Spectrally- and time-resolved vibrational surface spectroscopy: Ultrafast hydrogen-bonding dynamics at D2O/CaF2 interface

Bordenyuk, Andrey N.; Benderskii, Alexander V.

doi:10.1063/1.1873652

Cited by 62 publications

(84 citation statements)

References 70 publications

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“…In fact, Bordenyuk and Benderskii [119] have used such an approach with VSFG to study D 2 O on a calcium fluoride surface ( Figure 14). They collected the broadband VSFG spectrum as a function of delay time, and were able to extract a considerable amount of dynamic information on hydrogen bonding in this system.…”

Section: Comparison Of Vsfg Spectra Obtained With Different Techniquesmentioning

confidence: 98%

Reexamining the interpretation of vibrational sum-frequency generation spectra

Rivera

Fourkas

2011

International Reviews in Physical Chemistry

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Vibrational sum-frequency generation (VSFG) has become a widely used technique for studying molecular orientation and intermolecular structure at interfaces. Due to the interfacial and vibrational selectivity of this technique, it can be used to probe molecular monolayers that are buried within bulk materials. Here, we present a critical review and examination of the assumptions that are generally used in the interpretation of VSFG spectra. This review focuses on three different aspects of VSFG spectroscopy. First, we examine the effect of dynamics (both reorientation and energy transfer) on the interpretation of VSFG spectra. Second, we consider whether (and under what circumstances) VSFG spectra cannot be interpreted solely in terms of the spectral properties of individual molecules. Third, we consider whether VSFG spectra obtained in different modes (frequency-domain, time-domain and broadband) should provide identical information. We conclude with a discussion of the challenges and opportunities provided by the revised viewpoint of VSFG that we present.

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Section: Comparison Of Vsfg Spectra Obtained With Different Techniquesmentioning

confidence: 98%

Reexamining the interpretation of vibrational sum-frequency generation spectra

Rivera

Fourkas

2011

International Reviews in Physical Chemistry

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“…4,23,31 Thus, the upconversion pulse power, and with it the measured BB-SFG signal intensity, decreases with increasing spectral resolution. 4,23,31 Thus, the upconversion pulse power, and with it the measured BB-SFG signal intensity, decreases with increasing spectral resolution.…”

Section: Temporal Effects On Spectroscopic Line Shapes Resolution Amentioning

confidence: 99%

Temporal effects on spectroscopic line shapes, resolution, and sensitivity of the broad-band sum frequency generation

Stiopkin

Jayathilake

Weeraman

et al. 2010

The Journal of Chemical Physics

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Sum frequency generation (SFG) is a surface-selective spectroscopy that provides a wealth of molecular-level information on the structure and dynamics at surfaces and interfaces. This paper addresses the general issue of spectral resolution and sensitivity of the broad-band (BB) SFG that involves a spectrally narrow nonresonant (usually visible) and a BB resonant (usually infrared) laser pulses. We examine how the spectral width and temporal shape of the two pulses, and the time delay between them, relate to the spectroscopic line shape and signal level in the BB-SFG measurement. By combining experimental and model calculations, we show that the best spectral resolution and highest signal level are simultaneously achieved when the nonresonant narrow-band upconversion pulse arrives with a nonzero time delay after the resonant BB pulse. The nonzero time delay partially avoids the linear trade-off of improving spectral resolution at the expense of decreasing signal intensity, which is common in BB-SFG schemes utilizing spectral filtering to produce narrow-band visible pulses.

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“…[20][21][22][23][24][33][34][35][36] The signal generated at k 3 = k 1 + k 2 is represented by the diagram in Fig. 2͑a͒.…”

Section: B Infrared/raman Sfgmentioning

confidence: 99%

Controlling multidimensional off-resonant-Raman and infrared vibrational spectroscopy by finite pulse band shapes

Mukamel

2009

The Journal of Chemical Physics

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Sum-frequency vibrational spectroscopy of chiral liquids off and close to electronic resonance and the antisymmetric Raman tensor Closed expressions are derived which incorporate pulse shaping effects in femtosecond nonlinear optical signals involving various combinations of temporally well-separated vibrationally resonant infrared and electronically off-resonant Raman pulses. Combinations of broadband and narrow band pulses that yield multidimensional extensions of coherent anti-Stokes Raman and sum frequency generation spectroscopy are presented.

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Spectrally- and time-resolved vibrational surface spectroscopy: Ultrafast hydrogen-bonding dynamics at D2O/CaF2 interface

Cited by 62 publications

References 70 publications

Reexamining the interpretation of vibrational sum-frequency generation spectra

Reexamining the interpretation of vibrational sum-frequency generation spectra

Temporal effects on spectroscopic line shapes, resolution, and sensitivity of the broad-band sum frequency generation

Controlling multidimensional off-resonant-Raman and infrared vibrational spectroscopy by finite pulse band shapes

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