Synergy of Experiment and Broadened Exploration of Ab Initio Calculations for Understanding of Lanthanide-Pentacyanidocobaltate Molecular Nanomagnets and Their Optical Properties.

We present a synergistic experimental-theoretical methodology for the investigation of lanthanide-based single-molecule magnets (SMMs), demonstrated using the example of novel heterometallic molecules incorporating Nd/Ce ions combined with three different, rarely explored, pentacyanidocobaltate(III) metalloligands, [Co(CN)(azido/nitrito-/iodido)]. The theoretical part of our approach broadens the exploration of calculations for lanthanide(III) complexes toward the convenient simulations of such physical characteristics as directional dependences of Helmholtz energy, magnetization, susceptibility, and their thermal and field evolution, as well as light absorption and emission bands. This work was conducted using newly designed SlothPy software (https://slothpy.

SHG-active luminescent thermometers based on chiral cyclometalated dicyanidoiridate(iii) complexes.

Multifunctional optical materials can be realized by combining stimuli-responsive photoluminescence (PL), , optical thermometry, with non-linear optical (NLO) effects, such as second-harmonic generation (SHG). We report a novel approach towards SHG-active luminescent thermometers achieved by constructing unique iridium(iii) complexes, -[Ir(CN)(,-pinppy)] (,-pinppy = (,)-2-phenyl-4,5-pinenopyridine), bearing both a chiral 2-phenylpyridine derivative and cyanido ligands, the latter enabling the formation of a series of molecular materials: (TBA)[Ir(CN)(,-pinppy)]·2MeCN (1) (TBA = tetrabutylammonium) and (Bu-DABCO)[Ir(CN)(,-pinppy)](i)·MeCN (2) (Bu-DABCO = 1-(-butyl)-1,4-diazabicyclo-[2.2.