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Journal Article

A General Approach To Combine the Advantages of Collinear and Noncollinear Spectrometer Designs in Phase-Resolved Second-Order Nonlinear Spectroscopy

MPS-Authors
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Garling,  Tobias
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Campen,  R. Kramer
Physical Chemistry, Fritz Haber Institute, Max Planck Society;
Faculty of Physics, University of Duisburg-Essen;

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Wolf,  Martin
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Thämer,  Martin
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Fulltext (public)

manuscript.pdf
(Any fulltext), 18MB

acs.jpca.9b09927.pdf
(Publisher version), 3MB

Supplementary Material (public)

SI.pdf
(Supplementary material), 18MB

Citation

Garling, T., Campen, R. K., Wolf, M., & Thämer, M. (2019). A General Approach To Combine the Advantages of Collinear and Noncollinear Spectrometer Designs in Phase-Resolved Second-Order Nonlinear Spectroscopy. The Journal of Physical Chemistry A, 123(51), 11022-11030. doi:10.17617/2.3177754.


Cite as: http://hdl.handle.net/21.11116/0000-0005-3CF8-1
Abstract
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 in­ volve the nonlinear interaction between three short laser pulses with the sample. ln 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. ln 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 spectrurneter to achieve a precise tirning control. The combination of this technique with a balanced detection scheme al­lows for the acquisition of highly accurate phase resolved nonlinear spectra without any loss in experimental flexibility. In fact, we show that the irnplernentation of this technique allows us to employ advanced pulse timing schemes inside the spectrometer, which can be used to sup­press nonlinear background signals and extend the capabilities of our spectrormeter to measure phase resolved sum frequency spectra of inter­faces in a liquid cell.