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利用粒子模拟方法对傅里叶变换离子回旋共振池中离子云运动进行逼真建模。

Realistic modeling of ion cloud motion in a Fourier transform ion cyclotron resonance cell by use of a particle-in-cell approach.

作者信息

Nikolaev Eugene N, Heeren Ron M A, Popov Alexander M, Pozdneev Alexander V, Chingin Konstantin S

机构信息

The Institute for Energy Problems of Chemical Physics, Russian Academy of Sciences, Leninskij pr.38, k.2, Moscow, Russia 119334.

出版信息

Rapid Commun Mass Spectrom. 2007;21(22):3527-46. doi: 10.1002/rcm.3234.

Abstract

Using a 'Particle-In-Cell' approach taken from plasma physics we have developed a new three-dimensional (3D) parallel computer code that today yields the highest possible accuracy of ion trajectory calculations in electromagnetic fields. This approach incorporates coulombic ion-ion and ion-image charge interactions into the calculation. The accuracy is achieved through the implementation of an improved algorithm (the so-called Boris algorithm) that mathematically eliminates cyclotron motion in a magnetic field from digital equations for ion motion dynamics. It facilitates the calculation of the cyclotron motion without numerical errors. At every time-step in the simulation the electric potential inside the cell is calculated by direct solution of Poisson's equation. Calculations are performed on a computational grid with up to 128 x 128 x 128 nodes using a fast Fourier transform algorithm. The ion populations in these simulations ranged from 1000 up to 1,000,000 ions. A maximum of 3,000,000 time-steps were employed in the ion trajectory calculations. This corresponds to an experimental detection time-scale of seconds. In addition to the ion trajectories integral time-domain signals and mass spectra were calculated. The phenomena observed include phase locking of particular m/z ions (high-resolution regime) inside larger ion clouds. A focus was placed on behavior of a cloud of ions of a single m/z value to understand the nature of Fourier transform ion cyclotron resonance (FTICR) resolution and mass accuracy in selected ion mode detection. The behavior of two and three ion clouds of different but close m/z was investigated as well. Peak coalescence effects were observed in both cases. Very complicated ion cloud dynamics in the case of three ion clouds was demonstrated. It was found that magnetic field does not influence phase locking for a cloud of ions of a single m/z. The ion cloud evolution time-scale is inversely proportional to magnetic field. The number of ions needed for peak coalescence depends quadratically on the magnetic field.

摘要

我们采用等离子体物理学中的“粒子模拟”方法,开发了一种新的三维(3D)并行计算机代码,该代码目前在电磁场中离子轨迹计算方面具有最高的精度。这种方法将库仑离子 - 离子和离子镜像电荷相互作用纳入计算。通过实施一种改进算法(即所谓的鲍里斯算法)实现了高精度,该算法从离子运动动力学的数字方程中数学上消除了磁场中的回旋运动。它有助于无数值误差地计算回旋运动。在模拟的每个时间步,通过直接求解泊松方程来计算单元内的电势。使用快速傅里叶变换算法在多达128×128×128个节点的计算网格上进行计算。这些模拟中的离子数量从1000到1000000不等。在离子轨迹计算中最多采用3000000个时间步。这对应于秒级的实验检测时间尺度。除了离子轨迹外,还计算了积分时域信号和质谱。观察到的现象包括较大离子云内部特定质荷比离子的锁相(高分辨率状态)。重点关注了单种质荷比离子云的行为,以了解在选定离子模式检测中傅里叶变换离子回旋共振(FTICR)分辨率和质量精度的本质。还研究了不同但相近质荷比的两个和三个离子云的行为。在这两种情况下都观察到了峰合并效应。展示了三个离子云情况下非常复杂的离子云动力学。发现磁场不会影响单种质荷比离子云的锁相。离子云演化时间尺度与磁场成反比。峰合并所需的离子数量与磁场呈二次方关系。

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