We report a comprehensive Raman scattering study on layered MPS_3(M = Mn, Fe, Ni), a two-dimensional magnetic compound with weak van der Waals interlayer coupling. The observed Raman phonon modes have been well assign...We report a comprehensive Raman scattering study on layered MPS_3(M = Mn, Fe, Ni), a two-dimensional magnetic compound with weak van der Waals interlayer coupling. The observed Raman phonon modes have been well assigned by the combination of first-principles calculations and the polarization-resolved spectra. Careful symmetry analysis on the angle-dependent spectra demonstrates that the crystal symmetry is strictly described by C_(2h)but can be simplified to D_(3d) with good accuracy. Interestingly, the three compounds share exactly the same lattice structure but show distinct magnetic structures. This provides us with a unique opportunity to study the effect of different magnetic orders on lattice dynamics in MPS_3. Our results reveal that the in-plane Nel antiferromagnetic(AF) order in MnPS_3 favors a spin–phonon coupling compared to the in-plane zig-zag AF in NiPS_3 and FePS_3. We have discussed the mechanism in terms of the folding of magnetic Brillouin zones. Our results provide insights into the relation between lattice dynamics and magnetism in the layered MPX_3(M = transition metal, X = S, Se) family and shed light on the magnetism of monolayer MPX_3 materials.展开更多
By combining temperature-dependent x-ray diffraction(XRD) with temperature-dependent Raman scattering, we have characterized the structural transitions and lattice dynamics of the hybrid organic–inorganic perovskite ...By combining temperature-dependent x-ray diffraction(XRD) with temperature-dependent Raman scattering, we have characterized the structural transitions and lattice dynamics of the hybrid organic–inorganic perovskite CH3NH3PbI3.The XRD measurements cover distinct phases between 15 K and 370 K and demonstrate a general positive thermal expansion.Clear anomalies are found around the transition temperatures.The temperature evolution of the lattice constants reveals that the transition at 160 K/330 K is of the first-/second-order type.Raman measurements uncover three strong lowfrequency modes, which can be ascribed to the vibration of the Pb/I atoms.The temperature evolution of the modes clearly catches these transitions at 160 K and 330 K, and confirms the transition types, which are exactly consistent with the XRD results.The present study may set an experimental basis to understand the high conversion efficiency in methylammonium lead iodide.展开更多
The layered magnetic van der Waals materials have generated tremendous interest due to their potential applications and importance in fundamental research.Previous x-ray diffraction(XRD)studies on the magnetic van der...The layered magnetic van der Waals materials have generated tremendous interest due to their potential applications and importance in fundamental research.Previous x-ray diffraction(XRD)studies on the magnetic van der Waals compound VI3,revealed a structural transition above the magnetic transition but output controversial analysis on symmetry.In this paper we carried out polarized Raman scattering measurements on VI3 from 10 K to 300 K,with focus on the two Ag phonon modes at^71.1 cm^-1 and 128.4 cm-1.Our careful symmetry analysis based on the angle-dependent spectra demonstrates that the crystal symmetry can be well described by C2h rather than D3d both above and below structural phase transition.We further performed temperature-dependent Raman experiments to study the magnetism in VI3.Fano asymmetry and anomalous linewidth drop of two Ag phonon modes at low temperatures,point to a significant spin-phonon coupling.This is also supported by the softening of 71.1-cm^-1 mode above the magnetic transition.The study provides the fundamental information on lattice dynamics and clarifies the symmetry in VI3.And spin-phonon coupling existing in a wide temperature range revealed here may be meaningful in applications.展开更多
The Kitaev spin liquid(KSL) system has attracted tremendous attention in recent years because of its fundamental significance in condensed matter physics and promising applications in fault-tolerant topological quantu...The Kitaev spin liquid(KSL) system has attracted tremendous attention in recent years because of its fundamental significance in condensed matter physics and promising applications in fault-tolerant topological quantum computation.Material realization of such a system remains a major challenge in the field due to the unusual configuration of anisotropic spin interactions,though great effort has been made before.Here we reveal that rare-earth chalcohalides REChX(RE=rare earth;Ch=O,S,Se,Te;X=F,Cl,Br,I) can serve as a family of KSL candidates.Most family members have the typical SmSI-type structure with a high symmetry of R3m,and rare-earth magnetic ions form an undistorted honeycomb lattice.The strong spin-orbit coupling of 4f electrons intrinsically offers anisotropic spin interactions as required by the Kitaev model.We have grown the crystals of YbOCl and synthesized the polycrystals of SmSI,ErOF,HoOF and DyOF,and made careful structural characterizations.We carry out magnetic and heat capacity measurements down to 1.8 K and find no obvious magnetic transition in all the samples but DyOF.The van der Waals interlayer coupling highlights the true two-dimensionality of the family which is vital for the exact realization of Abelian/non-Abelian anyons,and the graphene-like feature will be a prominent advantage for developing miniaturized devices.The family is expected to act as an inspiring material platform for the exploration of KSL physics.展开更多
基金Project supported by the Ministry of Science and Technology of China(Grant Nos.2016YFA0300504 and 2017YFA0302904)the National Natural Science Foundation of China(Grant Nos.11474357 and 11774419)the Fundamental Research Funds for the Central Universities,China,and the Research Funds of Renmin University of China(Grant No.14XNLQ03)
文摘We report a comprehensive Raman scattering study on layered MPS_3(M = Mn, Fe, Ni), a two-dimensional magnetic compound with weak van der Waals interlayer coupling. The observed Raman phonon modes have been well assigned by the combination of first-principles calculations and the polarization-resolved spectra. Careful symmetry analysis on the angle-dependent spectra demonstrates that the crystal symmetry is strictly described by C_(2h)but can be simplified to D_(3d) with good accuracy. Interestingly, the three compounds share exactly the same lattice structure but show distinct magnetic structures. This provides us with a unique opportunity to study the effect of different magnetic orders on lattice dynamics in MPS_3. Our results reveal that the in-plane Nel antiferromagnetic(AF) order in MnPS_3 favors a spin–phonon coupling compared to the in-plane zig-zag AF in NiPS_3 and FePS_3. We have discussed the mechanism in terms of the folding of magnetic Brillouin zones. Our results provide insights into the relation between lattice dynamics and magnetism in the layered MPX_3(M = transition metal, X = S, Se) family and shed light on the magnetism of monolayer MPX_3 materials.
基金Project supported by the National Natural Science Foundation of China(Grant No.11774419)the Ministry of Science and Technology of China(Grant Nos.2016YFA0300504 and 2017YFA0302904)
文摘By combining temperature-dependent x-ray diffraction(XRD) with temperature-dependent Raman scattering, we have characterized the structural transitions and lattice dynamics of the hybrid organic–inorganic perovskite CH3NH3PbI3.The XRD measurements cover distinct phases between 15 K and 370 K and demonstrate a general positive thermal expansion.Clear anomalies are found around the transition temperatures.The temperature evolution of the lattice constants reveals that the transition at 160 K/330 K is of the first-/second-order type.Raman measurements uncover three strong lowfrequency modes, which can be ascribed to the vibration of the Pb/I atoms.The temperature evolution of the modes clearly catches these transitions at 160 K and 330 K, and confirms the transition types, which are exactly consistent with the XRD results.The present study may set an experimental basis to understand the high conversion efficiency in methylammonium lead iodide.
基金Project supported by the Science Fund from the Ministry of Science and Technology of China(Grant Nos.2017YFA0302904 and 2016YFA0300504)the National Natural Science Foundation of China(Grant Nos.11774419,U1932215,11774423,and 11822412)+1 种基金the Fundamental Research Funds for the Central Universities,Chinathe Research Funds of Renmin University of China(RUC)(Grant Nos.15XNLQ07,18XNLG14,and 19XNLG17).
文摘The layered magnetic van der Waals materials have generated tremendous interest due to their potential applications and importance in fundamental research.Previous x-ray diffraction(XRD)studies on the magnetic van der Waals compound VI3,revealed a structural transition above the magnetic transition but output controversial analysis on symmetry.In this paper we carried out polarized Raman scattering measurements on VI3 from 10 K to 300 K,with focus on the two Ag phonon modes at^71.1 cm^-1 and 128.4 cm-1.Our careful symmetry analysis based on the angle-dependent spectra demonstrates that the crystal symmetry can be well described by C2h rather than D3d both above and below structural phase transition.We further performed temperature-dependent Raman experiments to study the magnetism in VI3.Fano asymmetry and anomalous linewidth drop of two Ag phonon modes at low temperatures,point to a significant spin-phonon coupling.This is also supported by the softening of 71.1-cm^-1 mode above the magnetic transition.The study provides the fundamental information on lattice dynamics and clarifies the symmetry in VI3.And spin-phonon coupling existing in a wide temperature range revealed here may be meaningful in applications.
基金the National Key Research and Development Program of China(Grant Nos.2017YFA0302904 and 2016YFA0300504)the National Natural Science Founation of China(Grant Nos.U1932215 and 11774419)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB33010100)。
文摘The Kitaev spin liquid(KSL) system has attracted tremendous attention in recent years because of its fundamental significance in condensed matter physics and promising applications in fault-tolerant topological quantum computation.Material realization of such a system remains a major challenge in the field due to the unusual configuration of anisotropic spin interactions,though great effort has been made before.Here we reveal that rare-earth chalcohalides REChX(RE=rare earth;Ch=O,S,Se,Te;X=F,Cl,Br,I) can serve as a family of KSL candidates.Most family members have the typical SmSI-type structure with a high symmetry of R3m,and rare-earth magnetic ions form an undistorted honeycomb lattice.The strong spin-orbit coupling of 4f electrons intrinsically offers anisotropic spin interactions as required by the Kitaev model.We have grown the crystals of YbOCl and synthesized the polycrystals of SmSI,ErOF,HoOF and DyOF,and made careful structural characterizations.We carry out magnetic and heat capacity measurements down to 1.8 K and find no obvious magnetic transition in all the samples but DyOF.The van der Waals interlayer coupling highlights the true two-dimensionality of the family which is vital for the exact realization of Abelian/non-Abelian anyons,and the graphene-like feature will be a prominent advantage for developing miniaturized devices.The family is expected to act as an inspiring material platform for the exploration of KSL physics.