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1. 发明申请

US20050103992A1 Mass spectrometer and method of determining mass-to-charge ratio of ion 有权
标题翻译：质谱仪和离子质荷比的测定方法
公开(公告)号：US20050103992A1
公开(公告)日：2005-05-19
申请号：US10983571
申请日：2004-11-09
申请人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda
发明人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda
IPC分类号： G01N27/62 , B01D59/44 , H01J49/00 , H01J49/06 , H01J49/40
CPC分类号： H01J49/408 , H01J49/0027
摘要： The present invention provides a time of flight mass spectrometer having a spiral flight path, whose mass resolution can be appropriately changed with respect to the analysis object or other factor without any complicated alteration or addition of the mechanical construction. In a specific form of the invention, the mass spectrometer includes deflecting electrodes 20-23 located between semi-cylindrical electrodes 11 and 12 for making ions fly along a spiral path. The deflecting electrodes 20-23 generate deflecting electric fields for shifting the ions in the axial direction of the semi-cylindrical electrodes 11 and 12. The voltage applied to the deflecting electrodes 20-23 is changed according to the mass resolution required. The deflecting electric fields are generated or removed with the change of the voltage, which makes the ions fly either along a spiral path or in the same loop orbit. The flight distance of the ions can be controlled as desired by regulating the voltage so that the ions fly in the loop orbit an appropriate number of times. Thus, the mass resolution can be arbitrarily controlled.
摘要翻译：本发明提供了具有螺旋飞行路径的飞行时间质谱仪，其质量分辨率可以相对于分析对象或其他因素适当地改变，而没有任何复杂的改变或添加机械结构。在本发明的具体形式中，质谱仪包括位于半圆柱形电极11和12之间的偏转电极20-23，用于使离子沿着螺旋路线飞行。偏转电极20-23产生用于使离子沿半圆柱形电极11和12的轴向移动的偏转电场。施加到偏转电极20-23的电压根据所需的质量分辨率而改变。随着电压的变化产生或去除偏转电场，这使得离子沿着螺旋路径或相同的环轨道飞行。通过调节电压可以根据需要控制离子的飞行距离，使得离子在环轨道中飞行适当次数。因此，质量分辨率可以任意控制。

2. 发明申请

US20050194528A1 Time of flight mass spectrometer 有权
标题翻译：飞行时间质谱仪
公开(公告)号：US20050194528A1
公开(公告)日：2005-09-08
申请号：US10929768
申请日：2004-08-31
申请人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda , Daisuke Okumura
发明人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda , Daisuke Okumura
IPC分类号： G01N27/62 , G01N27/64 , H01J49/00 , H01J49/40
CPC分类号： H01J49/408 , H01J49/406
摘要： A time of flight type mass spectrometer (TOF-MS) of the present invention includes: a flight space containing a loop orbit on which ions fly once or more than once; a flight controller for making ions of a same mass to charge ratio fly the loop orbit at several values of number of turns; a flight time measurer for measuring a length of flight time of the ions; and a processor for determining the mass to charge ratio of the ions based on a relationship between the value of number of turns and the length of flight time of the ions. The speed of ions flying a loop orbit depends on their mass to charge ratios. For ions of the same mass to charge ratio, the difference between the lengths of flight time of the ions flying the loop orbit N turns and of the ions flying the loop orbit N+1 turns depends on the speed of the ions, so that the difference depends on the mass to charge ratio of the ions. The difference in the length of flight time is unrelated to the variation in the starting time (jitter), variation in the detection timing (jitter), etc, so that the value of the mass to charge ratio can be precisely determined free from errors caused by such disturbing factors.
摘要翻译：本发明的飞行时间型质谱仪（TOF-MS）包括：包含离子飞行一次或多次的循环轨道的飞行空间; 用于使相同质荷比的离子的飞行控制器以匝数的几个值飞行环路轨道; 用于测量离子的飞行时间长度的飞行时间测量器; 以及用于基于匝数与离子的飞行时间长度之间的关系来确定离子的质荷比的处理器。飞行环路轨道的离子速度取决于其质荷比。对于相同质荷比的离子，飞越环轨道N圈的离子的飞行时间长度和飞行环轨道N + 1圈的离子之间的差异取决于离子的速度，因此差异取决于离子的质荷比。飞行时间长度的差异与启动时间（抖动）的变化，检测定时（抖动）等的变化无关，从而可以精确地确定质荷比值，从而避免误差受到这样的扰乱因素。

3. 发明授权

US07227131B2 Time of flight mass spectrometer 有权
标题翻译：飞行时间质谱仪
公开(公告)号：US07227131B2
公开(公告)日：2007-06-05
申请号：US10929768
申请日：2004-08-31
申请人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda , Daisuke Okumura
发明人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda , Daisuke Okumura
IPC分类号： H01J49/40
CPC分类号： H01J49/408 , H01J49/406
摘要： A time of flight type mass spectrometer (TOF-MS) of the present invention includes: a flight space containing a loop orbit on which ions fly once or more than once; a flight controller for making ions of a same mass to charge ratio fly the loop orbit at several values of number of turns; a flight time measurer for measuring a length of flight time of the ions; and a processor for determining the mass to charge ratio of the ions based on a relationship between the value of number of turns and the length of flight time of the ions. The speed of ions flying a loop orbit depends on their mass to charge ratios. For ions of the same mass to charge ratio, the difference between the lengths of flight time of the ions flying the loop orbit N turns and of the ions flying the loop orbit N+1 turns depends on the speed of the ions, so that the difference depends on the mass to charge ratio of the ions. The difference in the length of flight time is unrelated to the variation in the starting time (jitter), variation in the detection timing (jitter), etc, so that the value of the mass to charge ratio can be precisely determined free from errors caused by such disturbing factors.
摘要翻译：本发明的飞行时间型质谱仪（TOF-MS）包括：包含离子飞行一次或多次的循环轨道的飞行空间; 用于使相同质荷比的离子的飞行控制器以匝数的几个值飞行环路轨道; 用于测量离子的飞行时间长度的飞行时间测量器; 以及用于基于匝数与离子的飞行时间长度之间的关系来确定离子的质荷比的处理器。飞行环路轨道的离子速度取决于其质荷比。对于相同质荷比的离子，飞越环轨道N圈的离子的飞行时间长度和飞行环轨道N + 1圈的离子之间的差异取决于离子的速度，因此差异取决于离子的质荷比。飞行时间长度的差异与启动时间（抖动）的变化，检测定时（抖动）等的变化无关，从而可以精确地确定质荷比值，从而避免误差受到这样的扰乱因素。

4. 发明授权

US07211792B2 Mass spectrometer 有权
标题翻译：质谱仪
公开(公告)号：US07211792B2
公开(公告)日：2007-05-01
申请号：US11032002
申请日：2005-01-11
申请人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda , Daisuke Okumura
发明人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda , Daisuke Okumura
IPC分类号： B01D59/44 , H01J49/00
CPC分类号： H01J49/408
摘要： In the mass spectrometer of the present invention, a flight space is provided before the mass analyzer, and the flight space includes a loop orbit on which ions fly repeatedly. While ions fly on the loop orbit repeatedly, ion selecting electrodes placed on the loop orbit selects object ions having a specific mass to charge ratio in such a manner that, for a limited time period when the object ions are flying through the ion selecting electrodes, an appropriate voltage is applied to the ion selecting electrodes to make them continue to fly on the loop orbit, but otherwise to make or let other ions deflect from the loop orbit. If ions having various mass to charge ratios are introduced in the loop orbit almost at the same time, the object ions having the same mass to charge ratio continue to fly on the loop orbit in a band, but ions having mass to charge ratios different from that are separated from the object ions while flying on the loop orbit repeatedly. Even if the difference in the mass to charge ratio is small, the separation becomes large when the number of turns of the flight becomes large. After such a separation is adequately achieved, the ion selecting electrodes can select the object ions with high selectivity, or at high mass resolution. By adding dissociating means, fragment ions originated only from the selected object ions can be analyzed, which enables the identification and structural analysis of the sample at high accuracy.
摘要翻译：在本发明的质谱仪中，在质量分析器之前提供飞行空间，并且飞行空间包括离子重复飞行的环轨道。当离子重复地在环路轨道上飞行时，放置在环路轨道上的离子选择电极以这样的方式选择具有特定质荷比的物体离子，使得在物体离子飞过离子选择电极的有限时间段内，对离子选择电极施加适当的电压使它们继续在环轨道上飞行，而另外使其它离子从环轨道偏转。如果几乎同时在环路轨道中引入具有各种质荷比的离子，则具有相同质荷比的物体离子在带内的环路轨道上继续飞行，但质量与电荷比的离子不同于它们与物体离子分离，同时在环路轨道上重复飞行。即使质荷比的差小，当飞行匝数变大时，分离也变大。在这种分离充分实现之后，离子选择电极可以以高选择性或高质量分辨率选择目标离子。通过添加解离手段，可以分析仅从所选择的对象离子产生的碎片离子，这使得能够高精度地鉴定和结构分析样品。

5. 发明授权

US07148473B2 Time of flight mass spectrometer 有权
标题翻译：飞行时间质谱仪
公开(公告)号：US07148473B2
公开(公告)日：2006-12-12
申请号：US10929770
申请日：2004-08-31
申请人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda , Daisuke Okumura
发明人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda , Daisuke Okumura
IPC分类号： H01J49/40
CPC分类号： H01J49/408 , H01J49/027
摘要： In a time of flight mass spectrometer (TOF-MS) of the present invention, a flight controller makes ions fly a loop orbit a predetermined number of turns, and an ion detector detects the ions at each turn of the flight. A flight time measurer measures the length of flight time of ions of a same mass to charge ratio at every turn, and a data processor constructs a spectrum of flight time. The data processor further computes the Fourier transformation of the spectrum, and determines the mass to charge ratio of the ions based on a frequency peak appearing in the Fourier transformation.
摘要翻译：在本发明的飞行时间质谱仪（TOF-MS）中，飞行控制器使离子飞行预定匝数的环路轨道，并且离子检测器在飞行的每一回合处检测离子。飞行时间测量器可以测量每一回合具有相同质荷比的离子的飞行时间长度，并且数据处理器构建飞行时间谱。数据处理器进一步计算光谱的傅立叶变换，并且基于在傅立叶变换中出现的频率峰值来确定离子的质荷比。

6. 发明授权

US07038198B2 Mass spectrometer 有权
标题翻译：质谱仪
公开(公告)号：US07038198B2
公开(公告)日：2006-05-02
申请号：US10957642
申请日：2004-10-05
申请人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda
发明人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda
IPC分类号： H01J49/40
CPC分类号： H01J49/0036 , H01J49/408
摘要： A mass spectrometer includes a flight control device for allowing ions from an ion source to repeatedly fly along an orbit in a flight space for predetermined times; a detecting device for detecting the ions after the ions repeatedly fly along the orbit for the predetermined times; and a data processing device for starting collection of ion strength data detected by the detecting device. The ion strength data is obtained during the flight of the ions along the orbit, or when the ions are headed toward the detecting device after departing from the orbit, or when one of the above situations is estimated.
摘要翻译：质谱仪包括用于允许来自离子源的离子在飞行空间中沿着轨道重复飞行预定次数的飞行控制装置; 检测装置，用于在离子重复沿着轨道飞行预定时间之后检测离子; 以及用于开始由检测装置检测的离子强度数据的收集的数据处理装置。离子强度数据是在沿着轨道的离子飞行过程中获得的，或者离子离开轨道时离子朝向检测装置，或当估计出上述情况之一时获得。

7. 发明申请

US20050151076A1 Mass spectrometer 有权
标题翻译：质谱仪
公开(公告)号：US20050151076A1
公开(公告)日：2005-07-14
申请号：US11032002
申请日：2005-01-11
申请人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda , Daisuke Okumura
发明人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda , Daisuke Okumura
IPC分类号： G01N27/62 , B01D59/44 , H01J49/06 , H01J49/16 , H01J49/26 , H01J49/40
CPC分类号： H01J49/408
摘要： In the mass spectrometer of the present invention, a flight space is provided before the mass analyzer, and the flight space includes a loop orbit on which ions fly repeatedly. While ions fly on the loop orbit repeatedly, ion selecting electrodes placed on the loop orbit selects object ions having a specific mass to charge ratio in such a manner that, for a limited time period when the object ions are flying through the ion selecting electrodes, an appropriate voltage is applied to the ion selecting electrodes to make them continue to fly on the loop orbit, but otherwise to make or let other ions deflect from the loop orbit. If ions having various mass to charge ratios are introduced in the loop orbit almost at the same time, the object ions having the same mass to charge ratio continue to fly on the loop orbit in a band, but ions having mass to charge ratios different from that are separated from the object ions while flying on the loop orbit repeatedly. Even if the difference in the mass to charge ratio is small, the separation becomes large when the number of turns of the flight becomes large. After such a separation is adequately achieved, the ion selecting electrodes can select the object ions with high selectivity, or at high mass resolution. By adding dissociating means, fragment ions originated only from the selected object ions can be analyzed, which enables the identification and structural analysis of the sample at high accuracy.
摘要翻译：在本发明的质谱仪中，在质量分析器之前提供飞行空间，并且飞行空间包括离子重复飞行的环轨道。当离子重复地在环路轨道上飞行时，放置在环路轨道上的离子选择电极以这样的方式选择具有特定质荷比的物体离子，使得在物体离子飞过离子选择电极的有限时间段内，对离子选择电极施加适当的电压使它们继续在环轨道上飞行，而另外使其它离子从环轨道偏转。如果几乎同时在环路轨道中引入具有各种质荷比的离子，则具有相同质荷比的物体离子在带内的环路轨道上继续飞行，但质量与电荷比的离子不同于它们与物体离子分离，同时在环路轨道上重复飞行。即使质荷比的差小，当飞行匝数变大时，分离也变大。在这种分离充分实现之后，离子选择电极可以以高选择性或高质量分辨率选择目标离子。通过添加解离手段，可以分析仅从所选择的对象离子产生的碎片离子，这使得能够高精度地鉴定和结构分析样品。

8. 发明申请

US20050077462A1 Method of determining mass-to-charge ratio of ions and mass spectrometer using the methhod 有权
标题翻译：使用该方法确定离子和质谱仪的质荷比的方法
公开(公告)号：US20050077462A1
公开(公告)日：2005-04-14
申请号：US10959433
申请日：2004-10-07
申请人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda
发明人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda
IPC分类号： G01N27/62 , H01J49/04 , H01J49/40
CPC分类号： H01J49/408
摘要： In an analysis using a mass spectrometer having a loop orbit along which ions are made to fly a plurality of times, the present invention provides a method of determining the mass-to-charge ratio of an ion without limiting the range of the mass-to-charge ratio of the ions to be brought into the loop orbit while allowing the lapping of the orbiting ions. The measurement is carried out two or more times under different conditions (Tg=500[μs], 400[μs]) under which the number of turns of the ion concerned is different. Flight times are determined from the flight time spectrums obtained by at least two measurements. Though the numbers of turns themselves are unknown, it is possible to calculate possible mass-to-charge ratios for each flight time by incrementally setting the number of turns at plural values. The two sets of possible mass-to-charge ratios derived from the two flight time values (525[μs], 441[μs]) determined by the two measurements are compared with each other, and a value that is found in both measurement results is selected as the mass-to-charge ratio of the ion concerned. Thus, it is possible to determine the mass-to-charge ratio without limiting the range of the mass-to-charge ratio before the ions are brought into the loop orbit.
摘要翻译：在使用具有环形轨道的质谱仪进行分析时，离子通过该轨道多次飞行，本发明提供了一种确定离子的质荷比而不限制质量 - 进入环轨道的离子的充电比例，同时允许研磨轨道离子。在不同条件下（Tg = 500 [mus]，400 [mus]）进行两次以上的测定，在该条件下，有关离子的匝数不同。从通过至少两次测量获得的飞行时间谱确定飞行时间。虽然转弯数量本身是未知的，但是可以通过逐个设定多个值的匝数来计算每个飞行时间的可能的质荷比。将由两个测量确定的两个飞行时间值（525 [mus]，441 [mus]）得到的两组可能的质荷比相互比较，并在两个测量结果中找到被选为相关离子的质荷比。因此，可以在离子进入环轨道之前不限制质荷比的范围来确定质荷比。

9. 发明申请

US20050077461A1 Mass spectrometer 有权
标题翻译：质谱仪
公开(公告)号：US20050077461A1
公开(公告)日：2005-04-14
申请号：US10957642
申请日：2004-10-05
申请人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda
发明人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda
IPC分类号： G01N27/62 , H01J49/06 , H01J49/10 , H01J49/40
CPC分类号： H01J49/0036 , H01J49/408
摘要： A mass spectrometer includes a flight control device for allowing ions from an ion source to repeatedly fly along an orbit in a flight space for predetermined times; a detecting device for detecting the ions after the ions repeatedly fly along the orbit for the predetermined times; and a data processing device for starting collection of ion strength data detected by the detecting device. The ion strength data is obtained during the flight of the ions along the orbit, or when the ions are headed toward the detecting device after departing from the orbit, or when one of the above situations is estimated.
摘要翻译：质谱仪包括用于允许来自离子源的离子在飞行空间中沿着轨道重复飞行预定次数的飞行控制装置; 检测装置，用于在离子重复沿着轨道飞行预定时间之后检测离子; 以及用于开始由检测装置检测的离子强度数据的收集的数据处理装置。离子强度数据是在沿着轨道的离子飞行过程中获得的，或者离子离开轨道时离子朝向检测装置，或当估计出上述情况之一时获得。

10. 发明授权

US07091480B2 Method of determining mass-to-charge ratio of ions and mass spectrometer using the method 有权
标题翻译：使用该方法确定离子和质谱仪的质荷比的方法
公开(公告)号：US07091480B2
公开(公告)日：2006-08-15
申请号：US10959433
申请日：2004-10-07
申请人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda
发明人： Shinichi Yamaguchi , Morio Ishihara , Michisato Toyoda
IPC分类号： H01J49/40
CPC分类号： H01J49/408
摘要： In an analysis using a mass spectrometer having a loop orbit along which ions are made to fly a plurality of times, the present invention provides a method of determining the mass-to-charge ratio of an ion without limiting the range of the mass-to-charge ratio of the ions to be brought into the loop orbit while allowing the lapping of the orbiting ions. The measurement is carried out two or more times under different conditions (Tg=500[μs], 400[μs]) under which the number of turns of the ion concerned is different. Flight times are determined from the flight time spectrums obtained by at least two measurements. Though the numbers of turns themselves are unknown, it is possible to calculate possible mass-to-charge ratios for each flight time by incrementally setting the number of turns at plural values. The two sets of possible mass-to-charge ratios derived from the two flight time values (525[μs], 441[μs]) determined by the two measurements are compared with each other, and a value that is found in both measurement results is selected as the mass-to-charge ratio of the ion concerned. Thus, it is possible to determine the mass-to-charge ratio without limiting the range of the mass-to-charge ratio before the ions are brought into the loop orbit.
摘要翻译：在使用具有环形轨道的质谱仪进行分析时，离子通过该轨道多次飞行，本发明提供了一种确定离子的质荷比而不限制质量 - 进入环轨道的离子的充电比例，同时允许研磨轨道离子。在不同条件下（Tg = 500 [mus]，400 [mus]）进行两次以上的测定，在该条件下，有关离子的匝数不同。从通过至少两次测量获得的飞行时间谱确定飞行时间。虽然转弯数量本身是未知的，但是可以通过逐个设定多个值的匝数来计算每个飞行时间的可能的质荷比。将由两个测量确定的两个飞行时间值（525 [mus]，441 [mus]）得到的两组可能的质荷比相互比较，并在两个测量结果中找到被选为相关离子的质荷比。因此，可以在离子进入环轨道之前不限制质荷比的范围来确定质荷比。

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