A thiazolo[5,4-d]thiazole-bridged porphyrin organic framework as a promising nonlinear optical material.

Porphyrin-based porous organic frameworks are an important group of materials gaining interest due to their structural diversity and distinct opto-electronic properties. However, these materials are seldom explored for nonlinear optical (NLO) applications. In this work, we investigate a thiazolo[5,4-d]thiazole-bridged porous, porphyrin framework (Por-TzTz-POF) with promising NLO properties. The planar TzTz moiety coupled with integrated porphyrin units enables efficient π-conjugation and charge distribution in the Por-TzTz-POF resulting in a high nonlinear absorption coefficient (ß = 1100 cm GW-1) with figure of merit (FoM) σ1/σ0 = 5571, in contrast to analogous molecules and material counterparts e.g. metal-organic frameworks (MOFs; ß = ∼0.3-0.5 cm GW-1), molecular porphyrins (ß = ∼100-400 cm GW-1), graphene (ß = 900 cm GW-1), and covalent organic frameworks (Por-COF-HH; ß = 1040 cm GW-1 and FoM = 3534).

Nonlinear Optical Switching in Regioregular Porphyrin Covalent Organic Frameworks.

Covalent organic frameworks (COFs) have garnered immense scientific interest among porous materials because of their structural tunability and diverse properties. However, the response of such materials toward laser-induced nonlinear optical (NLO) applications is hardly understood and demands prompt attention. Three novel regioregular porphyrin (Por)-based porous COFs-Por-COF-HH and its dual metalated congeners Por-COF-ZnCu and Por-COF-ZnNi-have been prepared and present excellent NLO properties. Notably, intensity-dependent NLO switching behavior was observed for these Por-COFs, which is highly desirable for optical switching and optical limiting devices. Moreover, the efficient π-conjugation and charge-transfer transition in ZnCu-Por-COF enabled a high nonlinear absorption coefficient (ß=4470 cm/GW) and figure of merit (FOM=σ1 /σo , 3565) value compared to other state-of-the-art materials, including molecular porphyrins (ß≈100-400 cm/GW), metal-organic frameworks (MOFs; ß≈0.3-0.5 cm/GW), and graphene (ß=900 cm/GW).

Ultrashort vortex from a Gaussian pulse - An achromatic-interferometric approach.

The more than a century old Sagnac interferometer is put to first of its kind use to generate an achromatic single-charge vortex equivalent to a Laguerre-Gaussian beam possessing orbital angular momentum (OAM). The interference of counter-propagating polychromatic Gaussian beams of beam waist ωλ with correlated linear phase (ϕ 0 ≥ 0.025 λ) and lateral shear (y 0 ≥ 0.05 ωλ) in orthogonal directions is shown to create a vortex phase distribution around the null interference. Using a wavelength-tunable continuous-wave laser the entire range of visible wavelengths is shown to satisfy the condition for vortex generation to achieve a highly stable white-light vortex with excellent propagation integrity. The application capablitiy of the proposed scheme is demonstrated by generating ultrashort optical vortex pulses, its nonlinear frequency conversion and transforming them to vector pulses. We believe that our scheme for generating robust achromatic vortex (implemented with only mirrors and a beam-splitter) pulses in the femtosecond regime, with no conceivable spectral-temporal range and peak-power limitations, can have significant advantages for a variety of applications.