Showing 1–50 of 84 results for author: Xiao, Q

Tunable Multistage Refrigeration via Geometrically Frustrated Triangular Lattice Antiferromagnet for Space Cooling

Authors: Jianqiao Wang, Chushu Fang, Zhibin Qiu, Yang Zhao, Quan Xiao, Xiying Sun, Zhaoyi Li, Laifeng Li, Yuan Zhou, Changzhao Pan, Shu Guo

Abstract: Low-temperature refrigeration technology constitutes a crucial component in space exploration. The small-scale, low-vibration Stirling-type pulse tube refrigerators hold significant application potential for space cooling. However, the efficient operation of current Stirling-type pulse tube cryocoolers in space cooling applications remains challenging due to the rapid decay of the heat capacity of… ▽ More Low-temperature refrigeration technology constitutes a crucial component in space exploration. The small-scale, low-vibration Stirling-type pulse tube refrigerators hold significant application potential for space cooling. However, the efficient operation of current Stirling-type pulse tube cryocoolers in space cooling applications remains challenging due to the rapid decay of the heat capacity of regenerative materials below 10 K. This study adopts a novel material strategy: using a novel high-spin S = 7/2 magnetic regenerative material, Gd2O2Se, we construct a multistage tunable regenerative material structure to achieve an efficient cooling approach to the liquid helium temperature range. Under substantial geometric frustration from a double-layered triangular lattice, it exhibits two-step specific heat transition peaks at 6.22 K and 2.11 K, respectively. Its ultrahigh specific heat and broad two-step transition temperature range effectively bridge the gap between commercially used high-heat-capacity materials. Experimental verification shows that when Gd2O2Se is combined with Er3Ni and HoCu2 in the Stirling-type pulse tube cryocooler, the cooling efficiency of the pulse tube increases by 66.5 % at 7 K, and the minimum achievable temperature reaches 5.85 K. These results indicate that Gd2O2Se is an ideal magnetic regenerative material for space cooling △ Less

Submitted 5 November, 2025; originally announced November 2025.

CoNi-MOF laccase-like nanozymes prepared by dielectric barrier discharge plasma for treatment of antibiotic pollution

Authors: Chao Liu, Yi Cao, Qi Xia, Amil Aligayev, Qing Huang

Abstract: Laccase is a natural green catalyst and utilized in pollution treatment. Nevertheless, its practical application is constrained by limitations including high cost, poor stability, and difficulties in recovery. Herein, with inspiration from catalytic mechanism of natural laccase, we designed and prepared a bimetallic metal-organic framework, namely, CoNi-MOF, using low-temperature plasma (LTP) tech… ▽ More Laccase is a natural green catalyst and utilized in pollution treatment. Nevertheless, its practical application is constrained by limitations including high cost, poor stability, and difficulties in recovery. Herein, with inspiration from catalytic mechanism of natural laccase, we designed and prepared a bimetallic metal-organic framework, namely, CoNi-MOF, using low-temperature plasma (LTP) technology. We employed dielectric barrier discharge (DBD) plasma to prepare CoNi-MOF, and by precisely modulating the N2/O2 gas ratio, we could modulate the distribution concentration of oxygen vacancies in CoNi-MOF. Experimental investigations and density functional theory (DFT) calculations elucidated that the critical role of the oxygen vacancies in enhancing the laccase-like activity, which promoted the activation of molecular oxygen (O2) for generation of reactive oxygen species (ROS). Compared to natural laccase, CoNi-MOF exhibited superior catalytic performance in the degradation of antibiotic tetracycline (TC), along with enhanced resistance to harsh environmental conditions, improved stability, and low biotoxicity. Notably, aeration increased the dissolved oxygen (DO) content, further improving the TC degradation efficiency. As such, this study not only proposes a facile and efficient low-temperature plasma technology for synthesizing high-performance laccase-like nanozymes but also provides a promising and environmentally friendly strategy for the remediation of antibiotic contamination in the environment. △ Less

Submitted 17 October, 2025; originally announced October 2025.

Distinct orbital contributions to electronic and magnetic structures in La$_{4}$Ni$_{3}$O$_{10}$

Authors: Shilong Zhang, Hengyuang Zhang, Zehao Dong, Jie Li, Qian Xiao, Mengwu Huo, Hsiao-Yu Huang, Di-Jing Huang, Yayu Wang, Yi Lu, Zhen Chen, Meng Wang, Yingying Peng

Abstract: High-T$_c$ superconductivity has recently been discovered in Ruddlesden-Popper phase nickelates under pressure, where the low-energy electronic structure is dominated by Ni $d_{x^2 - y^2}$ and $d_{z^2}$ orbitals. However, the respective roles of these orbitals in superconductivity remain unclear. Here, by combining X-ray absorption, electron energy loss spectroscopy, and density functional theory… ▽ More High-T$_c$ superconductivity has recently been discovered in Ruddlesden-Popper phase nickelates under pressure, where the low-energy electronic structure is dominated by Ni $d_{x^2 - y^2}$ and $d_{z^2}$ orbitals. However, the respective roles of these orbitals in superconductivity remain unclear. Here, by combining X-ray absorption, electron energy loss spectroscopy, and density functional theory calculations on La$_{4}$Ni$_{3}$O$_{10}$ single crystals, we identify ligand holes in the $p_{x,y}$ orbitals of planar oxygen and the $p_z$ orbitals of apical oxygen, which hybridize with the Ni $d_{x^2-y^2}$ and $d_{z^2}$ orbitals, respectively. These ligand holes enable orbital-selective O K-edge resonant inelastic X-ray scattering (RIXS) study, which reveals that $d_{x^2-y^2}$ states dominate the low-energy charge excitations and are more itinerant. We also observe a $\sim$0.1 eV bimagnon through RIXS and Raman spectroscopy, which leads to an interlayer superexchange interaction J$_z$ of $\sim$50 meV. Our results reveal distinct contributions of Ni $d_{x^2-y^2}$ and $d_{z^2}$ orbitals to the electronic and magnetic structure and provide direct experimental insights to understand the RP-phase nickelate superconductors. △ Less

Submitted 25 September, 2025; originally announced September 2025.

Probing Magnetic Properties of RuO$_{2}$ Heterostructures Through the Ferromagnetic Layer

Authors: Frank M. Abel, Subhash Bhatt, Shelby S. Fields, Vinay Sharma, Dai Q. Ho, Daniel Wines, D. Quang To, Joseph C. Prestigiacomo, Tehseen Adel, Riccardo Torsi, Maria F. Munoz, David T. Plouff, Xinhao Wang, Brian Donovan, Don Heiman, Gregory M. Stephen, Adam L. Friedman, Garnett W. Bryant, Anderson Janotti, Michelle E. Jamer, Angela R. Hight Walker, John Q. Xiao, Steven P. Bennett

Abstract: RuO$_{2}$ has been proposed as the prototypical altermagnetic material. However, several reports have recently questioned its intrinsic magnetic ordering, leading to conflicting findings, especially in thin film heterostructures pointing to possible interface effects being convoluted with supposed antiferromagnetic/altermagnetic signatures. Here, extensive magnetometry measurements were performed… ▽ More RuO$_{2}$ has been proposed as the prototypical altermagnetic material. However, several reports have recently questioned its intrinsic magnetic ordering, leading to conflicting findings, especially in thin film heterostructures pointing to possible interface effects being convoluted with supposed antiferromagnetic/altermagnetic signatures. Here, extensive magnetometry measurements were performed on two independently grown thin film heterostructures of RuO$_{2}$ interfaced with either NiFe or Fe acting as the ferromagnetic layer. Below about 15 K, both samples exhibit exchange bias fields when cooled to approximately 2 K in a $+$1 T field, and a spin transitional feature is observed around 31 K. Magneto-Raman measurements on RuO$_{2}$ thin films only reveal a magnon mode when there is a NiFe layer, suggesting that RuO$_{2}$ does not intrinsically possess long range magnetic ordering.. When in contact with a ferromagnet, RuO$_2$ displays effects that could be ascribed to antiferromagnetism. However, the lack of intrinsic magnon modes points toward possible diffusion between the layers or spin disorder at the interface as seen by density functional theory (DFT) calculations. △ Less

Submitted 20 August, 2025; originally announced August 2025.

Mixed spin states for robust ferromagnetism in strained SrCoO$_3$ thin films

Authors: Xiquan Zheng, Nicholas B. Brookes, Flora Yakhou-Harris, Yingjie Lyu, Jianbing Zhang, Qian Xiao, Xinyi Jiang, Qingzheng Qiu, Qizhi Li, Shilong Zhang, Xinqiang Cai, Pu Yu, Yi Lu, Yingying Peng

Abstract: Epitaxial strain in transition-metal oxides can induce dramatic changes in electronic and magnetic properties. A recent study on the epitaxially strained SrCoO$_3$ thin films revealed persistent ferromagnetism even across a metal-insulator transition. This challenges the current theoretical predictions, and the nature of the local spin state underlying this robustness remains unresolved. Here, we… ▽ More Epitaxial strain in transition-metal oxides can induce dramatic changes in electronic and magnetic properties. A recent study on the epitaxially strained SrCoO$_3$ thin films revealed persistent ferromagnetism even across a metal-insulator transition. This challenges the current theoretical predictions, and the nature of the local spin state underlying this robustness remains unresolved. Here, we employ high-resolution resonant inelastic x-ray scattering (RIXS) at the Co-$L_3$ edge to probe the spin states of strained SrCoO$_3$ thin films. Compared with CoO$_6$ cluster multiplet calculations, we identify a ground state composed of a mixed high- and low-spin configuration, distinct from the previously proposed intermediate-spin state. Our results demonstrate that the robustness of ferromagnetism arises from the interplay between this mixed spin state and the presence of ligand holes associated with negative charge transfer. These findings provide direct experimental evidence for a nontrivial magnetic ground state in SrCoO$_3$ and offer new pathways for designing robust ferromagnetic systems in correlated oxides. △ Less

Submitted 2 August, 2025; originally announced August 2025.

Comments: 6 pages, 4 figures

Nature of nonanalytic chemical short-range order in metallic alloys

Authors: Hao Deng, Jue-Yi Qi, Qin-Han Xia, Jinshan Li, Xie Zhang

Abstract: Nonanalytic chemical short-range order (SRO) has long been observed in diffuse scattering experiments for metallic alloys. However, considerable debate surrounds the validity of these observations due to the unresolved nature of the nonanalyticity. Using prototypical face-centered cubic alloys as an example, here we demonstrate that SRO in metallic alloys is mostly nonanalytic at Γ. The nonanalyti… ▽ More Nonanalytic chemical short-range order (SRO) has long been observed in diffuse scattering experiments for metallic alloys. However, considerable debate surrounds the validity of these observations due to the unresolved nature of the nonanalyticity. Using prototypical face-centered cubic alloys as an example, here we demonstrate that SRO in metallic alloys is mostly nonanalytic at Γ. The nonanalyticity stems from the elastic anisotropy and long-range atomic interactions of the \emph{host} lattice. The physical insights substantially improve our understanding of chemical order in alloys and resolves the long-standing debate in the field. Nonanalytic SRO is expected to be general in alloys and the nonanalyticity may serve as a unique feature to verify the intensely debated existence of SRO in compositionally complex alloys. △ Less

Submitted 5 June, 2025; originally announced June 2025.

Comments: 6 pages, 4 figures, submitted to PRL

Ultrafast Laser Induces Macroscopic Symmetry-Breaking of Diamond Color Centers

Authors: Yang Gao, Qi-Zheng Ji, Chao-Bo Liu, Qi Xiao, Chao Lian

Abstract: We employ real-time time-dependent density functional theory (RT-TDDFT) to investigate the electron-phonon-spin correlated dynamics in negatively charged nitrogen-vacancy centers (NV$^{-}$) and construct a comprehensive dynamical picture. Laser excitation promotes minority-spin electrons within 100~fs, establishing a three-fold rotation symmetry breaking (3RSB) charge ordering. Subsequently, ionic… ▽ More We employ real-time time-dependent density functional theory (RT-TDDFT) to investigate the electron-phonon-spin correlated dynamics in negatively charged nitrogen-vacancy centers (NV$^{-}$) and construct a comprehensive dynamical picture. Laser excitation promotes minority-spin electrons within 100~fs, establishing a three-fold rotation symmetry breaking (3RSB) charge ordering. Subsequently, ionic motion on the potential energy surface of the excited electrons generates two distinct dynamical modes: (1) symmetric oscillations of carbon-nitrogen bonds and (2) dynamic Jahn-Teller distortions (DJT) with 3RSB. These distortions induce nonlocal coherent phonons in the diamond lattice, which propagate with 3RSB at the sound velocity ($\sim$2~Å/fs). Furthermore, the NV$^{-}$ spin state remains preserved during photoexcitation but undergoes rapid reorientation within 100~fs via enhanced spin-orbit-phonon coupling. Our RT-TDDFT simulations provide direct time-resolved visualization of these processes, offering novel insights into the microscopic interplay of electrons, phonons, and spins in NV$^{-}$ centers. These results advance the fundamental understanding of dynamical mechanisms in solid-state quantum systems, with implications for optimizing NV$^{-}$-based quantum sensing technologies. △ Less

Submitted 19 May, 2025; originally announced May 2025.

Time-Reversal Symmetry Protected Transport at Correlated Oxide Interfaces

Authors: Mengke Ha, Qing Xiao, Zhiyuan Qin, Dawei Qiu, Longbing Shang, Xinyi Liu, Pu Yan, Changjian Ma, Danqing Liu, Chengyuan Huang, Zhenlan Chen, Haoyuan Wang, Chang-Kui Duan, Zhaoliang Liao, Wei-Tao Liu, Yang Gao, Kecheng Cao, Jiangfeng Du, Guanglei Cheng

Abstract: Time-reversal symmetry (TRS) protection is core to topological physics, yet its role in correlated oxides-typically non-topological-remains underexplored. This limit hampers the potential in engineering exotic quantum states by fusing TRS protection and the rich emergent phenomena in the oxide platform. Here, we report evidence of a TRS-protected subband at oxygen vacancy-free LaAlO3/SrTiO3 interf… ▽ More Time-reversal symmetry (TRS) protection is core to topological physics, yet its role in correlated oxides-typically non-topological-remains underexplored. This limit hampers the potential in engineering exotic quantum states by fusing TRS protection and the rich emergent phenomena in the oxide platform. Here, we report evidence of a TRS-protected subband at oxygen vacancy-free LaAlO3/SrTiO3 interfaces. This subband causes a low-field quantum oscillation with anomalous characters: exceptionally light electron mass, aperiodicity, and susceptibility to magnetic fields. All findings align with a Rashba model in which TRS-protected transport occurs along quasi-1D ferroelastic domain walls, which possess a Dirac band topology and a giant Rashba spin-orbit coupling, two orders stronger than the 2D interface. Our results deepen the understanding of SrTiO3-based electron systems, unveiling an appealing new platform for quantum engineering. △ Less

Submitted 4 May, 2025; originally announced May 2025.

Dominant apical-oxygen electron-phonon coupling in HgBa$_2$Ca$_2$Cu$_3$O$_{8+δ}$

Authors: Wenshan Hong, Qizhi Li, Shilong Zhang, Qian Xiao, Sahil Tippireddy, Jie Li, Yuchen Gu, Shichi Dong, Taimin Miao, Xiangyu Luo, Xianghong Jin, Lin Zhao, Xingjiang Zhou, Ke-Jin Zhou, Yi Lu, Yingying Peng, Yuan Li

Abstract: How electron-phonon interactions influence high-temperature superconductivity in cuprates remains contested, and their role outside the CuO$_2$ planes has been largely overlooked. The most conspicuous evidence for such coupling is the ubiquitous 70-meV dispersion kink seen by photoemission, yet its microscopic origin is still debated. Here we use oxygen-$K$-edge resonant inelastic X-ray scattering… ▽ More How electron-phonon interactions influence high-temperature superconductivity in cuprates remains contested, and their role outside the CuO$_2$ planes has been largely overlooked. The most conspicuous evidence for such coupling is the ubiquitous 70-meV dispersion kink seen by photoemission, yet its microscopic origin is still debated. Here we use oxygen-$K$-edge resonant inelastic X-ray scattering (RIXS) to probe the trilayer cuprate HgBa$_2$Ca$_2$Cu$_3$O$_{8+δ}$ (Hg1223). When both incident photon energy and polarization are tuned to the apical-oxygen $1s\!\rightarrow\!2p_z$ transition, the RIXS spectra exhibit a ladder of at least ten phonon overtones, evenly spaced by 70 meV, whose intensities follow a Franck-Condon envelope, signalling exceptionally strong electron-phonon coupling. Quantitative modelling that incorporates core-hole lifetime evaluation yields an apical-phonon coupling energy of 0.25(1) eV, significantly larger than that of the planar stretching mode. Such a coupling strength offers a strong contender for explaining the universal 70-meV kink and suggests that the dominant electron-phonon channel resides outside the CuO$_2$ planes. By elevating inter-layer lattice dynamics from a peripheral factor to a central actor, our results provide a fresh starting point for theories seeking to reconcile strong correlations, lattice dynamics and high-temperature superconductivity. △ Less

Submitted 30 April, 2025; originally announced May 2025.

Comments: 33 pages, 15 figures; comments are welcome

Interaction of Shear Horizontal Acoustic and Plasma Waves in Hexagonal Piezoelectric Semiconductors

Authors: Qingguo Xia, Jianke Dua, Jiashi Yangb

Abstract: We study coupled acoustic and plasma waves in piezoelectric semiconductor crystals of hexagonal symmetry. We focus on the so called shear-horizontal or antiplane motions with one mechanical displacement. A set of two dimensional equations is reduced from the three-dimensional equations. Since the material is effectively isotropic in the two dimensional plane under consideration, the equations are… ▽ More We study coupled acoustic and plasma waves in piezoelectric semiconductor crystals of hexagonal symmetry. We focus on the so called shear-horizontal or antiplane motions with one mechanical displacement. A set of two dimensional equations is reduced from the three-dimensional equations. Since the material is effectively isotropic in the two dimensional plane under consideration, the equations are relatively simple. Dispersion curves of coupled elastic and acoustic waves are obtained analytically and examined numerically along with the effects of some parameters. △ Less

Submitted 10 February, 2025; originally announced February 2025.

Photo-induced Dynamics and Momentum Distribution of Chiral Charge Density Waves in 1T-TiSe$_{2}$

Authors: Qingzheng Qiu, Sae Hwan Chun, Jaeku Park, Dogeun Jang, Li Yue, Yeongkwan Kim, Yeojin Ahn, Mingi Jho, Kimoon Han, Xinyi Jiang, Qian Xiao, Tao Dong, Jia-Yi Ji, Nanlin Wang, Jeroen van den Brink, Jasper van Wezel, Yingying Peng

Abstract: Exploring the photoinduced dynamics of chiral states offers promising avenues for advanced control of condensed matter systems. Photoinduced or photoenhanced chirality in 1T-TiSe$_{2}$ has been suggested as a fascinating platform for optical manipulation of chiral states. However, the mechanisms underlying chirality training and its interplay with the charge density wave (CDW) phase remain elusive… ▽ More Exploring the photoinduced dynamics of chiral states offers promising avenues for advanced control of condensed matter systems. Photoinduced or photoenhanced chirality in 1T-TiSe$_{2}$ has been suggested as a fascinating platform for optical manipulation of chiral states. However, the mechanisms underlying chirality training and its interplay with the charge density wave (CDW) phase remain elusive. Here, we use time-resolved X-ray diffraction (tr-XRD) with circularly polarized pump lasers to probe the photoinduced dynamics of chirality in 1T-TiSe$_{2}$. We observe a notable ($\sim$20%) difference in CDW intensity suppression between left- and right-circularly polarized pumps. Additionally, we reveal momentum-resolved circular dichroism arising from domains of different chirality, providing a direct link between CDW and chirality. An immediate increase in CDW correlation length upon laser pumping is detected, suggesting the photoinduced expansion of chiral domains. These results both advance the potential of light-driven chirality by elucidating the mechanism driving chirality manipulation in TiSe$_2$, and they demonstrate that tr-XRD with circularly polarized pumps is an effective tool for chirality detection in condensed matter systems. △ Less

Submitted 4 February, 2025; originally announced February 2025.

Comments: 6 pages, 4 figures

Journal ref: Phys. Rev. Lett. 135, 116904 (2025)

Revisiting altermagnetism in RuO2: a study of laser-pulse induced charge dynamics by time-domain terahertz spectroscopy

Authors: David T. Plouff, Laura Scheuer, Shreya Shrestha, Weipeng Wu, Nawsher J. Parvez, Subhash Bhatt, Xinhao Wang, Lars Gundlach, M. Benjamin Jungfleisch, John Q. Xiao

Abstract: Altermagnets are a recently discovered class of magnetic material with great potential for applications in the field of spintronics, owing to their non-relativistic spin-splitting and simultaneous antiferromagnetic order. One of the most studied candidates for altermagnetic materials is rutile structured RuO2. However, it has recently come under significant scrutiny as evidence emerged for its lac… ▽ More Altermagnets are a recently discovered class of magnetic material with great potential for applications in the field of spintronics, owing to their non-relativistic spin-splitting and simultaneous antiferromagnetic order. One of the most studied candidates for altermagnetic materials is rutile structured RuO2. However, it has recently come under significant scrutiny as evidence emerged for its lack of any magnetic order. In this work, we study bilayers of epitaxial RuO2 and ferromagnetic permalloy (Fe19Ni81) by time-domain terahertz spectroscopy, probing for three possible mechanisms of laser-induced charge dynamics: the inverse spin Hall effect (ISHE), electrical anisotropic conductivity (EAC), and inverse altermagnetic spin-splitting effect (IASSE). We examine films of four common RuO2 layer orientations: (001), (100), (110), and (101). If RuO2 is altermagnetic, then the (100) and (101) oriented samples are expected to produce anisotropic emission from the IASSE, however, our results do not indicate the presence of IASSE for either as-deposited or field annealed samples. The THz emission from all samples is instead consistent with charge dynamics induced by only the relativistic ISHE and the non-relativistic and non-magnetic EAC, casting further doubt on the existence of altermagnetism in RuO2. In addition, we find that in the (101) oriented RuO2 sample, the combination of ISHE and EAC emission mechanisms produces THz emission which is tunable between linear and elliptical polarization by modulation of the external magnetic field. △ Less

Submitted 15 December, 2024; originally announced December 2024.

Effect of Ti-doping on the dimer transition in Lithium Ruthenate

Authors: Sheetal Jain, Zhengbang Zhou, Ezekiel Horsley, Christopher J. S. Heath, Mohsen Shakouri, Qunfeng Xiao, Ning Chen, Weifeng Chen, Graham King, Young-June Kim

Abstract: We carried out a comprehensive crystal structure characterization of Ti-doped lithium ruthenate (Li$_2$Ti$_x$Ru$_{1-x}$O$_3$), to investigate the effect of Ti-doping on the structural phase transition. Experimental tools sensitive to the average structure (X-ray diffraction), as well as those sensitive to local structure (Extended X-ray Absorption Fine Structure, EXAFS; pair distribution function,… ▽ More We carried out a comprehensive crystal structure characterization of Ti-doped lithium ruthenate (Li$_2$Ti$_x$Ru$_{1-x}$O$_3$), to investigate the effect of Ti-doping on the structural phase transition. Experimental tools sensitive to the average structure (X-ray diffraction), as well as those sensitive to local structure (Extended X-ray Absorption Fine Structure, EXAFS; pair distribution function, PDF) are used. We observed non-monotonic dependence of the structural transition temperature on the Ti-doping level. At low doping, the transition temperature slightly increases with doping, while at high doping, the temperature decreases significantly with doping. We note two important observations from our studies. First, Ti K-edge EXAFS data shows persistent Ti-Ru dimerization even with substantial Ti doping. Second, we were able to use the PDF data to estimate the dimer correlation length above the transition temperature, which would correspond to the size of the proposed local `dimer clusters' formed by Ru-Ru and Ti-Ru neighbours. The dimer correlation length is found to be around 10~Å, which remains robust regardless of doping. Our study therefore suggests that Ti$^{4+}$ with its $d^0$ electronic configuration is a special type of dopant when replacing Ru. △ Less

Submitted 15 October, 2024; originally announced October 2024.

Comments: 12 pages, 11 figures

Deciphering the origin of spin current in spintronic terahertz emitters and its imprint on their electromagnetic radiation via time-dependent density functional theory

Authors: Ali Kefayati, Yafei Ren, M. Benjamin Jungfleisch, Lars Gundlach, John Q. Xiao, Branislav K. Nikolic

Abstract: Spin current flowing between femtosecond laser pulse (fsLP)-driven ferromagnetic metal and adjacent normal metal (NM) hosting strong spin-orbit coupling is invariably invoked to explain terahertz (THz) radiation believed to be emitted solely by NM layer. Despite being such a central concept, the microscopic origin of interlayer spin current remains vague. Here, we employ recently developed [A. Kef… ▽ More Spin current flowing between femtosecond laser pulse (fsLP)-driven ferromagnetic metal and adjacent normal metal (NM) hosting strong spin-orbit coupling is invariably invoked to explain terahertz (THz) radiation believed to be emitted solely by NM layer. Despite being such a central concept, the microscopic origin of interlayer spin current remains vague. Here, we employ recently developed [A. Kefayati {\em et al.}, Phys. Rev. Lett. {\bf 133}, 136704 (2024)] time-dependent density functional theory plus Jefimenko equations approach to extract spin current between Co and NM=Pt or NM=W layer where Co is driven by fsLP responsible for its demagnetization, i.e., shrinking of its magnetization vector, $M^y(t)/M^y(t=0)<1$. By comparing time dependence of spin current with those of other relevant quantities, we find that: ({\em i}) spin current is generated by demagnetization dynamics because it {\em follows} closely $dM^y/dt$, thus it is an example of quantum pumping phenomenon that cannot be captured by phenomenological notions (such as ``spin voltage'') and related semiclassical transport theories; ({\em ii}) time dependence of pumped spin current {\em does not follow} closely that of charge current emerging within NM layer via spin-to-charge conversion mechanisms; ({\em iii}) THz emission can be governed by {\em both} charge current (i.e., its time derivative entering the Jefimenko equations) within Co layer or NM layer, but in different times frames. We also unravel a special case of NM=W where spin-to-charge conversion by the inverse spin Hall effect and its contribution to THz emission is suppressed, despite large spin Hall angle of W, because of localization of excited electrons onto the outer unfilled $d$-orbitals of W. △ Less

Submitted 27 February, 2025; v1 submitted 9 October, 2024; originally announced October 2024.

Comments: 9 pages, 3 figures, 90 references

Journal ref: Phys. Rev. B 111, L140415 (2025)

Broken intrinsic symmetry induced magnon-magnon coupling in synthetic ferrimagnets

Authors: Mohammad Tomal Hossain, Hang Chen, Subhash Bhatt, Mojtaba Taghipour Kaffash, John Q. Xiao, Joseph Sklenar, M. Benjamin Jungfleisch

Abstract: Synthetic antiferromagnets offer rich magnon energy spectra in which optical and acoustic magnon branches can hybridize. Here, we demonstrate a broken intrinsic symmetry induced coupling of acoustic and optical magnons in a synthetic ferrimagnet consisting of two dissimilar antiferromagnetically interacting ferromagnetic metals. Two distinct magnon modes hybridize at degeneracy points, as indicate… ▽ More Synthetic antiferromagnets offer rich magnon energy spectra in which optical and acoustic magnon branches can hybridize. Here, we demonstrate a broken intrinsic symmetry induced coupling of acoustic and optical magnons in a synthetic ferrimagnet consisting of two dissimilar antiferromagnetically interacting ferromagnetic metals. Two distinct magnon modes hybridize at degeneracy points, as indicated by an avoided level-crossing. The avoided level-crossing gap depends on the interlayer exchange interaction between the magnetic layers, which can be controlled by adjusting the non-magnetic interlayer thickness. An exceptionally large avoided level crossing gap of 6 GHz is revealed, exceeding the coupling strength that is typically found in other magnonic hybrid systems based on a coupling of magnons with photons or magnons and phonons. △ Less

Submitted 8 October, 2024; originally announced October 2024.

Electric polarization induced by magnons and magnon Nernst effects

Authors: D. Quang To, Federico Garcia-Gaitan, Yafei Ren, Joshua M. O. Zide, John Q. Xiao, Branislav K. Nikolić, Garnett W. Bryant, Matthew F. Doty

Abstract: Magnons offer a promising path toward energy-efficient information transmission and the development of next-generation classical and quantum computing technologies. However, methods to efficiently excite, manipulate, and detect magnons remain a critical need. Here, we show that magnons, despite their charge-neutrality, can induce electric polarization as a result of both their spin and orbital mom… ▽ More Magnons offer a promising path toward energy-efficient information transmission and the development of next-generation classical and quantum computing technologies. However, methods to efficiently excite, manipulate, and detect magnons remain a critical need. Here, we show that magnons, despite their charge-neutrality, can induce electric polarization as a result of both their spin and orbital moments. We demonstrate this by calculating the electric polarization induced by magnons in two-dimensional (2D) honeycomb antiferromagnets. The electric polarization becomes finite when the Dzyaloshinskii-Moriya Interaction (DMI) is present and its magnitude can be increased by symmetries of the system. We illustrate this by computing and comparing the electric polarizations induced by the magnon Nernst effects in 2D materials with Néel and Zigzag ordering. Our findings show that in the Zigzag order, where the effect is dominated by the magnon orbital moment, the induced electric polarization is approximately three orders of magnitude greater than in the Néel phase. These findings reveal that electric fields could enable both detection and manipulation of magnons under certain conditions by leveraging their spin and orbital angular moment. They also suggest that the discovery or engineering of materials with substantial magnon orbital moments could lead to more practical use of magnons for future computing and information transmission device applications. △ Less

Submitted 13 December, 2024; v1 submitted 22 July, 2024; originally announced July 2024.

Journal ref: PNAS, 2025

Charge and spin current pumping by ultrafast demagnetization dynamics

Authors: Jalil Varela-Manjarres, Ali Kefayati, M. Benjamin Jungfleisch, John Q. Xiao, Branislav K. Nikolic

Abstract: The surprising discovery of ultrafast demagnetization -- where electric field of femtosecond laser pulse couples to electrons of a ferromagnetic (FM) layer causing its magnetization vector {\em to shrink while not rotating}, is also assumed to be accompanied by generation of spin current in the direction orthogonal to electric field. However, understanding of the microscopic origin of such spin cu… ▽ More The surprising discovery of ultrafast demagnetization -- where electric field of femtosecond laser pulse couples to electrons of a ferromagnetic (FM) layer causing its magnetization vector {\em to shrink while not rotating}, is also assumed to be accompanied by generation of spin current in the direction orthogonal to electric field. However, understanding of the microscopic origin of such spin current and how efficiently it can be converted into charge current, as the putative source of THz radiation, is lacking despite nearly three decades of intense studies. Here we connect the standard pumping phenomena driven by microwave precession of magnetization vector replacing periodic time-dependence of magnetization precession with nonperiodic time-dependence of demagnetization, as obtained from experiments on ultrafast-light-driven Ni layer. Applying time-dependent nonequilibrium Green's functions, able to evolve such setup with arbitrary time dependence, reveals how demagnetization dynamics pumps both charge and spin currents in directions both parallel and orthogonal to electric field of laser pulse, even in the absence of spin-orbit coupling and thereby induced spin-to-charge conversion mechanisms. Although pumped currents follow $dM_z/dt$ in some setups, this becomes obscured when NM layers are disconnected and pumped currents start to reflect from FM boundaries (as is the case of experimental setups). Finally, we use the Jefimenko equations to compute electromagnetic radiation by charge current pumped in disconnected setup during demagnetization, or later during its slow recovery, unraveling that radiated electric field only in the former time interval exhibits features in 0.1--30 THz frequency range probed experimentally or explored for applications of spintronic THz emitters. △ Less

Submitted 27 August, 2024; v1 submitted 31 March, 2024; originally announced April 2024.

Comments: 8 pages, 4 figures; Supplemental Material with two additional figure is available from https://wiki.physics.udel.edu/qttg/Publications ; Highlighlight at physics.aps.org is available from https://physics.aps.org/articles/v17/s97

Journal ref: Phys. Rev. B 110, L060410 (2024)

Diamond Micro-Chip for Quantum Microscopy

Authors: Shahidul Asif, Hang Chen, Johannes Cremer, Shantam Ravan, Jeyson Tamara-Isaza, Saurabh Lamsal, Reza Ebadi, Yan Li, Ling-Jie Zhou, Cui-Zu Chang, John Q. Xiao, Amir Yacoby, Ronald L. Walsworth, Mark J. H. Ku

Abstract: The nitrogen vacancy (NV) center in diamond is an increasingly popular quantum sensor for microscopy of electrical current, magnetization, and spins. However, efficient NV-sample integration with a robust, high-quality interface remains an outstanding challenge to realize scalable, high-throughput microscopy. In this work, we characterize a diamond micro-chip (DMC) containing a (111)-oriented NV e… ▽ More The nitrogen vacancy (NV) center in diamond is an increasingly popular quantum sensor for microscopy of electrical current, magnetization, and spins. However, efficient NV-sample integration with a robust, high-quality interface remains an outstanding challenge to realize scalable, high-throughput microscopy. In this work, we characterize a diamond micro-chip (DMC) containing a (111)-oriented NV ensemble; and demonstrate its utility for high-resolution quantum microscopy. We perform strain imaging of the DMC and find minimal detrimental strain variation across a field-of-view of tens of micrometer. We find good ensemble NV spin coherence and optical properties in the DMC, suitable for sensitive magnetometry. We then use the DMC to demonstrate wide-field microscopy of electrical current, and show that diffraction-limited quantum microscopy can be achieved. We also demonstrate the deterministic transfer of DMCs with multiple materials of interest for next-generation electronics and spintronics. Lastly, we develop a polymer-based technique for DMC placement. This work establishes the DMC's potential to expand the application of NV quantum microscopy in materials, device, geological, biomedical, and chemical sciences. △ Less

Submitted 15 March, 2024; originally announced March 2024.

Comments: Includes supplementary materials section

Magnon spectrum of altermagnets beyond linear spin wave theory: Magnon-magnon interactions via time-dependent matrix product states vs. atomistic spin dynamics

Authors: Federico Garcia-Gaitan, Ali Kefayati, John Q. Xiao, Branislav K. Nikolic

Abstract: The energy-momentum dispersion of magnons, as collective low-energy excitations of magnetic material, is computed from an effective quantum spin Hamiltonian but simplified via linearized Holstein-Primakoff transformations to describe noninteracting magnons. The dispersion produced by such linear spin wave theory (LSWT) is then plotted as ``sharp bands'' of infinitely long-lived quasiparticles. How… ▽ More The energy-momentum dispersion of magnons, as collective low-energy excitations of magnetic material, is computed from an effective quantum spin Hamiltonian but simplified via linearized Holstein-Primakoff transformations to describe noninteracting magnons. The dispersion produced by such linear spin wave theory (LSWT) is then plotted as ``sharp bands'' of infinitely long-lived quasiparticles. However, magnons are prone to many-body interactions with other quasiparticles -- such as electrons, phonons or other magnons -- which can lead to shifting (i.e., band renormalization) and broadening of ``sharp bands'' as the signature of finite quasiparticle lifetime. The magnon-magnon interactions can be particularly important in antiferromagnets (AFs), and, therefore, possibly in newly classified altermagnets sharing many features of collinear AFs. Here, we employ nonperturbative quantum many-body calculations, via time-dependent matrix product states (TDMPS), to obtain magnon spectral function for RuO$_2$ altermagnet whose effective quantum spin Hamiltonian is put onto 4-leg cylinder. Its upper band is shifted away from upper ``sharp band'' of LSWT, as well as broadened, which is explained as the consequence of {\em hybridization} of the latter with three-magnon continuum. This implies that two-magnon Raman scattering spectra {\em cannot} be computed from LSWT bands, which offers a litmus test for the relevance of magnon-magnon interactions. Finally, we employ atomistic spin dynamics (ASD) simulations, based on classical Landau-Lifshitz-Gilbert (LLG) equation, to obtain magnon spectrum at finite temperature and/or at a fraction of the cost of TDMPS calculations. Despite including magnon-magnon interactions via nonlinearity of LLG equation, ASD simulations {\em cannot} match the TDMPS-computed magnon spectrum, thereby signaling {\em nonclassical} effects harbored by AFs and altermagnets. △ Less

Submitted 21 January, 2025; v1 submitted 29 February, 2024; originally announced February 2024.

Comments: 8 pages, 2 figures, 82 references; Supplemental Material is available from https://wiki.physics.udel.edu/qttg/Publications

Journal ref: Phys. Rev. B 111, L020407 (2025)

Hybridized magnonic materials for THz frequency applications

Authors: D. -Q. To, A. Rai, J. M. O. Zide, S. Law, J. Q. Xiao, M. B. Jungfleisch, M. F. Doty

Abstract: The capability of magnons to hybridize and strongly couple with diverse excitations offers a promising avenue for realizing and controlling emergent properties that hold significant potential for applications in devices, circuits, and information processing. In this letter, we present recent theoretical and experimental developments in magnon-based hybrid systems, focusing on the combination of ma… ▽ More The capability of magnons to hybridize and strongly couple with diverse excitations offers a promising avenue for realizing and controlling emergent properties that hold significant potential for applications in devices, circuits, and information processing. In this letter, we present recent theoretical and experimental developments in magnon-based hybrid systems, focusing on the combination of magnon excitation in an antiferromagnet with other excitations, namely plasmons in a topological insulator, phonons in a 2D AFM, and photons. The existence of THz frequency magnons, plasmons, and phonons makes magnon-based hybrid systems particularly appealing for high-operating-speed devices. In this context, we explore several directions to advance magnon hybrid systems, including strong coupling between a surface plasmon and magnon polariton in a TI/AFM bilayer, a giant spin Nernst effect induced by magnon phonon coupling in 2D AFMs, and control of magnon-photon coupling using spin torque. △ Less

Submitted 27 January, 2024; v1 submitted 19 January, 2024; originally announced January 2024.

Journal ref: Appl. Phys. Lett. 2024

Anomalous size effects with fixed criticality in bistable flexible mechanical metamaterials

Authors: Zehuan Tang, Tingfeng Ma, Boyue Su, Qing Xia, Pengfei Kang, Bowei Wu

Abstract: When the structure deformation is dominated by the low-energy deformation mode, the structure hardens with the increase in the size (number of units) at small sizes. This anomalous behavior will eventually disappear with the decay length of the finite structure converging to a size-independent characteristic quantity, but the specific critical point at which the anomalous behavior disappears still… ▽ More When the structure deformation is dominated by the low-energy deformation mode, the structure hardens with the increase in the size (number of units) at small sizes. This anomalous behavior will eventually disappear with the decay length of the finite structure converging to a size-independent characteristic quantity, but the specific critical point at which the anomalous behavior disappears still cannot be accurately and concisely described. Here, under two steady states of the bistable chain, we observed anomalous size effects with constant and oscillating criticality (the proportion of inhomogeneous deformation), two criticalities exactly separate the increasing and decreasing intervals of stiffness variation. They are interrelated due to the implied symmetries between the two steady states. On the other hand, they are distinguished because of the opposite superposition modes under the two steady states. Specifically, the constant criticality corresponds to the anomalous size effect achieved by the competition mechanism, while the oscillating criticality reveals an anomalous size effect achieved by the new mechanism (cancellation mechanism). In the anomalous size effect achieved by the cancellation mechanism, the singular characteristics generated by the completely cancelled deformation make it very robust. This robustness reflects in that the anomalous effect is no longer limited to linear small deformation, but it can still be observed stably in nonlinear large deformation. Our study reinterprets the anomalous size effect at a quantitative level, and the proposed cancellation mechanism expands the possible application range of this anomalous effect. △ Less

Submitted 9 August, 2025; v1 submitted 30 December, 2023; originally announced January 2024.

Observation of giant circular dichroism induced by electronic chirality

Authors: Qian Xiao, Oleg Janson, Sonia Francoual, Qingzheng Qiu, Qizhi Li, Shilong Zhang, Wu Xie, Pablo Bereciartua, Jeroen van den Brink, Jasper van Wezel, Yingying Peng

Abstract: Chiral phases of matter, characterized by a definite handedness, abound in nature, ranging from the crystal structure of quartz to spiraling spin states in helical magnets. In $1T$-TiSe$_2$ a source of chirality has been proposed that stands apart from these classical examples as it arises from combined electronic charge and quantum orbital fluctuations. This may allow its chirality to be accessed… ▽ More Chiral phases of matter, characterized by a definite handedness, abound in nature, ranging from the crystal structure of quartz to spiraling spin states in helical magnets. In $1T$-TiSe$_2$ a source of chirality has been proposed that stands apart from these classical examples as it arises from combined electronic charge and quantum orbital fluctuations. This may allow its chirality to be accessed and manipulated without imposing either structural or magnetic handedness. However, direct bulk evidence that broken inversion symmetry and chirality are intrinsic to TiSe$_2$ remains elusive. Here, employing resonant elastic scattering of x-rays, we reveal the presence of giant circular dichroism up to $\sim$ 40$\%$ at forbidden Bragg peaks that emerge at the charge and orbital ordering transition. The dichroism varies dramatically with incident energy and azimuthal angle. Comparison to calculated scattering intensities unambiguously traces its origin to bulk chiral electronic order in ${\mathrm{TiSe}}_2$ and establishes resonant elastic x-ray scattering as a sensitive probe to electronic chirality. △ Less

Submitted 19 December, 2023; originally announced December 2023.

Comments: 6 pages, 4 figures

Journal ref: Phys. Rev. Lett. 133, 126402 (2024)

Highly Anisotropic Elastic Properties of Suspended Black Arsenic Nanoribbons

Authors: Yunfei Yu, Guoshuai Du, Shang Chen, Jingjing Zhang, Yubing Du, Qinglin Xia, Ke Jin, Yabin Chen

Abstract: Anisotropy, as an exotic degree of freedom, enables us to discover the emergent two-dimensional (2D) layered nanomaterials with low in-plane symmetry and to explore their outstanding properties and promising applications. 2D black arsenic (b-As) with puckered structure has garnered increasing attention these years owing to its extreme anisotropy with respect to the electrical, thermal, and optical… ▽ More Anisotropy, as an exotic degree of freedom, enables us to discover the emergent two-dimensional (2D) layered nanomaterials with low in-plane symmetry and to explore their outstanding properties and promising applications. 2D black arsenic (b-As) with puckered structure has garnered increasing attention these years owing to its extreme anisotropy with respect to the electrical, thermal, and optical properties. However, the investigation on mechanical properties of 2D b-As is still lacking, despite much effort on theoretical simulations. Herein, we report the highly anisotropic elastic properties of suspended b-As nanoribbons via atomic force microscope-based nanoindentation. It was found that the extracted Young's modulus of b-As nanoribbons exhibits remarkable anisotropy, which approximates to 72.2 +- 5.4 and 44.3 +- 1.4 GPa along zigzag and armchair directions, respectively. The anisotropic ratio reaches up to ~ 1.6. We expect that these results could lay a solid foundation for the potential applications of 2D anisotropic nanomaterials in the next-generation nanomechanics and optoelectronics. △ Less

Submitted 31 October, 2023; originally announced October 2023.

Comments: 17 pages, 5 figures

Experimental observation of highly anisotropic elastic properties of two-dimensional black arsenic

Authors: Jingjing Zhang, Shang Chen, Guoshuai Du, Yunfei Yu, Wuxiao Han, Qinglin Xia, Ke Jin, Yabin Chen

Abstract: Anisotropic two-dimensional layered materials with low-symmetric lattices have attracted increasing attention due to their unique orientation-dependent mechanical properties. Black arsenic (b-As), with the puckered structure, exhibits extreme in-plane anisotropy in optical, electrical and thermal properties. However, experimental research on mechanical properties of b-As is very rare, although the… ▽ More Anisotropic two-dimensional layered materials with low-symmetric lattices have attracted increasing attention due to their unique orientation-dependent mechanical properties. Black arsenic (b-As), with the puckered structure, exhibits extreme in-plane anisotropy in optical, electrical and thermal properties. However, experimental research on mechanical properties of b-As is very rare, although theoretical calculations predicted the exotic elastic properties of b-As, such as anisotropic Young's modulus and negative Poisson's ratio. Herein, experimental observations on highly anisotropic elastic properties of b-As were demonstrated using our developed in situ tensile straining setup based on the effective microelectromechanical system. The cyclic and repeatable load-displacement curves proved that Young's modulus along zigzag direction was ~1.6 times greater than that along armchair direction, while the anisotropic ratio of ultimate strain reached ~2.5, attributed to hinge structure in armchair direction. This study could provide significant insights to design novel anisotropic materials and explore their potential applications in nanomechanics and nanodevices. △ Less

Submitted 27 September, 2023; originally announced September 2023.

Comments: 19 pages, 5 figures

Thermodynamic Origins of Structural Metastability in Two-Dimensional Black Arsenic

Authors: Guoshuai Du, Feng Ke, Wuxiao Han, Bin Chen, Qinglin Xia, Jun Kang, Yabin Chen

Abstract: Two-dimensional (2D) materials have aroused considerable research interests owing to their potential applications in nanoelectronics and optoelectronics. Thermodynamic stability of 2D structures inevitably affects the performance and power consumption of the fabricated nanodevices. Black arsenic (b-As), as a cousin of black phosphorus, has presented the extremely high anisotropy in physical proper… ▽ More Two-dimensional (2D) materials have aroused considerable research interests owing to their potential applications in nanoelectronics and optoelectronics. Thermodynamic stability of 2D structures inevitably affects the performance and power consumption of the fabricated nanodevices. Black arsenic (b-As), as a cousin of black phosphorus, has presented the extremely high anisotropy in physical properties. However, the systematic research on structural stability of b-As is still lack. Herein, we demonstrated the detailed analysis on structural metastability of the natural b-As, and determined its existence conditions in terms of two essential thermodynamic variables as hydrostatic pressure and temperature. Our results confirmed that b-As can only survive below 0.7 GPa, and then irreversibly transform to gray arsenic, in consistent with our theoretical calculations. Furthermore, thermal annealing strategy was developed to precisely control the thickness of b-As flake, and it sublimates at 300 oC. These results could pave the way for 2D b-As in many promising applications. △ Less

Submitted 7 September, 2023; originally announced September 2023.

Comments: 28 pages, 4 figures

Intralayer Negative Poisson's Ratio in Two-Dimensional Black Arsenic by Strain Engineering

Authors: Jingjing Zhang, Weihan Zhang, Leining Zhang, Guoshuai Du, Yunfei Yu, Qinglin Xia, Xu Wu, Yeliang Wang, Wei Ji, Jingsi Qiao, Feng Ding, Yabin Chen

Abstract: Negative Poisson's ratio as the anomalous characteristic generally exists in artificial architectures, such as re-entrant and honeycomb structures. The structures with negative Poisson's ratio have attracted intensive attention due to their unique auxetic effect and many promising applications in shear resistant and energy absorption fields. However, experimental observation of negative Poisson's… ▽ More Negative Poisson's ratio as the anomalous characteristic generally exists in artificial architectures, such as re-entrant and honeycomb structures. The structures with negative Poisson's ratio have attracted intensive attention due to their unique auxetic effect and many promising applications in shear resistant and energy absorption fields. However, experimental observation of negative Poisson's ratio in natural materials barely happened, although various two-dimensional layered materials are predicted in theory. Herein, we report the anisotropic Raman response and the intrinsic intralayer negative Poisson's ratio of two-dimensional natural black arsenic (b-As) via strain engineering strategy. The results were evident by the detailed Raman spectrum of b-As under uniaxial strain together with density functional theory calculations. It is found that b-As was softer along the armchair than zigzag direction. The anisotropic mechanical features and van der Waals interactions play essential roles in strain-dependent Raman shifts and negative Poisson's ratio in the natural b-As along zigzag direction. This work may shed a light on the mechanical properties and potential applications of two-dimensional puckered materials. △ Less

Submitted 7 September, 2023; originally announced September 2023.

Comments: 23 pages, 4 figures

Charge redistribution, charge order and plasmon in La$_{2-x}$Sr$_{x}$CuO$_{4}$/La$_{2}$CuO$_{4}$ superlattices

Authors: Qizhi Li, Lele Ju, Hsiaoyu Huang, Yuxuan Zhang, Changwei Zou, Tianshuang Ren, A. Singh, Shilong Zhang, Qingzheng Qiu, Qian Xiao, Di-Jing Huang, Yanwu Xie, Zhen Chen, Yingying Peng

Abstract: Interfacial superconductors have the potential to revolutionize electronics, quantum computing, and fundamental physics due to their enhanced superconducting properties and ability to create new types of superconductors. The emergence of superconductivity at the interface of La$_{2-x}$Sr$_{x}$CuO$_{4}$/La$_{2}$CuO$_{4}$ (LSCO/LCO), with a T$_c$ enhancement of $\sim$ 10 K compared to the La… ▽ More Interfacial superconductors have the potential to revolutionize electronics, quantum computing, and fundamental physics due to their enhanced superconducting properties and ability to create new types of superconductors. The emergence of superconductivity at the interface of La$_{2-x}$Sr$_{x}$CuO$_{4}$/La$_{2}$CuO$_{4}$ (LSCO/LCO), with a T$_c$ enhancement of $\sim$ 10 K compared to the La$_{2-x}$Sr$_{x}$CuO$_{4}$ bulk single crystals, provides an exciting opportunity to study quantum phenomena in reduced dimensions. To investigate the carrier distribution and excitations in interfacial superconductors, we combine O K-edge resonant inelastic X-ray scattering and atomic-resolved scanning transmission electron microscopy measurements to study La$_{2-x}$Sr$_{x}$CuO$_{4}$/La$_{2}$CuO$_{4}$ superlattices (x=0.15, 0.45) and bulk La$_{1.55}$Sr$_{0.45}$CuO$_{4}$ films. We find direct evidence of charge redistribution, charge order and plasmon in LSCO/LCO superlattices. Notably, the observed behaviors of charge order and plasmon deviate from the anticipated properties of individual constituents or the average doping level of the superlattice. Instead, they conform harmoniously to the effective doping, a critical parameter governed by the T$_c$ of interfacial superconductors. △ Less

Submitted 4 September, 2023; originally announced September 2023.

Comments: 8 pages, 5 figures

Giant spin Nernst effect in a two-dimensional antiferromagnet due to magnetoelastic coupling-induced gaps and interband transitions between magnon-like bands

Authors: D. -Q. To, C. Y. Ameyaw, A. Suresh, S. Bhatt, M. J. H. Ku, M. B. Jungfleisch, J. Q. Xiao, J. M. O. Zide, B. K. Nikolic, M. F. Doty

Abstract: We analyze theoretically the origin of the spin Nernst and thermal Hall effects in FePS3 as a realization of two-dimensional antiferromagnet (2D AFM). We find that a strong magnetoelastic coupling, hybridizing magnetic excitation (magnon) and elastic excitation (phonon), combined with time-reversal-symmetry-breaking, results in a Berry curvature hotspots in the region of anticrossing between the t… ▽ More We analyze theoretically the origin of the spin Nernst and thermal Hall effects in FePS3 as a realization of two-dimensional antiferromagnet (2D AFM). We find that a strong magnetoelastic coupling, hybridizing magnetic excitation (magnon) and elastic excitation (phonon), combined with time-reversal-symmetry-breaking, results in a Berry curvature hotspots in the region of anticrossing between the two distinct hybridized bands. Furthermore, large spin Berry curvature emerges due to interband transitions between two magnon-like bands, where a small energy gap is induced by magnetoelastic coupling between such bands that are energetically distant from anticrossing of hybridized bands. These nonzero Berry curvatures generate topological transverse transport (i.e., the thermal Hall effect) of hybrid excitations, dubbed magnon-polaron, as well as of spin (i.e., the spin Nernst effect) carried by them, in response to applied longitudinal temperature gradient. We investigate the dependence of the spin Nernst and thermal Hall conductivities on the applied magnetic field and temperature, unveiling very large spin Nernst conductivity even at zero magnetic field. Our results suggest FePS3 AFM, which is already available in 2D form experimentally, as a promising platform to explore the topological transport of the magnon-polaron quasiparticles at THz frequencies. △ Less

Submitted 16 May, 2023; v1 submitted 10 May, 2023; originally announced May 2023.

Comments: 11 pages, 7 figures; Supplemental Materials is available from https://mrsec.udel.edu/publications/

Journal ref: Physical Review B, 2023

Evolution of charge density waves from three-dimensional to quasi-two-dimensional in Kagome superconductors Cs(V$_{1-x}M_{x}$)$_3$Sb$_5$ ($M$ = Nb, Ta)

Authors: Qian Xiao, Qizhi Li, Jinjin Liu, Yongkai Li, Wei Xia, Xiquan Zheng, Yanfeng Guo, Yugui Yao, Zhiwei Wang, Yingying Peng

Abstract: The Kagome material $A{\mathrm{V}}_3{\mathrm{Sb}}_5$ ($A$ = K, Rb, Cs) with geometry frustration hosts non-trivial topological electronic structures, electronic nematicity, charge density wave (CDW) and superconductivity, providing an ideal platform to study the interplay between these phases. Specifically, in pressurized- or substituted-${\mathrm{CsV}}_3{\mathrm{Sb}}_5$, the relationship between… ▽ More The Kagome material $A{\mathrm{V}}_3{\mathrm{Sb}}_5$ ($A$ = K, Rb, Cs) with geometry frustration hosts non-trivial topological electronic structures, electronic nematicity, charge density wave (CDW) and superconductivity, providing an ideal platform to study the interplay between these phases. Specifically, in pressurized- or substituted-${\mathrm{CsV}}_3{\mathrm{Sb}}_5$, the relationship between CDW and superconductivity is unusual and remains to be fully understood. Recently, coexisting and competing 2 $\times$ 2 $\times$ 4 and 2 $\times$ 2 $\times$ 2 CDW phases were discovered in ${\mathrm{CsV}}_3{\mathrm{Sb}}_5$. To investigate the evolution of the CDW phases with the substitution of V atoms, we performed x-ray diffraction (XRD) experiments on ${\mathrm{Cs(V}}_{1-x}{\mathrm{Ta}}_{x}{\mathrm{)}}_3{\mathrm{Sb}}_5$ and ${\mathrm{Cs(V}}_{1-x}{\mathrm{Nb}}_{x}{\mathrm{)}}_3{\mathrm{Sb}}_5$. Our results indicate that in all substituted samples, the discrete CDW reflection points in pristine ${\mathrm{CsV}}_3{\mathrm{Sb}}_5$ change to rod-like structures along the $c^\star$ direction. This suggests that the long-ranged three-dimensional CDW becomes quasi-two-dimensional by the substitution of V by Ta/Nb. Moreover, our temperature-dependent measurements show that there is no hysteresis behavior of CDW signals, indicating that the 2 $\times$ 2 $\times$ 4 CDW phase is easily suppressed by even a slight substitution of V with Nb/Ta. These findings uncover the CDW evolution upon substitution of V atoms in CsV$_3$Sb$_5$, providing insights into the microscopic mechanism of CDW and helping to understand the interplay between intertwined phases and superconductivity. △ Less

Submitted 4 April, 2023; originally announced April 2023.

Comments: 7 pages, 6 figures

Journal ref: Phys. Rev. Materials 7, 074801 (2023)

Absence of localized $5d^1$ electrons in KTaO$_3$ interface superconductors

Authors: Xinqiang Cai, Jungho Kim, Leonardo Martinelli, Piero Florio, Matteo Corti, Weiliang Qiao, Yanqiu Sun, Jiasen Niu, Quentin Faure, Christoph Sahle, Qingzheng Qiu, Qian Xiao, Xiquan Zheng, Qizhi Li, Changwei Zou, Xinyi Jiang, Giacomo Ghiringhelli, Wei Han, Yanwu Xie, Yi Lu, Marco Moretti Sala, Yingying Peng

Abstract: Recently, an exciting discovery of orientation-dependent superconductivity was made in two-dimensional electron gas (2DEG) at the interfaces of LaAlO$_3$/KTaO$_3$ (LAO/KTO) or EuO/KTaO$_3$ (EuO/KTO). The superconducting transition temperature can reach a $T_c$ of up to $\sim$ 2.2 K, which is significantly higher than its 3$d$ counterpart LaAlO$_3$/SrTiO$_3$ (LAO/STO) with a $T_c$ of $\sim$ 0.2 K.… ▽ More Recently, an exciting discovery of orientation-dependent superconductivity was made in two-dimensional electron gas (2DEG) at the interfaces of LaAlO$_3$/KTaO$_3$ (LAO/KTO) or EuO/KTaO$_3$ (EuO/KTO). The superconducting transition temperature can reach a $T_c$ of up to $\sim$ 2.2 K, which is significantly higher than its 3$d$ counterpart LaAlO$_3$/SrTiO$_3$ (LAO/STO) with a $T_c$ of $\sim$ 0.2 K. However, the underlying origin remains to be understood. To uncover the nature of electrons in KTO-based interfaces, we employ x-ray absorption spectroscopy (XAS) and resonant inelastic x-ray spectroscopy (RIXS) to study LAO/KTO and EuO/KTO with different orientations. We reveal the absence of $dd$ orbital excitations in all the measured samples. Our RIXS results are well reproduced by calculations that considered itinerant $5d$ electrons hybridized with O $2p$ electrons. This suggests that there is a lack of localized Ta $5d^1$ electrons in KTO interface superconductors, which is consistent with the absence of magnetic hysteresis observed in magneto-resistance (MR) measurements. These findings offer new insights into our understanding of superconductivity in Ta $5d$ interface superconductors and their potential applications. △ Less

Submitted 3 March, 2023; originally announced March 2023.

Comments: 8 pages, 6 figures

Journal ref: Phys. Rev. B 108, 235167 (2023)

Phonon-mediated strong coupling between a three-dimensional topological insulator and a two-dimensional antiferromagnetic material

Authors: D. Quang To, Weipeng Wu, Subhash Bhatt, Yongchen Liu, Anderson Janotti, Joshua M. O. Zide, Mark J. H. Ku, John Q. Xiao, M. Benjamin Jungfleisch, Stephanie Law, Matthew F. Doty

Abstract: Van der Waals antiferromagnetic and topological insulator materials provide powerful platforms for modern optical, electronic, and spintronic devices applications. The interaction between an antiferromagnet (AFM) and a topological insulator (TI), if sufficiently strong, could offer emergent hybrid material properties that enable new functionality exceeding what is possible in any individual materi… ▽ More Van der Waals antiferromagnetic and topological insulator materials provide powerful platforms for modern optical, electronic, and spintronic devices applications. The interaction between an antiferromagnet (AFM) and a topological insulator (TI), if sufficiently strong, could offer emergent hybrid material properties that enable new functionality exceeding what is possible in any individual material constituent. In this work, we study strong coupling between THz excitations in a three dimensional (3D) topological insulator and a quasi-two dimensional (2D) antiferromagnetic material resulting in a new hybridized mode, namely a surface Dirac plasmon-phonon-magnon polariton. We find that the interaction between a surface Dirac plasmon polariton in the 3D TI and a magnon polariton in the 2D AFM is mediated by the phonon coupling in the 3D TI material. The coupling of phonons with an electromagnetic wave propagating in the 3D TI enhances the permittivity of the TI thin film in a way that results in a strong correlation between the dispersion of Dirac plasmon polaritons on the surfaces of the TI with the thickness of the TI. As a result, the dispersion of surface Dirac plasmon polaritons in the TI can be tuned toward resonance with the magnon polariton in the AFM material by varying the TI's thickness, thereby enhancing the strength of the coupling between the excitations in the two materials. The strength of this coupling, which results in the surface Dirac plasmon-phonon-magnon polariton, can be parameterized by the amplitude of the avoided-crossing splitting between the two polariton branches at the magnon resonance frequency... △ Less

Submitted 5 December, 2022; originally announced December 2022.

Report number: 7, 045201

Journal ref: Phys. Rev. Materials 2023

Negative GMR Effect in current perpendicular-to-plane (Zn,Cr)Te/Cu/Co spin salves

Authors: W. G. Wang, C. Ni, L. R. Shah, X. M. Kou, J. Q. Xiao

Abstract: Magnetic and transport properties are explored in the current perpendicular-to-plane (CPP) spin salves with Cr doped wide band gap semiconductor ZnTe as one of the ferromagnetic electrodes. A negative magnetoresistance is observed in these CPP spin valves at low temperature, with a strong temperature dependence. This effect can be explained by the large difference of spin scattering asymmetry coef… ▽ More Magnetic and transport properties are explored in the current perpendicular-to-plane (CPP) spin salves with Cr doped wide band gap semiconductor ZnTe as one of the ferromagnetic electrodes. A negative magnetoresistance is observed in these CPP spin valves at low temperature, with a strong temperature dependence. This effect can be explained by the large difference of spin scattering asymmetry coefficients in (Zn,Cr)Te and Cobalt, due to the very different spin polarizations of the two materials as revealed by the DFT calculation. △ Less

Submitted 10 November, 2022; originally announced November 2022.

Spin-polarized transport in magnetic tunnel junctions with ZnTe barriers

Authors: W. G. Wang, C. Ni, A. Ozbay, L. R. Shah, X. Fan, X. M. Kou, E. R. Nowak, J. Q. Xiao

Abstract: Magnetic tunnel junctions with wide band gap semiconductor ZnTe barrier were fabricated. A very low barrier height and sizable magnetoresistance were observed in the Fe/ZnTe/Fe junctions at room temperature. The nonlinear I-V characteristic curve confirmed the observed magnetoresistance is due to spin-dependent tunneling effect. Temperature dependent study indicated that the total conductance of t… ▽ More Magnetic tunnel junctions with wide band gap semiconductor ZnTe barrier were fabricated. A very low barrier height and sizable magnetoresistance were observed in the Fe/ZnTe/Fe junctions at room temperature. The nonlinear I-V characteristic curve confirmed the observed magnetoresistance is due to spin-dependent tunneling effect. Temperature dependent study indicated that the total conductance of the junction is dominated by direct tunneling, with only a small portion from the hopping conduction through the defect states inside the barrier. △ Less

Submitted 29 October, 2022; originally announced October 2022.

Large Bilinear Magnetoresistance from Rashba Spin-Splitting on the Surface of a Topological Insulator

Authors: Yang Wang, Binbin Liu, Yue-Xin Huang, Sivakumar V. Mambakkam, Yong Wang, Shengyuan A. Yang, Xian-Lei Sheng, Stephanie A. Law, John Q. Xiao

Abstract: In addition to the topologically protected linear dispersion, a band-bending-confined two-dimensional electron gas with tunable Rashba spin-splitting (RSS) was found to coexist with the topological surface states on the surface of topological insulators (TIs). Here, we report the observation of large bilinear magnetoresistance (BMR) in Bi2Se3 films decorated with transition metal atoms. The magnit… ▽ More In addition to the topologically protected linear dispersion, a band-bending-confined two-dimensional electron gas with tunable Rashba spin-splitting (RSS) was found to coexist with the topological surface states on the surface of topological insulators (TIs). Here, we report the observation of large bilinear magnetoresistance (BMR) in Bi2Se3 films decorated with transition metal atoms. The magnitude of the BMR sensitively depends on the type and amount of atoms deposited, with a maximum achieved value close to those of strong Rashba semiconductors. Our first-principles calculations reproduce the quantum well states and reveal sizable RSS in all Bi2Se3 heterostructures with broken inversion symmetry. Our results show that charge-spin interconversion through RSS states in TIs can be fine-tuned through surface atom deposition and easily detected via BMR for potential spintronic applications. △ Less

Submitted 16 December, 2022; v1 submitted 15 September, 2022; originally announced September 2022.

Comments: Typos in Fig. 4 caption and Ref. [27] were corrected in this version

Observation of electronic nematicity driven by three-dimensional charge density wave in kagome lattice KV$_3$Sb$_5$

Authors: Zhicheng Jiang, Haiyang Ma, Wei Xia, Zhengtai Liu, Qian Xiao, Zhonghao Liu, Yichen Yang, Jianyang Ding, Zhe Huang, Jiayu Liu, Yuxi Qiao, Jishan Liu, Yingying Peng, Soohyun Cho, Yanfeng Guo, Jianpeng Liu, Dawei Shen

Abstract: Kagome superconductors AV$_3$Sb$_5$ (A = K, Rb, Cs) provide a fertile playground for studying intriguing phenomena, including non-trivial band topology, superconductivity, giant anomalous Hall effect and charge density wave (CDW). Recently, a $C_2$ symmetric nematic phase prior to the superconducting state in AV$_3$Sb$_5$ drew enormous attention due to its potential inheritance of the symmetry of… ▽ More Kagome superconductors AV$_3$Sb$_5$ (A = K, Rb, Cs) provide a fertile playground for studying intriguing phenomena, including non-trivial band topology, superconductivity, giant anomalous Hall effect and charge density wave (CDW). Recently, a $C_2$ symmetric nematic phase prior to the superconducting state in AV$_3$Sb$_5$ drew enormous attention due to its potential inheritance of the symmetry of the unusual superconductivity. However, direct evidence on the rotation symmetry breaking of the electronic structure in the CDW state from the reciprocal space is still rare, and the underlying mechanism remains ambiguous. The observation shows unconventional unidirectionality, indicative of rotation symmetry breaking from six-fold to two-fold. The interlayer coupling between adjacent planes with $π$-phase offset in the 2$\times$2$\times$2 CDW phase leads to the preferred two-fold symmetric electronic structure. These rarely observed unidirectional back-folded bands in KV$_3$Sb$_5$ may provide important insights into its peculiar charge order and superconductivity. △ Less

Submitted 15 June, 2023; v1 submitted 2 August, 2022; originally announced August 2022.

Above-room-temperature ferromagnetism in ultrathin van der Waals magnet

Authors: Hang Chen, Shahidul Asif, Kapildeb Dolui, Yang Wang, Jeyson Tamara Isaza, V. M. L. Durga Prasad Goli, Matthew Whalen, Xinhao Wang, Zhijie Chen, Huiqin Zhang, Kai Liu, Deep Jariwala, M. Benjamin Jungfleisch, Chitraleema Chakraborty, Andrew F. May, Michael A. McGuire, Branislav K. Nikolic, John Q. Xiao, Mark J. H. Ku

Abstract: Two-dimensional (2D) magnetic van der Waals materials provide a powerful platform for studying fundamental physics of low-dimensional magnetism, engineering novel magnetic phases, and enabling ultrathin and highly tunable spintronic devices. To realize high quality and practical devices for such applications, there is a critical need for robust 2D magnets with ordering temperatures above room temp… ▽ More Two-dimensional (2D) magnetic van der Waals materials provide a powerful platform for studying fundamental physics of low-dimensional magnetism, engineering novel magnetic phases, and enabling ultrathin and highly tunable spintronic devices. To realize high quality and practical devices for such applications, there is a critical need for robust 2D magnets with ordering temperatures above room temperature that can be created via exfoliation. Here the study of exfoliated flakes of cobalt substituted Fe5GeTe2 (CFGT) exhibiting magnetism above room temperature is reported. Via quantum magnetic imaging with nitrogen-vacancy centers in diamond, ferromagnetism at room temperature was observed in CFGT flakes as thin as 16 nm. This corresponds to one of the thinnest room-temperature 2D magnet flakes exfoliated from robust single crystals, reaching a thickness relevant to practical spintronic applications. The Curie temperature Tc of CFGT ranges from 310 K in the thinnest flake studied to 328 K in the bulk. To investigate the prospect of high-temperature monolayer ferromagnetism, Monte Carlo calculations were performed which predicted a high value of Tc ~270 K in CFGT monolayers. Pathways towards further enhancing monolayer Tc are discussed. These results support CFGT as a promising platform to realize high-quality room-temperature 2D magnet devices. △ Less

Submitted 14 June, 2022; originally announced June 2022.

Surface plasmon-phonon-magnon polariton in a topological insulator-antiferromagnetic bilayer structure

Authors: D. Quang To, Zhengtianye Wang, Yongchen Liu, Weipeng Wu, M. Benjamin Jungfleisch, John Q. Xiao, Joshua M. O. Zide, Stephanie Law, Matthew F. Doty

Abstract: We present a robust technique for computationally studying surface polariton modes in hybrid materials. We use a semi-classical model that allows us to understand the physics behind the interactions between collective excitations of the hybrid system and develop a scattering and transfer matrix method that imposes the proper boundary conditions to solve Maxwell equations and derive a general equat… ▽ More We present a robust technique for computationally studying surface polariton modes in hybrid materials. We use a semi-classical model that allows us to understand the physics behind the interactions between collective excitations of the hybrid system and develop a scattering and transfer matrix method that imposes the proper boundary conditions to solve Maxwell equations and derive a general equation describing the surface polariton in a heterostructure consisting of N constituent materials. We apply this method to a test structure composed of a topological insulator (TI) and an antiferromagnetic material (AFM) to study the resulting surface Dirac plasmon-phonon-magnon polariton (DPPMP). We find that interactions between the excitations of the two constituents result in the formation of hybridized modes and the emergence of avoided-crossing points in the dispersion relations for the DPPMP. For the specific case of a Bi2Se3 TI material, the polariton branch with low frequency below 2 THz redshifts upon increasing the thickness of TI thin film, which leads to an upper bound on the thickness of the TI layer that will allow an observable signature of strong coupling and the emergence of hybridized states. We also find that the strength of the coupling between the TI and the AFM, which is parameterized by the amplitude of the avoided-crossing splitting between the two polariton branches at the magnon resonance frequency, depends on the magnitude of the magnetic dipole and the line width of the magnon in the AFM material as well as on the Fermi energy of Dirac plasmon in the TI. Finally, we predict that materials with extremely high quality, i.e. low scattering loss rate, are essential to achieve an experimentally-observable strong coupling between a TI and AFM. △ Less

Submitted 15 May, 2022; originally announced May 2022.

Comments: 16 pages, 12 figures

Journal ref: Phys. Rev. Materials 6, 085201 (2022)

Domain wall nature of sketched LaAlO3/SrTiO3 nanowires

Authors: Dawei Qiu, Mengke Ha, Qing Xiao, Zhiyuan Qin, Danqing Liu, Changjian Ma, Guanglei Cheng, Jiangfeng Du

Abstract: The rich electron correlations and highly coherent transport in reconfigurable devices sketched by a conductive atomic force microscope tip at the LaAlO3/SrTiO3 interface have enabled the oxide platform an ideal playground for studying correlated electrons and quantum technological applications. Why these one-dimensional devices possess enhanced properties over the two-dimensional interface, howev… ▽ More The rich electron correlations and highly coherent transport in reconfigurable devices sketched by a conductive atomic force microscope tip at the LaAlO3/SrTiO3 interface have enabled the oxide platform an ideal playground for studying correlated electrons and quantum technological applications. Why these one-dimensional devices possess enhanced properties over the two-dimensional interface, however, has remained elusive. Here we provide evidence that one-dimensional LaAlO3/SrTiO3 nanowires are intrinsically ferroelastic domain walls by nature through thermodynamic study. We have observed spreading resistance anomalies under thermo-stimulus and temperature cycles, with characteristic temperatures matching domain wall polarity. This information is crucial in understanding the novel phenomena including superconductivity and high mobility quantum transport. △ Less

Submitted 15 June, 2023; v1 submitted 25 April, 2022; originally announced April 2022.

$2^{1296}$ Exponentially Complex Quantum Many-Body Simulation via Scalable Deep Learning Method

Authors: Xiao Liang, Mingfan Li, Qian Xiao, Hong An, Lixin He, Xuncheng Zhao, Junshi Chen, Chao Yang, Fei Wang, Hong Qian, Li Shen, Dongning Jia, Yongjian Gu, Xin Liu, Zhiqiang Wei

Abstract: For decades, people are developing efficient numerical methods for solving the challenging quantum many-body problem, whose Hilbert space grows exponentially with the size of the problem. However, this journey is far from over, as previous methods all have serious limitations. The recently developed deep learning methods provide a very promising new route to solve the long-standing quantum many-bo… ▽ More For decades, people are developing efficient numerical methods for solving the challenging quantum many-body problem, whose Hilbert space grows exponentially with the size of the problem. However, this journey is far from over, as previous methods all have serious limitations. The recently developed deep learning methods provide a very promising new route to solve the long-standing quantum many-body problems. We report that a deep learning based simulation protocol can achieve the solution with state-of-the-art precision in the Hilbert space as large as $2^{1296}$ for spin system and $3^{144}$ for fermion system , using a HPC-AI hybrid framework on the new Sunway supercomputer. With highly scalability up to 40 million heterogeneous cores, our applications have measured 94% weak scaling efficiency and 72% strong scaling efficiency. The accomplishment of this work opens the door to simulate spin models and Fermion models on unprecedented lattice size with extreme high precision. △ Less

Submitted 16 April, 2022; originally announced April 2022.

Comments: Massive ground state optimizations of CNN-based wave-functions for $J1$-$J2$ model and $t$-$J$ model carried out on a heterogeneous cores supercomputer

Journal ref: 2023 Mach. Learn.: Sci. Technol. 4 015035

Giant magnetic in-plane anisotropy and competing instabilities in Na3Co2SbO6

Authors: Xintong Li, Yuchen Gu, Yue Chen, V. Ovidiu Garlea, Kazuki Iida, Kazuya Kamazawa, Yangmu Li, Guochu Deng, Qian Xiao, Xiquan Zheng, Zirong Ye, Yingying Peng, I. A. Zaliznyak, J. M. Tranquada, Yuan Li

Abstract: We report magnetometry data obtained on twin-free single crystals of Na3Co2SbO6, which is considered a candidate material for realizing the Kitaev honeycomb model for quantum spin liquids. Contrary to a common belief that such materials can be modeled with the symmetries of an ideal honeycomb lattice, our data reveal a pronounced two-fold symmetry and in-plane anisotropy of over 200%, despite the… ▽ More We report magnetometry data obtained on twin-free single crystals of Na3Co2SbO6, which is considered a candidate material for realizing the Kitaev honeycomb model for quantum spin liquids. Contrary to a common belief that such materials can be modeled with the symmetries of an ideal honeycomb lattice, our data reveal a pronounced two-fold symmetry and in-plane anisotropy of over 200%, despite the honeycomb layer's tiny orthorhombic distortion of less than 0.2%. We further use magnetic neutron diffraction to elucidate a rich variety of field-induced phases observed in the magnetometry. These phases manifest themselves in the paramagnetic state as diffuse scattering signals associated with competing ferro- and antiferromagnetic instabilities, consistent with a theory that also predicts a quantum spin liquid phase nearby. Our results call for theoretical understanding of the observed in-plane anisotropy, and render Na3Co2SbO6 a promising ground for finding exotic quantum phases by targeted external tuning. △ Less

Submitted 15 October, 2022; v1 submitted 9 April, 2022; originally announced April 2022.

Comments: 19 pages, 15 figures, 1 animation; to appear in Phys. Rev. X

Journal ref: Phys. Rev. X 12, 041024 (2022)

Observation of nonlinear planar Hall effect in magnetic insulator/topological insulator heterostructures

Authors: Yang Wang, Sivakumar V. Mambakkam, Yue-Xin Huang, Yong Wang, Yi Ji, Cong Xiao, Shengyuan A. Yang, Stephanie A. Law, John Q. Xiao

Abstract: Interfacing topological insulators (TIs) with magnetic insulators (MIs) has been widely used to study the interaction between topological surface states and magnetism. Previous transport studies typically interpret the suppression of weak antilocalization or appearance of the anomalous Hall effect as signatures of magnetic proximity effect (MPE) imposed to TIs. Here, we report the observation of n… ▽ More Interfacing topological insulators (TIs) with magnetic insulators (MIs) has been widely used to study the interaction between topological surface states and magnetism. Previous transport studies typically interpret the suppression of weak antilocalization or appearance of the anomalous Hall effect as signatures of magnetic proximity effect (MPE) imposed to TIs. Here, we report the observation of nonlinear planar Hall effect (NPHE) in Bi2Se3 films grown on MI thulium and yttrium iron garnet (TmIG and YIG) substrates, which is an order of magnitude larger than that in Bi2Se3 grown on nonmagnetic gadolinium gallium garnet (GGG) substrate. The nonlinear Hall resistance in TmIG/Bi2Se3 depends linearly on the external magnetic field, while that in YIG/Bi2Se3 exhibits an extra hysteresis loop around zero field. The magnitude of the NPHE is found to scale inversely with carrier density. We speculate the observed NPHE is related to the MPE-induced exchange gap opening and out-of-plane spin textures in the TI surface states, which may be used as an alternative transport signature of the MPE in MI/TI heterostructures. △ Less

Submitted 15 September, 2022; v1 submitted 11 March, 2022; originally announced March 2022.

Direct probing of strong magnon-photon coupling in a planar geometry

Authors: Mojtaba Taghipour Kaffash, Dinesh Wagle, Anish Rai, Thomas Meyer, John Q. Xiao, M. Benjamin Jungfleisch

Abstract: We demonstrate direct probing of strong magnon-photon coupling using Brillouin light scattering spectroscopy in a planar geometry. The magnonic hybrid system comprises a split-ring resonator loaded with epitaxial yttrium iron garnet thin films of 200 nm and 2.46 $μ$m thickness. The Brillouin light scattering measurements are combined with microwave spectroscopy measurements where both biasing magn… ▽ More We demonstrate direct probing of strong magnon-photon coupling using Brillouin light scattering spectroscopy in a planar geometry. The magnonic hybrid system comprises a split-ring resonator loaded with epitaxial yttrium iron garnet thin films of 200 nm and 2.46 $μ$m thickness. The Brillouin light scattering measurements are combined with microwave spectroscopy measurements where both biasing magnetic field and microwave excitation frequency are varied. The cooperativity for the 200 nm-thick YIG films is 4.5, and larger cooperativity of 137.4 is found for the 2.46 $μ$m-thick YIG film. We show that Brillouin light scattering is advantageous for probing the magnonic character of magnon-photon polaritons, while microwave absorption is more sensitive to the photonic character of the hybrid excitation. A miniaturized, planar device design is imperative for the potential integration of magnonic hybrid systems in future coherent information technologies, and our results are a first stepping stone in this regard. Furthermore, successfully detecting the magnonic hybrid excitation by Brillouin light scattering is an essential step for the up-conversion of quantum signals from the optical to the microwave regime in hybrid quantum systems. △ Less

Submitted 25 February, 2022; originally announced February 2022.

Report number: 8 01LT02

Journal ref: Quantum Sci. Technol. (2023)

Coexistence of Multiple Stacking Charge Density Waves in Kagome Superconductor ${\mathrm{CsV}}_3{\mathrm{Sb}}_5$

Authors: Qian Xiao, Yihao Lin, Qizhi Li, Xiquan Zheng, Sonia Francoual, Christian Plueckthun, Wei Xia, Qingzheng Qiu, Shilong Zhang, Yanfeng Guo, Ji Feng, Yingying Peng

Abstract: The recently discovered Kagome family ${\mathrm{AV}}_3{\mathrm{Sb}}_5$ (A = K, Rb, Cs) exhibits rich physical phenomena, including non-trivial topological electronic structure, giant anomalous Hall effect, charge density waves (CDW) and superconductivity. Notably, CDW in ${\mathrm{AV}}_3{\mathrm{Sb}}_5$ is evidenced to intertwine with its superconductivity and topology, but its nature remains elus… ▽ More The recently discovered Kagome family ${\mathrm{AV}}_3{\mathrm{Sb}}_5$ (A = K, Rb, Cs) exhibits rich physical phenomena, including non-trivial topological electronic structure, giant anomalous Hall effect, charge density waves (CDW) and superconductivity. Notably, CDW in ${\mathrm{AV}}_3{\mathrm{Sb}}_5$ is evidenced to intertwine with its superconductivity and topology, but its nature remains elusive. Here, we combine x-ray scattering experiments and density-functional theory calculations to investigate the CDWs in ${\mathrm{CsV}}_3{\mathrm{Sb}}_5$ and demonstrate the coexistence of 2 $\times$ 2 $\times$ 2 and 2 $\times$ 2 $\times$ 4 CDW stacking phases. Competition between these CDW phases is revealed by tracking the temperature evolution of CDW intensities, which also manifests in different transition temperatures during warming- and cooling measurements. We also identify a meta-stable quenched state of ${\mathrm{CsV}}_3{\mathrm{Sb}}_5$ after fast-cooling process. Our study demonstrates the coexistence of competing CDW stacking in ${\mathrm{CsV}}_3{\mathrm{Sb}}_5$, offering new insights in understanding the novel properties of this system. △ Less

Submitted 10 March, 2023; v1 submitted 13 January, 2022; originally announced January 2022.

Comments: 6 pages, 5 figures

Journal ref: Phys. Rev. Research 5, L012032 (2023)

Dispersionless orbital excitations in (Li,Fe)OHFeSe superconductors

Authors: Qian Xiao, Wenliang Zhang, Teguh Citra Asmara, Dong Li, Qizhi Li, Shilong Zhang, Yi Tseng, Xiaoli Dong, Yao Wang, Cheng-Chien Chen, Thorsten Schmitt, Yingying Peng

Abstract: The superconducting critical temperature $T_{\mathrm{c}}$ of intercalated iron-selenide superconductor (Li,Fe)OHFeSe (FeSe11111) can be increased to 42 K from 8 K of bulk FeSe. It shows remarkably similar electronic properties as the high-$T_{\mathrm{c}}$ monolayer FeSe and provides a bulk counterpart to investigate the origin of enhanced superconductivity. Unraveling the nature of excitations is… ▽ More The superconducting critical temperature $T_{\mathrm{c}}$ of intercalated iron-selenide superconductor (Li,Fe)OHFeSe (FeSe11111) can be increased to 42 K from 8 K of bulk FeSe. It shows remarkably similar electronic properties as the high-$T_{\mathrm{c}}$ monolayer FeSe and provides a bulk counterpart to investigate the origin of enhanced superconductivity. Unraveling the nature of excitations is crucial for understanding the pairing mechanism in high-$T_{\mathrm{c}}$ iron selenides. Here we use resonant inelastic x-ray scattering (RIXS) to investigate the excitations in FeSe11111. Our high-quality data exhibit several Raman-like excitations, which are dispersionless and isotropic in momentum transfer and robust against varying $T_{\mathrm{c}}$. Using atomic multiplet calculations, we assign the low-energy $\sim 0.3$ and 0.7 eV Raman peaks as local $e_g-e_g$ and $e_g-t_{2g}$ orbital excitations. The intensity of these two features decreases with increasing temperature, suggesting a primary contribution of the orbital fluctuations. Our results highlight the importance of orbital degree of freedom for high-$T_{\mathrm{c}}$ iron selenides. △ Less

Submitted 23 December, 2021; v1 submitted 11 October, 2021; originally announced October 2021.

Comments: 11 pages, 4 figures

Journal ref: npj Quantum Materials 7, 80 (2022)

Revealing room temperature ferromagnetism in exfoliated Fe$_5$GeTe$_2$ flakes with quantum magnetic imaging

Authors: Hang Chen, Shahidul Asif, Matthew Whalen, Jeyson Tamara-Isaza, Brennan Luetke, Yang Wang, Xinhao Wang, Millicent Ayako, Saurabh Lamsal, Andrew F. May, Michael A. McGuire, Chitraleema Chakraborty, John Q. Xiao, Mark J. H. Ku

Abstract: Van der Waals material Fe$_5$GeTe$_2$, with its long-range ferromagnetic ordering near room temperature, has significant potential to become an enabling platform for implementing novel spintronic and quantum devices. To pave the way for applications, it is crucial to determine the magnetic properties when the thickness of Fe5GeTe2 reaches the few-layers regime. However, this is highly challenging… ▽ More Van der Waals material Fe$_5$GeTe$_2$, with its long-range ferromagnetic ordering near room temperature, has significant potential to become an enabling platform for implementing novel spintronic and quantum devices. To pave the way for applications, it is crucial to determine the magnetic properties when the thickness of Fe5GeTe2 reaches the few-layers regime. However, this is highly challenging due to the need for a characterization technique that is local, highly sensitive, artifact-free, and operational with minimal fabrication. Prior studies have indicated that Curie temperature TC can reach up to close to room temperature for exfoliated Fe$_5$GeTe$_2$ flakes, as measured via electrical transport; there is a need to validate these results with a measurement that reveals magnetism more directly. In this work, we investigate the magnetic properties of exfoliated thin flakes of van der Waals magnet Fe$_5$GeTe$_2$ via a quantum magnetic imaging technique based on nitrogen vacancy diamond. Through imaging the stray fields, we confirm room-temperature magnetic order in Fe$_5$GeTe$_2$ thin flakes with thickness down to 7 units cell. The stray field patterns and their response to magnetizing fields with different polarities point to a perpendicular easy-axis anisotropy. Furthermore, we perform imaging at different temperatures and determine the Curie temperature of the flakes at Tc~300 K. These results provide the basis for realizing a room-temperature monolayer ferromagnet with Fe$_5$GeTe$_2$. This work also demonstrates that the imaging technique enables a rapid screening of multiple flakes simultaneously, thereby paving the way towards high throughput characterization of potential 2D magnets near room temperature. △ Less

Submitted 20 March, 2022; v1 submitted 11 October, 2021; originally announced October 2021.

Journal ref: 2D Mater. (2022) 9 025017

Hot electron cooling in InSb probed by ultrafast time-resolved terahertz cyclotron resonance

Authors: Chelsea Q. Xia, Maurizio Monti, Jessica L. Boland, Laura M. Herz, James Lloyd-Hughes, Marina R. Filip, Michael B. Johnston

Abstract: Measuring terahertz (THz) conductivity on an ultrafast time scale is an excellent way to observe charge-carrier dynamics in semiconductors as a function of time after photoexcitation. However, a conductivity measurement alone cannot separate the effects of charge-carrier recombination from effective mass changes as charges cool and experience different regions of the electronic band structure. Her… ▽ More Measuring terahertz (THz) conductivity on an ultrafast time scale is an excellent way to observe charge-carrier dynamics in semiconductors as a function of time after photoexcitation. However, a conductivity measurement alone cannot separate the effects of charge-carrier recombination from effective mass changes as charges cool and experience different regions of the electronic band structure. Here we present a form of time-resolved magneto-THz spectroscopy which allows us to measure cyclotron effective mass on a picosecond time scale. We demonstrate this technique by observing electron cooling in the technologically-significant narrow-bandgap semiconductor indium antimonide (InSb). A significant reduction of electron effective mass from 0.032$m_\mathrm{e}$ to 0.017$m_\mathrm{e}$ is observed in the first 200ps after injecting hot electrons. Measurement of electron effective mass in InSb as a function of photo-injected electron density agrees well with conduction band non-parabolicity predictions from ab initio calculations of the quasiparticle band structure. △ Less

Submitted 11 September, 2021; originally announced September 2021.

Journal ref: Phys. Rev. B, 2021, 103, 245205

Limits to Electrical Mobility in Lead-Halide Perovskite Semiconductors

Authors: Chelsea Q. Xia, Jiali Peng, Samuel Poncé, Jay B. Patel, Adam D. Wright, Timothy W. Crothers, Mathias Uller Rothmann, Juliane Borchert, Rebecca L. Milot, Hans Kraus, Qianqian Lin, Feliciano Giustino, Laura M. Herz, Michael B. Johnston

Abstract: Semiconducting polycrystalline thin films are cheap to produce and can be deposited on flexible substrates, yet high-performance electronic devices usually utilize single-crystal semiconductors, owing to their superior electrical mobilities and longer diffusion lengths. Here we show that the electrical performance of polycrystalline films of metal-halide perovskites (MHPs) approaches that of singl… ▽ More Semiconducting polycrystalline thin films are cheap to produce and can be deposited on flexible substrates, yet high-performance electronic devices usually utilize single-crystal semiconductors, owing to their superior electrical mobilities and longer diffusion lengths. Here we show that the electrical performance of polycrystalline films of metal-halide perovskites (MHPs) approaches that of single crystals at room temperature. Combining temperature-dependent terahertz conductivity measurements and ab initio calculations we uncover a complete picture of the origins of charge scattering in single crystals and polycrystalline films of CH$_3$NH$_3$PbI$_3$. We show that Fröhlich scattering of charge carriers with multiple phonon modes is the dominant mechanism limiting mobility, with grain-boundary scattering further reducing mobility in polycrystalline films. We reconcile the large discrepancy in charge diffusion lengths between single crystals and films by considering photon reabsorption. Thus, polycrystalline films of MHPs offer great promise for devices beyond solar cells, including transistors and modulators. △ Less

Submitted 10 September, 2021; originally announced September 2021.

Comments: 33 pages, 4 figures (including the toc figure)

Journal ref: J. Phys. Chem. Lett. 2021, 12, 3607

Bridging the Gap between Deep Learning and Frustrated Quantum Spin System for Extreme-scale Simulations on New Generation of Sunway Supercomputer

Authors: Mingfan Li, Junshi Chen, Qian Xiao, Qingcai Jiang, Xuncheng Zhao, Rongfen Lin, Fei Wang, Hong An, Xiao Liang, Lixin He

Abstract: Efficient numerical methods are promising tools for delivering unique insights into the fascinating properties of physics, such as the highly frustrated quantum many-body systems. However, the computational complexity of obtaining the wave functions for accurately describing the quantum states increases exponentially with respect to particle number. Here we present a novel convolutional neural net… ▽ More Efficient numerical methods are promising tools for delivering unique insights into the fascinating properties of physics, such as the highly frustrated quantum many-body systems. However, the computational complexity of obtaining the wave functions for accurately describing the quantum states increases exponentially with respect to particle number. Here we present a novel convolutional neural network (CNN) for simulating the two-dimensional highly frustrated spin-$1/2$ $J_1-J_2$ Heisenberg model, meanwhile the simulation is performed at an extreme scale system with low cost and high scalability. By ingenious employment of transfer learning and CNN's translational invariance, we successfully investigate the quantum system with the lattice size up to $24\times24$, within 30 million cores of the new generation of sunway supercomputer. The final achievement demonstrates the effectiveness of CNN-based representation of quantum-state and brings the state-of-the-art record up to a brand-new level from both aspects of remarkable accuracy and unprecedented scales. △ Less

Submitted 14 April, 2022; v1 submitted 31 August, 2021; originally announced August 2021.

Comments: This paper reviews the technical details of calculating spin-1/2 J1-J2 model using convolutional neural network ansatz on Sunway Supercomputer

Observation of van der Waals phonons in the single-layer cuprate (Bi,Pb)$_2$(Sr,La)$_2$CuO$_{6+δ}$

Authors: Y. Y. Peng, I. Boukahil, K. Krongchon, Q. Xiao, A. A. Husain, Sangjun Lee, Q. Z. Li, A. Alatas, A. H. Said, H. T. Yan, Y. Ding, L. Zhao, X. J. Zhou, T. P. Devereaux, L. K. Wagner, C. D. Pemmaraju, P. Abbamonte

Abstract: Interlayer van der Waals (vdW) coupling is generic in two-dimensional materials such as graphene and transition metal dichalcogenides, which can induce very low-energy phonon modes. Using high-resolution inelastic hard x-ray scattering, we uncover the ultra-low energy phonon mode along the Cu-O bond direction in the high-$T_c$ cuprate (Bi,Pb)$_2$(Sr,La)$_2$CuO$_{6+δ}$ (Bi2201). This mode is indepe… ▽ More Interlayer van der Waals (vdW) coupling is generic in two-dimensional materials such as graphene and transition metal dichalcogenides, which can induce very low-energy phonon modes. Using high-resolution inelastic hard x-ray scattering, we uncover the ultra-low energy phonon mode along the Cu-O bond direction in the high-$T_c$ cuprate (Bi,Pb)$_2$(Sr,La)$_2$CuO$_{6+δ}$ (Bi2201). This mode is independent of temperature, while its intensity decreases with doping in accordance with an increasing c-axis lattice parameter. We compare the experimental results to first-principles density functional theory simulations and identify the observed mode as a van der Waals phonon, which arises from the shear motion of the adjacent Bi-O layers. This shows that Bi-based cuprate has similar vibrational properties as graphene and transition metal dichalcogenides, which can be exploited to engineer novel heterostructures. △ Less

Submitted 21 June, 2021; originally announced June 2021.

Journal ref: Physical Review Materials 8, 024804 (2024)

Observation of orbital order in the Van der Waals material 1T-TiSe2

Authors: Yingying Peng, Xuefei Guo, Qian Xiao, Qizhi Li, Jörg Strempfer, Yongseong Choi, Dong Yan, Huixia Luo, Yuqing Huang, Shuang Jia, Oleg Janson, Peter Abbamonte, Jeroen van den Brink, Jasper van Wezel

Abstract: Besides magnetic and charge order, regular arrangements of orbital occupation constitute a fundamental order parameter of condensed matter physics. Even though orbital order is difficult to identify directly in experiments, its presence was firmly established in a number of strongly correlated, three-dimensional Mott insulators. Here, reporting resonant X-ray scattering experiments on the layered… ▽ More Besides magnetic and charge order, regular arrangements of orbital occupation constitute a fundamental order parameter of condensed matter physics. Even though orbital order is difficult to identify directly in experiments, its presence was firmly established in a number of strongly correlated, three-dimensional Mott insulators. Here, reporting resonant X-ray scattering experiments on the layered Van der Waals compound $1T$-TiSe$_2$, we establish the emergence of orbital order in a weakly correlated, quasi-two-dimensional material. Our experimental scattering results are consistent with first-principles calculations that bring to the fore a generic mechanism of close interplay between charge redistribution, lattice displacements, and orbital order. It demonstrates the essential role that orbital degrees of freedom play in TiSe$_2$, and their importance throughout the family of correlated Van der Waals materials. △ Less

Submitted 27 May, 2021; originally announced May 2021.

Journal ref: Physical Review Research 4, 033053 (2022)