Structure and dynamics of molecular liquids investigated by optical-heterodyne detected Raman-induced Kerr effect spectroscopy (OHD-RIKES)

Cong, Peijun; Deuel, Hans P.; Simon, John D.

doi:10.1016/0009-2614(95)00492-m

Cited by 53 publications

(62 citation statements)

References 18 publications

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“…28–34 This technique has been applied to study various processes, including the dynamics of pure and mixed solvents, 35–38 electrolyte solutions, 39 ionic liquids, 40–42 polymer solutions, 43 and peptides and globular protein 44 at high concentrations. Studies involving multiplexed RIKES using a broad-band probe are limited.…”

Section: Introductionmentioning

confidence: 99%

Ultrafast Charge Transfer in Nickel Phthalocyanine Probed by Femtosecond Raman-Induced Kerr Effect Spectroscopy

et al. 2014

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The recently developed technique of femtosecond stimulated Raman spectroscopy, and its variant, femtosecond Raman-induced Kerr effect spectroscopy (FRIKES), offer access to ultrafast excited-state dynamics via structurally specific vibrational spectra. We have used FRIKES to study the photoexcitation dynamics of nickel(II) phthalocyanine with eight butoxy substituents, NiPc(OBu)8. NiPc(OBu)8 is reported to have a relatively long-lived ligand-to-metal charge-transfer (LMCT) state, an essential characteristic for efficient electron transfer in photocatalysis. Following photoexcitation, vibrational transitions in the FRIKES spectra, assignable to phthalocyanine ring modes, evolve on the femtosecond to picosecond time scales. Correlation of ring core size with the frequency of the ν10 (asymmetric C–N stretching) mode confirms the identity of the LMCT state, which has a ∼500 ps lifetime, as well as that of a precursor d-d excited state. An even earlier (∼0.2 ps) transient is observed and tentatively assigned to a higher-lying Jahn–Teller-active LMCT state. This study illustrates the power of FRIKES spectroscopy in elucidating ultrafast molecular dynamics.

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Section: Introductionmentioning

confidence: 99%

Ultrafast Charge Transfer in Nickel Phthalocyanine Probed by Femtosecond Raman-Induced Kerr Effect Spectroscopy

et al. 2014

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“…In a liquid, where the mean free path before collisions is small, the molecules do not execute complete rotations and the frequencies of the librational motion are primordially determined by the moment of inertia. 26 The moment of inertia for rotations around the axes that produces changes to the anisotropic ellipsoid is higher for the CS 2 molecules in comparison to the C 6 H 6 molecules. 26 According to this model, CS 2 molecules have a lower librational frequency and this originates a narrower spectral band, as measured by the ⌬ parameter.…”

Section: Resultsmentioning

confidence: 90%

“…26 The moment of inertia for rotations around the axes that produces changes to the anisotropic ellipsoid is higher for the CS 2 molecules in comparison to the C 6 H 6 molecules. 26 According to this model, CS 2 molecules have a lower librational frequency and this originates a narrower spectral band, as measured by the ⌬ parameter.…”

Section: Resultsmentioning

confidence: 90%

“…This relaxation times confirm the well known literature results for these liquids. 21,26,27 At shorter times ͑typically 100-1000 fs͒ the dynamics consist of complex, nondiffusive intermolecular motions ͑degrees of freedom͒ associated with the potential formed by nearby molecules through intermolecular forces. There are various contributions 28 to the nondiffusive response ͑albeit yet neither all known nor well separated͒: interaction induced anisotropy ͑I-I͒ ͑including binary colli-sions͒ that arises from distortions of the molecular polarizabilities induced by the intermolecular interactions, intermolecular vibrational which include orientational ͑librational͒ and translational degrees of freedom, molecular frame distor-tions associated with molecular collisions, and others.…”

Section: Resultsmentioning

confidence: 99%

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Molecular dynamics investigation with the time resolved optical Kerr effect on the CS2–C6H6 mixtures

Heisler

Correia

Cunha

2006

The Journal of Chemical Physics

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An investigation of the molecular dynamics in pure liquids and in mixtures through the technique of time resolved optical Kerr effect is performed. The samples studied were the mixtures of carbon disulfide (CS(2)) with benzene (C(6)H(6)). The molecular dynamics of the pure liquids is briefly discussed while the main results are obtained for the mixtures. A slow dynamics component is observed for the optical heterodyne detected optical Kerr effect transient decaying exponentially with time constants on picosecond time scale. The fast subpicosend time relaxations are analyzed in terms of the nondiffusive component of the spectral response that is associated with the molecular dynamics. The modifications of the spectrum are quantified, and the explanation of the observed changes is given in terms of the structural interaction configurations that produced changes in the intermolecular potential within which the molecules execute librational motions.

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“…Далее S R (τ ) подвергается процедуре деконволюции (6), в результате чего получают функцию РСП T RSD (ω). В качестве примера рассмотрим зависимость формы T RSD (ω) от параметра γ для сигнала бензонитрила C 6 H 5 CN, экспериментальные данные которого представлены, например, в работах [24][25][26][27][28]. Рисунок 1 показывает сигнал ОЭК, полученный в работе [24], где огибающая интенсивности лазерных импульсов с несущей длиной волны 790 nm имела вид…”

Section: оптический нелинейный отклик среды третьего порядка и редуцированная рспunclassified

Низкочастотные Молекулярные Отклики В Жидкости При Регистрации Сверхбыстрого Оптического Эффекта Керра

Никифоров¹

2019

Журнал Технической Физики

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Low-frequency molecular rotations recorded in a region of 0–150 cm^–1 with a high “signal/noise” ratio in the ultrafast optical Kerr effect (OKE), which is a third-order nonlinear optical response upon nonresonant excitation of a liquid by femtosecond laser pulses, are analyzed in detail. It is shown that the reduced Raman spectral density (RSD) derived from experimental data using the well-known deconvolution procedure is ambiguous due to the problem of separating the orientational and librational contributions to the total OKE signal. This fact significantly limits the reliability of information derived about molecular motions in a liquid. For the example of an ultrafast OKE in benzonitrile, it is shown that, in the range of 0–300 fs, rotational responses cannot be considered independent, and the application of a number of additional criteria resulting from the assumption of their correlation allows this ambiguity in deriving the RSD function from experimental data to be removed.

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Structure and dynamics of molecular liquids investigated by optical-heterodyne detected Raman-induced Kerr effect spectroscopy (OHD-RIKES)

Cited by 53 publications

References 18 publications

Ultrafast Charge Transfer in Nickel Phthalocyanine Probed by Femtosecond Raman-Induced Kerr Effect Spectroscopy

Ultrafast Charge Transfer in Nickel Phthalocyanine Probed by Femtosecond Raman-Induced Kerr Effect Spectroscopy

Molecular dynamics investigation with the time resolved optical Kerr effect on the CS2–C6H6 mixtures

Низкочастотные Молекулярные Отклики В Жидкости При Регистрации Сверхбыстрого Оптического Эффекта Керра

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