arXiv subjects

Baiqiang Liu

Publications and source records attributed to Baiqiang Liu.

5 recordsLinked to original sources

arXiv2026

Hydrogen s-electrons as the origin of crystal magnetism beyond spin-orbit coupling

Magnetism has long been attributed to localized d, f, and even p electrons with strong correlations, whereas s electrons exemplified by hydrogen are reactive and tend to have their spins quenched, making s-electron-derived magnetism and long-range ordered magnetic crystals seem unattainable. Here we report a low-Z ferromagnetic crystal H13@(BN)12 using first-principles calculations, where thirteen hydrogen atoms are encapsulated within a (BN)12 cage and magnetism originates from the 1s electron of the central hydrogen atom. The crystal remains stable under ambient pressure owing to chemical precompression. Notably, the central hydrogen atom retains a magnetic moment of 1 μB, with long-range magnetic order established through multicenter bonding within the H13 aggregate and the intercell B-B network, while the zero orbital angular momentum of s electrons renders spin-orbit coupling (SOC) negligible as expected. Electronic structure analyses reveal that the large cavity and central negative electrostatic potential of the (BN)12 cage localize the hydrogen 1s electron, preventing spin quenching. Interestingly, under 16 GPa compression, the system transforms into a nonmagnetic metallic state driven by delocalized electrons of the central hydrogen atom. This study opens a pathway for constructing s-electron-driven magnetic materials and lays the foundation for developing low-energy consumption magnetic devices without SOC.

cond-mat.mtrl-sci↗

arXiv2026

Hydrogen-atom roaming reactions in water clusters: Unveiling an unusual dimension of water reactivity through first-principles calculations and machine learning

Water mediates a broad range of chemical reactions, including proton transfer, bond rearrangement, and conventional radical processes, defining a continuously expanding repertoire of intrinsic reactivity. However, roaming, a fundamental reaction mechanism that a departing fragment bypasses the minimum energy path to recombine, has not been identified in water itself. Here, we report the discovery of hydrogen-atom roaming reactions in water clusters through high-precision ab initio calculations of first-principles. A neutral hydrogen atom departs as a radical, roams across the flat potential energy surface, and recombines along pathways that connect the same reactants and products as known hydrogen-bond network rearrangements. Interpretable machine learning analysis identifies the reactant dipole moment as the decisive switch governing whether roaming occurs, underpinned by exchange-repulsion and electrostatic interactions. Once roaming is initiated, polarizability and spin population determine barrier heights, while the charge distribution of the roaming hydrogen atom governs barrier widths, collectively shaped by electrostatic, orbital, and dispersion contributions. These findings establish hydrogen-atom roaming as a previously unrecognized intrinsic reaction class in water, complementing a fundamental dimension to the mechanistic picture of water reactivity.

physics.chem-ph↗

arXiv2025

Metallic solid-state hydrogen storage crystals achieved through chemical precompression under ambient conditions

Improving hydrogen storage density is essential for reducing the extreme conditions required in applications such as nuclear fusion. However, the recognition of metallic hydrogen as the "Holy Grail" of high-pressure science highlights the difficulty of high-density hydrogen aggregation. Here, we report a solid-state crystal H9@C20 formed by embedding hydrogen atoms into C20 fullerene cages and utilizing chemical precompression, which remains stable under ambient pressure and temperature conditions and exhibits metallic properties. This precompression effect is reflected in the formation of C-H bonds within the cage and C-C bonds between cages, resulting in the transformation of all C atoms from sp2 to sp3 hybridization with inward and outward distortions, while promoting delocalized multicenter bonding within the H9 aggregate. In particular, the hydrogen density inside the C20 cage exceeds that of solid hydrogen, achieving a uniform discrete distribution with H9 as monomers. Further study reveals that filling hydrogen molecules into voids between H9@C20 primitive cells can increase hydrogen content while maintaining structural stability, forming a solid-gas mixed hydrogen storage crystal. Our findings provide a basis for developing high-density hydrogen storage materials under ambient conditions.

cond-mat.mtrl-sci↗

arXiv2025

Superatomic hydrogen: achieving effective aggregation of hydrogen atoms at pressures lower than that of metallic hydrogen

Metal hydrogen exhibiting electron delocalization properties has been recognized as an important prospect for achieving controlled nuclear fusion, but the extreme pressure conditions required exceeding hundreds of GPa remain a daunting challenge. Here, we propose a model of superatomic hydrogen, aiming to reduce the pressure conditions required for the effective aggregation of elemental hydrogen atoms. High-precision ab initio calculations indicate that the pressure required to compress the H13 system with one central atom and 12 surrounding atoms into a superatomic state is approximately two orders of magnitude lower than that of metallic hydrogen. Atomic-level analyses reveal that in the superatomic state of compressed H13, the central H atom donates its electron, and all electrons are delocalized on the superatomic molecular orbitals, which conforms to properties of metallic hydrogen. Our discovery in principle opens up the prospect of superatomic hydrogen in areas such as nuclear fusion.

physics.comp-ph↗

arXiv2024

Double Layer-Interlocked Crystals of Nitrogen-Rich Compounds under Zero-Pressure Conditions

Stabilizing nitrogen-rich compound crystals under conventional conditions is a key issue in the development and application of high-energy density materials (HEDMs). Herein, a two-dimensional double-layer interlocked Li4(N5)2 nitrogen-rich compound crystals, in which the two N5 rings are locked to by sharing four Li atoms, was found to maintain structural stability at zero pressure conditions. Dynamics studies reliably confirm crystal stability below 250 K. Furthermore, the stability of Li4(N5)2 crystal mainly arises from the ionic interaction between Li atoms and N5 rings, formed by the charge transfer from Li atoms to N5 rings. This study highlights the feasibility of stabilizing nitrogen-rich compound crystals under conventional conditions, paving the way for atomic level advancements in HEDMs.

cond-mat.mtrl-sci↗