Spiral Graphene Nanoribbons with Azulene Defects as Potential Nonlinear Optical Materials

Abstract

Inducing new nonlinear optical (NLO) properties while keeping the thermal stability of carbon-based nanomaterials paves a new path for the application of carbon nanomaterials in optoelectronics. In the present work, azulene units are introduced to spiral carbon nanoribbons to enhance the polarity of the charge distribution in spiral carbon nanoribbons, significantly enhancing the first hyperpolarizabilities of those nanoribbons and making the nanoribbons potential nonlinear optical materials. For example, the static first hyperpolarizability of azulene-defected spiral graphene nanoribbon with eight units (ADSGN8) is 2499.0 × 10–30 esu, whereas that of azulene spiral graphene nanoribbon (SGN8) is only 12.0 × 10–30 esu. The two-dimensional second-order NLO spectra predicted by the sum-over-states model reveal the strong second-order NLO responses of the nanomaterials under external fields, particularly within the visible region of approximately 600.0 nm. The origin of the first hyperpolarizability of azulene-defected spiral carbon nanoribbons is scrutinized and further improvement on the NLO responses of those systems is proposed.

PCM-DFT Investigation on the Linear and Nonlinear Optical Properties of Two Triazole Derivatives in Different Solvents

“…Here the large 6-311+G(d) Pople split-valence basis set is used combined with the CAM-B3LYP. In favor of usingthe PCM model, recent theoretical studies of NLO properties of molecules immersed in solvent media have shown a good agreement with the experimental data for the Hyper-Rayleigh Scattering first hyperpolarizability [5,13,21,25].…”

Tuning the edge states in X-type carbon based molecules for applications in nonlinear optics

“…, azulene-embedded nanographene 26,27 and azulene-defected GNRs. 21,28 In this work, the designed X-type molecules are polyacene based molecules with azulenes at four end-corners (Fig. 1) and similar systems have been successfully synthesized.…”

“…Accordingly, considerable efforts have been devoted toward synthesizing and predicting carbon based molecules fused with azulenes in various patterns, e.g., azulene-embedded nanographene 26,27 and azulene-defected GNRs. 21,28 In this work, the designed X-type molecules are polyacene based molecules with azulenes at four end-corners (Fig. 1) and similar systems have been successfully synthesized.…”

A new isostructural halogenated chalcone with optical properties

“…The sum-over-state (SOS) approach will be used to calculate the second hyperpolarizability. The SOS approach has been widely used to calculate the second molecular hyperpolarizability in organic compounds [49][50][51][52][53][54][55][56][57][58][59]. The benefit of the SOS approach is that it truncates the sum of states, as the significant contribution occurs in only a few excited states.…”