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Impact energy measurement in time-of-flight mass spectrometry with cryogenic microcalorimeters.

机译:飞行时间质谱仪中具有低温微热量计的冲击能量测量。

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Time-of-flight mass spectrometry-most notably matrix-assisted laser-desorption-ionization time-of-flight (MALDI-TOF) spectrometry-is an important class of techniques for the study of proteins and other biomolecules. Although these techniques provide excellent performance for masses up to about 20,000 daltons, there has been limited success in achieving good mass resolution at higher masses. This is because the sensitivity of the microchannel plate (MCP) detectors used in most systems decreases rapidly with increasing particle mass, limiting the utility of MCP detectors for very large masses. It has recently been proposed that cryogenic particle detectors may provide a solution to these difficulties. Cryogenic detectors measure the thermal energy deposited by the particle impact, and thus have a sensitivity that is largely independent of particle mass. Recent experiments have demonstrated the sensitivity of cryogenic particle detectors to single biomolecules, a quantum efficiency several orders of magnitude larger than the MCP detectors, and sensitivity to masses as large as 750,000 daltons. Here we present results demonstrating an order of magnitude better energy resolution than previous measurements, allowing direct determination of particle charge state during acceleration. Although application of these detectors to practical mass spectrometry will require further development of the detectors and cryogenics, these detectors can be used to elucidate the performance-limiting processes that occur in such systems.
机译:飞行时间质谱法-最著名的是基质辅助激光解吸电离飞行时间(MALDI-TOF)光谱法-是研究蛋白质和其他生物分子的重要技术类别。尽管这些技术为高达20,000道尔顿的质量提供了出色的性能,但是在更高质量下获得良好质量分辨率的成功有限。这是因为在大多数系统中使用的微通道板(MCP)检测器的灵敏度会随着颗粒质量的增加而迅速降低,从而限制了MCP检测器对非常大质量的应用。最近已经提出,低温粒子检测器可以为这些困难提供解决方案。低温检测器可测量粒子撞击所沉积的热能,因此其灵敏度在很大程度上与粒子质量无关。最近的实验证明了低温粒子检测器对单个生物分子的灵敏度,比MCP检测器大几个数量级的量子效率以及对高达750,000道尔顿的质量的灵敏度。在这里,我们提供的结果证明了比以前的测量结果更好的能量分辨率,从而可以直接确定加速过程中的粒子电荷状态。尽管将这些检测器应用于实际质谱将需要对检测器和低温技术进行进一步开发,但这些检测器可用于阐明此类系统中出现的性能限制过程。

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