Lateral hopping and desorption of a single CO molecule on a Cu(110) surface induced by
Lateral hopping and desorption of a single CO molecule on a Cu(110) surface induced by
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Cu(110)表面上单个CO分子的横向跳跃和解吸
DOI：
10.1103/physrevb.87.205403
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发表时间：
2013
影响因子：
3.7
通讯作者：
H. Ueba
中科院分区：
文献类型：
--
作者：
蔡萍根;水谷祐輔;土屋雅博;岡嶋孝治;Masahito Yamazaki;H. Ueba
利用间接传热模型研究了飞秒激光脉冲诱导的单个CO分子在Cu（110）表面上的横向跳跃和脱附[Bartels，Science 305，648（2004）SCIEAS 0036 -807510.1126/science. 1099770]。除了直接加热的反应坐标（RC）模式[受抑平移（FT）模式的跳跃和质量中心（CM）模式的解吸]由激光产生的热电子在衬底中，我们认为间接加热的RC模式之间的模间耦合的受抑旋转（FR）模式和RC模式。我们计算的FT和CM模式的有效温度的瞬态行为，和归一化的反应产率。计算了Cu（110）表面上沿沿着行和跨行跳跃产额之比的实验结果。虽然没有任何信息是可用的尝试频率的形式的阿克里尼乌斯方程的热活化反应，它是预测在何种条件下的解吸率成为在相同的数量级的跳跃率，虽然脱附的势垒高度是远远高于跳跃。本分析突出了FR模式的激发在CO分子的反应中的作用，如已经在实时观察中确认的[Backus，Science 310，1790（2005）SCIEAS 0036 -807510.1126/science.1120693]。
Lateral hopping and desorption of a single CO molecule on a Cu(110) surface [Bartels , Science 305, 648 (2004)SCIEAS0036-807510.1126/science.1099770] induced by femtosecond laser pulses are studied using an indirect heat-transfer model. In addition to a direct heating of the reaction coordinate (RC) mode [frustrated translation (FT) mode for hopping and center-of-mass (CM) mode for desorption] by laser-generated hot electrons in the substrate, we consider an indirect heating of the RC mode through intermode coupling between the frustrated rotation (FR) mode and the RC mode. We calculate the transient behavior of the effective temperature of the FT and the CM modes, and of the normalized reaction yield. The experimental result of a ratio of the hopping yield along and across a row on a Cu(110) surface is nicely calculated. Although no information is available for the attempt frequency in a form of the Arrhenius equation for thermally activated reactions, it is predicted under which condition the desorption rate becomes in the same order of magnitude as the hopping rate, although the barrier height for desorption is much higher than for hopping. The present analysis highlights the role of excitation of the FR mode in reactions of a CO molecule as has been confirmed in the real-time observation [Backus , Science 310, 1790 (2005)SCIEAS0036-807510.1126/science.1120693].