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首页> 外文期刊>The Journal of Chemical Physics >Dynamics of relaxation and fragmentation in size-selected icosahedral ArnNO-(v 1) clusters
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Dynamics of relaxation and fragmentation in size-selected icosahedral ArnNO-(v 1) clusters

机译:尺寸选择的二十面体ArnNO-(v 1)团簇的弛豫和断裂动力学

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We study the vibrational relaxation and solvation dynamics in size-selected icosahedral Arn(NO-) at 300 K, where NO -(X~(3-)) is in v 1 and n 1-12, using a classical dynamics method and an interaction model consisting of detailed host-guest and host-host interactions. Two relaxation time scales are found: (i) the short-time (200 ps), in which rate is nearly independent of cluster size, and (ii) the ns scale, in which a slow energy transfer process occurs between NO- vibration and argon modes at a rate (~108 s-1) decreasing slightly from n 12 to 6 and rapidly from n 5 to 1 (~10 6 s-1). In Ar12(NO-), less than one-quarter of the host atoms sampled evaporate, nearly 60 of evaporation occurring within 200 ps caused by rapid energy transfer from NO- at short time. The fraction of evaporation decreases nearly exponentially with increasing evaporation time, but ~16 of evaporation still occurs on a time scale longer than 1 ns. Evaporation from one hemisphere of Ar _(12)(NO-) dominates the rest. Final cluster sizes commonly produced from the fragmentation of Ar_(12)(NO-) are n 6-11 (evaporation of 6-1 atoms) and n 12 (no evaporation).
机译:我们使用经典的动力学方法和一个有限元方法研究了尺寸选定的二十面体Arn(NO-)在300 K时的振动弛豫和溶剂化动力学,其中NO-(X〜(3-))在v 1和n 1-12中。交互模型,由详细的来宾与来宾交互组成。发现了两个弛豫时间尺度:(i)短时间(200 ps),其速率几乎与团簇大小无关;(ii)ns尺度,其中在NO振动和振动之间发生缓慢的能量传递过程氩气模式的速率(〜108 s-1)从n 12减小到6,然后迅速从n 5减小到1(〜10 6 s-1)。在Ar12(NO-)中,不到四分之一的被采样原子蒸发,由于在短时间内从NO-快速转移能量,在200 ps内发生了近60蒸发。蒸发分数随蒸发时间的增加几乎成指数下降,但在大于1 ns的时间尺度上仍会发生〜16的蒸发。从Ar _(12)(NO-)的一个半球蒸发占主导。通常由Ar_(12)(NO-)断裂产生的最终簇尺寸为n 6-11(蒸发6-1个原子)和n 12(不蒸发)。

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