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We bring together synchrotron-based infrared and Raman spectroscopies, diamond anvil cell techniques, and an analysis of frequency shifts and lattice dynamics to unveil the vibrational properties of multiwall WS2 nanotubes under compression. While most of the vibrational modes display similar hardening trends, the Raman-active A1g breathing mode is almost twice as responsive, suggesting that the nanotube breakdown pathway under strain proceeds through this displacement. At the same time, the previously unexplored high pressure infrared response provides unexpected insight into the electronic properties of the multiwall WS2 tubes. The development of the localized absorption is fit to a percolation model, indicating that the nanotubes display a modest macroscopic conductivity due to hopping from tube to tube.

Vibrations play a prominent role in magnetic relaxation processes of molecular spin qubits as they couple to spin states, leading to the loss of quantum information. Direct experimental determination of vibronic coupling is crucial to understand and control the spin dynamics of these nano-objects, which represent the limit of miniaturization for quantum devices. Herein, we measure the magneto-infrared properties of the molecular spin qubit system Na9[Ho­(W5O18)2]·35H2O. Our results place significant constraints on the pattern of crystal field levels and the vibrational excitations allowing us to unravel vibronic decoherence pathways in this system. We observe field-induced spectral changes near 63 and 370 cm–1 that are modeled in terms of odd-symmetry vibrations mixed with f-manifold crystal field excitations. The overall extent of vibronic coupling in Na9[Ho­(W5O18)2]·35H2O is limited by a modest coupling constant (on the order of 0.25) and a transparency window in the phonon density of states that acts to keep the intramolecular vibrations and M J levels apart. These findings advance the understanding of vibronic coupling in a molecular magnet with atomic clock transitions and suggest strategies for designing molecular spin qubits with improved coherence lifetimes.

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We report the growth of single-phase (0001)-oriented epitaxial films of the purported electronically driven multiferroic, LuFe2O4, on (111) MgAl2O4, (111) MgO, and (0001) 6H-SiC substrates. Film stoichiometry was regulated using an adsorption-controlled growth process by depositing LuFe2O4 in an iron-rich environment at pressures and temperatures where excess iron desorbs from the film surface during growth. Scanning transmission electron microscopy reveals reaction-free film-substrate interfaces. The magnetization increases rapidly below 240 K, consistent with the paramagnetic-to-ferrimagnetic phase transition of bulk LuFe2O4. In addition to the ∼0.35 eV indirect band gap, optical spectroscopy reveals a 3.4 eV direct band gap at the gamma point.

Nonreciprocal directional dichroism is an unusual light-matter interaction that gives rise to diode-like behavior in low-symmetry materials. The chiral varieties are particularly scarce due to the requirements for strong spin-orbit coupling, broken time-reversal symmetry, and a chiral axis. Here we bring together magneto-optical spectroscopy and first-principles calculations to reveal highenergy, broadband nonreciprocal directional dichroism in Ni 3 TeO 6 with special focus on behavior in the metamagnetic phase above 52 T. In addition to demonstrating this effect in the magnetochiral configuration, we explore the transverse magnetochiral orientation in which applied field and light propagation are orthogonal to the chiral axis and, by so doing, uncover an additional configuration with a unique nonreciprocal response in the visible part of the spectrum. In a significant conceptual advance, we use first-principles methods to analyze how the Ni 2+ d-to-d on-site excitations develop magneto-electric character and present a microscopic model that unlocks the door to theory-driven discovery of chiral magnets with nonreciprocal properties.

Hydrogen bonding plays a foundational role in the life, earth, and chemical sciences, with its richness and strength depending on the situation. In molecular materials, these interactions determine assembly mechanisms, control superconductivity, and even permit magnetic exchange. In spite of its long-standing importance, exquisite control of hydrogen bonding in molecule-based magnets has only been realized in limited form and remains as one of the major challenges. Here, we report the discovery that pressure can tune the dimensionality of hydrogen bonding networks in CuF2(H2O)2(3-chloropyridine) to induce magnetic switching. Specifically, we reveal how the development of exchange pathways under compression combined with an enhanced ab-plane hydrogen bonding network yields a three dimensional superexchange web between copper centers that triggers a reversible magnetic crossover. Similar pressure- and strain-driven crossover mechanisms involving coordinated motion of hydrogen bond networks may play out in other quantum magnets.

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