Oron Dan, Dudovich Nirit, Silberberg Yaron
Department of Physics of Complex Systems, Weizmann Institute of Science, Rehovot 76100, Israel.
Phys Rev Lett. 2002 Dec 30;89(27):273001. doi: 10.1103/PhysRevLett.89.273001. Epub 2002 Dec 17.
High spectral resolution nonlinear vibrational spectroscopy with a single ultrashort pulse is demonstrated on a variety of samples. The spectral data are obtained by shaping the excitation pulse in order to control the relative phase between the weak resonant signal and the strong nonresonant background, in analogy with phase-contrast microscopy techniques. This is unlike the more conventional approach to nonlinear spectroscopy, in which the nonresonant background is reduced to a minimum. By measuring the spectrum of the coherent anti-Stokes Raman signal, it is possible to infer the vibrational energy levels in a band spanning almost an entire octave.
利用单个超短脉冲的高光谱分辨率非线性振动光谱技术在多种样品上得到了验证。通过对激发脉冲进行整形以控制弱共振信号与强非共振背景之间的相对相位来获取光谱数据，这类似于相衬显微镜技术。这与非线性光谱学中更传统的方法不同，在传统方法中，非共振背景被降至最低。通过测量相干反斯托克斯拉曼信号的光谱，可以推断出几乎跨越整个倍频程的一个能带中的振动能级。
