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1. Quantum electronic control on chemical activation of methane by collision with spin–orbit state selected vanadium cation

   https://doi.org/10.1039/D0CP04333H  

   Ng, Cheuk-Yiu; Xu, Yuntao; Chang, Yih-Chung; Wannenmacher, Anna; Parziale, Matthew; Armentrout, P. B. (January 2021, Physical Chemistry Chemical Physics)

   null (Ed.)

   By coupling a newly developed quantum-electronic-state-selected supersonically cooled vanadium cation (V + ) beam source with a double quadrupole-double octopole (DQDO) ion–molecule reaction apparatus, we have investigated detailed absolute integral cross sections ( σ 's) for the reactions, V + [a 5 D J ( J = 0, 2), a 5 F J ( J = 1, 2), and a 3 F J ( J = 2, 3)] + CH 4 , covering the center-of-mass collision energy range of E cm = 0.1–10.0 eV. Three product channels, VH + + CH 3 , VCH 2 + + H 2 , and VCH 3 + + H, are unambiguously identified based on E cm -threshold measurements. No J -dependences for the σ curves ( σ versus E cm plots) of individual electronic states are discernible, which may indicate that the spin–orbit coupling is weak and has little effect on chemical reactivity. For all three product channels, the maximum σ values for the triplet a 3 F J state [ σ (a 3 F J )] are found to be more than ten times larger than those for the quintet σ (a 5 D J ) and σ (a 5 F J ) states, showing that a reaction mechanism favoring the conservation of total electron spin. Without performing a detailed theoretical study, we have tentatively interpreted that a weak quintet-to-triplet spin crossing is operative for the activation reaction. The σ (a 5 D 0 , a 5 F 1 , and a 3 F 2) measurements for the VH + , VCH 2 + , and VCH 3 + product ion channels along with accounting of the kinetic energy distribution due to the thermal broadening effect for CH 4 have allowed the determination of the 0 K bond dissociation energies: D 0 (V + –H) = 2.02 (0.05) eV, D 0 (V + –CH 2 ) = 3.40 (0.07) eV, and D 0 (V + –CH 3 ) = 2.07 (0.09) eV. Detailed branching ratios of product ion channels for the titled reaction have also been reported. Excellent simulations of the σ curves obtained previously for V + generated by surface ionization at 1800–2200 K can be achieved by the linear combination of the σ (a 5 D J , a 5 F J , and a 3 F J ) curves weighted by the corresponding Boltzmann populations of the electronic states. In addition to serving as a strong validation of the thermal equilibrium assumption for the populations of the V + electronic states in the hot filament ionization source, the agreement between these results also confirmed that the V + (a 5 D J , a 5 F J , and a 3 F J ) states prepared in this experiment are in single spin–orbit states with 100% purity. 

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2. Motion of a spinning particle under the conservative piece of the self-force is Hamiltonian to first order in mass and spin

   https://doi.org/10.1103/PhysRevD.107.124017  

   Blanco, Francisco M; Flanagan, Éanna É (June 2023, Physical Review D)

   We consider the motion of a point particle with spin in a stationary spacetime. We define, following Witzany et al. [Classical Quantum Gravity 36, 075003 (2019)] and later Ramond [arXiv:2210.03866], a 12-dimensional Hamiltonian dynamical system whose orbits coincide with the solutions of the Mathisson- Papapetrou-Dixon equations of motion with the Tulczyjew-Dixon spin supplementary condition, to linear order in spin. We then perturb this system by adding the conservative pieces of the leading order gravitational self-force and self-torque sourced by the particle’s mass and spin. We show that this perturbed system is Hamiltonian and derive expressions for the Hamiltonian function and symplectic form. This result extends a previous result for spinless point particles [F. M. Blanco and E. E. Flanagan, Phys. Rev. Lett. 130, 051201 (2023)]. 

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3. Quantum state control on the chemical reactivity of a transition metal vanadium cation in carbon dioxide activation

   https://doi.org/10.1039/C9CP00575G  

   Chang, Yih Chung; Xu, Yuntao; Ng, Cheuk-Yiu (March 2019, Physical Chemistry Chemical Physics)

   By combining a newly developed two-color laser pulsed field ionization-photoion (PFI-PI) source and a double-quadrupole–double-octopole (DQDO) mass spectrometer, we investigated the integral cross sections ( σ s) of the vanadium cation (V + ) toward the activation of CO 2 in the center-of-mass kinetic energy ( E cm ) range from 0.1 to 10.0 eV. Here, V + was prepared in single spin–orbit levels of its lowest electronic states, a 5 D J ( J = 0–4), a 5 F J ( J = 1–5), and a 3 F J ( J = 2–4), with well-defined kinetic energies. For both product channels VO + + CO and VCO + + O identified, V + (a 3 F 2,3 ) is found to be greatly more reactive than V + (a 5 D 0,2 ) and V + (a 5 F 1,2 ), suggesting that the V + + CO 2 reaction system mainly proceeds via a “weak quintet-to-triplet spin-crossing” mechanism favoring the conservation of total electron spins. In addition, no J -state dependence was observed. The distinctive structures of the quantum electronic state selected integral cross sections observed as a function of E cm and the electronic state of the V + ion indicate that the difference in the chemical reactivity of the title reaction originated from the quantum-state instead of energy effects. Furthermore, this work suggests that the selection of the quantum electronic states a 3 F J ( J = 2–4) of the transition metal V + ion can greatly enhance the efficiency of CO 2 activation. 

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4. Impact of strain on the SOT-driven dynamics of thin film Mn3Sn

   https://doi.org/10.1063/5.0179669  

   Shukla, Ankit; Qian, Siyuan; Rakheja, Shaloo (March 2024, Journal of Applied Physics)

   Mn 3 Sn, a metallic antiferromagnet with an anti-chiral 120° spin structure, generates intriguing magneto-transport signatures such as a large anomalous Hall effect, spin-polarized current with novel symmetries, anomalous Nernst effect, and magneto-optic Kerr effect. When grown epitaxially as MgO(110)[001]∥Mn3Sn(01¯1¯0)[0001], Mn3Sn experiences a uniaxial tensile strain, which changes the bulk sixfold anisotropy to a twofold perpendicular magnetic anisotropy (PMA). Here, we investigate the field-assisted spin–orbit-torque (SOT)-driven dynamics in single-domain Mn3Sn with PMA. We find that for non-zero external magnetic fields, the magnetic octupole moment of Mn3Sn can be switched between the two stable states if the input current is between two field-dependent critical currents. Below the lower critical current, the magnetic octupole moment exhibits a stationary state in the vicinity of the initial stable state. On the other hand, above the higher critical current, the magnetic octupole moment shows oscillatory dynamics which could, in principle, be tuned from the 100s of megahertz to the terahertz range. We obtain approximate analytic expressions of the two critical currents that agree very well with the numerical simulations for experimentally relevant magnetic fields. We also obtain a unified functional form of the switching time vs the input current for different magnetic fields. Finally, we show that for lower values of Gilbert damping (α≲2×10−3), the critical currents and the final steady states depend significantly on α. The numerical and analytic results presented in our work can be used by both theorists and experimentalists to understand the SOT-driven order dynamics in PMA Mn3Sn and design future experiments and devices. 

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5. Mapping of Spin‐Wave Transport in Thulium Iron Garnet Thin Films Using Diamond Quantum Microscopy

   https://doi.org/10.1002/aelm.202300648  

   Timalsina, Rupak; Wang, Haohan; Giri, Bharat; Erickson, Adam; Xu, Xiaoshan; Laraoui, Abdelghani (March 2024, Advanced Electronic Materials)

   Abstract Spin waves, collective dynamic magnetic excitations, offer crucial insights into magnetic material properties. Rare‐earth iron garnets offer an ideal spin‐wave (SW) platform with long propagation length, short wavelength, gigahertz frequency, and applicability to magnon spintronic platforms. Of particular interest, thulium iron garnet (TmIG) has attracted huge interest recently due to its successful growth down to a few nanometers, observed topological Hall effect, and spin‐orbit torque‐induced switching effects. However, there is no direct spatial measurement of its SW properties. This work uses diamond nitrogen‐vacancy (NV) magnetometry in combination with SW electrical transmission spectroscopy to study SW transport properties in TmIG thin films. NV magnetometry allows probing spin waves at the sub‐micrometer scale, seen by the amplification of the local microwave magnetic field due to the coupling of NV spin qubits with the stray magnetic field produced by the microwave‐excited spin waves. By monitoring the NV spin resonances, the SW properties in TmIG thin films are measured as a function of the applied magnetic field, including their amplitude, decay length (≈50 µm), and wavelength (0.8–2 µm). These results pave the way for studying spin qubit‐magnon interactions in rare‐earth magnetic insulators, relevant to quantum magnonics applications. 

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