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Zhangyu Yuan

Publications and source records attributed to Zhangyu Yuan.

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Strongly entangled Quantum Spin Rings driven by Hückel rule

Quantum spin rings represent an intriguing platform for studying unconventional magnetic order and exotic quantum phases, and they are also promising materials for emerging quantum technologies. Conventional spin systems consist of a set of weakly interacting localized spins that are well described by the Heisenberg spin models. Here, we demonstrate that strong interactions between radical centers in macrocycles of different sizes lead to fluctuations in the total number of unpaired electrons and to non-trivial antiferromagnetic order that extends beyond the Heisenberg picture. We demonstrate that the electronic structure of these spin rings is governed by the concept of 4n/4n+2 Hückel (anti)aromaticity for even-membered rings, whereas odd-membered rings possess a highly degenerate frustrated magnetic ground state. The strongly coupled spin rings are experimentally realized through the on-surface synthesis of π-magnetic carbon-based macrocycles, which consist of [2]triangulene units. The close correlation between the electronic structure and the Hückel aromaticity rule is revealed by scanning tunneling spectroscopy and multireference calculations. This work establishes a novel design principle employing the concept of Hückel aromaticity for quantum spin macrocycles.

cond-mat.mes-hall

Atomic-Scale Imaging of Fractional Spinon Quasiparticles in Open-Shell Triangulene Spin-$\frac{1}{2}$ Chains

The emergence of spinon quasiparticles, which carry spin but lack charge, is a hallmark of collective quantum phenomena in low-dimensional quantum spin systems. While the existence of spinons has been demonstrated through scattering spectroscopy in ensemble samples, real-space imaging of these quasiparticles within individual spin chains has remained elusive. In this study, we construct individual Heisenberg antiferromagnetic spin-$\frac{1}{2}$ chains using open-shell [2]triangulene molecules as building blocks. Each [2]triangulene unit, owing to its sublattice imbalance, hosts a net spin-$\frac{1}{2}$ in accordance with Lieb's theorem, and these spins are antiferromagnetically coupled within covalent chains with a coupling strength of $J = 45$ meV. Through scanning tunneling microscopy and spectroscopy, we probe the spin states, excitation gaps, and their spatial excitation weights within covalent spin chains of varying lengths with atomic precision. Our investigation reveals that the excitation gap decreases as the chain length increases, extrapolating to zero for long chains, consistent with Haldane's gapless prediction. Moreover, inelastic tunneling spectroscopy reveals an m-shaped energy dispersion characteristic of confined spinon quasiparticles in a one-dimensional quantum box. These findings establish a promising strategy for exploring the unique properties of excitation quasiparticles and their broad implications for quantum information.

cond-mat.mtrl-sci

Local Probe Structure Isomerization in a One-Dimensional Molecular Array

Synthesis of one-dimensional molecular arrays with tailored stereoisomers is challenging yet has a great potential for application in molecular opto-, electronic- and magnetic-devices, where the local array structure plays a decisive role in the functional properties. Here, we demonstrate construction and characterization of dehydroazulene isomer and diradical units in three-dimensional organometallic compounds on Ag(111) with a combination of low-temperature scanning tunneling microscopy and density functional theory calculations. Tip-induced voltage pulses firstly result in the formation of a diradical species via successive homolytic fission of two C-Br bonds in the naphthyl groups, which are subsequently transformed into chiral dehydroazulene moieties. The delicate balance of the reaction rates among the diradical and two stereoisomers, arising from an in-line configuration of tip and molecular unit, allows directional azulene-to-azulene and azulene-to-diradical local probe structural isomerization in a controlled manner. Furthermore, our theoretical calculations suggest that the diradical moiety hosts an open-shell singlet with antiferromagnetic coupling between the unpaired electrons, which can undergo an inelastic spin transition of 91 meV to the ferromagnetically coupled triplet state.

cond-mat.mtrl-sci