Measuring Complex Sum Frequency Spectra with a Nonlinear Interferometer

<div> <div> <p>Recent years have seen a huge progress in the development of phase sensitive second order laser spectroscopy which has proven to be a very powerful tool for the investigation of interfaces. These interferometric techniques involve the nonlinear interaction between three short laser pulses with the sample. In order to obtain accurate phase information, the relative phases between the pulses must be stabilized and their timings precisely controlled. Despite much progress made, fulfilling both requirements remains a formidable experimental challenge. The two common approaches employ different beam geometries which each yields its particular advantages and deficiencies. While non-collinear spectrometers allow for a relatively simple timing control they typically yield poor phase stability and require a challenging alignment. Collinear approaches in contrast come with a simplified alignment and improved phase stability but typically suffer from a highly limited timing control. In this contribution we present a general experimental solution which allows for combining the advantages of both approaches while being compatible with most of the common spectrometer types. Based on a collinear geometry we exploit different selected polarization states of the light pulses in well- defined places in the spectrometer to achieve a precise timing control. The combination of this technique with a balanced detection scheme al- lows for the acquisition of highly accurate phase resolved nonlinear spectra without any loss in experimental flexibility. In fact, we show that the implementation of this technique allows us to employ advanced pulse timing schemes inside the spectrometer, which can be used to sup- press nonlinear background signals and extend the capabilities of our spectrometer to measure phase resolved sum frequency spectra of inter- faces in a liquid cell.</p> </div> </div>

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Interpreting Vibrational Sum-Frequency Spectra of Sulfur Dioxide at the Air/Water Interface: A Comprehensive Molecular Dynamics Study

The Journal of Physical Chemistry B ◽

10.1021/jp100310s ◽

2010 ◽

Vol 114 (21) ◽

pp. 7245-7249 ◽

Cited By ~ 20

Author(s):

Marcel Baer ◽

Christopher J. Mundy ◽

Tsun-Mei Chang ◽

Fu-Ming Tao ◽

Liem X. Dang

Keyword(s):

Molecular Dynamics ◽

Sulfur Dioxide ◽

Water Interface ◽

Frequency Spectra ◽

Sum Frequency ◽

Air Water Interface

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Intensity relation between IR–UV doubly resonant sum-frequency spectra and antisymmetric resonant vibrational Raman scattering of chiral solutions

Chemical Physics Letters ◽

10.1016/j.cplett.2007.12.057 ◽

2008 ◽

Vol 452 (1-3) ◽

pp. 215-219

Author(s):

Hai-Long Wang ◽

Ming He ◽

Dong-Ming Chen ◽

Tian-Jing He ◽

Fan-Chen Liu

Keyword(s):

Raman Scattering ◽

Frequency Spectra ◽

Sum Frequency

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Molecular dynamics simulations of surface-specific bonding of the hydrogen network of water: A solution to the low sum-frequency spectra

Physical Review B ◽

10.1103/physrevb.86.035408 ◽

2012 ◽

Vol 86 (3) ◽

Cited By ~ 22

Author(s):

Tatsuya Ishiyama ◽

Hideaki Takahashi ◽

Akihiro Morita

Keyword(s):

Molecular Dynamics ◽

Molecular Dynamics Simulations ◽

Frequency Spectra ◽

Sum Frequency ◽

Hydrogen Network ◽

Dynamics Simulations

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Limitations in the Analysis of Vibrational Sum-Frequency Spectra Arising from the Nonresonant Contribution

The Journal of Physical Chemistry C ◽

10.1021/jp200915z ◽

2011 ◽

Vol 115 (23) ◽

pp. 11550-11559 ◽

Cited By ~ 21

Author(s):

Alexander D. Curtis ◽

Scott R. Burt ◽

Angela R. Calchera ◽

James E. Patterson

Keyword(s):

Frequency Spectra ◽

Sum Frequency

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Phase-Sensitive Sum-Frequency Generation Measurements Using a Femtosecond Nonlinear Interferometer

The Journal of Physical Chemistry C ◽

10.1021/acs.jpcc.9b00861 ◽

2019 ◽

Vol 123 (12) ◽

pp. 7266-7270 ◽

Cited By ~ 3

Author(s):

Shumei Sun ◽

Patrick J. Bisson ◽

Mischa Bonn ◽

Mary Jane Shultz ◽

Ellen H. G. Backus

Keyword(s):

Sum Frequency Generation ◽

Sum Frequency ◽

Phase Sensitive ◽

Nonlinear Interferometer ◽

Frequency Generation

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Sum Frequency Spectra in the C-H Stretch Region of Adsorbates on Iron

Applied Spectroscopy ◽

10.1366/0003702934048361 ◽

1993 ◽

Vol 47 (2) ◽

pp. 167-172 ◽

Cited By ~ 9

Author(s):

C. R. Maechling ◽

D. A. V. Kliner ◽

D. Klenerman

Keyword(s):

Acetic Acid ◽

Iron Oxide ◽

Stearic Acid ◽

Vibrational Spectra ◽

Analytical Tool ◽

Hydrocarbon Contamination ◽

Frequency Spectra ◽

Sum Frequency ◽

Langmuir Blodgett ◽

Langmuir Blodgett Films

Infrared-visible sum frequency generation (SFG) was used to record vibrational spectra in the C-H stretch region of single monolayer Langmuir-Blodgett films of stearic acid, octadecylamine, and p-octadecylphenyl acetic acid on iron oxide, demonstrating the sensitivity of SFG to about 0.1 monolayer. Within our present signal-to-noise limitations, it was not possible to obtain SFG spectra of the aromatic C-H stretch in p-octadecylphenyl acetic acid or the N-H stretch in octadecylamine. Vibrational spectra in the C-H stretch region have also been obtained for chemically adsorbed monolayers of stearic acid and oleic imidazoline on iron oxide; however an undetermined fraction of these spectra result from hydrocarbon contamination. Finally, an SFG spectrum was obtained at a buried interface, that of p-octadecylphenyl acetic acid on iron oxide under water. The potential of SFG as a surface analytical tool is discussed.

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