Simultaneous measurement of magnitude and phase in interferometric sum-frequency vibrational spectroscopy

Covert, Paul A.; Fitzgerald, William; Hore, Dennis K.

doi:10.1063/1.4731282

Cited by 42 publications

(64 citation statements)

References 31 publications

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“…Third, a) shoichi@apc.saitama-u.ac.jp because | χ (2) | 2 is proportional to the square of the density of interfacial molecules, conventional SFG is not very suitable for quantitative spectrometric experiments where an isosbestic point can be a good marker for measurement reliability. [16][17][18] Phase-sensitive SFG [19][20][21] and multiplex heterodynedetected SFG (HD-SFG) [22][23][24][25][26][27] have solved these problems of conventional SFG. In these methods, optical interference between SF signal light and local oscillator (LO) light permits the separate acquisition of the real and imaginary parts of χ (2) (Re χ (2) and Im χ (2) ).…”

Section: Introductionmentioning

confidence: 99%

Development of single-channel heterodyne-detected sum frequency generation spectroscopy and its application to the water/vapor interface

Yamaguchi

2015

The Journal of Chemical Physics

113

124

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Single-channel heterodyne-detected sum frequency generation (HD-SFG) spectroscopy for selectively measuring vibrational spectra of liquid interfaces is presented. This new methodology is based on optical interference between sum frequency signal light from a sample interface and phase-controlled local oscillator light. In single-channel HD-SFG, interferometric and spectrometric measurements are simultaneously carried out with an input IR laser scanned in a certain wavenumber range, which results in a less task than existing phase-sensitive sum frequency spectroscopy. The real and imaginary parts of second-order nonlinear optical susceptibility (χ((2))) of interfaces are separately obtained with spectral resolution as high as 4 cm(-1) that is approximately six times better than existing multiplex HD-SFG. In this paper, the experimental procedure and theoretical background of single-channel HD-SFG are explicated, and its application to the water/vapor interface is demonstrated, putting emphasis on the importance of a standard for the complex phase of χ((2)).

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Section: Introductionmentioning

confidence: 99%

Development of single-channel heterodyne-detected sum frequency generation spectroscopy and its application to the water/vapor interface

Yamaguchi

2015

The Journal of Chemical Physics

113

124

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“…In order to perform heterodyne detection, a local oscillator (LO) pulse that is at the same frequency as the VSFG signals has to be generated separately and collinearly aligned with the VSFG signals. 39,30,31,[33][34][35][36] To date, the only reported HD VSFG microscopy used a Michelson Interferometric geometry. 40 In this geometry, LO is generated in one of the Michelson Interferometer arms and combined with VSFG signals in the other arm.…”

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confidence: 99%

Self-Phase-Stabilized Heterodyne Vibrational Sum Frequency Generation Microscopy

2017

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Vibrational sum frequency generation (VSFG) spectroscopy has been a powerful technique to probe molecular structures at non-centrosymmetric media. Recent developed heterodyne (HD) detection can further reveal spectral phase and molecular orientations. Adding imaging capability to an HD VSFG signal can bring spatial visualization capability into this non-linear optical technique. However, it has been a challenge to build an HD VSFG microscope that is both easy to align and has good spectral phase stability -two necessary criterions for the broad application of this technique into various areas of science. Here, we report a fully-collinear HD VSFG microscope, which meets both phase stability and optical alignment requirements that can spatially resolve images of molecular interfaces and domains, with chemical and structural sensitivities. The phase stability is more than nine times better than a Michelson Interferometric HD VSFG microscope. Using this HD VSFG microscope, we study the structures of molecular selfassembly films. Because of the superior phase sensitivity, we successfully identify two molecular domains with different molecular orientations, which we show is not possible to extract from an ensemble-averaged VSFG spectrum or homodyne-detected VSFG image.

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“…The PSU and lens phase shifts were calculated using established expressions. 14,15 The wavelength-dependent phase shift by the lens is a function of its thickness (d), refractive index (n), and the speed 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 of light (c)…”

Section: Resultsmentioning

confidence: 98%

“…A direct measurement of the phase of (2) was made using a heterodyne SFG technique, the details of which are presented in prior publications. 14,15 Experimental conditions were the same as for the homodyne measurements with the addition 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60…”

Section: Acs Paragon Plus Environmentmentioning

confidence: 99%

“…[7][8][9] However, the absolute phase can be resolved only by interference with an SFG signal of known phase. This has been accomplished using a nonresonant signal generated in the far field (commonly from quartz or GaAs), 6,[10][11][12][13][14][15] or by interference with a nonresonant SFG signal from an internal source (commonly gold or silver) in the near field. 16,17 In cases where internal SFG phase references are available, the experimental technique is greatly simplified as it avoids the use of heterodyning.…”

Section: Introductionmentioning

confidence: 99%

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Assessing the Gold Standard: The Complex Vibrational Nonlinear Susceptibility of Metals

Covert

Hore

2014

J. Phys. Chem. C

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Sum-frequency generation techniques can o↵er molecular-level, structural details of surfaces and interfaces. The incorporation of a metallic layer, either exposed or buried, is frequently used to provide a non-vibrationally resonant reference to which the phase of the resonant responses may be compared. This in turn provides further structural information, such as the polarity of interfacial groups. Since the phase of the metal depends strongly on factors that alter the electronic structure of the interface, such as the wavelength of the visible beam, chemical bonding, and surface coverage, it is beneficial to characterize the phase of the nonresonant response. A direct measurement of the absolute phase of a commonly prepared model hydrophobic surface, 1-octadecanethiol bound to gold, is presented and compared with relative phase measurements. Assignment of the phase of metallic samples requires careful consideration of the e↵ects of the local field upon phase in both the near and far fields. We have outlined an approach that is suitable for the characterization of any dielectric or metal surface.

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Simultaneous measurement of magnitude and phase in interferometric sum-frequency vibrational spectroscopy

Cited by 42 publications

References 31 publications

Development of single-channel heterodyne-detected sum frequency generation spectroscopy and its application to the water/vapor interface

Development of single-channel heterodyne-detected sum frequency generation spectroscopy and its application to the water/vapor interface

Self-Phase-Stabilized Heterodyne Vibrational Sum Frequency Generation Microscopy

Assessing the Gold Standard: The Complex Vibrational Nonlinear Susceptibility of Metals

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