Nitrogen-14(^(14)N)overtone(OT)spectroscopy under fast magic angle spinning(MAS)conditions(>60 kHz)has emerged as a powerful technique for observing correlations and distances between ^(14)N and ^(1)H,owing to the ...Nitrogen-14(^(14)N)overtone(OT)spectroscopy under fast magic angle spinning(MAS)conditions(>60 kHz)has emerged as a powerful technique for observing correlations and distances between ^(14)N and ^(1)H,owing to the absence of the first-order quadrupolar broadenings.In addition,^(14)N^(OT) allows selective manipulation of ^(14)N nuclei for each site.Despite extensive theoretical and experimental studies,the spin dynamics of ^(14)N^(OT) remains under debate.In this study,we conducted experimental investigations to assess the spin dynamics of ^(14)N^(OT) using the rotational-echo saturation-pulse double-resonance(RESPDOR)sequence,which monitors population transfer induced by a^(14)N^(OT) pulse.The ^(14)N^(OT) spin dynamics is well represented by a model of a two-energy-level system.Unlike spin-1/2,the maximum excitation efficiency of ^(14)N^(OT) coherences of powdered solids,denoted by p,depends on the radiofrequency field(rf-field)strength due to orientation dependence of effective nutation fields even when pulse lengths are optimized.It is also found that the p factor,contributing to the ^(14)N^(OT) spin dynamics,is nearly independent of the B0 field.Consequently,the filtering efficiency of RESPDOR experiments exhibits negligible dependence on B0 when the ^(14)N^(OT) pulse length is optimized.The study also identifies the optimal experimental conditions for ^(14)N^(OT)/^(1)H RESPDOR correlation experiments.展开更多
This paper presents a detailed investigation of unsteady supersonic flows around a typical two-body configuration, which consists of a capsule and a canopy. The cases with different trailing distances between the caps...This paper presents a detailed investigation of unsteady supersonic flows around a typical two-body configuration, which consists of a capsule and a canopy. The cases with different trailing distances between the capsule and canopy are simulated. The objective of this study is to examine the detailed effects of trailing distance on the flow fields and analyze the flow physics of the different flow modes around the parachute-like two-body model. The computational results show unsteady pulsating flow fields in the small trailing distance cases and are in reasonable agree- ment with the experimental data. As the trailing distance increases, this unsteady flow mode takes different forms along with the wake/shock and shock/shock interactions, and then gradually fades away and transits to oscillate mode, which is very different from the former. As the trailing distance keeps increasing, only the capsule wake/canopy shock interaction is present in the flow field around the two-body model, which reveals that the unsteady capsule shock/canopy shock interaction is a key mechanism for the pulsation mode.展开更多
文摘Nitrogen-14(^(14)N)overtone(OT)spectroscopy under fast magic angle spinning(MAS)conditions(>60 kHz)has emerged as a powerful technique for observing correlations and distances between ^(14)N and ^(1)H,owing to the absence of the first-order quadrupolar broadenings.In addition,^(14)N^(OT) allows selective manipulation of ^(14)N nuclei for each site.Despite extensive theoretical and experimental studies,the spin dynamics of ^(14)N^(OT) remains under debate.In this study,we conducted experimental investigations to assess the spin dynamics of ^(14)N^(OT) using the rotational-echo saturation-pulse double-resonance(RESPDOR)sequence,which monitors population transfer induced by a^(14)N^(OT) pulse.The ^(14)N^(OT) spin dynamics is well represented by a model of a two-energy-level system.Unlike spin-1/2,the maximum excitation efficiency of ^(14)N^(OT) coherences of powdered solids,denoted by p,depends on the radiofrequency field(rf-field)strength due to orientation dependence of effective nutation fields even when pulse lengths are optimized.It is also found that the p factor,contributing to the ^(14)N^(OT) spin dynamics,is nearly independent of the B0 field.Consequently,the filtering efficiency of RESPDOR experiments exhibits negligible dependence on B0 when the ^(14)N^(OT) pulse length is optimized.The study also identifies the optimal experimental conditions for ^(14)N^(OT)/^(1)H RESPDOR correlation experiments.
基金supported by the National Natural Science Foundation of China(No.11702332)
文摘This paper presents a detailed investigation of unsteady supersonic flows around a typical two-body configuration, which consists of a capsule and a canopy. The cases with different trailing distances between the capsule and canopy are simulated. The objective of this study is to examine the detailed effects of trailing distance on the flow fields and analyze the flow physics of the different flow modes around the parachute-like two-body model. The computational results show unsteady pulsating flow fields in the small trailing distance cases and are in reasonable agree- ment with the experimental data. As the trailing distance increases, this unsteady flow mode takes different forms along with the wake/shock and shock/shock interactions, and then gradually fades away and transits to oscillate mode, which is very different from the former. As the trailing distance keeps increasing, only the capsule wake/canopy shock interaction is present in the flow field around the two-body model, which reveals that the unsteady capsule shock/canopy shock interaction is a key mechanism for the pulsation mode.