Isotope and mode selectivity in two-dimensional vibrational four wave mixing spectroscopy

Murdoch, Keith M.; Condon, Nicholas J.; Zhao, Wei; Besemann, Daniel M.; Meyer, Kent A.; Wright, John

doi:10.1016/s0009-2614(00)01392-0

Cited by 16 publications

(22 citation statements)

References 20 publications

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“…The Raman spectrum shows that there are two C Ð Ð ÐN stretch modes separated by 9 cm ¡1 . The coherent 2D DOVE FWM spectrum is shown in ®gure 26 [201]. In addition to the same features that were observed in ®gure 22, there is an additional DOVE IR peak at …!…”

Section: Experimental Observationssupporting

confidence: 53%

“…The 2D spectrum of the mixture was modelled using equation (37). The results are shown in ®gure 26(b) [201]. Again, the simulation reproduces the general features of the spectrum.…”

Section: Experimental Observationsmentioning

confidence: 59%

“…The ®rst example of CMDVS mode selectivity is shown in ®gure 27 [201]. This spectrum was taken with the same sample as ®gure 26 but with an expanded range for !…”

Section: Experimental Observationsmentioning

confidence: 99%

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Coherent multidimensional vibrational spectroscopy

Wright¹

2002

International Reviews in Physical Chemistry

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108

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Coherent multidimensional vibrational spectroscopy (CMDVS) is an emerging ®eld that o ers new oportunities to probe speci®cally intramolecular and intermolecular interactions in complex samples with the improved resolution and selectivity expected of a multidimensional method. In particular, it provides structural and dynamical information about correlations between modes. It provides this information on the picosecond time scales characteristic of vibrational dephasing. CMDVS is based on the perturbations that are induced in a mode when other coupled modes are excited. It is the vibrational analogue to multidimensional nucler magnetic resonance (NMR). In this review, we present the background that led to the development of CMDVS, a brief summary of the di erent methods of non-linear laser spectroscopy and how they can achieve CMDVS, the relationships between CMDVS and multidimensional NMR, and the theory necessary to understand the experimental results. The experimental approaches reviewed fall into three main classes: non-degenerate four-wave mixing which is doubly vibrationally enhanced, degenerate four-wave mixing which is triply vibrationally enhanced and six-wave mixing which has three Raman transitions. CMDVS has been implemented in both the time domain and the frequency domain. Finally, the review describes possible extensions of CMDVS and speculates on its future.

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Section: Experimental Observationssupporting

confidence: 53%

“…The 2D spectrum of the mixture was modelled using equation (37). The results are shown in ®gure 26(b) [201]. Again, the simulation reproduces the general features of the spectrum.…”

Section: Experimental Observationsmentioning

confidence: 59%

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Coherent multidimensional vibrational spectroscopy

Wright¹

2002

International Reviews in Physical Chemistry

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108

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“…Figure 2 shows the two dimensional DOVE-FWM spectra of a mixture of CH3CN, CD3CN, and C6D6 along with the infrared spectrum in the region of the DOVE resonances. 24 The x and y axes represent the ω 1 and ω 2 frequencies, respectively, and the colors indicate the signal intensity at ). There are diagonal features extending through these features that come from the Raman process when ω 1 − ω 2 matches the C-C stretch vibrational modes at 828 cm −1 and 917 cm −1 for CD3CN and CH3CN, respectively.…”

Section: Dove Methodsmentioning

confidence: 99%

Experimental Determinations of Coherent Multidimensional Vibrational Spectroscopy

Besemann¹,

Condon²,

Meyer³

et al. 2003

Bulletin of the Korean Chemical Society

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Coherent multidimensional vibrational spectroscopy is a new technique for establishing correlations between features in vibrational spectra that are caused by intra-and intermolecular interactions. These interactions cause cross-peaks between vibrational transitions that reflect the coupling. In this paper, we use Doubly Vibrationally Enhanced Infrared Spectroscopy (DOVE-IR) and DOVE-Raman processes to obtain coherent two dimensional vibrational spectra. The spectra are fitted to obtain the dephasing rates and third order susceptibilities (χ (3) ) for the nonlinear processes. We show that the DOVE χ (3) values are directly related to the molar absorptivities and Raman χ (3) . We then use these relationships to obtain estimates for the χ (3) of the stimulated photon echo and χ (5) of the six wave mixing spectroscopies, respectively. We also predict the ratio of the cascaded four wave mixing signal to the six wave mixing signal.

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“…CMDVS four-wave mixing (FWM) methods include pump-probe [5], stimulated photon echo (SPE) [6][7][8][9][10][11], and doubly vibrationally enhanced (DOVE) methods [12][13][14][15]. The pump-probe and DOVE methods are performed in the frequency domain and the SPE measurement is performed in the time domain.…”

Section: Introductionmentioning

confidence: 99%