Diprose Jake A, Richardson Vincent, Regan Paul, Roberts Adam, Burdin Sergey, Tsikritea Andriana, Mavrokoridis Konstantinos, Heazlewood Brianna R
Department of Physics, University of Liverpool, Liverpool L69 7ZE, U.K.
Department of Physics, TU Dortmund, Dortmund 44227, Germany.
J Phys Chem A. 2024 May 16;128(19):3900-3909. doi: 10.1021/acs.jpca.3c08132. Epub 2024 Apr 8.
Coulomb crystals have proven to be powerful and versatile tools for the study of ion-molecule reactions under cold and controlled conditions. Reactions in Coulomb crystals are typically monitored through a combination of fluorescence imaging of the laser-cooled ions and destructive time-of-flight mass spectrometry measurements of the ejected ions. However, neither of these techniques is able to provide direct structural information on the positions of nonfluorescing "dark" ions within the crystal. In this work, structural information is obtained using a phosphor screen and a microchannel plate detector in conjunction with a Timepix3 camera. The Timepix3 camera simultaneously records the spatial and temporal distribution of all ions that strike the phosphor screen detector following crystal ejection at a selected reaction time. A direct comparison can be made between the observed Timepix3 ion distributions and the distributions established from SIMION simulations of the ion trajectories through the apparatus and onto the detector. Quantitative agreement is found between the measured Timepix3 signal and the properties of Coulomb crystals assigned using fluorescence imaging─independently confirming that the positions and numbers of nonfluorescing ions within Coulomb crystals can be accurately determined using molecular dynamics simulations. It is anticipated that the combination of high-resolution spatial and temporal data will facilitate new measurements of the ion properties within Coulomb crystals.
库仑晶体已被证明是在低温和可控条件下研究离子 - 分子反应的强大且通用的工具。库仑晶体中的反应通常通过激光冷却离子的荧光成像和对 ejected 离子的破坏性飞行时间质谱测量相结合来监测。然而,这些技术都无法提供关于晶体中不发荧光的“暗”离子位置的直接结构信息。在这项工作中,使用磷光屏和微通道板探测器结合 Timepix3 相机获得结构信息。Timepix3 相机在选定的反应时间同时记录晶体 ejection 后撞击磷光屏探测器的所有离子的空间和时间分布。可以直接比较观察到的 Timepix3 离子分布与通过该装置并到达探测器的离子轨迹的 SIMION 模拟所建立的分布。在测量的 Timepix3 信号与使用荧光成像指定的库仑晶体性质之间发现了定量一致性——独立地证实了可以使用分子动力学模拟准确确定库仑晶体中不发荧光离子的位置和数量。预计高分辨率空间和时间数据的结合将有助于对库仑晶体中的离子性质进行新的测量。