Surface-enhanced Raman scattering (SERS) has attracted much attention as an important technique for studying and monitoring the behavior of molecules. Coherent control by shaping femtosecond pulses is an efficient method for controlling molecular vibration state, rotation state, ionization state, and other molecule dynamics. In this paper, we propose a theoretical scheme of selective excitation of SERS from a single porphycene molecule with two Raman peaks at 327[Formula: see text]cm[Formula: see text] and 367[Formula: see text]cm[Formula: see text] placed in the gap between silver dimer nanospheres. Based on the theory of quantum coherent control, selective excitation of the peak at 327[Formula: see text]cm[Formula: see text] and depression of another at 367[Formula: see text]cm[Formula: see text] are demonstrated by properly shaping femtosecond laser pulses with central frequency of 12500[Formula: see text]cm[Formula: see text] and a full width at half maximum (FWHM) of 300[Formula: see text]cm[Formula: see text]. Ultrafast dynamics of the response of dimer nanospheres to the shaped pump and Stokes pulses are simulated by finite difference time domain (FDTD) method followed by Fourier transform. The enhanced and selected single molecule SERS is realized simultaneously. The SERS probability is enhanced by more than six orders in magnitude compared with the case in air environment, and the FWHMs of the enhanced and the depressed Raman peaks are both larger than 17[Formula: see text]cm[Formula: see text] despite the narrow gap of only 40[Formula: see text]cm[Formula: see text] between the two Raman peaks.

中文翻译：

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通过整形泵和斯托克斯脉冲对单分子表面增强拉曼散射的超快选择性激发

表面增强拉曼散射（SERS）作为研究和监测分子行为的重要技术而备受关注。通过塑造飞秒脉冲的相干控制是控制分子振动状态、旋转状态、电离状态和其他分子动力学的有效方法。在本文中，我们提出了一种从单个卟啉分子选择性激发 SERS 的理论方案，该分子在 327[公式：见文本]cm[公式：见文本]和 367[公式：见文本]cm[公式：见正文] 置于银二聚体纳米球之间的空隙中。基于量子相干控制理论，在 327[公式：见正文]cm[公式：见正文]处选择性激发峰，在 367[公式：见正文]cm[公式：见文本]通过适当塑造中心频率为 12500[公式：见文本]cm[公式：见文本]和半高全宽 (FWHM) 为 300[公式：见文本]cm[公式: 见正文]。二聚体纳米球对成形泵和斯托克斯脉冲的响应的超快动力学通过有限差分时域 (FDTD) 方法和傅里叶变换来模拟。增强和选择的单分子SERS同时实现。与空气环境相比，SERS概率提高了6个数量级以上，增强和降低的拉曼峰的半高宽均大于17[公式：见正文]cm[公式：见正文]尽管两个拉曼峰之间只有 40[公式：见正文]cm[公式：见正文]的狭窄间隙。