Publications by authors named "Venkatram Nalla"

Metal-halide perovskites are rapidly emerging as solution-processable optical materials for light-emitting applications. Here, we adopt a plasmonic metamaterial approach to enhance photoluminescence emission and extraction of methylammonium lead iodide (MAPbI) thin films based on the Purcell effect. We show that hybridization of the active metal-halide film with resonant nanoscale sized slits carved into a gold film can yield more than 1 order of magnitude enhancement of luminescence intensity and nearly 3-fold reduction of luminescence lifetime corresponding to a Purcell enhancement factor of more than 300.

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Diamond is introduced as a material platform for visible/near-infrared photonic metamaterials, with a nanostructured polycrystalline diamond metasurface only 170 nm thick providing an experimental demonstration of coherent light-by-light modulation at few-optical-cycle (6 fs) pulse durations. "Coherent control" of absorption in planar (subwavelength-thickness) materials has emerged recently as a mechanism for high-contrast all-optical gating, with a speed of response that is limited only by the spectral width of the absorption line. It is shown here that a free-standing diamond membrane structured by focused ion beam milling can provide strong, spectrally near-flat absorption over a visible to near-infrared wavelength range that is wide enough (wider than is characteristically achievable in plasmonic metal metasurfaces) to facilitate coherent modulation of ultrashort optical pulses comprising only a few oscillations of electromagnetic field.

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Recently, coherent control of the optical response of thin films in standing waves has attracted considerable attention, ranging from applications in excitation-selective spectroscopy and nonlinear optics to all-optical image processing. Here, we show that integration of metamaterial and optical fibre technologies allows the use of coherently controlled absorption in a fully fiberized and packaged switching metadevice. With this metadevice, which controls light with light in a nanoscale plasmonic metamaterial film on an optical fibre tip, we provide proof-of-principle demonstrations of logical functions XOR, NOT and AND that are performed within a coherent fibre network at wavelengths between 1530 and 1565 nm.

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We demonstrate generation of the shortest reported 11fs dark pulses using the coherent absorption process on a plasmonic absorber with a gating pulse. The dark pulses appear as a power dip on the envelope of a long carrier pulse and are characterized using the cross-correlation technique. The principal difference and advantage of our approach in comparison with previously developed laser sources of dark pulses is that, in principle, it allows transferring arbitrary pattern of bright pulses into a pattern of dark pulses in another optical signal channel.

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Multi-photon absorption (MPA) is among the most prominent nonlinear optical (NLO) effects and has applications, for example in telecommunications, defense, photonics, and bio-medicines. Established MPA materials include dyes, quantum dots, organometallics and conjugated polymers, most often dispersed in solution. We demonstrate how metal-organic frameworks (MOFs), a novel NLO solid-state materials class, can be designed for exceptionally strong MPA behavior.

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With regards to developing miniaturized coherent light sources, the temperature-insensitivity in gain spectrum and threshold is highly desirable. Quantum dots (QDs) are predicted to possess a temperature-insensitive threshold by virtue of the separated electronic states; however, it is never observed in colloidal QDs due to the poor thermal stability. Besides, for the classical II-VI QDs, the gain profile generally redshifts with increasing temperature, plaguing the device chromaticity.

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Blue-color stimulated emission with low threshold power is observed from In- and Zn-MOFs, which feature a highly fluorescent chromophore densely packed and rigidly linked to the metal-ion centers in the solid state. The density-of-states and transition dipole moments are calculated and the stimulated emission phenomenon is correlated with these properties.

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Iron pyrite has received significant attention due to its high optical absorption. However, the loss of open circuit voltage (Voc) prevents its further application in photovoltaics. Herein, we have studied the photophysics of pyrite by ultrafast laser spectroscopy to understand fundamental limitation of low Voc by quantifying photocarrier losses in high quality, stoichiometric, and phase pure {100} faceted pyrite nanocubes.

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Second harmonic generation (SHG) is a well known non-linear optical phenomena which can be observed only in non-centrosymmetric crystals due to non-zero hyperpolarizability. In the current work we observed SHG from a Zn(II) complex which was originally thought to have crystallized in the centrosymmetric space group C2/c. This has been attributed to the unequal antiparallel packing of the metal complexes in the non-symmetric space group Cc or residual non-centrosymmetry in C2/c giving rise to polarizability leading to strong SHG.

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A blue (ca. 440 nm) liquid laser with an ultra-low threshold through which quasi-continuous wave pumping is accessible is achieved by engineering unconventional ternary CdZnS/ZnS alloyed-core/shell QDs. Such an achievement is enabled by exploiting the novel gain media with minimal defects, suppressed Auger recombination, and large gain cross-section in combination with high-quality-factor whispering gallery mode resonators.

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Silicon based nonlinear photonics has been extensively researched at telecom wavelengths in recent years. However, studies of Kerr nonlinearity in silicon at mid-infrared wavelengths still remain limited. Here, we report the wavelength dependency of third-order nonlinearity in the spectral range from 1.

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Two C-(antenna) analogous compounds having branched hybrid triad C(>DPAF-C)(>CPAF-C) and tetrad C(>DPAF-C)(>CPAF-C) nanostructures were synthesized and characterized. The structural design was intended to facilitate the ultrafast fs intramolecular energy-transfer from photoexcited C[>(DPAF)*-C](>CPAF-C) or C(>DPAF-C)[>(CPAF)*-C] to the C> cage moiety upon two-photon pumping at either 780 or 980 nm, respectively. The latter nanostructure showed approximately equal extinction coefficients of optical absorption over 400-550 nm that corresponds to near-IR two-photon based excitation wavelengths at 780-1100 nm for broadband nonlinear optical (NLO) applications.

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Highly sensitive, multicomponent broadband photodetector devices are made from PbSe/graphene/TiO(2). TiO(2) and PbSe nanoparticles act as light harvesting photoactive materials from the UV to IR regions of the electromagnetic spectrum, while the graphene acts as a charge collector for both photogenerated holes and electrons under an applied electric field.

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We demonstrated ultrafast femtosecond nonlinear optical (NLO) absorption characteristics of bilayered fullerosome vesicle nanostructures derived from molecular self-assembly of amphiphilic oligo(ethylene glycolated) C(60)-(light-harvesting diphenylaminofluorene antenna). Fullerene conjugates were designed to enhance photoresponse in a femtosecond time scale by applying an isomerizable periconjugation linker between the C(60) cage and diphenylaminofluorene antenna subunit in an intramolecular contact distance of only < 3.0 Å.

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Large-area patterning of epitaxial graphene for Schottky junction photodetectors has been demonstrated with a simple laser irradiation method. In this method, semimetal-semiconductor Schottky junctions are created in a controllable pattern between epitaxial graphene (EG) and laser-modified epitaxial graphene (LEG). The zero-biased EG-LEG-EG photodetector exhibits a nanosecond and wavelength-independent photoresponse in a broad-band spectrum from ultraviolet (200 nm) through visible to infrared light (1064 nm), distinctively different from conventional photon detectors.

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A water soluble conjugated thiophene polymer, sodium salt of poly[2-(3-thienyl)ethoxy-4-butylsulfonate] (TPP), and graphene oxide (GO) composite film (GO-TPP) device was prepared. Transient photoconductivity measurements were carried out on the GO-TPP composite film using 150 ns laser pulses of 527 nm wavelength. Highly efficient photocurrent generation was observed from the GO-TPP film.

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