SearcharxivSearch

arXiv subjects

Wencan Jin

Publications and source records attributed to Wencan Jin.

At least 19 recordsLinked to original sources

Optical poling of a quantum ferroelectric metal across the order-disorder phase transition

Electron-doped strontium titanate has emerged as a prototypical quantum ferroelectric metal. It provides a fertile ground to explore how ferroelectric instability intertwined with itinerant electrons creates quantum phenomena, including unconventional superconductivity. Despite extensive studies, the microscopic origin of the ferroelectric transition remains unsettled, with distinct interpretations based on displacive mechanism driven by soft mode and order-disorder alignment of local dipoles. In particular, the local dipoles form nanoscale, spatially heterogeneous clusters, termed polar nanoregions, posing a significant challenge for probing or manipulating them. Here, using rotational anisotropy second harmonic generation, a symmetry-resolved probe, we quantify the orientational statistics of polar nanoregions in dilute electron-doped Sr$_{0.95}$Ba$_{0.05}$Ti$_{1-x}$Nb$_x$O$_3$. By tracking the alignment and meltdown of polar nanoregions in thermal cycles, we unambiguously demonstrate the order-disorder nature of the ferroelectric transition. We further show that, above transition temperature, femtosecond optical fields enable deterministic control of otherwise disordered polar nanoregions, realizing reversible write and readout of polar textures on ultrafast timescales. Our findings provide new insight into ferroelectric instability and establish an all-optical route of controlling polar metal systems where conventional electrical approaches are not feasible.

cond-mat.mtrl-sci

Co2SeO3Cl2: Studies of Emerging Magnetoelectric Coupling in a Polar, Buckled Honeycomb Material

The development of magnetoelectric materials requires chemical design strategies that integrate structural polarity with magnetic lattices capable of supporting competing spin interactions. Here, we demonstrate such an approach in the polar, buckled honeycomb magnet Co2SeO3Cl2. Magnetization and heat-capacity measurements reveal strong magnetic anisotropy and four successive magnetic transitions at 25.4, 16.8, 11, and 3 K. The recovered magnetic entropy through the ordering regime is only around half of the expected 2Rln(2), indicating persistent spin fluctuations. Second-harmonic generation measurements show three pronounced intensity anomalies at 11, 17, and 26 K that coincide with magnetic transitions while revealing that the crystallographic symmetry is preserved. Together, these results demonstrate that polar, buckled honeycomb magnets offer an unconventional phase space for coupling magnetic and electric dipoles in magnetoelectric materials.

cond-mat.mtrl-sci

Magneto-optical spectroscopy based on pump-probe strobe light

We demonstrate a pump-probe strobe light spectroscopy for sensitive detection of magneto-optical dynamics in the context of hybrid magnonics. The technique uses a combinatorial microwave-optical pump-probe scheme, leveraging both the high-energy resolution of microwaves and the high-efficiency detection using optical photons. In contrast to conventional stroboscopy using a continuous-wave light, we apply microwave and optical pulses with varying pulse widths, and demonstrate magnetooptical detection of magnetization dynamics in Y3Fe5O12 films. The detected magneto-optical signals strongly depend on the characteristics of both the microwave and the optical pulses as well as their relative time delays. We show that good magneto-optical sensitivity and coherent stroboscopic character are maintained even at a microwave pump pulse of 1.5 ns and an optical probe pulse of 80 ps, under a 7 megahertz clock rate, corresponding to a pump-probe footprint of ~1% in one detection cycle. Our results show that time-dependent strobe light measurement of magnetization dynamics can be achieved in the gigahertz frequency range under a pump-probe detection scheme.

cond-mat.mes-hall

Multimode magnon-phonon cavity driven by symmetry-locked strain fields

Hybrid magnon-phonon cavities with precise control knobs are highly sought after for coherent energy and signal transduction in solid-state platforms. While strain offers a powerful means to tune magnonic characteristics, extending strain engineering into magnon-phonon hybridization has remained elusive. Moreover, implementing controllable strain at the meso- or nanoscale poses a formidable challenge, as spatial inhomogeneity of strain fields often leads to enhanced damping and reduced coherence, thereby hindering device integration and scalability. Here, we present an epitaxial La0.7Sr0.3MnO3/SrTiO3 (LSMO/STO) heterostructure that exhibits strong coupling between the Kittel magnon and acoustic phonon. Leveraging the emergence of structural domains when STO undergoes a cubic-to-tetragonal phase transition, we create anisotropic local strains at the interface. Remarkably, the anisotropic local strain of less than 0.1 % drives the pronounced splitting of the magnon into three branches. Each branch independently hybridizes with acoustic phonons, forming a matrix of magnon-phonon avoided crossings that underpins multimode transduction and programmable networks in frequency and magnetic field space. An analytical model reveals that the split magnon branches are deterministically locked to the three main crystalline axes, enabling robust, orientation-selective control of the hybridized magnon-phonon spectrum against spatial inhomogeneity. Our results establish designed local strain as an exceptionally sensitive trigger for multimode magnon-phonon hybridization in magnetoelastic oxide heterostructures, and highlight local strain engineering as a viable strategy for designing tunable hybrid magnonic and phononic devices.

cond-mat.mtrl-sci

Emergent Topological Hall Effect in Fe-doped Monolayer WSe2

The topological Hall effect (THE) has attracted great attention since it provides an important probe of the interaction between electron and topological spin textures. THE has been considered an experimental signature of the topological spin texture of skyrmions. While THE has been widely reported in chiral magnets, oxide heterostructures, and hybrid systems such as ferromagnet/heavy metal and ferromagnet/topological insulators, the study of monolayer structures is lacking, hindering the understanding of noncollinear spin textures at the atomically thin scale. Here, we show a discernible THE via proximity coupling of Fe-doped monolayer WSe2 (Fe:WSe2) synthesized using chemical vapor deposition on a Pt Hall bar. Multiple characterization methods were employed to demonstrate that Fe atoms substitutionally replace W atoms, making a two-dimensional (2D) van der Waals (vdW) dilute magnetic semiconductor (DMS) at room temperature. Distinct from the intrinsic anomalous Hall effect, we found the transverse Hall resistivity of Fe:WSe2 displaying two additional dip/peak features in the temperature-dependent measurements, consistent with the contribution of THE. The topological Hall effect is attributed to the magnetic skyrmions that emerge from the Dzyaloshinskii-Moriya interactions at the Fe:WSe2 and Pt interface. Our work shows that a DMS synthesized from 2D vdW transition metal dichalcogenides is promising for realizing magnetic skyrmions and spintronic applications.

physics.atom-ph

Strain Effects in SrHfO$_{3}$ Films Grown by Hybrid Molecular Beam Epitaxy

Perovskite oxides hetero-structures are host to a large number of interesting phenomena such as ferroelectricity and 2D-superconductivity. Ferroelectric perovskite oxides have been of significant interest due to their possible use in MOSFETs and FRAM. SrHfO$_3$ (SHO) is a perovskite oxide with pseudo-cubic lattice parameter of 4.1 $\mathring{A}$ that previous DFT calculations suggest can be stabilized in a ferroelectric P4mm phase, similar to STO, when stabilized with sufficient compressive strain. Additionally, it is insulating, possesses a large band gap, and a high dielectric constant, making it an ideal candidate for oxide electronic devices. In this work, SHO films were grown by hybrid molecular beam epitaxy with a tetrakis(ethylmethylamino)hafnium(IV) source on GdScO$_3$ and TbScO$_3$ substrates. Equilibrium and strained SHO phases were characterized using X-ray diffraction, X-ray absorption spectroscopy, and scanning transmission electron microscopy to determine the perovskite phase of the strained films, with the results compared to density functional theory models of phase stability versus strain. Contrary to past reports, we find that compressively-strained SrHfO$_3$ undergoes octahedral tilt distortions and most likely takes on the I4/mcm phase with the a$^0$a$^0$c$^-$ tilt pattern.

cond-mat.mtrl-sci

Exciton-activated effective phonon magnetic moment in monolayer MoS2

Optical excitation of chiral phonons plays a vital role in studying the phonon-driven magnetic phenomena in solids. Transition metal dichalcogenides host chiral phonons at high symmetry points of the Brillouin zone, providing an ideal platform to explore the interplay between chiral phonons and valley degree of freedom. Here, we investigate the helicity-resolved magneto-Raman response of monolayer MoS2 and identify a doubly degenerate Brillouin-zone-center chiral phonon mode at ~270 cm-1. Our wavelength- and temperature-dependent measurements show that this chiral phonon is activated through the resonant excitation of A exciton. Under an out-of-plane magnetic field, the chiral phonon exhibits giant Zeeman splitting, which corresponds to an effective magnetic moment of ~2.5mu_B. Moreover, we carry out theoretical calculations based on the morphic effects in nonmagnetic crystals, which reproduce the linear Zeeman splitting and Raman cross-section of the chiral phonon. Our study provides important insights into lifting the chiral phonon degeneracy in an achiral covalent material, paving a new route to excite and control chiral phonons.

cond-mat.mtrl-sci

Spin Dynamics in van der Waals Magnetic Systems

The discovery of atomic monolayer magnetic materials has stimulated intense research activities in the two-dimensional (2D) van der Waals (vdW) materials community. The field is growing rapidly and there has been a large class of 2D vdW magnetic compounds with unique properties, which provides an ideal platform to study magnetism in the atomically thin limit. In parallel, based on tunneling magnetoresistance and magneto-optical effect in 2D vdW magnets and their heterostructures, emerging concepts of spintronic and optoelectronic applications such as spin tunnel field-effect transistors and spin-filtering devices are explored. While the magnetic ground state has been extensively investigated, reliable characterization and control of spin dynamics play a crucial role in designing ultrafast spintronic devices. Ferromagnetic resonance (FMR) allows direct measurements of magnetic excitations, which provides insight into the key parameters of magnetic properties such as exchange interaction, magnetic anisotropy, gyromagnetic ratio, spin-orbit coupling, damping rate, and domain structure. In this review article, we present an overview of the essential progress in probing spin dynamics of 2D vdW magnets using FMR techniques. Given the dynamic nature of this field, we focus mainly on broadband FMR, optical FMR, and spin-torque FMR, and their applications in studying prototypical 2D vdW magnets. We conclude with the recent advances in laboratory- and synchrotron-based FMR techniques and their opportunities to broaden the horizon of research pathways into atomically thin magnets.

cond-mat.mtrl-sci

Magnetism and Spin Dynamics in Room-Temperature van der Waals Magnet Fe$_5$GeTe$_2$

Two-dimensional (2D) van der Waals (vdWs) materials have gathered a lot of attention recently. However, the majority of these materials have Curie temperatures that are well below room temperature, making it challenging to incorporate them into device applications. In this work, we synthesized a room-temperature vdW magnetic crystal Fe$_5$GeTe$_2$ with a Curie temperature T$_c = 332$ K, and studied its magnetic properties by vibrating sample magnetometry (VSM) and broadband ferromagnetic resonance (FMR) spectroscopy. The experiments were performed with external magnetic fields applied along the c-axis (H$\parallel$c) and the ab-plane (H$\parallel$ab), with temperatures ranging from 300 K to 10 K. We have found a sizable Landé g-factor difference between the H$\parallel$c and H$\parallel$ab cases. In both cases, the Landé g-factor values deviated from g = 2. This indicates contribution of orbital angular momentum to the magnetic moment. The FMR measurements reveal that Fe$_5$GeTe$_2$ has a damping constant comparable to Permalloy. With reducing temperature, the linewidth was broadened. Together with the VSM data, our measurements indicate that Fe$_5$GeTe$_2$ transitions from ferromagnetic to ferrimagnetic at lower temperatures. Our experiments highlight key information regarding the magnetic state and spin scattering processes in Fe$_5$GeTe$_2$, which promote the understanding of magnetism in Fe$_5$GeTe$_2$, leading to implementations of Fe$_5$GeTe$_2$ based room-temperature spintronic devices.

cond-mat.mtrl-sci

Correlating surface stoichiometry and termination in SrTiO$_{3}$ films grown by hybrid molecular beam epitaxy

Hybrid oxide molecular beam epitaxy (hMBE), a thin-film deposition technique in which transition metal cations are delivered using a metal-organic precursor, has emerged as the state-of-the-art approach to the synthesis of electronic-grade complex oxide films with a stoichiometric growth window. However, numerous questions remain regarding the chemical mechanisms of the growth process and the surface properties of the resulting films. To examine these properties, thin film SrTiO$_{3}$ (STO) was prepared by hMBE using a titanium tetraisopropoxide (TTIP) precursor for Ti delivery and an elemental Sr source on annealed STO and Nb-doped STO substrates with varying TTIP:Sr flux ratios to examine the conditions for the reported stoichiometric growth window. The films were transferred in vacuo to an x-ray photoelectron spectroscopy system to study the surface elemental composition. Samples were examined using x-ray diffraction to compare our surface sensitive results with previously reported measurements of the bulk of the films in the literature. Ex situ studies by atomic force microscopy, scanning tunneling microscopy and low energy electron microscopy confirmed the presence of surface reconstructions and an Ehrlich-Schwoebel barrier consistent with an A-site SrO termination. We find that a surface exhibiting a mixture of SrO and TiO$_{2}$ termination, or a full SrO termination is necessary to obtain stoichiometric adsorption-controlled growth. These results indicate that surface Sr is necessary to maintain chemical equilibrium for stoichiometric growth during the hMBE process, which is important for the design of future interfacial systems using this technique.

cond-mat.mtrl-sci

Structural Monoclinicity and Its Coupling to Layered Magnetism in Few-Layer $\mathrm{CrI_{3}}$

Using polarization-resolved Raman spectroscopy, we investigate layer number, temperature, and magnetic field dependence of Raman spectra in one- to four-layer $\mathrm{CrI_{3}}$. Layer-number-dependent Raman spectra show that in the paramagnetic phase a doubly degenerated $E_{g}$ mode of monolayer $\mathrm{CrI_{3}}$ splits into one $A_{g}$ and one $B_{g}$ mode in N-layer (N > 1) $\mathrm{CrI_{3}}$ due to the monoclinic stacking. Their energy separation increases in thicker samples until an eventual saturation. Temperature-dependent measurements further show that the split modes tend to merge upon cooling but remain separated until 10 K, indicating a failed attempt of the monoclinic-to-rhombohedral structural phase transition that is present in the bulk crystal. Magnetic-field-dependent measurements reveal an additional monoclinic distortion across the magnetic-field-induced layered antiferromagnetism-to-ferromagnetism phase transition. We propose a structural change that consists of both a lateral sliding toward the rhombohedral stacking and a decrease in the interlayer distance to explain our experimental observations.

cond-mat.mes-hall

Tunable layered-magnetism-assisted magneto-Raman effect in a two-dimensional magnet $\mathrm{CrI_3}$

We use a combination of polarized Raman spectroscopy experiment and model magnetism-phonon coupling calculations to study the rich magneto-Raman effect in the two-dimensional (2D) magnet $\mathrm{CrI_3}$. We reveal a novel layered-magnetism-assisted phonon scattering mechanism below the magnetic onset temperature, whose Raman excitation breaks time-reversal symmetry, has an antisymmetric Raman tensor, and follows the magnetic phase transitions across critical magnetic fields, on top of the presence of the conventional phonon scattering with symmetric Raman tensors in $N$-layer $\mathrm{CrI_3}$. We resolve in data and by calculations that the 1st-order $A_g$ phonon of monolayer splits into a $N$-fold multiplet in $N$-layer $\mathrm{CrI_3}$ due to the interlayer coupling ($N$>=2) and that the phonons with the multiple show distinct magnetic field dependence because of their different layered-magnetism-phonon coupling. We further find that such a layered-magnetism-phonon coupled Raman scattering mechanism extends beyond 1st-order to higher-order multi-phonon scattering processes. Our results on magneto-Raman effect of the 1st-order phonons in the multiplet and the higher-order multi-phonons in $N$-layer $\mathrm{CrI_3}$ demonstrate the rich and strong behavior of emergent magneto-optical effects in 2D magnets and underlines the unique opportunities of new spin-phonon physics in van der Waals layered magnets.

cond-mat.mtrl-sci

Observation of the polaronic character of excitons in a two-dimensional semiconducting magnet $\mathrm{CrI_3}$

Exciton dynamics can be strongly affected by lattice vibrations through electron-phonon coupling. This is rarely explored in two-dimensional magnetic semiconductors. Focusing on bilayer CrI3, we first show the presence of strong electron-phonon coupling through temperature-dependent photoluminescence and absorption spectroscopy. We then report the observation of periodic broad modes up to the 8th order in Raman spectra, attributed to the polaronic character of excitons. We establish that this polaronic character is dominated by the coupling between the charge-transfer exciton at 1.96 eV and a longitudinal optical phonon at 120.6 cm-1. We further show that the emergence of long-range magnetic order enhances the electron-phonon coupling strength by about 50$\%$ and that the transition from layered antiferromagnetic to ferromagnetic order tunes the spectral intensity of the periodic broad modes, suggesting a strong coupling among the lattice, charge and spin in two-dimensional CrI3. Our study opens opportunities for tailoring light-matter interactions in two-dimensional magnetic semiconductors.

cond-mat.mes-hall

Second-order nonlinear optical and linear UV-VIS absorption properties of type-II multiferroic candidates RbFe(AO4)2 (A = Mo, Se, S)

Motivated by the search for type-II multiferroics, we present a comprehensive optical study of a complex oxide family of type-II multiferroic candidates: RbFe(MoO4)2, RbFe(SeO4)2, and RbFe(SO4)2. We employ rotational-anisotropy second harmonic generation spectroscopy (RA SHG), a technique sensitive to point symmetries, to address discrepancies in literature-assigned point/space groups and to identify the correct crystal structures. At room temperature we find that our RA SHG patterns rotate away from the crystal axes in RbFe(AO4)2 (A = Se, S), which identifies the lack of mirror symmetry and in-plane two-fold rotational symmetry. Also, the SHG efficiency of RbFe(SeO4)2 is two orders of magnitude stronger than RbFe(AO4)2 (A = Mo, S), which suggests broken inversion symmetry. Additionally, we present temperature-dependent linear optical characterizations near the band edge of this family of materials using ultraviolet-visible (UV-VIS) absorption spectroscopy. Included is experimental evidence of the band gap energy and band gap transition type for this family. Previously unreported sub-band gap absorption is also presented, which reveals prominent optical transitions, some with an unusual central energy temperature dependence. Furthermore, we find that by substituting the A-site in RbFe(AO4)2 (A = Mo, Se, S), the aforementioned transitions are spectrally tunable. Finally, we discuss the potential origin and impact of these tunable transitions.

cond-mat.mtrl-sci

Symmetry-resolved two-magnon excitations in a strong spin-orbit-coupled bilayer antiferromagnet

We used a combination of polarized Raman spectroscopy and spin wave calculations to study magnetic excitations in the strong spin-orbit-coupled (SOC) bilayer perovskite antiferromagnet $Sr_3Ir_2O_7$. We observed two broad Raman features at ~ 800 $cm^{-1}$ and ~ 1400 $cm^{-1}$ arising from magnetic excitations. Unconventionally, the ~ 800 $cm^{-1}$ feature is fully symmetric ($A_{1g}$) with respect to the underlying tetragonal ($D_{4h}$) crystal lattice which, together with its broad line shape, definitively rules out the possibility of a single magnon excitation as its origin. In contrast, the ~ 1400 $cm^{-1}$ feature shows up in both the $A_{1g}$ and $B_{2g}$ channels. From spin wave and two-magnon scattering cross-section calculations of a tetragonal bilayer antiferromagnet, we identified the ~ 800 $cm^{-1}$ (~ 1400 $cm^{-1}$) feature as two-magnon excitations with pairs of magnons from the zone-center $Γ$ point (zone-boundary van Hove singularity X point). We further found that this zone-center two-magnon scattering is unique to bilayer perovskite magnets which host an optical branch in addition to the acoustic branch, as compared to their single layer counterparts. This zone-center two-magnon mode is distinct in symmetry from the time-reversal symmetry broken spin wave gap and phase mode proposed to explain the ~ 92 meV (742 $cm^{-1}$) gap in RIXS magnetic excitation spectra of $Sr_3Ir_2O_7$.

cond-mat.str-el

Observation of a ferro-rotational order coupled with second-order nonlinear optical fields

The ferro-rotational order, whose order parameter (OP) is an axial vector invariant under both time reversal (TR) and spatial inversion (SI) operations, is the last remaining category of ferroics to be observed after the ferroelectric, ferromagnetic, and ferro-toroidal orders. This order has become increasingly popular in many new quantum materials, especially in complex oxides, and is considered responsible for a number of novel phenomena such as polar vortices, giant magnetoelectric coupling, and type-II multiferroics. However, physical properties of the ferro-rotational order have been rarely studied either theoretically or experimentally. Here, using high sensitivity rotational anisotropy second harmonic generation (RA SHG), we have, for the first time, exploited the electric quadrupole (EQ) contribution to the SHG to directly couple to this centrosymmetric ferro-rotational order in an archetype of type-II multiferroics, RbFe(MoO4)2. Surprisingly, we have found that two types of domains with opposite ferro-rotational vectors emerge with distinct populations at the critical temperature Tc ~195 K and gradually evolve to reach an even ratio at lower temperatures. Moreover, we have identified the ferro-rotational order phase transition as weak first order, and have revealed its conjugate coupling field as a unique combination of the induced EQ SHG and the incident fundamental electric fields. Our results on physical properties of a ferro-rotational order provide crucial knowledge for understanding and searching for novel phases of matter built upon the ferro-rotational order. Further, these results open the possibility of revealing unconventional centrosymmetric orders and identifying their conjugate coupling fields with second order nonlinear optics.

cond-mat.mtrl-sci

Polarized Raman spectroscopy study of metallic $(Sr_{1-x}La_{x})_{3}Ir_{2}O_{7}$: a consistent picture of disorder-interrupted unidirectional charge order

We have used rotational anisotropic polarized Raman spectroscopy to study the symmetries, the temperature and the doping dependence of the charge ordered state in metallic $(Sr_{1-x}La_{x})_{3}Ir_{2}O_{7}$. Although the Raman probe size is greater than the charge ordering length, we establish that the charge ordering breaks the fourfold rotational symmetry of the underlying tetragonal crystal lattice into twofold, as well as the translational symmetry, and forms short-range domains with $90^{\circ}$ rotated charge order wave vectors, as soon as the charge order sets in below $T_{CO} = \sim$ 200K and across the doping-induced insulator metal transition. We observe that this charge order mode frequency remains nearly constant over a wide temperature range and up to the highest doping level. These above features are highly reminiscent of the ubiquitous unidirectional charge order in underdoped high-$T_C$ copper-oxide-based superconductors (cuprates). We further resolve that the charge order damping rate diverges when approaching $T_{CO}$ from below and increases significantly as increasing the La doping level, which resembles the behaviors for a disorder-interrupted ordered phase and has not been observed for the charge order in cuprates.

cond-mat.str-el

Raman fingerprint of two terahertz spin wave branches in a two-dimensional honeycomb Ising ferromagnet

Two-dimensional (2D) magnetism has been long sought-after and only very recently realized in atomic crystals of magnetic van der Waals materials. So far, a comprehensive understanding of the magnetic excitations in such 2D magnets remains missing. Here we report polarized micro-Raman spectroscopy studies on a 2D honeycomb ferromagnet CrI3. We show the definitive evidence of two sets of zero-momentum spin waves at frequencies of 2.28 terahertz (THz) and 3.75 THz, respectively, that are three orders of magnitude higher than those of conventional ferromagnets. By tracking the thickness dependence of both spin waves, we reveal that both are surface spin waves with lifetimes an order of magnitude longer than their temporal periods. Our results of two branches of high-frequency, long-lived surface spin waves in 2D CrI3 demonstrate intriguing spin dynamics and intricate interplay with fluctuations in the 2D limit, thus opening up opportunities for ultrafast spintronics incorporating 2D magnets.

cond-mat.mes-hall