Two-dimensional time-frequency ultrafast infrared vibrational echo spectroscopy
Two-dimensional time-frequency ultrafast infrared vibrational echo spectroscopy
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DOI：
10.1103/physrevlett.86.3899
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发表时间：
2001-04-23
影响因子：
8.6
通讯作者：
Fayer, MD
中科院分区：
文献类型：
--
作者：
Merchant, KA;Thompson, DE;Fayer, MD
在 Rh(CO)(2)acac [(乙酰丙酮)二羰基铑 (I)] 上进行二维光谱分辨超快 (< 200 fs) 红外振动回波实验。二维光谱显示的特征反映了 0-1 和 1-2 跃迁以及对称 (S) 和反对称 (A) CO 拉伸模式的组合能带跃迁。数据中的三个振荡是由 S 和 A 模式（量子拍）之间的频率差以及 C 和 A 非谐波引起的。对这些“非谐波”振荡给出了新的解释。计算表明，光谱分辨率可以独立测量 0-1 和 1-2 相移。
2D spectrally resolved ultrafast (< 200 fs) IR vibrational echo experiments were performed on Rh(CO)(2)acac [(acetylacetonato)dicarbonylrhodium (I)]. The 2D spectra display features that reflect the 0-1 and 1-2 transitions and the combination band transition of the symmetric (S) and antisymmetric (A) CO stretching modes. Three oscillations in the data arise from the frequency difference between the S and A modes (quantum beats) and the,C and A anharmonicities. A new explanation is given for these "anharmonic" oscillations. Calculations show that spectral resolution enables the 0-1 and 1-2 dephasing to be measured independently.