Multiresonant coherent multidimensional spectroscopy.

Multiresonant coherent multidimensional spectroscopy.
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多共振相干多维光谱。

DOI:
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发表时间:
2011
期刊:
Annual review of physical chemistry (Print)
影响因子:
--
通讯作者:
J. C. Wright
J. C. Wright
中科院分区:
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文献类型:
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作者:
J. C. Wright

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多共振相干多维光谱学是一种频域方法,其使用可调谐激发脉冲来激发多个量子相干态(MQCs)和/或使用完全相干或部分相干激发路径的态布居。通过分子内和分子间相互作用耦合的状态对以它们的频率差重新发射光。MQCs是相干的并且相长干涉以产生相位匹配的输出光束。用固定的激励脉冲时间延迟扫描激励频率产生多维光谱,而用固定的激励频率扫描时间延迟测量MQCs的相干和非相干动力学。多共振方法可以激发振动和/或电子状态的任何组合,并使用任何相干路径。当一个状态的激发扰动另一个状态时,状态之间就会出现交叉峰。这种耦合要求用于消除频谱拥塞。光谱分辨率的提高是因为多共振方法缩小了不均匀加宽,增强了特定组分的峰,并将分辨率扩展到多个维度。
Multiresonant coherent multidimensional spectroscopy is a frequency-domain method that uses tunable excitation pulses to excite multiple quantum coherences (MQCs) and/or state populations using fully coherent or partially coherent excitation pathways. Pairs of states that are coupled by intra- and intermolecular interactions re-emit light at their frequency differences. The MQCs are coherent and interfere constructively to create phase-matched output beams. Scanning the excitation frequencies with fixed-excitation-pulse time delays creates multidimensional spectra, whereas scanning the time delays with fixed excitation frequencies measures the MQCs' coherent and incoherent dynamics. Multiresonant methods can excite any combination of vibrational and/or electronic states and use any coherence pathway. Cross-peaks occur between states when the excitation of one perturbs the other. This requirement for coupling acts to eliminate spectral congestion. Spectral resolution is increased because multiresonant methods narrow inhomogeneous broadening, enhance peaks from specific components, and spread the resolution over multiple dimensions.
DOI: 10.1529/biophysj.105.074534
发表时间: 2006-07-15
影响因子: 3.4
作者:
Nan, Xiaolin;Potma, Eric O.;Xie, X. Sunney
通讯作者: Xie, X. Sunney
DOI: 10.1103/physrevlett.86.3899
发表时间: 2001-04-23
影响因子: 8.6
作者:
Merchant, KA;Thompson, DE;Fayer, MD
通讯作者: Fayer, MD