We propose a new scheme for realizing deterministic quantum state transfer (QST) between two spatially separated single molecule magnets (SMMs) with the framework of cavity quantum eleetrodynamics (QED). In the ...We propose a new scheme for realizing deterministic quantum state transfer (QST) between two spatially separated single molecule magnets (SMMs) with the framework of cavity quantum eleetrodynamics (QED). In the present scheme, two SMMs are trapped in two spatially separated optical cavities coupled by an optical fiber. Through strictly numerically simulating, we demonstrate that our scheme is robust with respect to the SMMs' spontaneous decay and fiber loss under the conditions of dispersive SMMs-field interaction and strong coupling of cavity fiber. In addition, we also discuss the influence of photon leakage out of cavities and show that our proposal is good enough to demonstrate the generation of QST with high fidelity utilizing the current experimental technology. The present investigation provides research opportunities for realizing QST between solid-state qubits and may result in a substantial impact on the progress of solid-state-based quantum communications network.展开更多
The syntheses, crystal structures, magnetic and luminescent properties of three isornorphous compounds [LnIII6(,u4-O)2(C4A)2- (NO3)2(HCOO)2(CH30)2(DMF)4(CH3OH)4] (Ln = Gd (1), Tb (2) and Dy (3); H...The syntheses, crystal structures, magnetic and luminescent properties of three isornorphous compounds [LnIII6(,u4-O)2(C4A)2- (NO3)2(HCOO)2(CH30)2(DMF)4(CH3OH)4] (Ln = Gd (1), Tb (2) and Dy (3); H4C4A = p-tert-butylcalix[4]arene) are reported. These three compounds are featured with the sandwich-like units constructed by two tail-to-tail calixarene molecules and an in-between Lnm6 octahedron. The DyTM compound exhibits both single molecule magnet behavior and photoluminescence.展开更多
Molecules with multifunctional properties are of immense interest in hybrid materials, while challenges still existed because of the limited compatibility of multiple functionalities in a single system. In this work, ...Molecules with multifunctional properties are of immense interest in hybrid materials, while challenges still existed because of the limited compatibility of multiple functionalities in a single system. In this work, a series of metal-organic complexes were synthesized and characterized under the assembly of electron donor phosphonate, electron acceptor polypyridine ligand and spin carrier rare earth ions. All the compounds exhibited remarkable and reversible responses with photochromism and photomodulated fluorescence, originated from photogenerated radicals via electron transfer from phosphonates to polypyridine ligands. For the Dy analog, slow magnetic relaxation was observed at cryogenic temperature, indicating the single-molecule magnetic behavior. Furthermore, photogenerated radicals could enhance the proton conductive behavior, with about 2 times larger in magnitude after light irradiation for Dy and Y compounds. The introduction of photoluminescence, magnetism and proton conduction into metallic phosphonates can provide potential applications for photochromic materials.展开更多
Reaction of [Mn(TTF-salphen)][OAc] (TTF-salphen2=2,2'-((2-(4,5-bis(methylthio)-1,3-dithiol-2-ylidene)-1,3-benzodithiole- 5,6-diyl)bis(nitrilomethylidyne)bis(pbenolate)dianion) and the cyanometalate bui...Reaction of [Mn(TTF-salphen)][OAc] (TTF-salphen2=2,2'-((2-(4,5-bis(methylthio)-1,3-dithiol-2-ylidene)-1,3-benzodithiole- 5,6-diyl)bis(nitrilomethylidyne)bis(pbenolate)dianion) and the cyanometalate building blocks [n-Bu4N][(Tp)Fe(CN)3] (Tp =Tris(pyrazolyl)hydroborate) or [n-Bu4N][Ru(salen)(CN)2] (salen2 =N,N'-ethylenebis(salicylideneimine)dianion) resulted in the formation of two redox-active complexes, the dinuclear heterometallic complex [(Tp)Fe(CN)3Mn(TTF-salphen)'CH3OH] (1) and the one dimensional complex [Ru(salen)(CN)2Mn(TTF-salphen)]n (2). Both complexes were characterized by X-ray crystallography and solid state electrochemistry, in addition to static and dynamic magnetic measurements. Antiferromagnetic couplings are found to be operative between metal ion centers bridged by cyanide in both complexes. Complex 1 exhibited field-induced SMM behavior with an energy barrier of 13.8 K. The introduction of the redox-active TTF unit into cyanidebridged complexes with interesting magnetic properties renders them promising candidates for the construction of new hybrid inorganic-organic materials.展开更多
In considering next-nearest neighbor (NNN) coupling, we numerically investigate the magnetoelastic instability in ring-shaped mesoscopic antiferromagnetic Heisenberg spin 1/2 systems with spin-phonon interaction. Th...In considering next-nearest neighbor (NNN) coupling, we numerically investigate the magnetoelastic instability in ring-shaped mesoscopic antiferromagnetic Heisenberg spin 1/2 systems with spin-phonon interaction. The results indicate that, for antiferromagnetic NNN coupling J2, there may be a critical value J2^c, at which the ground state is dimerized for arbitrary lattice spring constant and beyond and below which the magnetoelastic instability behavior is different from each other. The values of J2^c are irrelevant to the system size. For ferromagnetic NNN coupling, only continuous transition is present from dimerized phase to uniform phase as lattice spring constant is increased.展开更多
Single molecule magnets(SMMs) with large magnetic anisotropy energy(MAE) have great potential applications in magnetic recording.Using the first-principles calculations,we investigate the MAE of 5 d transition metal-p...Single molecule magnets(SMMs) with large magnetic anisotropy energy(MAE) have great potential applications in magnetic recording.Using the first-principles calculations,we investigate the MAE of 5 d transition metal-porphyrin-based SMMs by using the PBE and PBE+U with different U values,respectively.The results indicate that W-P,Re-P,Os-P,and Ir-P possess the considerably large MAE among 5 d TM-P SMMs.Furthermore,the MAE of 5 d TM-P can be facilely manipulated by tensile strain.The reduction of the absolute value of MAE for Ir-P molecule caused by tensile strain makes it easier to implement the writing operation.The decreasing of the occupation number of minority-spin channels of Ir-d_(x^(2)-y^(2)) orbital leads the MAE to decrease when the tensile strain increases.展开更多
Dephasing mechanism of quantum tunnelling in molecular magnets has been studied by means of the spin-coherentstate path integral in a mean field approximation. It is found that the fluctuating uncompensated transverse...Dephasing mechanism of quantum tunnelling in molecular magnets has been studied by means of the spin-coherentstate path integral in a mean field approximation. It is found that the fluctuating uncompensated transverse field from the dipolar-dipolar interaction between molecular magnets contributes a random phase to the quantum interference phase. The resulting transition rate is determined by the average tunnel splitting over the random phase. Such a dephasing process leads to the suppression of quenching due to the quantum phase interference, and to the steps due to odd resonances in hysteresis loop survived, which is in good agreement with experimental observations in molecular nanomagnets Fes and Mn12.展开更多
Spin parity effect on magnetic relaxation by quantum tunneling in the biaxial spin model is studied by taking into account the transverse local stray field. It is shown that the square root time dependence in the even...Spin parity effect on magnetic relaxation by quantum tunneling in the biaxial spin model is studied by taking into account the transverse local stray field. It is shown that the square root time dependence in the even resonance occurs in the presence of a distribution of transverse anisotropic parameters, while the odd resonance always shows exponential relaxation. Magnetic relaxation under a sweeping field is also studied. The variation of the relaxation curve with the increasing distribution width of the local stray field for even resonance is qualitatively different from that of the odd resonance. The theoretical result on even resonance is in agreement with experimental results on Fe8 system, while the prediction for odd resonance awaits the experimental verification.展开更多
The quantum tunnelling of magnetization (QTM) in single crystals of the single molecule magnet (Mn1-xCrx)12- Ac (x=0, 0.03, 0.04, 0.05) has been investigated. In comparison with its parent Mnl2-Ac, a greater rat...The quantum tunnelling of magnetization (QTM) in single crystals of the single molecule magnet (Mn1-xCrx)12- Ac (x=0, 0.03, 0.04, 0.05) has been investigated. In comparison with its parent Mnl2-Ac, a greater rate of magnetization relaxation and a lower effective potential-energy barrier have been observed in Cr-doping samples. This modulation of QTM due to the Cr-doping could be attributed to the small change of Sz due to the smaller spin of Cr itself and additional intrinsic but distributed transverse and longitudinal anisotropy raised by a subtle change of the local environment in the magnetic Mn12 core.展开更多
Dysprosium compounds with high magnetic anisotropy are widely studied as single molecule magnets(SMMs).Here the anisotropic magnetocaloric effect in a Dy(Ⅲ)SMM,{[Dy(OSiMe_(3))_(2)(4-Mepy)5(BPh_(4))]0.5 Toluene},was s...Dysprosium compounds with high magnetic anisotropy are widely studied as single molecule magnets(SMMs).Here the anisotropic magnetocaloric effect in a Dy(Ⅲ)SMM,{[Dy(OSiMe_(3))_(2)(4-Mepy)5(BPh_(4))]0.5 Toluene},was studied by single crystals.Angular dependent magnetization can be observed at 300 K because of its high magnetic anisotropy.SMM behavior measured along the easy axis direction is identical to that of the polycrystalline sample.Rotating magnetization from the easy axis to the hard plane gives a maximum magnetic entropy change(-ΔSR)of 3.05 J/(kg·K)at 19 K atΔB=5 T,which enables the Dy(Ⅲ)SMM to be used as a low-temperature rotating magnetic refrigerant.展开更多
Metal-organic frameworks(MOFs)with inherent porosity and suspended acidic groups are promising proton conducting materials in water or aqua-ammonia media.Herein we report a new lanthanide phosphonate,namely,Dy_(2)(amp...Metal-organic frameworks(MOFs)with inherent porosity and suspended acidic groups are promising proton conducting materials in water or aqua-ammonia media.Herein we report a new lanthanide phosphonate,namely,Dy_(2)(amp_(2)H_(2))_(2)(mal)(H_(2)O)_(2)·5H2O(MDAF-6).It possesses a 3D open-framework structure,and shows a high NH_(3)adsorption capacity of 142.4 cm^(3)/g at P/P0=0.98 at 298 K due to acid-base interaction.Interestingly,the proton conductivity of MDAF-6-NH3 is enhanced by five orders of magnitude compared to MDAF-6 after 8.5 h exposure in saturated NH_(3)-H_(2)O vapor,indicating the importance of coexistent conjugate acid-base pairs of H_(3)O+-H_(2)O and NH_(4)^(+)-NH_(3)in promoting proton conduction.Magnetic studies of MDAF-6 revealed slow magnetization relaxation under zero dc field,characteristic of singlemolecule magnet behavior.This work provides not only a new multifunctional MOF material,but also a new strategy to improve proton conduction in aqua-ammonia medium.展开更多
Dinuclear ytterbium and erbium based bifunction complexes Ln_(2) L_(2)(depma_(2))Cl_(2)(1-Ln,Ln=Yb and Er,H_(2) L=N~1,N~3-bis(salicylideneimino)diethylenetriamine,depma_(2)=dimerized 9-diethyl-phosphonomethylanthracen...Dinuclear ytterbium and erbium based bifunction complexes Ln_(2) L_(2)(depma_(2))Cl_(2)(1-Ln,Ln=Yb and Er,H_(2) L=N~1,N~3-bis(salicylideneimino)diethylenetriamine,depma_(2)=dimerized 9-diethyl-phosphonomethylanthracene)are reported.They undergo thermo-induced consecutive phase transitions,first the dissociation of depma_(2) ligand forming LnL(depma)Cl(2-Ln)and then the release of chloroethane forming LnL(epma)(3-Ln,epma=9-ethylphosphonomethylanthrancene).The structural transformations are accompanied with synergetic switch of the luminescence in visible and NIR regions and also magnetic dynamics.展开更多
基金Supported by the Natural Science Foundation of China under Grant Nos.10575040,90503010,10634060,and 10874050 National Basic Research Program of China under Grant No.2005CB724508+1 种基金the Foundation from the Ministry of the National Education of China under Grant No.200804870051 the Science Innovation Foundation of Huazhong University of Science and Technology under Grant No.HF-06-010-08-012
文摘We propose a new scheme for realizing deterministic quantum state transfer (QST) between two spatially separated single molecule magnets (SMMs) with the framework of cavity quantum eleetrodynamics (QED). In the present scheme, two SMMs are trapped in two spatially separated optical cavities coupled by an optical fiber. Through strictly numerically simulating, we demonstrate that our scheme is robust with respect to the SMMs' spontaneous decay and fiber loss under the conditions of dispersive SMMs-field interaction and strong coupling of cavity fiber. In addition, we also discuss the influence of photon leakage out of cavities and show that our proposal is good enough to demonstrate the generation of QST with high fidelity utilizing the current experimental technology. The present investigation provides research opportunities for realizing QST between solid-state qubits and may result in a substantial impact on the progress of solid-state-based quantum communications network.
基金financially supported by the National Natural Science Foundation of China (20971119, 51074148, 91026024)
文摘The syntheses, crystal structures, magnetic and luminescent properties of three isornorphous compounds [LnIII6(,u4-O)2(C4A)2- (NO3)2(HCOO)2(CH30)2(DMF)4(CH3OH)4] (Ln = Gd (1), Tb (2) and Dy (3); H4C4A = p-tert-butylcalix[4]arene) are reported. These three compounds are featured with the sandwich-like units constructed by two tail-to-tail calixarene molecules and an in-between Lnm6 octahedron. The DyTM compound exhibits both single molecule magnet behavior and photoluminescence.
基金supported by the National Natural Science Foundation of China (Nos. 21901133 and 22071126)Key Research and Development Project of Shandong Province (No. 2019GGX102006)the State Key Laboratory of Fine Chemicals (No. KF1905)。
文摘Molecules with multifunctional properties are of immense interest in hybrid materials, while challenges still existed because of the limited compatibility of multiple functionalities in a single system. In this work, a series of metal-organic complexes were synthesized and characterized under the assembly of electron donor phosphonate, electron acceptor polypyridine ligand and spin carrier rare earth ions. All the compounds exhibited remarkable and reversible responses with photochromism and photomodulated fluorescence, originated from photogenerated radicals via electron transfer from phosphonates to polypyridine ligands. For the Dy analog, slow magnetic relaxation was observed at cryogenic temperature, indicating the single-molecule magnetic behavior. Furthermore, photogenerated radicals could enhance the proton conductive behavior, with about 2 times larger in magnitude after light irradiation for Dy and Y compounds. The introduction of photoluminescence, magnetism and proton conduction into metallic phosphonates can provide potential applications for photochromic materials.
基金supported by the National Basic Research Program of China(2011CB808704,2013CB922101)the National Natural Science Foundation of China(51173075,91022031)the Australian Research Council
文摘Reaction of [Mn(TTF-salphen)][OAc] (TTF-salphen2=2,2'-((2-(4,5-bis(methylthio)-1,3-dithiol-2-ylidene)-1,3-benzodithiole- 5,6-diyl)bis(nitrilomethylidyne)bis(pbenolate)dianion) and the cyanometalate building blocks [n-Bu4N][(Tp)Fe(CN)3] (Tp =Tris(pyrazolyl)hydroborate) or [n-Bu4N][Ru(salen)(CN)2] (salen2 =N,N'-ethylenebis(salicylideneimine)dianion) resulted in the formation of two redox-active complexes, the dinuclear heterometallic complex [(Tp)Fe(CN)3Mn(TTF-salphen)'CH3OH] (1) and the one dimensional complex [Ru(salen)(CN)2Mn(TTF-salphen)]n (2). Both complexes were characterized by X-ray crystallography and solid state electrochemistry, in addition to static and dynamic magnetic measurements. Antiferromagnetic couplings are found to be operative between metal ion centers bridged by cyanide in both complexes. Complex 1 exhibited field-induced SMM behavior with an energy barrier of 13.8 K. The introduction of the redox-active TTF unit into cyanidebridged complexes with interesting magnetic properties renders them promising candidates for the construction of new hybrid inorganic-organic materials.
文摘In considering next-nearest neighbor (NNN) coupling, we numerically investigate the magnetoelastic instability in ring-shaped mesoscopic antiferromagnetic Heisenberg spin 1/2 systems with spin-phonon interaction. The results indicate that, for antiferromagnetic NNN coupling J2, there may be a critical value J2^c, at which the ground state is dimerized for arbitrary lattice spring constant and beyond and below which the magnetoelastic instability behavior is different from each other. The values of J2^c are irrelevant to the system size. For ferromagnetic NNN coupling, only continuous transition is present from dimerized phase to uniform phase as lattice spring constant is increased.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.21403144,11464038,11134005,and 51472113)the National Key Project for Basic Research of China(Grant Nos.2013CB922103 and 2015CB921203)。
文摘Single molecule magnets(SMMs) with large magnetic anisotropy energy(MAE) have great potential applications in magnetic recording.Using the first-principles calculations,we investigate the MAE of 5 d transition metal-porphyrin-based SMMs by using the PBE and PBE+U with different U values,respectively.The results indicate that W-P,Re-P,Os-P,and Ir-P possess the considerably large MAE among 5 d TM-P SMMs.Furthermore,the MAE of 5 d TM-P can be facilely manipulated by tensile strain.The reduction of the absolute value of MAE for Ir-P molecule caused by tensile strain makes it easier to implement the writing operation.The decreasing of the occupation number of minority-spin channels of Ir-d_(x^(2)-y^(2)) orbital leads the MAE to decrease when the tensile strain increases.
基金Project supported by the National Natural Science Foundation of China (Grant No 10575045)
文摘Dephasing mechanism of quantum tunnelling in molecular magnets has been studied by means of the spin-coherentstate path integral in a mean field approximation. It is found that the fluctuating uncompensated transverse field from the dipolar-dipolar interaction between molecular magnets contributes a random phase to the quantum interference phase. The resulting transition rate is determined by the average tunnel splitting over the random phase. Such a dephasing process leads to the suppression of quenching due to the quantum phase interference, and to the steps due to odd resonances in hysteresis loop survived, which is in good agreement with experimental observations in molecular nanomagnets Fes and Mn12.
基金National Natural Science Foundation of China under Grant No.10575045
文摘Spin parity effect on magnetic relaxation by quantum tunneling in the biaxial spin model is studied by taking into account the transverse local stray field. It is shown that the square root time dependence in the even resonance occurs in the presence of a distribution of transverse anisotropic parameters, while the odd resonance always shows exponential relaxation. Magnetic relaxation under a sweeping field is also studied. The variation of the relaxation curve with the increasing distribution width of the local stray field for even resonance is qualitatively different from that of the odd resonance. The theoretical result on even resonance is in agreement with experimental results on Fe8 system, while the prediction for odd resonance awaits the experimental verification.
基金Project supported by the National Natural Science Foundation of China (Grant No 10505029).
文摘The quantum tunnelling of magnetization (QTM) in single crystals of the single molecule magnet (Mn1-xCrx)12- Ac (x=0, 0.03, 0.04, 0.05) has been investigated. In comparison with its parent Mnl2-Ac, a greater rate of magnetization relaxation and a lower effective potential-energy barrier have been observed in Cr-doping samples. This modulation of QTM due to the Cr-doping could be attributed to the small change of Sz due to the smaller spin of Cr itself and additional intrinsic but distributed transverse and longitudinal anisotropy raised by a subtle change of the local environment in the magnetic Mn12 core.
基金Project supported by Shenzhen Science and Technology Program(JCYJ20180306170859634)National Natural Science Foundation of China(21620102002,21773130,21871219,21801202,21971203)+3 种基金China Postdoctoral Science Foundation(2019T120891,2019T120892,2018M643615,2018M631138)Postdoctoral Foundation of Shaanxi Province(2018BSHEDZZ100)Natural Science Basic Research Plan in Shaanxi Province(2019JQ-292)Key Laboratory Construction Program of Xi’an Municipal Bureau of Science and Technology(201805056ZD7CG40)。
文摘Dysprosium compounds with high magnetic anisotropy are widely studied as single molecule magnets(SMMs).Here the anisotropic magnetocaloric effect in a Dy(Ⅲ)SMM,{[Dy(OSiMe_(3))_(2)(4-Mepy)5(BPh_(4))]0.5 Toluene},was studied by single crystals.Angular dependent magnetization can be observed at 300 K because of its high magnetic anisotropy.SMM behavior measured along the easy axis direction is identical to that of the polycrystalline sample.Rotating magnetization from the easy axis to the hard plane gives a maximum magnetic entropy change(-ΔSR)of 3.05 J/(kg·K)at 19 K atΔB=5 T,which enables the Dy(Ⅲ)SMM to be used as a low-temperature rotating magnetic refrigerant.
基金the National Natural Science Foundation of China(No.21731003).
文摘Metal-organic frameworks(MOFs)with inherent porosity and suspended acidic groups are promising proton conducting materials in water or aqua-ammonia media.Herein we report a new lanthanide phosphonate,namely,Dy_(2)(amp_(2)H_(2))_(2)(mal)(H_(2)O)_(2)·5H2O(MDAF-6).It possesses a 3D open-framework structure,and shows a high NH_(3)adsorption capacity of 142.4 cm^(3)/g at P/P0=0.98 at 298 K due to acid-base interaction.Interestingly,the proton conductivity of MDAF-6-NH3 is enhanced by five orders of magnitude compared to MDAF-6 after 8.5 h exposure in saturated NH_(3)-H_(2)O vapor,indicating the importance of coexistent conjugate acid-base pairs of H_(3)O+-H_(2)O and NH_(4)^(+)-NH_(3)in promoting proton conduction.Magnetic studies of MDAF-6 revealed slow magnetization relaxation under zero dc field,characteristic of singlemolecule magnet behavior.This work provides not only a new multifunctional MOF material,but also a new strategy to improve proton conduction in aqua-ammonia medium.
基金supported by grants from the National Key R&D Program of China(Nos.2017YFA0303203,2018YFA0306004)the National Natural Science Foundation of China(No.21731003)。
文摘Dinuclear ytterbium and erbium based bifunction complexes Ln_(2) L_(2)(depma_(2))Cl_(2)(1-Ln,Ln=Yb and Er,H_(2) L=N~1,N~3-bis(salicylideneimino)diethylenetriamine,depma_(2)=dimerized 9-diethyl-phosphonomethylanthracene)are reported.They undergo thermo-induced consecutive phase transitions,first the dissociation of depma_(2) ligand forming LnL(depma)Cl(2-Ln)and then the release of chloroethane forming LnL(epma)(3-Ln,epma=9-ethylphosphonomethylanthrancene).The structural transformations are accompanied with synergetic switch of the luminescence in visible and NIR regions and also magnetic dynamics.