Remarkable advances in fast magic-angle spinning(MAS)techniques significantly improve the resolution of^(1)H solid-state nuclear magnetic resonance(NMR)spectra.Here,we introduce a heteronuclear-filtered^(1)H homonucle...Remarkable advances in fast magic-angle spinning(MAS)techniques significantly improve the resolution of^(1)H solid-state nuclear magnetic resonance(NMR)spectra.Here,we introduce a heteronuclear-filtered^(1)H homonuclear multi-quantum(MQ)correlation strategy available at a MAS rate of 100 kHz by combining^(1)H{X}heteronuclear-filtered methods and^(1)H homonuclear MQ correlation experiments.The proposed strategy was applied to selectively extract^(1)H signals of aluminum lactate(Al-Lac)in a mixture of Al-Lac and zinc lactate(Zn-Lac)using 27Al-filtered methods(i.e.,^(1)H{27Al}heteronuclear multiple quantum correlation(HMQC)or^(1)H{27Al}symmetry-based resonance-echo saturationpulse double-resonance(S-RESPDOR)).We demonstrate that incorporating these 27Al-filtered methods into two-dimensional(2D)^(1)He^(1)H double-quantum(DQ)/single-quantum(SQ),triple-quantum(TQ)/SQ,and even three-dimensional(3D)27Al/^(1)H(DQ)/^(1)H(SQ)experiments can facilitate the acquisition of spectra without signal overlap and targeted characterization of the^(1)H species surrounding 27Al sites.The proposed strategy is considered to efficiently extract key structural information from complex spin systems.展开更多
Proton NMR-spectra of Wang resin bound compounds were obtained using the magic angle spinning 1HNMR technique with standard equipment. It was possible to analyse the spectra to evaluate their utility in solid-phase ch...Proton NMR-spectra of Wang resin bound compounds were obtained using the magic angle spinning 1HNMR technique with standard equipment. It was possible to analyse the spectra to evaluate their utility in solid-phase chernistry. A typical example was presented, which could directly monitor solid-phase reactions展开更多
Some proteins perform their biological functions by changing their material states through liquid-liquid phase separation.Upon phase separation,the protein condenses into a concentrated liquid phase and sometimes into...Some proteins perform their biological functions by changing their material states through liquid-liquid phase separation.Upon phase separation,the protein condenses into a concentrated liquid phase and sometimes into a gel phase,changing its dynamic properties and intermolecular interactions,thereby regulating cellular functions.Although the biological significance of this phenomenon has been widely recognized by researchers,there is still a lack of a comprehensive understanding of the structural and dynamic properties of the protein in the condensed phase.In this phase,molecules usually contain domains with varied dynamic properties and undergo intermediate exchanges.Magic angle spinning(MAS)solid-state NMR(SSNMR)experiments are very powerful in studying rigid protein polymers such as amyloid.The incorporation of solution-like experiments into SSNMR and the development of J-coupling based MAS SSNMR techniques extend its ability to study partially mobile segments of proteins in a condensed liquid or gel phase which are not visible by solution NMR or dipolar-coupling based SSNMR.Therefore,it has been applied in studying protein condensation and has provided very important information that is hard to obtain by other techniques.展开更多
To construct pulsed high magnet, with rapid adjustments to large changes in the field strength, it is a mandatory acces-sory to development a special NMR probes to provide a precise real-time map of the magnetic field...To construct pulsed high magnet, with rapid adjustments to large changes in the field strength, it is a mandatory acces-sory to development a special NMR probes to provide a precise real-time map of the magnetic field. In order to do so, it is necessary to understand the variations of the spin transition and susceptibility of NMR samples in a time dependent longitudinal field. This work analyzes the effect on the spin transition by a time dependent longitudinal field. For a 1/2 spin system, we have derived a simple formula for the prediction of the probabilities of occupation of the 1/2 and ?1/2 states in a non-static field. We also calculate the magnetic susceptibility of the water and give an analysis of the effect on the magnetic susceptibility in a time dependent longitudinal field and RF frequency.展开更多
Cross polarization(CP)is a widely used solid-state nuclear magnetic resonance(NMR)technique for enhancing the polarization of dilute S spins from much larger polarization of abundant I spins such as 1 H.To achieve suc...Cross polarization(CP)is a widely used solid-state nuclear magnetic resonance(NMR)technique for enhancing the polarization of dilute S spins from much larger polarization of abundant I spins such as 1 H.To achieve such a polarization transfer,the I spin should either be spin-locked or be converted to the dipolar ordered state through adiabatic demagnetization in the rotating frame.In this work,we analyze the spin dynamics of the Hartmann-Hahn CP(HHCP)utilizing the 1 H spin-locking,and the dipolar-order CP(DOCP)having the 1 H adiabatic demagnetization.We further propose an adiabatic demagnetization CP(ADCP)where a constant radio-frequency pulse is applied on the S spin while 1 H is adiabatically demagnetized.Our analyses indicate that ADCP utilizes the adiabatic passage to effectively achieve the polarization transfer from the 1 H to S spins.In addition,the dipolar ordered state generated during the 1 H demagnetization process could also be converted into the observable S polarization through DOCP,further enhancing the polarized signals.It is shown by both static and magic-angle-spinning(MAS)NMR experiments that ADCP has dramatically broadened the CP matching condition over the other CP schemes.Various samples have been used to demonstrate the polarization transfer efficiency of this newly proposed ADCP scheme.展开更多
C spin-lattice relaxtion times for polystyrene nanolatex particles have been investigated. It was found that the dramatic increase at 80℃ annealing temperature is well below the Tg temperature of bulk polystyrene, t...C spin-lattice relaxtion times for polystyrene nanolatex particles have been investigated. It was found that the dramatic increase at 80℃ annealing temperature is well below the Tg temperature of bulk polystyrene, the increase of relaxation time of aromatic carbons is larger than that of for aliphatic carbons at transition annealing temperature.展开更多
This paper investigates the concept of Cross Polarization (CP) experiment in addition to revisiting the two potential expansion schemes recently developed in the field of solid-state nuclear magnetic resonance (SSNMR)...This paper investigates the concept of Cross Polarization (CP) experiment in addition to revisiting the two potential expansion schemes recently developed in the field of solid-state nuclear magnetic resonance (SSNMR): namely, the Floquet-Magnus expansion and the Fer expansion. We use the aforementioned expansion schemes for the calculation of effective Hamiltonians and propagators when the spin system undergoes Cross Polarization radiation. CP is the gateway experiment into SSNMR. An in-depth comprehension of the underlying mechanics of spin dynamics during the cross-polarization experiment is pivotal for further experimental developments and optimization of more complex solid-state NMR experiments. The main contribution of this work is a prospect related to spin physics;particularly regarding to generalization of the calculation. This work reports original yet interesting novel ideas and developments that include calculations performed on the CP experiment. In fact, the approach presented could play a major role in the interpretation of several fine NMR experiments in solids, which would in turn provide significant new insights in spin physics. The generality of the work points towards potential applications in problems related in solid-state NMR and theoretical developments of spectroscopy as well as interdisciplinary research areas as long as they include spin dynamics concepts.展开更多
基金the National Natural Science Foundation of China(Grants,22161132028,221721177,22127801,U1932218 and 21733013)Hubei Provincial Natural Science Foundation(2021CFA021)Youth Innovation Promotion Association,Chinese Academy of Sciences(2019326)。
文摘Remarkable advances in fast magic-angle spinning(MAS)techniques significantly improve the resolution of^(1)H solid-state nuclear magnetic resonance(NMR)spectra.Here,we introduce a heteronuclear-filtered^(1)H homonuclear multi-quantum(MQ)correlation strategy available at a MAS rate of 100 kHz by combining^(1)H{X}heteronuclear-filtered methods and^(1)H homonuclear MQ correlation experiments.The proposed strategy was applied to selectively extract^(1)H signals of aluminum lactate(Al-Lac)in a mixture of Al-Lac and zinc lactate(Zn-Lac)using 27Al-filtered methods(i.e.,^(1)H{27Al}heteronuclear multiple quantum correlation(HMQC)or^(1)H{27Al}symmetry-based resonance-echo saturationpulse double-resonance(S-RESPDOR)).We demonstrate that incorporating these 27Al-filtered methods into two-dimensional(2D)^(1)He^(1)H double-quantum(DQ)/single-quantum(SQ),triple-quantum(TQ)/SQ,and even three-dimensional(3D)27Al/^(1)H(DQ)/^(1)H(SQ)experiments can facilitate the acquisition of spectra without signal overlap and targeted characterization of the^(1)H species surrounding 27Al sites.The proposed strategy is considered to efficiently extract key structural information from complex spin systems.
文摘Proton NMR-spectra of Wang resin bound compounds were obtained using the magic angle spinning 1HNMR technique with standard equipment. It was possible to analyse the spectra to evaluate their utility in solid-phase chernistry. A typical example was presented, which could directly monitor solid-phase reactions
基金supported by the National Natural Science Foundation of China(No.32171185,No.31770790)the National Key R&D Program of China(No.2017YFA0504804).
文摘Some proteins perform their biological functions by changing their material states through liquid-liquid phase separation.Upon phase separation,the protein condenses into a concentrated liquid phase and sometimes into a gel phase,changing its dynamic properties and intermolecular interactions,thereby regulating cellular functions.Although the biological significance of this phenomenon has been widely recognized by researchers,there is still a lack of a comprehensive understanding of the structural and dynamic properties of the protein in the condensed phase.In this phase,molecules usually contain domains with varied dynamic properties and undergo intermediate exchanges.Magic angle spinning(MAS)solid-state NMR(SSNMR)experiments are very powerful in studying rigid protein polymers such as amyloid.The incorporation of solution-like experiments into SSNMR and the development of J-coupling based MAS SSNMR techniques extend its ability to study partially mobile segments of proteins in a condensed liquid or gel phase which are not visible by solution NMR or dipolar-coupling based SSNMR.Therefore,it has been applied in studying protein condensation and has provided very important information that is hard to obtain by other techniques.
文摘To construct pulsed high magnet, with rapid adjustments to large changes in the field strength, it is a mandatory acces-sory to development a special NMR probes to provide a precise real-time map of the magnetic field. In order to do so, it is necessary to understand the variations of the spin transition and susceptibility of NMR samples in a time dependent longitudinal field. This work analyzes the effect on the spin transition by a time dependent longitudinal field. For a 1/2 spin system, we have derived a simple formula for the prediction of the probabilities of occupation of the 1/2 and ?1/2 states in a non-static field. We also calculate the magnetic susceptibility of the water and give an analysis of the effect on the magnetic susceptibility in a time dependent longitudinal field and RF frequency.
基金supported by the NSF Cooperative Agreement DMR-1644779the State of Florida.X.H.P.acknowledges the supports from the National Key R&D Program of China(Grants No.2018YFA0306600)+1 种基金the National Science Foundation of China(Grants No.11927811,12150014)Anhui Initiative in Quantum Information Technologies(Grant No.AHY050000).
文摘Cross polarization(CP)is a widely used solid-state nuclear magnetic resonance(NMR)technique for enhancing the polarization of dilute S spins from much larger polarization of abundant I spins such as 1 H.To achieve such a polarization transfer,the I spin should either be spin-locked or be converted to the dipolar ordered state through adiabatic demagnetization in the rotating frame.In this work,we analyze the spin dynamics of the Hartmann-Hahn CP(HHCP)utilizing the 1 H spin-locking,and the dipolar-order CP(DOCP)having the 1 H adiabatic demagnetization.We further propose an adiabatic demagnetization CP(ADCP)where a constant radio-frequency pulse is applied on the S spin while 1 H is adiabatically demagnetized.Our analyses indicate that ADCP utilizes the adiabatic passage to effectively achieve the polarization transfer from the 1 H to S spins.In addition,the dipolar ordered state generated during the 1 H demagnetization process could also be converted into the observable S polarization through DOCP,further enhancing the polarized signals.It is shown by both static and magic-angle-spinning(MAS)NMR experiments that ADCP has dramatically broadened the CP matching condition over the other CP schemes.Various samples have been used to demonstrate the polarization transfer efficiency of this newly proposed ADCP scheme.
基金This work was supported by National Key Project for Fundamental Research (N.95-11) and National Natural Science Foundation of Ch
文摘C spin-lattice relaxtion times for polystyrene nanolatex particles have been investigated. It was found that the dramatic increase at 80℃ annealing temperature is well below the Tg temperature of bulk polystyrene, the increase of relaxation time of aromatic carbons is larger than that of for aliphatic carbons at transition annealing temperature.
文摘This paper investigates the concept of Cross Polarization (CP) experiment in addition to revisiting the two potential expansion schemes recently developed in the field of solid-state nuclear magnetic resonance (SSNMR): namely, the Floquet-Magnus expansion and the Fer expansion. We use the aforementioned expansion schemes for the calculation of effective Hamiltonians and propagators when the spin system undergoes Cross Polarization radiation. CP is the gateway experiment into SSNMR. An in-depth comprehension of the underlying mechanics of spin dynamics during the cross-polarization experiment is pivotal for further experimental developments and optimization of more complex solid-state NMR experiments. The main contribution of this work is a prospect related to spin physics;particularly regarding to generalization of the calculation. This work reports original yet interesting novel ideas and developments that include calculations performed on the CP experiment. In fact, the approach presented could play a major role in the interpretation of several fine NMR experiments in solids, which would in turn provide significant new insights in spin physics. The generality of the work points towards potential applications in problems related in solid-state NMR and theoretical developments of spectroscopy as well as interdisciplinary research areas as long as they include spin dynamics concepts.
