Search for: All records

The magnetic properties and phase diagrams of S = 1/2 quasi-one-dimensional Heisenberg antiferromagnets are well established with copper-containing coordination polymers as the platform of choice due to their low energy scales and ease of chemical substitution. The inability to uncover orbitally resolved components of the magnetization has, however, been a longstanding barrier to greater understanding of high field spin state transitions. In this work, we combine pulsed field magnetization, optical spectroscopy, and magnetic circular dichroism with complementary electronic structure calculations to unravel orbital-specific contributions to the magnetism in the linear chain quantum magnet [CuL2(H2O)2(pyz)](ClO4)2 [L = 5-methyl-2-pyridone; pyz = pyrazine]. In addition to revealing a spin flop and field-driven transition to the fully saturated spin state, we untangle the green → teal color change across the 185 K structural phase transition and employ what we learn about the different Cu2+ → pyrazine charge transfer excitations to decompose the magnetic circular dichroism. Analysis reveals that both eg-derived Cu2+ 3d orbitals play a role in the field-driven transition to the fully saturated state, not just those formally hosting unpaired electrons. We attribute the surprisingly strong dichroic signature at room temperature to the presence of uncorrelated spin. 

Abstract Kagomé metals are widely recognized, versatile platforms for exploring topological properties, unconventional electronic correlations, magnetic frustration, and superconductivity. In theRV₆Sn₆family of materials (R= Sc, Y, Lu), ScV₆Sn₆hosts an unusual charge density wave ground state as well as structural similarities with theAV₃Sb₅system (A= K, Cs, Rb). In this work, we combine Raman scattering spectroscopy with first-principles lattice dynamics calculations to reveal phonon mixing processes in the charge density wave state of ScV₆Sn₆. In the low temperature phase, we find at least four new peaks in the vicinity of the V-containing totally symmetric mode near 240 cm⁻¹suggesting that the density wave acts to mix modes ofP6/mmmand$$R\bar{3}m$$ $R\overline{3}m$symmetry - a result that we quantify by projecting phonons of the high symmetry state onto those of the lower symmetry structure. We also test the stability of the short-range ordered density wave state under compression and propose that both physical and chemical pressure quench the effect. We discuss these findings in terms of symmetry and the structure-property trends that can be unraveled in this system.