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Youwen Long

Publications and source records attributed to Youwen Long.

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$d$-wave altermagnetism revealed by resonant inelastic X-ray scattering

Altermagnetism defines a third fundamental class of collinear magnetic order, featuring compensated magnetic moments with antiparallel spin alignment, yet lifted Kramers degeneracy without the need for relativistic spin-orbit coupling. Its ability to host spin-polarized electronic bands and unconventional chiral magnons makes it a promising platform for functional materials. However, experimental verification has proven challenging; while circular dichroism in resonant inelastic X-ray scattering (RIXS) has been suggested as a signature of chiral magnons, it remains controversial whether this effect is an intrinsic property of altermagnetism or an artifact of experimental geometry. In this work, we resolve this debate and provide unambiguous experimental evidence of $d$-wave altermagnetism in the strongly correlated Lieb-lattice magnet La$_2$O$_3$Mn$_2$Se$_2$. The RIXS spectra exhibit a $d$-wave-symmetry circular dichroism in the magnetic excitations that vanishes in the paramagnetic phase. Through RIXS-operator symmetry analysis and exact-diagonalization calculations, we prove that the observed dichroism is a direct consequence of altermagnetic symmetry constraints, independent of magnon branch splitting. Our results provide definitive evidence for the experimental realization of $d$-wave altermagnetism in La$_2$O$_3$Mn$_2$Se$_2$ and establish circularly polarized RIXS as a highly symmetry-sensitive spectroscopic framework for detecting magnetic phases that evade conventional probes.

cond-mat.str-el

Long-range magnetic order with disordered spin orientations in a high-entropy antiferromagnet

Disorder in magnetic systems typically suppresses long-range order, promoting short-range states such as spin glasses and magnetic clusters. This is particularly prominent in high-entropy materials, characterized by the random distributions of local magnetic entities and exchange interactions. However, in rare exceptions, long-range magnetic order can persist in high-entropy systems, while the microscopic characters and underlying mechanisms remain elusive, especially the magnetic behaviors of individual elements. Here, combining neutron diffraction and resonant soft x-ray scattering, we have conducted an element-specific investigation into the magnetic order of a high-entropy honeycomb-lattice van der Waals material (Mn1/4Fe1/4Co1/4Ni1/4)PS3. Despite significant atomic disorder, long-range zigzag antiferromagnetic order is observed below 72 K, with all four transition-metal elements participating in a unified phase transition. However, the spin orientations of various elements are distinct, attributed to the competition between single-ion anisotropies and exchange interactions. Our findings showcase a novel form of long-range magnetic order with disordered spin orientations, which is synergically stabilized by distinct magnetic elements in a high entropy magnet, offering a new paradigm for understanding complex magnetic systems.

cond-mat.str-el

Anomalous lattice specific heat and rattling phonon modes in quadruple perovskites

Experimental data on the specific heat $C_p$ of quadruple perovskites ACu$_3$Fe$_2$Re$_2$O$_{12}$ (A = Mn, Cu, La, Ce, Dy) are presented, demonstrating an anomalous concave-down $C_p/T$ vs. $T^2$ curve and a bell-shaped feature in $\beta(T) = (C_p - \gamma T)/T^3$ plotted against $T$ on a logarithmic scale. This feature is most pronounced for A = Cu and Mn. These findings can be explained by the rattling phenomenon, previously identified in other systems such as filled skutterudites and $\beta$-pyrochlores. Using first-principles DFT+U calculations, the presence of a rattling mode in A = Mn system is directly confirmed. A qualitative interpretation of the rattling mechanism in terms of a pseudo-Jahn-Teller effect is proposed.

cond-mat.mtrl-sci

Exchange interaction in ACu3Fe2Re2O12 quadruple perovskites

Quadruple perovskites ACu$_3$Fe$_2$Re$_2$O$_{12}$ attract considerable interest due to their high Curie temperatures (up to $710$K), which strongly depend on the A-site cation. In this work, we employ first-principles calculations to investigate their electronic structure and magnetic exchange interactions. A band mechanism of magnetism that explains the antiferromagnetic character of the exchange interactions and their strong dependence on the filling of the Re $t_{2g}$ states is proposed. These antiferromagnetic interactions stabilize ferrimagnetic ground state. The calculated Curie temperatures, obtained within the Onsager reaction field theory, are in a good agreement with experimental data.

cond-mat.mtrl-sci

High Pressure Growth of Transition-Metal Monosilicide RhGe Single Crystals

Transition-metal monosilicide RhGe has been reported to exhibit weak itinerant ferromagnetism, superconductivity, and topological properties. In this study, we report the high-pressure growth of high-quality RhGe single crystals up to millimeter size using flux method. Transport measurements reveal the metallic behavior of RhGe between 2-300 K with Fermi liquid behavior at low temperature region. However, no superconductivity was observed with variations in Ge composition. Magnetic characterizations indicate that RhGe exhibits a paramagnetic behavior between 2-300 K. The high-quality, large-size RhGe single crystals pave the way for further investigation of their topological properties using spectroscopic techniques.

cond-mat.str-el

Mixed anion control of enhanced negative thermal expansion in the oxysulfide of PbTiO3

The rare physical property of negative thermal expansion (NTE) is intriguing because materials with large NTE over a wide temperature range can serve as high-performance thermal expansion compensators. However, applications of NTE are hindered by the fact that most of the available NTE materials show small magnitudes of NTE, and/or NTE occurs only in a narrow temperature range. Herein, for the first time, we investigated the effect of anion substitution instead of general Pb/Ti-site substitutions on the thermal expansion properties of a typical ferroelectric NTE material, PbTiO3. Intriguingly, the substitution of S for O in PbTiO3 further increases the tetragonality of PbTiO3. Consequently, an unusually enhanced NTE with an average volumetric coefficient of thermal expansion $\bar{\alpha}_V$ = -2.50 $\times$ 10$^{-5}$/K was achieved over a wide temperature range (300 -- 790 K), which is contrasted to that of pristine PbTiO3 ($\bar{\alpha}_V$ = -1.99 $\times$ 10$^{-5}$/K RT -- 763 K). The intensified NTE is attributed to the enhanced hybridization between Pb/Ti and O/S atoms by the substitution of S, as evidenced by our theoretical investigations. We therefore demonstrate a new technique for introducing mixed anions to achieve large NTE over a wide temperature range in PbTiO3-based ferroelectrics.

cond-mat.mtrl-sci

Pressure Induced 18 K Superconductivity and Two Superconducting Phases in CuIr2S4

We report pressure-induced superconductivity in the spinel CuIr$_{2}$S$_{4}$ with a transition temperature ($T_{\text{c}}$) reaching \textbf{18.2 K}, establishing a new record for this class of materials and surpassing the decades-old limit of 13.7 K. Our electrical transport and synchrotron X-ray diffraction studies up to 224 GPa reveal the emergence of \textbf{two distinct superconducting phases} from a charge-ordered insulating state. The first phase (SC-I) appears around 18 GPa, and forms a dome-shaped superconducting region in which the resistivity exhibits a pronounced, field- and current-sensitive drop without reaching strict zero above our base temperature. Above 111.8 GPa, a second, lower-$T_{\text{c}}$ phase (SC-II) emerges and coexists with SC-I over a broad pressure range, and SC-II ultimately develops a true zero-resistance state above 122.2 GPa. These superconducting phases are intimately linked to a cascade of structural transitions that systematically distort the frustrated pyrochlore lattice of Ir atoms. Our results expand the potential for superconductivity in spinels and demonstrate a pathway to high-$T_{\text{c}}$ pairing directly from a correlated insulating state driven by lattice tuning.

cond-mat.supr-con

Importance of the indirect exchange interaction $via$ $s$-states in altermagnetic HgMnO$_3$

The electronic and magnetic properties of recently synthesized new perovskite phase of HgMnO$_3$ are studied. By means of $ab$ $initio$ DFT calculations this material was shown to be altermagnetic. We discuss features of its electronic structure and unveil the physical mechanism of anomalous suppression of antiferromagnetic exchange interaction in this material. While it is tempting to ascribe unexpectedly weak exchange interaction between nearest neighbors to crystal structure distortions, this is the indirect ferromagnetic exchange via Hg $6s$ states, which strongly affects the magnetic properties. This effect can be important not only for HgMnO$_3$, but also for many other transition metal compounds having empty $s$ states, placed not far above the Fermi level.

cond-mat.str-el

Large low-field magnetocaloric response in a ferromagnetic gadolinium orthophosphate

Bulk magnetic and thermodynamic measurements, along with mean-field calculations, were conducted on the ferromagnetic K3Gd5(PO4)6 powders. No magnetic ordering was observed until 2 K, while the application of an external field B > 1 T resulted in the splitting of the Gd3+ ground state multiplet and induced a non-cooperative Schottky effect. The average nearest-neighbor exchange strength |J1/kB| is determined to be 0.017 K, which leads to a remarkably large low field magnetic entropy change {\Delta}Sm = 36.2 J kg-1 K-1 under applied field change B = 2 T at temperature T = 2 K, as well as a maximum adiabatic temperature change Tad = 10.9 K. We contend that ferromagnetic gadolinium orthophosphates serve as a promising reservoir for exploring advanced magnetic refrigerants applicable under low magnetic fields.

cond-mat.mtrl-sci

Percolation-induced resistivity drop in cold-pressed LuH2

The stoichiometric bulk LuH2 is a paramagnetic metal with high electrical conductivity comparable to simple metals. Here we show that the resistivity of cold-pressed (CP) LuH2 samples varies sensitively upon modifying the grain size or surface conditions via the grinding process, i.e., the CP pellets made of commercially purchased LuH2 powder remain metallic but exhibit thousands of times higher resistivity, while additional grinding of LuH2 powders in air further enhances the resistivity and even results in weakly localized behaviors. For these CP samples, interestingly, we can occasionally observe abrupt resistivity drops at high temperatures, which also show dependences on magnetic fields and electrical current. Measurements of variable-temperature XRD, magnetic susceptibility, and specific heat exclude the possibilities of structural, magnetic, and superconducting transitions for the observed resistivity drops. Instead, we tentatively attribute these above observations to the presence of insulating layers on the grain surface due to the modification of hydrogen stoichiometry or the pollution by oxygen/nitrogen. Percolation of the metallic grains through the insulating surfaces can explain the sudden drop in resistivity. The present results thus call for caution in asserting the resistivity drops as superconductivity and invalidate the background subtraction in analyzing the resistivity data.

cond-mat.supr-con

Discovery of a metallic oxide with ultralow thermal conductivity

A compound with metallic electrical conductivity usually has a considerable total thermal conductivity because both electrons and photons contribute to thermal transport. Here, we show an exceptional example of iridium oxide, Bi3Ir3O11, that concurrently displays metallic electrical conductivity and ultralow thermal conductivity approaching 0.61 W m-1 K-1 at 300 K. The compound crystallizes into a cubic structural framework with space group Pn-3. The edge- and corner-sharing IrO6 octahedra with a mixed Ir4.33+ charge state favor metallic electrical transport. Bi3Ir3O11 exhibits an extremely low lattice thermal conductivity close to the minimum limit in theory owing to its tunnel-like structure with filled heavy atoms Bi rattling inside. Theoretical calculations reveal the underlying mechanisms for the extraordinary compatibility between metallic electrical conductivity and ultralow thermal conductivity. This study may establish a new avenue for designing and developing unprecedented heat-insulation metals.

cond-mat.mtrl-sci

Ferroelectricity driven by magnetism in quasi-one-dimensional Ba9Fe3Se15

The spin-induced ferroelectricity in quasi-1D spin chain system is little known, which could be fundamentally different from those in three-dimensional (3D) system. Here, we report the ferroelectricity driven by a tilted screw spin order and its exotic dynamic in the spin-chain compound Ba9Fe3Se15. It is found that the spin-induced polarization has already occurred and exhibits magnetoelectric coupling behavior far above the long-range spin order (LRSO) at TN = 14 K. The polarized entities grow and their dynamic responses slow down gradually with decreasing temperature and permeate the whole lattice to form 3D ferroelectricity at TN. Our results reveal that the short-range spin orders (SRSOs) in the decoupled chains play a key role for the exotic dynamic in this dimension reduced system. Ba9Fe3Se15 is the only example so far which exhibits electric polarization above LRSO temperature because of the formation of SRSOs.

cond-mat.str-el

A ferrotoroidic candidate with well-separated spin chains

The search of novel quasi one-dimensional (1D) materials is one of the important aspects in the field of material science. Toroidal moment, the order parameter of ferrotoroidic order, can be generated by a head-to-tail configuration of magnetic moment. It has been theoretically proposed that one-dimensional (1D) dimerized and antiferromagnetic-like spin chain hosts ferrotoroidicity and has the toroidal moment composed of only two antiparallel spins. Here, we report a ferrotoroidic candidate of Ba6Cr2S10 with such a theoretical model of spin chain. The structure consists of unique dimerized face-sharing CrS6 octahedral chains along the c axis. An antiferromagnetic-like ordering at ~10 K breaks both space- and time-reversal symmetries and the magnetic point group of mm'2' allows three ferroic orders in Ba6Cr2S10: (anti)ferromagnetic, ferroelectric and ferrotoroidic orders. Our investigation reveals that Ba6Cr2S10 is a rare ferrotoroidic candidate with quasi 1D spin chain, which can be considered as a starting point for the further exploration of the physics and applications of ferrotoroidicity.

cond-mat.str-el

Physical realization of topological Roman surface by spin-induced ferroelectric polarization in cubic lattice

Topology, a mathematical concept in geometry, has become an ideal theoretical tool for describing topological states and phase transitions. Many topological concepts have found their physical entities in real or reciprocal spaces identified by topological/geometrical invariants, which are usually defined on orientable surfaces such as torus and sphere. It is natural to quest whether it is possible to find the physical realization of more intriguing non-orientable surfaces. Herein, we show that the set of spin-induced ferroelectric polarizations in cubic perovskite oxides AMn3Cr4O12 (A = La and Tb) resides on the topological Roman surface, a non-orientable two-dimensional manifold formed by sewing a Mobius strip edge to that of a disc. The induced polarization may travel in a loop along the non-orientable Mobius strip or orientable disc depending on how the spin evolves as controlled by external magnetic field. Experimentally, the periodicity of polarization can be the same or the twice of the rotating magnetic field, being well consistent with the orientability of disc and Mobius strip, respectively. This path dependent topological magnetoelectric effect presents a way to detect the global geometry of the surface and deepens our understanding of topology in both mathematics and physics

cond-mat.str-el

High-pressure synthesis and spin glass behavior of a Mn/Ir disordered quadruple perovskite CaCu3Mn2Ir2O12

A new 3d-5d hybridized quadruple perovskite oxide, CaCu3Mn2Ir2O12, was synthesized by high-pressure and high-temperature methods. The Rietveld structure analysis reveals that the compound crystallizes in an AA'3B4O12-type perovskite structure with space group Im-3, where the Ca and Cu are 1:3 ordered at fixed atomic positions. At the B site the 3d Mn and the 5d Ir ions are disorderly distributed due to a rare equal +4 charge states for both of them as determined by X-ray absorption spectroscopy. The competing antiferromagnetic and ferromagnetic interactions among Cu2+, Mn4+, and Ir4+ ions give rise to spin glass behavior, which follows a conventional dynamical slowing down model.

cond-mat.mtrl-sci

Evidence for pressure-induced node-pair annihilation in Cd3As2

As an intermediate state in the topological phase diagram, Dirac semimetals are of particular interest as a platform for studying topological phase transitions under external modulations. Despite a growing theoretical interest in this topic, it remains a substantial challenge to experimentally tune the system across topological phase transitions. Here, we investigate the Fermi surface evolution of Cd3As2 under high pressure through magnetotransport. A sudden change in Berry phase occurs at 1.3 GPa along with the unanticipated shrinkage of the Fermi surface, which occurs well below the structure transition point (~2.5 GPa). High pressure X-ray diffraction also reveals an anisotropic compression of the Cd3As2 lattice around a similar pressure. Corroborated by the first-principles calculations we show that an axial compression will shift the Dirac nodes towards the Brillouin zone center and eventually introduces a finite energy gap. The ability to tune the node position, a vital parameter of Dirac semimetals, can have dramatic impacts on the corresponding topological properties such as the Fermi arc surface states and the chiral anomaly. Our study demonstrates axial compression as an efficient approach for manipulating the band topology and exploring the critical phenomena near the topological phase transition in Cd3As2.

cond-mat.mtrl-sci