Transient Grating Optical Heterodyne Detected Impulsive Stimulated Raman Scattering in Simple Liquids

Vöhringer, Peter; Scherer, Norbert F.

doi:10.1021/j100009a027

Cited by 166 publications

(157 citation statements)

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“…28,29 Here it is important to note that such spikes do not require resonance enhancement; they are present even in transparent materials. 30 Because of this off-resonance contribution, we suggest that the glass cover slips and TiO 2 films (common to all samples) are primarily responsible for the spikes. The offsets in the TG signals measured at long delay times, A 2 , reflect the excited state electronic structures of RuCmp-TiO 2 and Catechol-TiO 2 .…”

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confidence: 86%

Communication: Uncovering molecule-TiO2 interactions with nonlinear spectroscopy

Miller

West

Curtis

et al. 2011

The Journal of Chemical Physics

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Femtosecond transient grating experiments are used to investigate electronic structures and transport mechanisms in dye-sensitized nanocrystalline TiO2 films. This study examines two molecular sensitizers spanning the weak (a phosphonated Ruthenium complex) and strong (catechol) molecule-TiO2 coupling regimes. It is shown that strong molecule-TiO2 interactions give rise to photoinduced vibrational coherences at the interface between species. We suggest that the amplitudes of these coherences reflect the molecule-TiO2 coupling strength and signify the delocalization of excited state wavefunctions.

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confidence: 86%

Communication: Uncovering molecule-TiO2 interactions with nonlinear spectroscopy

Miller

West

Curtis

et al. 2011

The Journal of Chemical Physics

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confidence: 99%

“…[23][24][25] Therefore, electric field-resolved signal detection is essential to the development of new higher-order methods as it allows the absolute sign of the signal to be extracted and unambiguously reveals the relative magnitudes of various competing terms in the nonlinear polarization response. 7,[26][27][28][29] In this Letter, we report the new method of electric fieldresolved coherent Stokes Raman spectroscopy (EFR-CSRS). The information content is demonstrated via measurements of cyclohexane and benzene in the C-H stretching region of the vibrational spectrum with a passively phase-stabilized, diffractive optic-based interferometer.…”

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confidence: 99%

“…Lettersstrong low-frequency intermolecular mode spectrum of liquid benzene, 28,40 which possesses higher frequency content than that of cyclohexane, 41 contributes to its prominent broadband signal component through the finite pulse durations of the laser pulses. This mechanism of signal emission may also be described with the NR1 and NR2 terms of Figure 2; it yields a frequency and bandwidth similar to that of the Stokes pulse.…”

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Field-Resolved Coherent Raman Spectroscopy of High Frequency Vibrational Resonances

2006

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Electric fields of coherent Raman signals are resolved with sensitivity for high-frequency vibrational resonances utilizing a four-pulse, trapezoidal beam geometry in a diffractive optic-based interferometer. Our experiments show that the heterodyne detected signal phase is stabilized for particular terms in the third-order response function by the cancellation of inter-pulse phases. The C-H stretching modes of cyclohexane and benzene are studied under two polarization conditions. The temporal profiles of signal fields for cyclohexane exhibit a low-frequency recurrence due to the interference between the signals associated with the symmetric and asymmetric C-H stretching modes. In contrast, the electronically nonresonant polarizability response of benzene gives rise to a significant broadband signal component in addition to that associated with its C-H vibrational resonance. Time-frequency shapes of the Raman signal fields are strongly dependent on the properties of the liquid and the polarizations of the laser pulses.Passively phase-stabilized heterodyned signal detection in transient grating and photon echo spectroscopies has recently been realized at optical frequencies by the incorporation of diffractive optics in four-wave mixing interferometers, thereby enhancing the sensitivity and information content of these techniques compared to that obtained with conventional homodyne detection. [1][2][3][4][5][6][7][8] This is more easily realized at infrared wavelengths due to significantly reduced mechanical stability requirements. Optical nonlinear spectroscopies are most useful for studying energy transfer dynamics in multilevel electronic systems, 5 whereas infrared spectroscopies provide more detailed information on molecular structure and dynamics through vibrational mode couplings. 9-13 By contrast, broadband stimulated Raman gain spectroscopy has the unique ability to resolve vibrational dynamics within a window of more than 1000 cm -1 with less than 100 fs time resolution in a single experiment. [14][15][16] Broadband optical measurements have long been undertaken 17 but pulse durations of less than 50 fs are more difficult to attain at infrared wavelengths, so the corresponding spectral range is reduced.Nonlinear spectroscopies intrinsically possess more information at higher orders. 15,16,[18][19][20][21][22] However, the interpretation of these experiments is complicated by interference between terms in the material response function. Dephasing-induced resonances in coherent anti-Stokes Raman spectroscopy are a good example at third order. [23][24][25] Therefore, electric field-resolved signal detection is essential to the development of new higher-order methods as it allows the absolute sign of the signal to be extracted and unambiguously reveals the relative magnitudes of various competing terms in the nonlinear polarization response. 7,[26][27][28][29]

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“…In this scheme the signal is proportional to the amplitude rather than intensity of the diffracted wave 17,18,16 . Considering that E dif f /E trans is typically of order 10 −5 − 10 −4 , coherent detection enhances the ratio of signal to stray light by four or five orders of magnitude.…”

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confidence: 99%

Optical Transient-Grating Measurements of Spin Diffusion andRelaxation in a Two-Dimensional Electron Gas

Weber¹

2005

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Spin diffusion in n-GaAs quantum wells, as measured by our optical transient-grating technique, is strongly suppressed relative to that of charge. Over a broad range of temperatures and dopings, the suppression of D s relative to D c agrees quantitatively with the prediction of "spin Coulomb drag" theory, which takes into account the exchange of spin in electron-electron collisions.Moreover, the spin-diffusion length, L s , is a nearly constant 1 µm over the same range of T and n, despite D s 's varying by nearly two orders of magnitude. This constancy supports the D'yakonov-Perel'-Kachorovskii model of spin relaxation through interrupted precessional dephasing in the spin-orbit field.

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Transient Grating Optical Heterodyne Detected Impulsive Stimulated Raman Scattering in Simple Liquids

Cited by 166 publications

References 11 publications

Communication: Uncovering molecule-TiO2 interactions with nonlinear spectroscopy

Communication: Uncovering molecule-TiO2 interactions with nonlinear spectroscopy

Field-Resolved Coherent Raman Spectroscopy of High Frequency Vibrational Resonances

Optical Transient-Grating Measurements of Spin Diffusion andRelaxation in a Two-Dimensional Electron Gas

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