Atomic-scale visualization of the toroidal order in a trimeric Dy(III) single-molecule toroic

Abstract: Single-molecule toroics (SMTs) offer a unique platform for next-generation quantum devices utilizing head-to-tail spin alignments in the compounds. Presence of toroidal moments in SMTs has been essentially based on magnetometry and ab initio calculations. Here, we report observation and probe of the toroidal moment in [Dy3(OH)(teaH2)3(paa)3]Cl(OMe) [teaH3: triethanolamine; paaH: N-(2-pyridyl)-acetoacetamide] from mapping of Dy3+ magnetic susceptibility tensors by polarized neutron diffraction (PND). Neutron diffraction under variable magnetic fields demonstrates field-induced magnetization along the c-axis with toroidal moments anti-parallelly stacked, providing definite proof of the toroidal moment. Magnetometry studies confirm the toroidal ground state. For the first time, the combined use of PND, variable-field neutron diffraction, ab initio calculations, and magnetometry is introduced as a robust and quantitative methodology to probe molecular-scale toroidal magnetism. This integrated approach overcomes limitations of earlier indirect methods, establishes a benchmark framework for investigating SMTs, and provides valuable insights for the design of molecular quantum materials.