Two-dimensional chirped-pulse Fourier transform microwave spectroscopy.

Two-dimensional chirped-pulse Fourier transform microwave spectroscopy.
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二维啁啾脉冲傅立叶变换微波光谱。

DOI:
10.1021/jp2043202
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发表时间:
2010
期刊:
The journal of physical chemistry. A
影响因子:
--
通讯作者:
B. C. Dian
B. C. Dian
中科院分区:
--
文献类型:
--
作者:
David S. Wilcox;K. M. Hotopp;B. C. Dian

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发展了啁啾脉冲傅里叶变换微波(CP-FTMW)光谱的二维相关技术。光谱仪的宽带特性与快速数字电子设备相结合,允许产生任意脉冲序列,并同时检测微波频谱的8-18 GHz区域。这显著地增加了可以同时探测的旋转转变的数量,以及两个频率维度中的带宽。我们从理论和实验上评估三能级和四能级系统的相干转移与以前的研究方法。然后,我们扩展了单量子和自相关的原则,将宽带激发和检测。转动能级结构的全局连通性是通过在一个单一的二维实验中的多个相干态的转移来证明的。此外,从辐照多能级系统中观察到开放系统效应。在间接测量的频率维度和相位循环中的正交检测也适用于2D CP-FTMW光谱。
Two-dimensional (2D) correlation techniques are developed for chirped-pulse Fourier transform microwave (CP-FTMW) spectroscopy. The broadband nature of the spectrometer coupled with fast digital electronics permits the generation of arbitrary pulse sequences and simultaneous detection of the 8-18 GHz region of the microwave spectrum. This significantly increases the number of rotation transitions that can be simultaneously probed, as well as the bandwidth in both frequency dimensions. We theoretically and experimentally evaluate coherence transfer of three- and four-level systems to relate the method with previous studies. We then extend the principles of single-quantum and autocorrelation to incorporate broadband excitation and detection. Global connectivity of the rotational energy level structure is demonstrated through the transfer of multiple coherences in a single 2D experiment. Additionally, open-system effects are observed from irradiating many-level systems. Quadrature detection in the indirectly measured frequency dimension and phase cycling are also adapted for 2D CP-FTMW spectroscopy.
DOI: 10.1073/pnas.0508833103
发表时间: 2006-03-07
影响因子: 11.1
作者:
Mukherjee, P;Kass, I;Zanni, MT
通讯作者: Zanni, MT