arXiv subjects

Caiyun Chen

Publications and source records attributed to Caiyun Chen.

10 recordsLinked to original sources

arXiv2026

Directionally Locked Heteroepitaxy with a Structurally Modulated van der Waals Material

Precise orientation of symmetry-mismatched epilayers on van der Waals (vdW) substrates via heteroepitaxy has commonly been achieved through surface treatment processes to accommodate weak interlayer registry and bonding strength, thereby limiting the range of material combinations for heterostructure design. In this study, we investigate the influence of lattice instabilities in a structurally modulated vdW TaCo2Te2 substrate on the growth and alignment of a symmetry-mismatched bulk CoxTey epilayer using in situ heating in a transmission electron microscope (TEM). We show that a Peierls-like lattice instability occurs in TaCo2Te2 at a transition temperature of ~523 K, which was corroborated by phonon calculations. Post-heat-treated samples reveal a thermally induced surface diffusion process and the dominant lateral growth of the CoxTey epilayer on the TaCo2Te2 vdW layers, as observed in cross-sectional TEM images. Temperature-dependent selected area electron diffraction (SAED) patterns reveal that the quasi-vdW CoxTey/TaCo2Te2 heterointerface acquires directional locking by aligning larger interlayer lattice mismatch along the lattice instability axis of TaCo2Te2, while preserving a strong lattice matching along the orthogonal direction. This heterostructure exhibits precise interlayer registry with one-dimensional lattice incommensuration along the lattice instability axis, resulting from structural distortion to accommodate lattice-mismatch strain. Moreover, the interfacial reconstruction of TaCo2Te2 back to the distorted phase stabilizes the lattice-locking of the quasi-vdW heterointerface at elevated temperatures. These findings encourage the expansion of material diversity for designing and predicting novel multi-dimensional heterostructures by leveraging lattice instabilities to guide epitaxy.

cond-mat.mtrl-sci↗

arXiv2026

Discovery of an odd-parity f-wave charge order in a kagome metal

The spontaneous breaking of symmetries is a cornerstone of physics, defining the phases of matter from the cosmological scale to the quantum realm. In condensed matter, electronic orders are classified by their behavior under fundamental symmetries like spatial inversion (parity). While even-parity orders, such as conventional superconductivity and charge density waves, are ubiquitous, their odd-parity counterparts--predicted to host exotic phenomena such as gapless quasiparticle excitations and novel collective modes--are comparatively elusive states of quantum matter. Here, using high-resolution scanning tunneling microscopy and angle-resolved photoemission spectroscopy on the kagome metal CsV$_3$Sb$_5$, we report the discovery of an inversion symmetry-breaking $f$-wave charge bond order. We show that this phase, which preserves translation symmetry, is stabilized by the spontaneous opening of a spectral gap at a previously overlooked Dirac point, providing a textbook condensed-matter realization of the Gross-Neveu model for dynamical mass generation and parity breaking. Intriguingly, this $f$-wave order is itself a intervening phase, vanishing abruptly below a temperature of 10\,K and pointing to a subsequent transition into a `hidden' electronic state that is invisible to local STM probes. Our findings establish odd-parity charge order as a novel phase of matter, here, embedded within the intricate hierarchy of correlated electronic orders on the kagome lattice.

cond-mat.str-el↗

arXiv2025

Orbital-resolved imaging of coherent femtosecond exciton dynamics in coupled molecules

Optical excitation and control of excitonic wavepackets in organic molecules is the basis to energy conversion processes. To gain insights into such processes, it is essential to establish the relationship between the coherence timescales of excitons with the electronic inhomogeneity in the molecules, as well as the influence of intermolecular interactions on exciton dynamics. Here, we demonstrate orbital-resolved imaging of optically induced coherent exciton dynamics in single copper napthalocyanine (CuNc) molecules, and selective coherent excitation of dark and bright triplet excitons in coupled molecular dimers. Ultrafast photon-induced tunneling current enabled atomic-scale imaging and control of the excitons in resonantly excited molecules by employing excitonic wavepacket interferometry. Our results reveal an ultrafast exciton coherence time of ~ 70 fs in a single molecule, which decreases for the triplet excitons in interacting molecules.

physics.optics↗

arXiv2025

Local spectroscopy of loop current order with individual magnetic atoms

Hidden ordered states--characterized by order parameters that elude conventional probes--pose a fundamental challenge for their identification in quantum materials. Recent experiments report evidence for time-reversal symmetry breaking orbital magnetic order and anomalous transport signatures in the $2a\times2a$ charge density wave state of the kagome metal CsV$_3$Sb$_5$ at a temperature $T<30\,$K. Theoretical analyses propose that a time-reversal symmetry breaking loop-current order could exist as the ground state of this charge density wave. However, this microscopic interpretation remains debated and experimentally unverified. In this work, we employ individual magnetic atoms as local quantum sensors to examine the quasiparticle excitations of the charge density wave in CsV$_3$Sb$_5$ with the scanning tunneling microscope. Our spectroscopic measurements show that the magnetic moment of Co induces a spatially localized $dI/dV$ peak inside the spectral gap of the charge density wave near the Fermi energy. Conducting temperature-dependent spectroscopy, we find that this spectral feature emerges at $T<30\,$K. By comparing our experimental observations with results of quantum many-body simulations and realistic tight-binding model calculations, we show that this spectroscopic signature can be naturally interpreted as a local flux defect in a loop current ordered state, arising from the Kondo coupling of the magnetic moment of Co with the loop current electrons. The excellent agreement between our experimental and theoretical results suggests the presence of loop-current order in the $2a\times2a$ charge density wave of CsV$_3$Sb$_5$ at $T<30\,$K. Our results provide a microscopic picture to the observation of time-reversal symmetry breaking orbital magnetism and anomalous transport signatures detected in measurements of the macroscopic material properties.

cond-mat.str-el↗

arXiv2025

Room temperature observation of the anomalous in-plane Hall effect in epitaxial thin films of a Weyl ferromagnet

Topologically nontrivial electronic states can give rise to novel anomalous Hall effects. The potential appearance of these effects at room temperature holds promise for their application in magnetic sensing, spintronics, and energy harvesting technology. The anomalous in-plane Hall effect (IPHE) is predicted to arise in topological magnetic materials when an external magnetic field is applied within the sample plane. Because of stringent symmetry requirements, the conclusive detection of the anomalous IPHE induced by topological electronic states remains challenging, and the study of anomalous Hall effects is often confined to cryogenic conditions. Combining molecular beam epitaxy of the kagome metal Fe$_3$Sn with measurements of the electric Hall effect and theoretical calculations, we propose and experimentally demonstrate that the interplay of the kagome lattice motif with spin-orbit coupling and canted ferromagnetism with large exchange interactions gives rise to the anomalous IPHE at room temperature that is induced by topological Weyl points in the electronic band structure. Synthesizing a topological heterostructure including layers of Fe$_3$Sn and ferromagnetic CoFeB, we further show the enhancement of the anomalous IPHE through the magnetic stray field of the CoFeB layer. Our work establishes a design paradigm for topological magnets and heterostructures to discover and control novel anomalous Hall effects toward their use in technological applications.

cond-mat.mes-hall↗

arXiv2024

Cascade of strongly correlated quantum states in a partially filled kagome flat band

Coulomb interactions among charge carriers that occupy an electronic flat band have a profound impact on the macroscopic properties of materials. At sufficient strength, these interactions can give rise to captivating phenomena such as quantum criticality, Mott-Hubbard states, and unconventional superconductivity. The appearance of these characteristics sensitively depends on the number of electrons occupying the flat band states. In this work, we present experimental evidence obtained from scanning tunneling microscopy measurements for a cascade of strongly correlated states appearing in the partially occupied kagome flat bands of Co$_{1-x}$Fe$_x$Sn whose filling can be controlled by the Fe-doping level $x$. At elevated temperatures ($T\geq16\,K$), we detect a nematic electronic state across a broad doping range $0.05 100\,$meV) blend the states of two $3d$-orbital derived flat bands and impart a nematic order parameter. This state serves as the parent phase of a strongly correlated phase diagram: At lower temperatures $T<16\,$K, we find spectroscopic evidence for an orbital-selective Mott state enabled by the $3d$-orbital degeneracy of the Co atom. This state can only be detected in samples with ideal Fe doping ($x=0.17$) and descends into pseudogap phases upon electron and hole doping. At $T<8\,$K, the pseudogap phase evolves into another nematic low temperature state. Our observations demonstrate that the electronic ground state of a kagome flat band depends on the complex interplay between strong Coulomb repulsion, $3d$-orbital degeneracy, and flat band filling fraction at different temperatures.

cond-mat.str-el↗

arXiv2023

Experimental evidence for Berry curvature multipoles in antiferromagnets

Berry curvature multipoles appearing in topological quantum materials have recently attracted much attention. Their presence can manifest in novel phenomena, such as nonlinear anomalous Hall effects (NLAHE). The notion of Berry curvature multipoles extends our understanding of Berry curvature effects on the material properties. Hence, research on this subject is of fundamental importance and may also enable future applications in energy harvesting and high-frequency technology. It was shown that a Berry curvature dipole can give rise to a 2nd order NLAHE in materials of low crystalline symmetry. Here, we demonstrate a fundamentally new mechanism for Berry curvature multipoles in antiferromagnets that are supported by the underlying magnetic symmetries. Carrying out electric transport measurements on the kagome antiferromagnet FeSn, we observe a 3rd order NLAHE, which appears as a transverse voltage response at the 3rd harmonic frequency when a longitudinal a.c. current drive is applied. Interestingly, this NLAHE is strongest at and above room temperature. We combine these measurements with a scaling law analysis, a symmetry analysis, model calculations, first-principle calculations, and magnetic Monte-Carlo simulations to show that the observed NLAHE is induced by a Berry curvature quadrupole appearing in the spin-canted state of FeSn. At a practical level, our study establishes NLAHE as a sensitive probe of antiferromagnetic phase transitions in other materials, such as moiré superlattices, two-dimensional van der Waal magnets, and quantum spin liquid candidates, that remain poorly understood to date. More broadly, Berry curvature multipole effects are predicted to exist for 90 magnetic point groups. Hence, our work opens a new research area to study a variety of topological magnetic materials through nonlinear measurement protocols.

cond-mat.mes-hall↗

arXiv2023

Visualizing the Localized Electrons of a Kagome Flat Band

Destructive interference between electron wavefunctions on the two-dimensional (2D) kagome lattice induces an electronic flat band, which could host a variety of interesting many-body quantum states. Key to realize these proposals is to demonstrate the real space localization of kagome flat band electrons. In particular, the extent to which the often more complex lattice structure and orbital composition of realistic materials counteract the localizing effect of destructive interference, described by the 2D kagome lattice model, is hitherto unknown. We used scanning tunneling microscopy (STM) to visualize the non-trivial Wannier states of a kagome flat band at the surface of CoSn, a kagome metal. We find that the local density of states associated with the flat bands of CoSn is localized at the center of the kagome lattice, consistent with theoretical expectations for their corresponding Wannier states. Our results show that these states exhibit an extremely small localization length of two to three angstroms concomitant with a strongly renormalized quasiparticle velocity, which is comparable to that of moiré superlattices. Hence, interaction effects in the flat bands of CoSn could be much more significant than previously thought. Our findings provide fundamental insight into the electronic properties of kagome metals and are a key step for future research on emergent many-body states in transition metal based kagome materials.

cond-mat.mes-hall↗

arXiv2022

Atomic-scale Manipulation of Single-Polaron in a Two-Dimensional Semiconductor

Polaron is a composite quasiparticle derived from an excess carrier trapped by local lattice distortion, and it has been studied extensively for decades both theoretically and experimentally. However, atomic-scale creation and manipulation of single-polarons in real space have still not been achieved so far, which precludes the atomistic understanding of the properties of polarons as well as their applications. Herein, using scanning tunneling microscopy, we succeeded to create single polarons in a monolayer two-dimensional semiconductor, CoCl2. Combined with first-principles calculations, two stable polaron configurations, centered at on-top and hollow sites, respectively, have been revealed. Remarkably, a series of manipulation progresses, from creation, erasure to transition, can be accurately implemented on individual polarons. Our results pave the way to understand the polaronic physics at atomic level, and the easy control of single polarons in 2D semiconductor may open the door to 2D polaronics including the data storage.

cond-mat.mes-hall↗

arXiv2017

Experimental realization of graphene-like borophene

We report a successful preparation of a purely honeycomb, graphene-like borophene, by using an Al(111) surface as the substrate and molecular beam epitaxy (MBE) growth in ultrahigh vacuum. Our scanning tunneling microscopy (STM) reveals perfect monolayer borophene with planar, non-buckled honeycomb lattice similar as graphene. Theoretical calculations show that the honeycomb borophene on Al(111) is energetically stable. Remarkably, nearly one electron charge is transferred to each boron atom from the Al(111) substrate and stabilizes the honeycomb borophene structure, in contrast to the little charge transfer in borophene/Ag(111) case. This work demonstrates that the borophene lattice can be manipulated by controlling the charge transfer between the substrate and the borophene film.

cond-mat.mes-hall↗