Ultrafast Production of NiCO and Ni Following 197 nm Photodissociation of Nickel Tetracarbonyl

IF 3.7 Q2 CHEMISTRY, PHYSICAL
Neil C. Cole-Filipiak, Jan Troß, Paul Schrader, Laura M. McCaslin, Krupa Ramasesha
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引用次数: 0

Abstract

Herein, we report on the ultrafast photodissociation of nickel tetracarbonyl─a prototypical metal–ligand model system─at 197 nm. Using mid-infrared transient absorption spectroscopy to probe the bound C≡O stretching modes, we find evidence for the picosecond time scale production of highly vibronically excited nickel dicarbonyl and nickel monocarbonyl, in marked contrast with a prior investigation at 193 nm. Further spectral evolution with a 50 ps time constant suggests an additional dissociation step; the absence of any corresponding growth in signal strongly indicates the production of bare Ni, a heretofore unreported product from single-photon excitation of nickel tetracarbonyl. Thus, by probing the deep UV-induced photodynamics of a prototypical metal carbonyl, this Letter adds time-resolved spectroscopic signatures of these dynamics to the sparse literature at high excitation energies.

Abstract Image

197 纳米波长光解离四羰基镍后超快生成 NiCO 和 Ni
在此,我们报告了在 197 纳米波长下四羰基镍--一种典型的金属配体模型系统--的超快光解离。利用中红外瞬态吸收光谱来探测结合的 C≡O 伸展模式,我们发现了皮秒时间尺度内产生高度振动激发的二羰基镍和一羰基镍的证据,这与之前在 193 纳米波长下进行的研究形成了鲜明对比。50 ps 时间常数的进一步光谱演变表明还存在一个解离步骤;信号没有任何相应的增长,这强烈表明产生了裸镍,这是迄今为止尚未报道的单光子激发四羰基镍的产物。因此,通过探测原型金属羰基的深紫外光诱导光动力学,这封信为高激发能量下这些动力学的稀少文献增添了时间分辨光谱特征。
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来源期刊
CiteScore
3.70
自引率
0.00%
发文量
0
期刊介绍: ACS Physical Chemistry Au is an open access journal which publishes original fundamental and applied research on all aspects of physical chemistry. The journal publishes new and original experimental computational and theoretical research of interest to physical chemists biophysical chemists chemical physicists physicists material scientists and engineers. An essential criterion for acceptance is that the manuscript provides new physical insight or develops new tools and methods of general interest. Some major topical areas include:Molecules Clusters and Aerosols; Biophysics Biomaterials Liquids and Soft Matter; Energy Materials and Catalysis
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