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1. The in-plane structure domain size of nm-thick MoSe 2 uncovered by low-momentum phonon scattering

   https://doi.org/10.1039/d0nr09099a  

   Lin, Huan ; Wang, Ridong ; Zobeiri, Hamidreza ; Wang, Tianyu ; Xu, Shen ; Wang, Xinwei ( April 2021 , Nanoscale)

   null (Ed.)

   Although 2D materials have been widely studied for more than a decade, very few studies have been reported on the in-plane structure domain (STD) size even though such a physical property is critical in determining the charge carrier and energy carrier transport. Grazing incidence X-ray diffraction (XRD) can be used for studying the in-plane structure of very thin samples, but it becomes more challenging to study few-layer 2D materials. In this work the nanosecond energy transport state-resolved Raman (nET-Raman) technique is applied to resolve this key problem by directly measuring the thermal reffusivity of 2D materials and determining the residual value at the 0 K-limit. Such a residual value is determined by low-momentum phonon scattering and can be directly used to characterize the in-plane STD size of 2D materials. Three suspended MoSe 2 (15, 50 and 62 nm thick) samples are measured using nET-Raman from room temperature down to 77 K. Based on low-momentum phonon scattering, the STD size is determined to be 58.7 nm and 84.5 nm for 50 nm and 62 nm thick samples, respectively. For comparison, the in-plane structure of bulk MoSe 2 that is used to prepare the measured nm-thick samples is characterized using XRD. It uncovers crystallite sizes of 64.8 nm in the (100) direction and 121 nm in the (010) direction. The STD size determined by our low momentum phonon scattering is close to the crystallite size determined by XRD, but still shows differences. The STD size by low-momentum phonon scattering is more affected by the crystallite sizes in all in-plane directions rather than that by XRD that is for a specific crystallographic orientation. Their close values demonstrate that during nanosheet preparation (peeling and transfer), the in-plane structure experiences very little damage. 

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2. High-harmonic generation in spin and charge current pumping at ferromagnetic or antiferromagnetic resonance in the presence of spin–orbit coupling

   https://doi.org/10.1088/2515-7639/aceaad  

   Varela-Manjarres, Jalil ; Nikolić, Branislav K. ( August 2023 , Journal of Physics: Materials)

   One of the cornerstone effects in spintronics is spin pumping by dynamical magnetization that is steadily precessing (around, for example, thez-axis) with frequencyω₀due to absorption of low-power microwaves of frequencyω₀under the resonance conditions and in the absence of any applied bias voltage. The two-decades-old ‘standard model’ of this effect, based on the scattering theory of adiabatic quantum pumping, predicts that component$I^{S_z}$of spin current vector$(I^{S_x}(t),I^{S_y}(t),I^{S_z})\propto {\omega }_0$is time-independent while$I^{S_x}(t)$and$I^{S_y}(t)$oscillate harmonically in time with a single frequencyω₀whereas pumped charge current is zero$I\equiv 0$in the same adiabatic$\propto {\omega }_0$limit. Here we employ more general approaches than the ‘standard model’, namely the time-dependent nonequilibrium Green’s function (NEGF) and the Floquet NEGF, to predict unforeseen features of spin pumping: namely precessing localized magnetic moments within a ferromagnetic metal (FM) or antiferromagnetic metal (AFM), whose conduction electrons are exposed to spin–orbit coupling (SOC) of either intrinsic or proximity origin, will pump both spin$I^{S_{\alpha }}(t)$and chargeI(t) currents. All four of these functions harmonically oscillate in time at both even and odd integer multiples$N{\omega }_0$of the driving frequencyω₀. The cutoff order of such high harmonics increases with SOC strength, reaching$N_{\mathrm{m}\mathrm{a}\mathrm{x}}\simeq 11$in the one-dimensional FM or AFM models chosen for demonstration. A higher cutoff$N_{\mathrm{m}\mathrm{a}\mathrm{x}}\simeq 25$can be achieved in realistic two-dimensional (2D) FM models defined on a honeycomb lattice, and we provide a prescription of how to realize them using 2D magnets and their heterostructures.

    

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3. Crossover of high-energy spin fluctuations from collective triplons to localized magnetic excitations in Sr14−xCaxCu24O41 ladders

   https://doi.org/10.1038/s41535-022-00502-1  

   Tseng, Y. ; Thomas, J. ; Zhang, W. ; Paris, E. ; Puphal, P. ; Bag, R. ; Deng, G. ; Asmara, T. C. ; Strocov, V. N. ; Singh, S. ; et al ( December 2022 , npj Quantum Materials)

   Abstract We studied the magnetic excitations in the quasi-one-dimensional (q-1D) ladder subsystem of Sr 14−x Ca x Cu 24 O 41 (SCCO) using Cu L 3 -edge resonant inelastic X-ray scattering (RIXS). By comparing momentum-resolved RIXS spectra with high ( x  = 12.2) and without ( x  = 0) Ca content, we track the evolution of the magnetic excitations from collective two-triplon (2 T) excitations ( x  = 0) to weakly-dispersive gapped modes at an energy of 280 meV ( x  = 12.2). Density matrix renormalization group (DMRG) calculations of the RIXS response in the doped ladders suggest that the flat magnetic dispersion and damped excitation profile observed at x  = 12.2 originates from enhanced hole localization. This interpretation is supported by polarization-dependent RIXS measurements, where we disentangle the spin-conserving Δ S  = 0 scattering from the predominant Δ S  = 1 spin-flip signal in the RIXS spectra. The results show that the low-energy weight in the Δ S  = 0 channel is depleted when Sr is replaced by Ca, consistent with a reduced carrier mobility. Our results demonstrate that off-ladder impurities can affect both the low-energy magnetic excitations and superconducting correlations in the CuO 4 plaquettes. Finally, our study characterizes the magnetic and charge fluctuations in the phase from which superconductivity emerges in SCCO at elevated pressures. 

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4. Applying Unconventional Spectroscopies to the Single‐Molecule Magnets, Co(PPh 3 ) 2 X 2 (X=Cl, Br, I): Unveiling Magnetic Transitions and Spin‐Phonon Coupling

   https://doi.org/10.1002/chem.202100705  

   Bone, Alexandria N. ; Widener, Chelsea N. ; Moseley, Duncan H. ; Liu, Zhiming ; Lu, Zhengguang ; Cheng, Yongqiang ; Daemen, Luke L. ; Ozerov, Mykhaylo ; Telser, Joshua ; Thirunavukkuarasu, Komalavalli ; et al ( August 2021 , Chemistry – A European Journal)

   Large separation of magnetic levels and slow relaxation in metal complexes are desirable properties of single‐molecule magnets (SMMs). Spin‐phonon coupling (interactions of magnetic levels with phonons) is ubiquitous, leading to magnetic relaxation and loss of memory in SMMs and quantum coherence in qubits. Direct observation of magnetic transitions and spin‐phonon coupling in molecules is challenging. We have found that far‐IR magnetic spectra (FIRMS) of Co(PPh₃)₂X₂(Co‐X; X=Cl, Br, I) reveal rarely observed spin‐phonon coupling as avoided crossings between magnetic andu‐symmetry phonon transitions. Inelastic neutron scattering (INS) gives phonon spectra. Calculations using VASP and phonopy programs gave phonon symmetries and movies. Magnetic transitions among zero‐field split (ZFS) levels of theS=3/2 electronic ground state were probed by INS, high‐frequency and ‐field EPR (HFEPR), FIRMS, and frequency‐domain FT terahertz EPR (FD‐FT THz‐EPR), giving magnetic excitation spectra and determining ZFS parameters (D, E) andgvalues. Ligand‐field theory (LFT) was used to analyze earlier electronic absorption spectra and give calculated ZFS parameters matching those from the experiments. DFT calculations also gave spin densities inCo‐X, showing that the larger Co(II) spin density in a molecule, the larger its ZFS magnitude. The current work reveals dynamics of magnetic and phonon excitations in SMMs. Studies of such couplings in the future would help to understand how spin‐phonon coupling may lead to magnetic relaxation and develop guidance to control such coupling.

    

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5. Fingerprints of an orbital-selective Mott phase in the block magnetic state of BaFe2Se3 ladders

   https://doi.org/10.1038/s42005-019-0155-3  

   Patel, N. D. ; Nocera, A. ; Alvarez, G. ; Moreo, A. ; Johnston, S. ; Dagotto, E. ( June 2019 , Communications Physics)

   Resonant Inelastic X-Ray Scattering (RIXS) experiments on the iron-based ladder BaFe₂Se₃unveiled an unexpected two-peak structure associated with local orbital (dd) excitations in a block-type antiferromagnetic phase. A mixed character between correlated band-like and localized excitations was also reported. Here, we use the density matrix renormalization group method to calculate the momentum-resolved charge- and orbital-dynamical response functions of a multi-orbital Hubbard chain. Remarkably, our results qualitatively resemble the BaFe₂Se₃RIXS data, while also capturing the presence of long-range magnetic order as found in neutron scattering, only when the model is in an exotic orbital-selective Mott phase (OSMP). In the calculations, the experimentally observed zero-momentum transfer RIXS peaks correspond to excitations between itinerant and Mott insulating orbitals. We provide experimentally testable predictions for the momentum-resolved charge and orbital dynamical structures, which can provide further insight into the OSMP regime of BaFe₂Se₃.

    

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