Large nonlinear optical electronic polarizabilities would be advantageous for a variety of devices and have been intensely studied for around three decades. This project examines the theoretical limits on the static first non-linear electronic susceptibility of a material, known as the hyperpolarizability. Numerical optimizations for a single fermion in a one-dimensional potential suggest that ...

The frequency-dependent vibrational second hyperpolarizability of CH42nFn molecules with n 50 – 4 has been computed for the most common nonlinear optical ~NLO! processes by adopting the perturbation approach due to Bishop and Kirtman @J. Chem. Phys. 95, 2646 ~1991!#. These calculations have been performed by using the Sadlej atomic basis set with the Hartree-Fock technique as well as with the M...

Motivated by a discrepancy of five orders of magnitude between three different hyperpolarizability measurements on the CGO fullerene, we calculated the optical response of this cluster using a tight-binding Hamiltonian and compared the results to those for a benzene molecule. Our Hamiltonian reproduces the linear polarizability and hyperpolarizability of benzene reasonably well. For C60, our ca...

The gas-phase thermal tautomerization reaction between imidazole-4-acetic (I) and imidazole-5-acetic (II) acids was monitored using the traditional hybrid functional (B3LYP) and the long-range corrected functionals (CAM-B3LYP and ωB97XD) with 6-311++G** and aug-cc-pvdz basis sets. The roles of the long-range and dispersion corrections on their geometrical parameters, thermodynamic functions, ki...

Several DFT functionals have been carried out to study the first hyperpolarizabilities βHRS of push-pull polyene as a function basis sets, electron correlation, size, frequency dispersion and geometry. These calculations confirm huge effects Møller– Plesset (MP2) results reproduces values hyperpolarizability obtained with reference CCSD(T) level. Among density functional theory exchange- correl...

Successfully predicting the frequency dispersion of electronic hyperpolarizabilities is an unresolved challenge in materials science and electronic structure theory. We show that the generalized Thomas-Kuhn sum rules, combined with linear absorption data and measured hyperpolarizability at one or two frequencies, may be used to predict the entire frequency-dependent electronic hyperpolarizabili...

Scaling laws for third-order susceptibilities are important in guiding efforts to develop better nonlinear-optical materials. Usually these scaling laws are derived by consideration of simplified model systems chosen for analytic or computational tractability, and they are mostly untested by experiment.'3 Here we derive a scaling law based on an essentially exact solution for the hyperpolarizab...

theoretical study of the electronic structure, and nonlinear optical properties (nlo) analysis of 12-crown-4were done using density functional theory (dft) evaluations at the b3lyp/6-311g (d,p) level of theory. the optimized structure is nonlinear compound as indicated from the dihedral angles were presented. the calculated ehomo and elumo energies of 12-crown-4 (12cn4) can be used to explain t...