A method to compute the numerical derivative of eigenvalues of parameterized crystal field Hamiltonian matrix is given, based on the numerical derivatives the general iteration methods such as Levenberg-Marquardt, New...A method to compute the numerical derivative of eigenvalues of parameterized crystal field Hamiltonian matrix is given, based on the numerical derivatives the general iteration methods such as Levenberg-Marquardt, Newton method, and so on, can be used to solve crystal field parameters by fitting to experimental energy levels. With the numerical eigenvalue derivative, a detailed iteration algorithm to compute crystal field parameters by fitting experimental energy levels has also been described. This method is used to compute the crystal parameters of Yb^3＋ in Sc2O3 crystal, which is prepared by a co-precipitation method and whose structure was refined by Rietveld method. By fitting on the parameters of a simple overlap model of crystal field, the results show that the new method can fit the crystal field energy splitting with fast convergence and good stability.展开更多
Nonlinear optical(NLO)crystals are the key fundamental materials in modern optoelectronic information technology,which play an irre-placeable role in modern quantum optics and photonics in addition to traditional lase...Nonlinear optical(NLO)crystals are the key fundamental materials in modern optoelectronic information technology,which play an irre-placeable role in modern quantum optics and photonics in addition to traditional laser frequency conversion applications[1,2].Especially at a time when the international competition of quantum information tech-nology is becoming increasingly intense,high-performing NLO crystals as the strategic materials for optical quantum technology have received continuous attention from physical chemists and materials scientists.展开更多
It is challenging to cooperatively improve the nonlinear optical(NLO)efficiency and the laser-induced damage threshold(LIDT).This work reports a novel IR NLO materials CsInP_(2)S_(7)(CIPS)designed by combination the s...It is challenging to cooperatively improve the nonlinear optical(NLO)efficiency and the laser-induced damage threshold(LIDT).This work reports a novel IR NLO materials CsInP_(2)S_(7)(CIPS)designed by combination the strategies of alkali metals substitution and microscopic NLO units PS4 introduction based on AgGaS_(2).CIPS was composed of strongly distorted[InS_(6)]^(9-)octahedra and[P_(2)S_(7)]4-dimers constructed by corner-sharing[PS_(4)]^(3-),which increase the NLO efficiency and decrease thermal expansion anisotropy simultaneously.Compared with AgGaS_(2),CIPS exhibited strong phase matchable NLO response ca.1.1×AGS@2.1μm,high LIDT ca.20.8×AgGaS_(2),and IR transparency up to 15.3μm.Structural analysis and theoretical investigation confirmed that large SHG effect and ultrahigh LIDT of CIPS originated from the synergistic contribution of[InS_(6)]^(9-)octahedra and[P_(2)S_(7)]4-dimers.These results indicate that CIPS is a promising NLO candidate in the mid-IR region,and this study provides a new approach for developing potential NLO-LIDT compatible materials.展开更多
Deep-ultraviolet (DUV, wavelength λ < 200 nm) nonlinear optical (NLO) crystal is the core component of frequency conversion to generate DUV laser, which plays an important role in cutting-edge laser technology and...Deep-ultraviolet (DUV, wavelength λ < 200 nm) nonlinear optical (NLO) crystal is the core component of frequency conversion to generate DUV laser, which plays an important role in cutting-edge laser technology and fundamental science. Significant progress has been made in both experimental exploration and theoretical design in the field of DUV NLO crystals over the past three decades. In-depth insight into “structure-property correlations”, in particular, allows for rigorous and precise identification of DUV NLO crystals. In this article, we reviewed the current experimental and theoretical research progress while elucidating the core concepts and stringent criteria of qualified DUV phase-matched second-harmonic generation crystals. We also discussed the development of the DUV NLO “structure-property correlations” from first principles and how it has sparked interest in related materials, as well as future directions for obtaining potential DUV NLO crystals.展开更多
Interlayer sliding modulation in van der Waals(vdW)layered materials opens opportunities to seek tunable applications for photonics and optoelectronics at the nanoscale.In this work,focusing on ternary chalcogenides,d...Interlayer sliding modulation in van der Waals(vdW)layered materials opens opportunities to seek tunable applications for photonics and optoelectronics at the nanoscale.In this work,focusing on ternary chalcogenides,dozens of typical vdW layered materials with the formula of A_(2)MZ_(4)(A,M=metal cation;Z=S/Se)were systematically classified and studied to illustrate the interlayer sliding modulation performance on nonlinear optical(NLO)effect and underlying mechanism.Based on first-principles analysis,the screened Cd_(2)GeSe_(4) exhibits large second harmonic generation(SHG)deviation(>36 times between high-and low-SHG states)under sliding among all studied materials.This phenomenon arises from the polarization modulation induced by the vdW interlayer charge redistribution of two tetrahedral primitives in the ternary edge-sharing tetrahedral structures.Our findings present a strategy to substantially modulate NLO properties by altering the interlayer charge coupling which is commonly thought to be very weak in vdW layered materials.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant Nos.50772112 and 50872135)the Natural Science Foundation of Anhui Province of China(Grant No.08040106820)the Knowledge Innovation Program of the Chinese Academy of Sciences(Grant No.YYYJ-1002)
文摘A method to compute the numerical derivative of eigenvalues of parameterized crystal field Hamiltonian matrix is given, based on the numerical derivatives the general iteration methods such as Levenberg-Marquardt, Newton method, and so on, can be used to solve crystal field parameters by fitting to experimental energy levels. With the numerical eigenvalue derivative, a detailed iteration algorithm to compute crystal field parameters by fitting experimental energy levels has also been described. This method is used to compute the crystal parameters of Yb^3＋ in Sc2O3 crystal, which is prepared by a co-precipitation method and whose structure was refined by Rietveld method. By fitting on the parameters of a simple overlap model of crystal field, the results show that the new method can fit the crystal field energy splitting with fast convergence and good stability.
基金supported by the National Natural Science Foundation of China(Grat Nos.12174404 and 22133004)the Open Research Fund Program of the State Key Laboratory of Low-Dimensional Quantum Physics
文摘Nonlinear optical(NLO)crystals are the key fundamental materials in modern optoelectronic information technology,which play an irre-placeable role in modern quantum optics and photonics in addition to traditional laser frequency conversion applications[1,2].Especially at a time when the international competition of quantum information tech-nology is becoming increasingly intense,high-performing NLO crystals as the strategic materials for optical quantum technology have received continuous attention from physical chemists and materials scientists.
基金the Natural Science Foundation of China(No.22105218).
文摘It is challenging to cooperatively improve the nonlinear optical(NLO)efficiency and the laser-induced damage threshold(LIDT).This work reports a novel IR NLO materials CsInP_(2)S_(7)(CIPS)designed by combination the strategies of alkali metals substitution and microscopic NLO units PS4 introduction based on AgGaS_(2).CIPS was composed of strongly distorted[InS_(6)]^(9-)octahedra and[P_(2)S_(7)]4-dimers constructed by corner-sharing[PS_(4)]^(3-),which increase the NLO efficiency and decrease thermal expansion anisotropy simultaneously.Compared with AgGaS_(2),CIPS exhibited strong phase matchable NLO response ca.1.1×AGS@2.1μm,high LIDT ca.20.8×AgGaS_(2),and IR transparency up to 15.3μm.Structural analysis and theoretical investigation confirmed that large SHG effect and ultrahigh LIDT of CIPS originated from the synergistic contribution of[InS_(6)]^(9-)octahedra and[P_(2)S_(7)]4-dimers.These results indicate that CIPS is a promising NLO candidate in the mid-IR region,and this study provides a new approach for developing potential NLO-LIDT compatible materials.
基金the National Natural Science Foundation of China(Grant Nos.12174404 and 22133004).
文摘Deep-ultraviolet (DUV, wavelength λ < 200 nm) nonlinear optical (NLO) crystal is the core component of frequency conversion to generate DUV laser, which plays an important role in cutting-edge laser technology and fundamental science. Significant progress has been made in both experimental exploration and theoretical design in the field of DUV NLO crystals over the past three decades. In-depth insight into “structure-property correlations”, in particular, allows for rigorous and precise identification of DUV NLO crystals. In this article, we reviewed the current experimental and theoretical research progress while elucidating the core concepts and stringent criteria of qualified DUV phase-matched second-harmonic generation crystals. We also discussed the development of the DUV NLO “structure-property correlations” from first principles and how it has sparked interest in related materials, as well as future directions for obtaining potential DUV NLO crystals.
基金This work is supported by the National Natural Science Foundation of China(Grant No.12174404 and 22133004)the Open Research Fund Program of the State Key Laboratory of Low-Dimensional Quantum Physics.The authors thank Dr.Bonan Zhu and Xuanlin Pan for helpful discussion.
文摘Interlayer sliding modulation in van der Waals(vdW)layered materials opens opportunities to seek tunable applications for photonics and optoelectronics at the nanoscale.In this work,focusing on ternary chalcogenides,dozens of typical vdW layered materials with the formula of A_(2)MZ_(4)(A,M=metal cation;Z=S/Se)were systematically classified and studied to illustrate the interlayer sliding modulation performance on nonlinear optical(NLO)effect and underlying mechanism.Based on first-principles analysis,the screened Cd_(2)GeSe_(4) exhibits large second harmonic generation(SHG)deviation(>36 times between high-and low-SHG states)under sliding among all studied materials.This phenomenon arises from the polarization modulation induced by the vdW interlayer charge redistribution of two tetrahedral primitives in the ternary edge-sharing tetrahedral structures.Our findings present a strategy to substantially modulate NLO properties by altering the interlayer charge coupling which is commonly thought to be very weak in vdW layered materials.
