Two‐Photon Luminescence and Second‐Harmonic Generation in Organic Nonlinear Surface Comprised of Self‐Assembled Frustum Shaped Organic Microlasers

Venkatakrishnarao, Dasari; Narayana, Yemineni S. L. V.; Mohaiddon, Mahamad A.; Mamonov, E. A.; Mitetelo, N. V.; Kolmychek, I. A.; Maydykovskiy, A. I.; Novikov, V. B.; Murzina, T. V.; Chandrasekar, Rajadurai

doi:10.1002/adma.201605260

Cited by 93 publications

(72 citation statements)

References 35 publications

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“…Further, the production of two‐photon pumped NLO cavities is in demand because they produce frequency upconverted optical signals and importantly, operated by infrared lasers. On the other hand, organic NLO crystalline cavities are intrinsic in nature, as a result, they are rarely realized, and to our knowledge, only less than a dozen reports are out there in the literature . The prerequisites for an intrinsic type of NLO cavity are: (i) strong NLO activity (e.g., two‐photon absorption) and (ii) high‐quality microcrystal or structure with high refractive index and smooth light‐reflecting mirror‐like facets for an effective feedback action .…”

Section: Methodsmentioning

confidence: 99%

Ambient Pressure Sublimation Technique Provides Polymorph‐Selective Perylene Nonlinear Optical Microcavities

Pradeep

Mitetelo

Annadhasan

et al. 2019

Advanced Optical Materials

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Highly pure, organic, crystalline materials with nonlinear optical (NLO) properties are in great demand due to their potential to be utilized in miniaturized nanophotonic device applications. Perylene dye is one of the celebrated near‐direct bandgap NLO materials. It crystallizes in two distinctive polymorphic forms (square‐shaped, α, and rhombus‐shaped, β) emitting yellow and green fluorescence, respectively. However, selective access to any one of the polymorphic microcrystals possessing qualities such as smooth‐surface and mirror‐like light‐reflecting sharp edges is a challenging task. On the other hand, these qualities are indispensable for a microcrystal to operate as an optical cavity. Here, a cost‐effective and straightforward, yet promising sublimation technique to grow microscale perylene crystals with the above qualities in a polymorph‐selective manner at ambient pressure is presented. As a result, both polymorphic microcrystals act as whispering gallery mode (WGM) cavities in the linear and notably, NLO regime as well. In agreement with the experiments, finite difference time domain numerical calculations support the WGM‐cavity‐type and also reveal the intricate localization of electric‐field within these cavities. Further, the quadratic dependence of emission intensity as a function of laser power establishes the two‐photon absorption nature of the optical cavities pumped by infrared lasers.

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Section: Methodsmentioning

confidence: 99%

Ambient Pressure Sublimation Technique Provides Polymorph‐Selective Perylene Nonlinear Optical Microcavities

Pradeep

Mitetelo

Annadhasan

et al. 2019

Advanced Optical Materials

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“…The quadratic dependence of the intensity on the fundamental beam power unambiguously confirmed the role of the two‐photon absorption in this NLO process (Figure B). Due to resonant coupling, the TPL signal intensity from these micro‐resonators is four times higher than from the thin films of comparable thickness (Figure S6) …”

Section: Methodsmentioning

confidence: 99%

“…Infra‐red laser pumped miniature organic non‐linear optical (NLO) resonators are important for the amplification of inherently weak up‐converted signals . Two‐photon luminescence (TPL) is one of the essential NLO up‐conversion processes which arises as a result of the absorption of two photons by the NLO materials .…”

Section: Methodsmentioning

confidence: 99%

A Two‐Photon Pumped Supramolecular Upconversion Microresonator

et al. 2018

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A two‐photon pumped non‐linear optical (NLO) Fabry‐Pèrot (F‐P) type organic micro‐crystal resonator useful for a myriad of upconversion‐based light technologies is presented. The resonator is parallelepiped‐shaped and composed of a self‐assembled donor‐acceptor‐donor type molecule namely, 9,9,9”,9”‐tetramethyl‐9H,9’H,9”H‐[2, 2’:7,2”‐terfluoren]‐9’‐one (TTO). X‐ray crystal structure of an orange‐yellow TTO micro‐crystal reveals C−H⋅⋅⋅O type weak intermolecular hydrogen bond between the oxygen atom of the fluorenone unit and fluorine hydrogen atom. For one‐ and two‐photon excitation the micro‐crystals exhibit F‐P type modes in their photoluminescence signal. The fundamental frequency‐dependent NLO intensity shows a continuous increase as the fundamental wavelength is decreasing down to 770 nm. The two‐photon luminescence signals from these micro‐resonators are several orders of magnitude higher than the thin films of similar thickness.

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“…Therefore, we envisioned the fabrication of MHS composed of two well‐known semi‐conductor molecules, namely, Dicyanomethylene)‐2‐methyl‐6‐( p ‐dimethylaminostyryl) 4H‐pyran (DCM) and perylene (Scheme ). The reasons for our choice are: (i) DCM forms one dimensional (1D) micro‐rods emitting red fluorescence (FL), (ii) perylene exist in two geometrically and optically different two dimensional (2D) polymorphs, the square‐shaped α and rhombus‐shaped β forms emitting yellow and green fluorescence, respectively . Further, DCM is a donor‐π‐bridge‐acceptor type molecule with low band gap optical material.…”

Section: Methodsmentioning

confidence: 99%

Vapour‐Phase Epitaxial Growth of Dual‐Colour‐Emitting DCM‐Perylene Micro‐Heterostructure Optical Waveguides

Pradeep

Annadhasan

Chandrasekar

2019

Chemistry An Asian Journal

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Organicm icro-heterostructures (MHS) with dual optical emissions are essential to produce miniaturized optical waveguidesf or wavelength divisionm ultiplexing technologies. The bimolecular MHS produced by solutionbased bottom-up self-assembly technique often leads to poor surface smoothness, edge imperfection, defects, and unwanted thin films deposits. Conversely,s equential sublimation technique at ambient pressure facilitates effective integration of a-perylene micro-square with dicyanomethylene-2-methyl-6-(p-dimethylaminostyryl) 4H-pyran (DCM) microrods in an epitaxial manner to produce MHS. The obtained DCM/perylene MHS act as optical waveguides to produce red (l max % 670 nm) or/and yellow (l max % 607 nm) dual optical outputs via an energy transfer mechanism depending upon the heterostructures geometry and optical excitation positions. The presented dualcolor emitting MHS opticalw aveguidesa re essential for the integratedn ano-photonic and optoelectronic device structures.Nano-and micro-scaleo rganic devices tructures are rapidly emerging as an alternative to inorganic ones. [1] Mainly,b ecause of the electronic properties of organic molecules are easily tunable via custom-made synthesis, andv ariousf lexible device structure can be fabricated by either solution-or physical vapor deposition techniques. [1] Direct applications of organic molecule-based materials include solid-state lasers, [2] lightemitting diodes and transistors, [3] photovoltaic cells, [4] and miniaturize photonic devices. [2] The micro-/nano-scale photonic device structures comprise of components such as optical waveguides, [5,6] modulators, [5d] filters, [7] cavities, [8] and lasers. [9] The above-mentioned photonic device structures are futuristic and are vital to the development of photon-based quantum information-processing, communication as well as integratedc ircuits. [10] One of the prime requirements for the implementation [a] V. V. Pradeep, Dr.M.A nnadhasan, Prof. R. Chandrasekar

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Two‐Photon Luminescence and Second‐Harmonic Generation in Organic Nonlinear Surface Comprised of Self‐Assembled Frustum Shaped Organic Microlasers

Cited by 93 publications

References 35 publications

Ambient Pressure Sublimation Technique Provides Polymorph‐Selective Perylene Nonlinear Optical Microcavities

Ambient Pressure Sublimation Technique Provides Polymorph‐Selective Perylene Nonlinear Optical Microcavities

A Two‐Photon Pumped Supramolecular Upconversion Microresonator

Vapour‐Phase Epitaxial Growth of Dual‐Colour‐Emitting DCM‐Perylene Micro‐Heterostructure Optical Waveguides

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