The photochemical deactivation process of HCFC-133a (C2H2F3Cl) was investigated by computing excited-state properties with a number of single-reference methods, including coupled cluster to approximated second order (CC2), algebraic diagrammatic construction to second order (ADC(2)), and time-dependent density functional theory (TDDFT). Excited states calculated with these methods, especially T...

Based on the equilibrium geometries of [Cu2(dbdmed)2O2](2+) and [Cu2(en)2O2](2+) obtained within density-functional theory, we investigate their molecular electronic structure and optical response. Thereby results from occupation-constrained as well as time-dependent DFT (ΔSCF and TDDFT) are compared with Green's function-based approaches within many-body perturbation theory such as the GW appr...

We present an efficient method to compute nonadiabatic couplings (NACs) between the electronically ground and excited states of molecules, within the framework of time-dependent density functional theory (TDDFT) in frequency domain. Based on the comparison of dynamic polarizability formulated both in the many-body wave function form and the Casida formalism, a rigorous expression is established...

We report a numerical study of strong-field ionization rates of the H2 molecule using time-dependent densityfunctional theory (TDDFT). In the dc field limit, TDDFT results for the rate of tunneling ionization agree with molecular Ammosov-Delone-Kralnov (MO-ADK) predictions, as well as results from a complex scaling method at the full configuration interaction level. Our study demonstrates the e...

Azobenzenes have a unique ability to undergo reversible isomerization between two geometrical isomer forms (the straight trans and the bent cis) when irradiated with the correct wavelength of UV or visible light. These systems are of interest because of their numerous potential applications as reversible photoswitchable absorbers. The azobenzenes can also be used as terminal groups in nickel di...

An extension of density functional theory to situations with significant nondynamical correlation is presented. The method is based on the spin–flip ~SF! approach which is capable of describing multireference wave functions within a single reference formalism as spin–flipping, e.g., a→b, excitations from a high-spin (M s51) triplet reference state. An implementation of the spin–flip approach wi...

Time-dependent density functional theory (TDDFT) is a powerful tool allowing for accurate description of excited states in many nanoscale molecular systems; however, its application to large molecules may be plagued with difficulties that are not immediately obvious from previous experiences of applying TDDFT to small molecules. In TDDFT, the appearance of spurious charge-transfer states below ...

The optoelectronic and excitonic properties in a series of linear acenes (naphthalene up to heptacene) are investigated using range-separated methods within time-dependent density functional theory (TDDFT). In these rather simple systems, it is well-known that TDDFT methods using conventional hybrid functionals surprisingly fail in describing the low-lying L(a) and L(b) valence states, resultin...

Fluorescent base analogues (FBAs) comprise a family of increasingly important molecules for the investigation of nucleic acid structure and dynamics. We recently reported the quantum chemical calculation supported development of four microenvironment sensitive analogues of the quadracyclic adenine (qA) scaffold, the qANs, with highly promising absorptive and fluorescence properties that were ve...