: The unpolarized absorption and circular dichroism spectra of the fundamental vibrational transitions of the chiral molecule, 4-methyl-2-oxetanone, are calculated ab initio. Harmonic force fields are obtained using Density Functional Theory (DFT), MP2, and SCF methodologies and a 5S4P2D/3S2P (TZ2P) basis set. DFT calculations use the Local Spin Density Approximation (LSDA), BLYP, and Becke3LYP (B3LYP) density functionals. Mid-IR spectra predicted using LSDA, BLYP, and B3LYP force fields are of significantly different quality, the B3LYP force field yielding spectra in clearly superior, and overall excellent, agreement with experiment. The MP2 force field yields spectra in slightly worse agreement with experiment than the B3LYP force field. The SCF force field yields spectra in poor agreement with experiment.The basis set dependence of B3LYP force fields is also explored: the 6-31G* and TZ2P basis sets give very similar results while the 3-21G basis set yields spectra in substantially worse agreements with experiment. jg

Ab initio calculation of vibrational absorption and circular dichroism spectra using density functional force fields

This review article provides an overview of recent advances in the study and understanding of dynamics of excitons in semiconductor nanocrystals (NCs) or quantum dots (QDs). Emphasis is placed on the relationship between exciton dynamics and optical properties, both linear and nonlinear. We also focus on the unique aspects of exciton dynamics in semiconductor NCs as compared to those in bulk crystals. Various experimental techniques for probing exciton dynamics, particularly time-resolved laser methods, are reviewed. Relevant models and computational studies are also briefly presented. By comparing different materials systems, a unifying picture is proposed to account for the major dynamic features of excitons in semiconductor QDs. While the specific dynamic processes involved are material-dependent, key processes can be identified for all the materials that include electronic dephasing, intraband relaxation, trapping, and interband recombination of free and trapped charge carriers (electron and hole). Exciton dynamics play a critical role in the fundamental properties and functionalities of nanomaterials of interest for a variety of applications including optical detectors, solar energy conversion, lasers, and sensors. A better understanding of exciton dynamics in nanomaterials is thus important both fundamentally and technologically.

Exciton Dynamics in Semiconductor Nanocrystals

Linear and nonlinear optical absorption coefficients and binding energy of a spherical quantum dot

Computation of the oscillator strength and absorption coefficients for the intersubband transitions of the spherical quantum dot

In this study, we have investigated the influence of an external electric field on the electronic properties of the ground and excited states and studied the linear and the third-order nonlinear optical properties (i.e., absorption coefficients and refractive indices) in a spherical semiconductor quantum dot of a parabolic confinement with an on-center shallow hydrogenic impurity. In the calculations, a variational procedure was employed within the effective-mass approximation. We found that the binding energies of the ground and excited states, the absorption coefficients, and the refractive index changes of 0s-1p and 1p-2d transitions depend on the applied electric field. The results show that the existence of the electric field has great influence on the optical absorption coefficients and the refractive index changes. Also, we have found that the magnitudes of the absorption coefficient and the refractive index change of the spherical quantum dot increase for transitions between higher levels.

Ayhan Özmen

Papers

Linear and nonlinear optical absorption coefficients and binding energy of a spherical quantum dot

Computation of the oscillator strength and absorption coefficients for the intersubband transitions of the spherical quantum dot

Calculation of linear and nonlinear optical absorption coefficients of a spherical quantum dot with parabolic potential

Refractive index changes and absorption coefficients in a spherical quantum dot with parabolic potential

Off-center hydrogenic impurity in spherical quantum dot with parabolic potential