Article
Multidisciplinary Sciences
Yuki Hibino, Tomohiro Taniguchi, Kay Yakushiji, Akio Fukushima, Hitoshi Kubota, Shinji Yuasa
Summary: The study elucidates a mechanism behind the enhancement of magnetic-dependent charge-to-spin conversion in ferromagnetic materials, highlighting the dominant role of interfacial contribution and the potential for control via interfacial band engineering. It shows that the efficiency of charge-to-spin conversion in ferromagnets surpasses other materials with reduced symmetry.
NATURE COMMUNICATIONS
(2021)
Article
Physics, Applied
Jinu Kurian, Aleena Joseph, Salia Cherifi-Hertel, Ciaran Fowley, Gregor Hlawacek, Peter Dunne, Michelangelo Romeo, Gwenael Atcheson, J. M. D. Coey, Bernard Doudin
Summary: He+ ion irradiation is used to pattern multiple areas of Pt/Co/W films with different irradiation doses in Hall bars, resulting in a landscape of perpendicular magnetic anisotropy. This enables selective multilevel current-induced switching, with full control of the position and order of the individual switching elements. Key pattern design parameters are specified, offering a scalable approach for multilevel switching devices.
APPLIED PHYSICS LETTERS
(2023)
Article
Materials Science, Multidisciplinary
L. L. Tao, Qin Zhang, Huinan Li, Xianjie Wang, Yi Wang, Yu Sui, Bo Song, M. Ye. Zhuravlev
Summary: Quasisymmetry is an approximate symmetry that emerges in low-energy effective theory and commutes with the Hamiltonian at a lower order. It adds desirable properties to the system, such as large Berry curvatures due to small band gaps, which are robust against perturbations.
Article
Optics
Peng Shi, Luping Du, Mingjie Li, Xiaocong Yuan
Summary: This research proposes a theoretical framework to show that photonic chiral spin textures in optical interfaces originate from the system's symmetry and relativity. The analysis of rotational symmetry in optical systems reveals the crucial role of the local spin momentum distribution in the chiral twisting of local spin vectors.
LASER & PHOTONICS REVIEWS
(2021)
Article
Materials Science, Multidisciplinary
Y. Chargui, A. Dhahbi, M. A. J. Ali
Summary: This paper considers a generalized version of the Duffin-Kemmer-Petiau oscillator (DKPO) model for spin-1 bosons by introducing an additional spin-orbit coupling (SOC). The model satisfies the requirements of Lorentz covariance and a conserved four-current, and provides exact solutions for both natural and unnatural parity states and any total angular momentum number. The obtained energy eigenvalues demonstrate that the additional SOC brings radical modifications to the spectroscopy of the DKPO, particularly making the spin-orbit splitting of energy levels independent from oscillator shells. Furthermore, interesting special cases of the model and its non-relativistic limit are discussed.
RESULTS IN PHYSICS
(2023)
Article
Physics, Multidisciplinary
Kun Jiang
Summary: The interplay between spin-orbit coupling (SOC) and electron correlation leads to the emergence of various quantum phases and transitions, particularly topological insulators and topological transitions. In multi-orbital systems under atomic SOC, electron correlation induces an extra large SOC and alters the topological properties of the ground state. The phase diagrams of the p(x)/p(y) orbital ionic Hubbard model on a honeycomb lattice are well studied using the Hartree-Fock mean field theory. Generally, the strength correction of SOC, Δλ, is proportional to (UMODIFIER LETTER PRIME-J). The form of SOC on multi-orbital materials is also affected by the breakdown of rotation symmetry under correlation. In addition, spontaneous generalized SOC can be found in a non-interacting system that is close to fermionic instability. Using renormalization group, SOC is found to lead to instability near the quadratic band-crossing point, and mean fields at this point are also studied.
CHINESE PHYSICS LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Xiaoming Zhang, Jiale Liu, Feng Liu
Summary: This study generalizes the effective p-wave theory to antisymmetric SOC (ASOC) and demonstrates that various 2D crystals can facilitate the desired ASOC. 314 TSC candidate materials are discovered by screening 2D material databases.
Article
Chemistry, Physical
Konstantin Komarov, Woojin Park, Seunghoon Lee, Tao Zeng, Cheol Ho Choi
Summary: Relativistic mixed-reference spin-flip (MRSF)-TDDFT is developed to consider spin-orbit coupling (SOC) within the mean-field approximation. It accurately reproduces experimental results and is consistent with four-component (4c) relativistic CASSCF and 4c-CASPT2 calculations for the C, Si, and Ge atoms. Even for Sn, it yields accurate splittings with a small error of about 3%. In the calculations for the molecular 4-thiothymine, SOC-MRSF values are in excellent agreement with SO-GMC-QDPT2 values regardless of geometries and exchange correlation functionals. SOC-MRSF also predicts the possible intersystem crossing of S1 (n7r*) -> T1 (7r7r*) even in thymine with only second-row elements. Therefore, SOC-MRSF is a promising electronic structure protocol for nonadiabatic molecular dynamics (NAMD) in large systems.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Multidisciplinary
Karolina Gornicka, Xin Gui, Bartlomiej Wiendlocha, Loi T. Nguyen, Weiwei Xie, Robert J. Cava, Tomasz Klimczuk
Summary: The search for new superconducting materials remains a challenge, even though superconductivity was first observed over a century ago. The newly reported materials, NbIr(2)B(2) and TaIr2B2, display unique noncentrosymmetric crystal structures and unconventional superconductivity, as indicated by experimental and theoretical evidence. These materials may serve as an excellent platform for studying unconventional superconductivity in intermetallic compounds.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Materials Science, Multidisciplinary
D. C. Cavanagh, Daniel F. Agterberg, P. M. R. Brydon
Summary: We investigate the effect of symmetry-breaking perturbations on superconductivity in multiorbital materials, focusing on the influence of an external magnetic field. We introduce the field-fitness function to characterize the disruption of pair formation due to the perturbation. In even-parity superconductors, the field-fitness function for an external magnetic field is unity, indicating that the paramagnetic response is determined solely by a generalized effective g-factor. For odd-parity superconductors, the interplay between the effective g-factor and the field-fitness function can result in counterintuitive outcomes. We demonstrate this phenomenon in the p-wave pairing of the effective j=32 electronic states in the Luttinger-Kohn model.
Article
Nanoscience & Nanotechnology
Satam Alotibi, Bryan J. Hickey, Gilberto Teobaldi, Mannan Ali, Joseph Barker, Emiliano Poli, David D. O'Regan, Quentin Ramasse, Gavin Burnell, James Patchett, Chiara Ciccarelli, Mohammed Alyami, Timothy Moorsom, Oscar Cespedes
Summary: The study found that the spin Hall magnetoresistance for Pt/C-60 and Ta/C-60 is up to a factor of 6 higher than those for pristine metals, indicating a 20-60% increase in the spin Hall angle. Additionally, the presence of C-60 increased the anisotropic magnetoresistance by up to 700% at low fields.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Optics
Lifu Zhang, Jie Jiang, Christian Multunas, Chen Ming, Zhizhong Chen, Yang Hu, Zonghuan Lu, Saloni Pendse, Ru Jia, Mani Chandra, Yi-Yang Sun, Toh-Ming Lu, Yuan Ping, Ravishankar Sundararaman, Jian Shi
Summary: Researchers demonstrate a persistent spin helix in an organic-inorganic hybrid ferroelectric halide perovskite. They show that the spin-polarized band structure can be switched via an intrinsic ferroelectric field. This discovery has the potential to resolve the control-relaxation dilemma in spintronic devices.
Article
Optics
Liang-Liang Wang, Wenjun Shao, Qing Sun, Jian Li
Summary: We investigate a fermionic superfluid with Raman-induced spin-orbit coupling immersed in a Bose-Einstein condensate. By minimizing the total free energy, we find that, with moderate repulsive interspecies interaction, a phase separation occurs where the otherwise nontopological uniform phase is divided into two parts: a purely fermionic one and a Bose-Fermi mix characterized by nontrivial topology with the winding number W = 1. We verify that Majorana zero modes emerge at the phase interfaces by numerical simulations of the coupled Bogoliubov-de Gennes and Gross-Pitaevskii equations in real space. The tunability of the phase interfaces enables a direct manipulation of the predicted Majorana zero modes.
Article
Astronomy & Astrophysics
Hsiao-Yi Chen, Andrea Mitridate, Tanner Trickle, Zhengkang Zhang, Marco Bernardi, Kathryn M. Zurek
Summary: This paper focuses on a class of materials in which narrow band gaps naturally arise as a consequence of spin-orbit coupling. The scattering and absorption rates of dark matter-electron in these materials are computed using state-of-the-art density functional theory techniques. The inclusion of spin-orbit coupling effects can substantially alter the projected constraints for dark matter.
Article
Physics, Applied
Long Liu, Xiaotian Zhao, Wei Liu, Yuhang Song, Xinguo Zhao, Zhidong Zhang
Summary: The study reveals that antiferromagnetic IEC between two GdCo layers through Ru can significantly enhance the SOT effect, leading to magnetization switching between parallel or antiparallel states. Current-induced multi-state switching processes, including four-steps-four-states and six-steps-four-states, are observed for samples with weakened IEC when t (Ru) is thicker than 0.57 nm.
JOURNAL OF PHYSICS D-APPLIED PHYSICS
(2021)
Article
Chemistry, Physical
Rene F. K. Spada, Mauricio P. Franco, Reed Nieman, Adelia J. A. Aquino, Ron Shepard, Felix Plasser, Hans Lischka
Summary: This work discusses the calculation of the spin-density matrix using the graphical unitary group approach. A general equation for the spin-density matrix is derived and the evaluation of this equation using Shavitt loop values is discussed. The spin-density matrix is then calculated for different structures and the physical meaning of spin-density is explained along with the quantification of negative contributions.
Article
Chemistry, Multidisciplinary
J. Patrick Zobel, Ayla Kruse, Omar Baig, Stefan Lochbrunner, Sergey I. I. Bokarev, Oliver Kuehn, Leticia Gonzalez, Olga S. S. Bokareva
Summary: This paper investigates the influence of optimally tuned parameters on the excited state dynamics, using the example of the iron complex [Fe(cpmp)(2)](2+) with push-pull ligands. The study finds that different sets of optimal parameters lead to different relaxation pathways and timescales. The set in better agreement with CASPT2 calculations predicts deactivation in the manifold of metal-centered states, in better agreement with the experimental reference data.
Article
Chemistry, Multidisciplinary
J. Patrick Zobel, Anna M. Wernbacher, Leticia Gonzalez
Summary: The mechanism of reverse intersystem crossing (rISC) in metal-based TADF emitters is still not clear, as the small singlet/triplet energy gaps necessary for thermal rISC in donor-acceptor systems with charge-transfer excited states have spin-orbit couplings that are too small for effective rISC. In this study, the first nonadiabatic dynamics simulation of rISC process in a carbene-copper(I)-carbazolyl TADF emitter is reported. Efficient rISC on a picosecond time scale is demonstrated, involving an intermediate higher-lying triplet state of metal-to-ligand charge transfer character ((MLCT)-M-3) that enables large spin-orbit couplings with the lowest singlet charge transfer state. The mechanism is completed in the S-1 state where the complex can return to a co-planar coordination geometry with high fluorescence efficiency.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Madlen Maria Reiner, Brigitta Bachmair, Maximilian Xaver Tiefenbacher, Sebastian Mai, Leticia Gonzalez, Philipp Marquetand, Christoph Dellago
Summary: We propose a rare event sampling scheme, the Nonadiabatic Forward Flux Sampling (NAFFS), which combines the trajectory surface hopping (TSH) method with the forward flux sampling (FFS) method. NAFFS is applied to two relevant excited-state models and provides insights into transition rate constants in regimes that cannot be explored through traditional TSH simulations. The comparison with brute-force TSH simulations shows that NAFFS is significantly more efficient, making it a valuable tool for studying rare nonadiabatic events in excited-state dynamics.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Biochemistry & Molecular Biology
J. Patrick Zobel, Hanna Radatz, Leticia Gonzalez
Summary: The introduction of strong-field ligands can promote luminescence in first-row transition-metal complexes. By using early 3d metals, earth-abundant near-infrared emitters can be obtained. The molecular ruby [Cr(ddpd)(2)](3+) is a prime example, achieving high phosphorescence quantum yields in aqueous solution at room temperature. Simulation of its photodynamics in water reveals a relaxation cascade through metal-centered states after excitation, leading to the experimentally observed emission. These processes are driven by bond elongation and twisting motion of the ligands.
Article
Chemistry, Physical
Ludwig Schwiedrzik, Tina Rajkovic, Leticia Gonzalez
Summary: In this study, the regeneration and degradation pathways of a highly active biomimetic water oxidation catalyst were investigated, completing its catalytic cycle. Mechanistic insights gained from this study are expected to advance the design of more efficient and stable Mn cubane water oxidation catalysts.
Article
Chemistry, Multidisciplinary
David Hernandez-Castillo, Roland E. P. Nau, Marie-Ann Schmid, Stefanie Tschierlei, Sven Rau, Leticia Gonzalez
Summary: Understanding the factors that determine the luminescence lifetime of transition metal compounds is crucial for applications in photocatalysis and photodynamic therapy. This study challenges the commonly accepted idea that emission lifetimes can be controlled by optimizing the energy barrier or gap between different excited states. Instead, an extended kinetic model that considers all the pathways related to multiple isomers is found to accurately predict temperature-dependent emission lifetimes.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Jin Wen, Sebastian Mai, Leticia Gonzalez
Summary: In this study, the excited-state dynamics of an overcrowded alkene in solution were investigated using a QM/MM approach. The results from spectroscopy and radial distribution function analysis revealed similar solvent orientation with the molecular motor between the electronic excited state and the ground state.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Physical
Nadja K. Singer, Katharina Schloegl, J. Patrick Zobel, Marko D. Mihovilovic, Leticia Gonzalez
Summary: Understanding the thermal isomerization mechanism of azobenzene derivatives is crucial for designing photoswitches with adjustable half-lives. Through quantum chemical calculations, nonadiabatic transition state theory, and photosensitized experiments, we unravel the thermal Z/E isomerization of a heteroaromatic azoswitch, phenylazo-1,3,5-trimethylpyrazole, and predict two pathways at room temperature, involving different reaction mechanisms and spin-orbit couplings.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Mark Stitch, Davide Avagliano, Daniel Graczyk, Ian P. Clark, Leticia Gonzalez, Michael Towrie, Susan J. Quinn
Summary: This study explores the sensitivity of an infrared probe to G-quadruplex structures and demonstrates its potential as a sensitive reporter of biological environments.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Troy L. R. Bennett, Adam V. Marsh, James M. Turner, Felix Plasser, Martin Heeney, Florian Gloecklhofer
Summary: Conjugated macrocycles can exhibit concealed antiaromaticity, displaying properties observed in antiaromatic molecules due to their formal macrocyclic 4n pi-electron system. Paracyclophanetetraene (PCT) and its derivatives are prime examples, showing potential applications in battery electrode materials and electronic applications. Two dibrominated PCTs were synthesized and functionalized via Suzuki cross-coupling reactions, with optical, electrochemical, and theoretical studies revealing the tunability of PCT properties by aryl substituents.
MOLECULAR SYSTEMS DESIGN & ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Megan L. Shipton, Fathima A. Jamion, Simon Wheeler, Andrew M. Riley, Felix Plasser, Barry V. L. Potter, Stephen J. Butler
Summary: We report the first molecular probe for the selective and sensitive detection of the most abundant cellular inositol pyrophosphate 5-PP-InsP(5), as well as an efficient new synthesis. Our probe offers a potential screening methodology to identify drug-like compounds that modulate the activity of enzymes of inositol pyrophosphate metabolism.
Article
Chemistry, Multidisciplinary
Mariana T. T. do Casal, Josene M. M. Toldo, Mario Barbatti, Felix Plasser
Summary: Electronic states with partial or complete doubly excited character are important in various areas, but the classification of these states has been controversial. In this study, a physically motivated definition of doubly excited character is proposed, which is based on operator expectation values and density matrices. A classification scheme is also developed to differentiate between three cases. The differences in energy terms and practical computations are discussed, and these three cases are illustrated using different computational methods. The study provides a deeper understanding of doubly excited states and can guide improvements in their computational description.
Article
Chemistry, Physical
Novitasari Sinambela, Richard Jacobi, David Hernandez-Castillo, Elisabeth Hofmeister, Nina Hagmeyer, Benjamin Dietzek-Ivansic, Leticia Gonzalez, Andrea Pannwitz
Summary: We have developed a method for enabling photochemical reactions in water using biomimetic, water-soluble liposomes and a specially functionalized perylene diimide chromophore. Our findings provide design principles for the functionalization of lipid bilayer membranes, which will be important for the molecular engineering of artificial cellular organelles and nano-reactors based on biomimetic vesicles and membranes. The results show that the reaction rate in the DOPG-membrane is slower compared to the acetonitrile-water reaction conditions.
MOLECULAR SYSTEMS DESIGN & ENGINEERING
(2023)
Article
Chemistry, Physical
Bowen Ding, Manik Bhosale, Troy L. R. Bennett, Martin Heeney, Felix Plasser, Birgit Esser, Florian Gloecklhofer
Summary: This study reports the development of an unsubstituted derivative, SqTI-H, of locally aromatic alkyl-N-substituted squarephaneic tetraimide (SqTI) conjugated macrocycles. By removing sidechains, the solubility of SqTI-H is reduced, resulting in improved thermal stability and low solubility. The unsubstituted SqTI-H also exhibits reversible solid state electrochemical reduction to a globally aromatic dianion state. However, further optimization of electrode fabrication procedures is needed to overcome the solubility issues and improve the cycling performance.
FARADAY DISCUSSIONS
(2023)
