Efficient Calculation of Magnetic Circular Dichroism Spectra Using Spin-Noncollinear Linear-Response Time-Dependent Density Functional Theory in Finite Magnetic Fields.

Excited-state calculations in finite magnetic fields are presented in the framework of spin-noncollinear linear-response time-dependent density functional theory. To ensure gauge-origin invariance, London atomic orbitals are employed throughout. An efficient implementation into the Turbomole package, which also includes the resolution of the identity approximation, allows for the investigation of excited states of large molecular systems. The implementation is used to investigate the magnetic circular dichroism spectra of sizable organometallic molecules such as a zinc tetraazaporphyrin with two fused naphthalene units, which is a molecule with 57 atoms.