the much believed rigidity of the glassy network.Comment: 26 pages, 9 figures (including the supplementary section

Nanosecond light induced, thermally tunable transient dual absorption bands in a-Ge5As30Se65 thin film

In this article, we report the first observation of nanosecond laser induced transient dual absorption bands, one in the bandgap (TA1) and another in the sub-bandgap (TA2) regions of a-Ge5As30Se65 thin films. Strikingly, these bands are thermally tunable and exhibit a unique contrasting characteristic: the magnitude of TA1 decreases while that of TA2 increases with increasing temperature. Further, the decay kinetics of these bands is strongly influenced by the temperature, which signifies a strong temperature-dependent exciton recombination mechanism. The induced absorption shows quadratic and the decay time constant shows linear dependence on the laser beam fluence.Comment: 17 pages, 6 figure

Coexistence of fast photodarkening and slow photobleaching in Ge19As21Se60 thin films

We experimentally demonstrate the coexistence of two opposite photo-effects, viz. fast photodarkening (PD) and slow photobleaching (PB) in Ge19As21Se60 thin films, when illuminated with a laser of wavelength 671nm, PD appears to begin instantaneously upon light illumination and saturates in tens of seconds. By comparison, PB is a slower process that starts only after PD has saturated. Although we could observe the coexistence of PD/PB even at moderate, one order of magnitude lower intensity of 0.2 W/cm2, the kinetics of transformation is significantly slowed down. However, both PD and PB follow stretched exponetial dependence on time. Modeling of overall change as a linear sum of two contributions suggests that the changes in As and Ge parts of glass network respond to light indepndent of each other.Comment: 6pages, 3 figures and 1 tabl

Near resonant nanosecond laser driven nonlinear optical response in As50S50 thin films

Nanosecond near resonant excitation in As50S50 thin films leads to strong nonlinear optical response, i.e. nonlinear absorption coefficient up to 4 x 106 cm/GW and nonlinear refractive index of 8.5 cm2/GW, both of which is the strongest ever reported in amorphous semiconductors. We propose a five-level energy model to explain such effect which indicates that nonlinear process is reverse saturable absorption in nature, mediated by excited state absorption from triplet-triplet transition. On the other hand, observation of negative nonlinear refractive index reveals the occurrence of self-defocusing effect. Finally, benefitting from the strong nonlinear response, we demonstrate a promising application of As50S50 thin films as an optical limiter for optoelectronic sensors.Comment: 26 pages, 6 figures, 3 table

Quantification of nonlinear absorption in ternary As-Sb-Se chalcogenide glasses

In this article, we studied intensity dependent third order nonlinear optical response in ternary As40Sb7Se53 and As40Sb10Se50 chalcogenide glasses by employing nanosecond Z-scan technique. At low intensity, we observed saturable absorption in As40Sb7Se53 which makes a remarkable transition to reverse saturable absorption at higher intensities. On the other hand, when the Sb concentration increased in As40Sb10Se50, saturable absorption disappears and the sample exhibits only two-photon absorption. Experimental results further indicate that the strong two-photon absorption in our samples can be exploited to fabricate high performance solid state optical limiting devices for next generation all-optical network.Comment: 16 pahes, 4 figure

Kinetics of photo-dissolution within Ag/As2S3 heterostructure

Chalcogenide glass-silver heterostructures are candidates for photoresist and diffractive optical applications. To optimize their processing, we report the kinetics of Ag photo-dissolution in As2S3 matrix using in-situ optical transmission/reflection measurements and real time atomic force microscopy (AFM) imaging under optical illumination. The results indicate that photodissolution occurs in three stages with the extent and kinetics of each stage depending strongly on Ag film thickness. By contrast, the photo-dissolution is found to be independent of As2S3 matrix thickness. The extent of three stages also depends strongly on the laser dose and can be reduced to two stages at higher laser fluence. A comparative study of two oppositely stacked sample configurations: As2S3/Ag/glass and Ag/As2S3/glass show that the heterostructures respond differently to light illumination. For the former, Ag dissolves completely into As2S3 matrix at a faster rate than for the latter case. The origin of this difference is established by energy dispersive X-ray spectroscopy and AFM measurements.Comment: 21 pages, 8 figures, 4 tables, Journal of Non-Crystalline Solids, 201

Intricate modulation of interlayer coupling at GO/MoSe2 interface: application in time-dependent optics and device transport

In GO/MoSe2 semiconductor heterostructure, we have demonstrated a subtle control on the doping dynamics by modulating interlayer coupling through the combination of strain-reducing relative rotation of the constituting layers and variation of ligand type and concentration. By first-principles calculations incorporating spin-orbital coupling, we have investigated the impact of variable interlayer coupling in introducing non-collinear magnetic behaviour in the heterostructure. The outcome of varying carrier type and their respective concentrations are investigated by static as well as time dependent density functional calculations, which indicates presence of optical anisotropy and time-dependent optical phenomena like exciton quenching and band-gap renormalization. Performance of such heterostructures as channel material in devices with top and edge metal contacts is analyzed. Our self-consistent quantum transport calculations have evinced that the nature of interface-induced variation in doping is extrapolated for devices only in the case of top contacts. The edge contact, although exhibits a better transmission, are inefficient for sensing the ligand-induced doping modulation introduced via vertical inter-layer charge transfer.Comment: 10 figure

Ultrafast light-induced softening of chalcogenide thin films above the rigidity percolation transition

Little is known about the role of network rigidity in light-induced structural rearrangements in network glasses due to a lack of supporting experiments and theories. In this report, we demonstrate for the first time the ultrafast structural rearrangements manifested as induced absorption (IA) over a broad spectral range in a-GexAs35-xSe65 thin films above the mean-field rigidity percolation transition, quantified by the mean coordination number = 2.40. The IA spectrum arising from self-trapped excitons, induced structural rearrangements by softening the glass network that strikingly reveal two relaxation mechanisms which differ by one order of magnitude. The fast kinetics of electron-lattice interaction occurs within 1 ps, exhibits a weak dependence on rigidity and dominates in the sub-bandgap region. In a stark contrast, the slow kinetics are associated with the structural changes in the bandgap region and depends strongly on network rigidity. Our results further demonstrate that amplitude of IA scales a linear relationship with excitation fluence which provides a unique way to induce structural rearrangements in over-coordinated network to exploit it for practical purposes. Our results modify the conventional concept of rigidity dependence of light-induced effects in network glasses, when excited with an ultrafast laser.Comment: 20 pages, 5 figures, Journal of Applied Physics, 201