Selectivity in vibrationally mediated single-molecule chemistry

被引:270
作者
Pascual, JI
Lorente, N
Song, Z
Conrad, H
Rust, HP
机构
[1] Max Planck Gesell, Fritz Haber Inst, D-14194 Berlin, Germany
[2] CSIC, Inst Ciencia Mat Barcelona, E-08193 Barcelona, Spain
[3] Univ Toulouse 3, Lab Collis Agregats React, UMR 5589, F-31062 Toulouse, France
[4] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA
基金
美国国家科学基金会;
关键词
D O I
10.1038/nature01649
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The selective excitation of molecular vibrations provides a means to directly influence the speed and outcome of chemical reactions. Such mode-selective chemistry(1) has traditionally used laser pulses to prepare reactants in specific vibrational states(2) to enhance reactivity(3,4) or modify the distribution of product species(5,6). Inelastic tunnelling electrons may also excite molecular vibrations(7,8) and have been used to that effect on adsorbed molecules, to cleave individual chemical bonds(9) and induce molecular motion(10-13) or dissociation(14-17). Here we demonstrate that inelastic tunnelling electrons can be tuned to induce selectively either the translation or desorption of individual ammonia molecules on a Cu(100) surface. We are able to select a particular reaction pathway by adjusting the electronic tunnelling current and energy during the reaction induction such that we activate either the stretching vibration of ammonia or the inversion of its pyramidal structure. Our results illustrate the ability of the scanning tunnelling microscope to probe single-molecule events in the limit of very low yield and very low power irradiation, which should allow the investigation of reaction pathways not readily amenable to study by more conventional approaches.
引用
收藏
页码:525 / 528
页数:5
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