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Role of pulse phase and direction in two-dimensional optical spectroscopy

Publication ,  Journal Article
Keusters, D; Tan, HS; Warren, WS
Published in: Journal of Physical Chemistry A
December 9, 1999

This paper examines the parallels between magnetic resonance and optical spectroscopy, with the goal of determining to what extent the benefits of 2DNMR might be extended into the optical regime. Precise optical analogues of the simplest 2DNMR sequences (collinear pulse sequences with phased laser pulse generation, phase sensitive detection, and phase cycling) are now feasible, and we demonstrate that they do generate cross-peaks which reveal common energy levels, even when averaged over the distribution of pulse flip angles expected in most optical experiments. One enormous difference between laser and NMR experiments-the use of pulses in different directions in optics-can be exploited to eliminate much of the phase cycling required in NMR. Phase control does permit rotating-frame detection, which is likely to be a substantial practical advantage. Finally, we point out optical analogues of the simplest 2DNMR sequences (COSY and NOESY) will likely add little to our understanding of ultrafast dynamics. Optical analogues of more complex 2D sequences, combining phase control for selective refocusing with noncollinear pulse generation for coherence pathway selection, show more promise. © 1999 American Chemical Society.

Duke Scholars

Published In

Journal of Physical Chemistry A

DOI

ISSN

1089-5639

Publication Date

December 9, 1999

Volume

103

Issue

49

Start / End Page

10369 / 10380

Related Subject Headings

  • 5102 Atomic, molecular and optical physics
  • 3407 Theoretical and computational chemistry
  • 3406 Physical chemistry
  • 0307 Theoretical and Computational Chemistry
  • 0306 Physical Chemistry (incl. Structural)
  • 0202 Atomic, Molecular, Nuclear, Particle and Plasma Physics
 

Citation

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Keusters, D., Tan, H. S., & Warren, W. S. (1999). Role of pulse phase and direction in two-dimensional optical spectroscopy. Journal of Physical Chemistry A, 103(49), 10369–10380. https://doi.org/10.1021/jp992325b
Keusters, D., H. S. Tan, and W. S. Warren. “Role of pulse phase and direction in two-dimensional optical spectroscopy.” Journal of Physical Chemistry A 103, no. 49 (December 9, 1999): 10369–80. https://doi.org/10.1021/jp992325b.
Keusters D, Tan HS, Warren WS. Role of pulse phase and direction in two-dimensional optical spectroscopy. Journal of Physical Chemistry A. 1999 Dec 9;103(49):10369–80.
Keusters, D., et al. “Role of pulse phase and direction in two-dimensional optical spectroscopy.” Journal of Physical Chemistry A, vol. 103, no. 49, Dec. 1999, pp. 10369–80. Scopus, doi:10.1021/jp992325b.
Keusters D, Tan HS, Warren WS. Role of pulse phase and direction in two-dimensional optical spectroscopy. Journal of Physical Chemistry A. 1999 Dec 9;103(49):10369–10380.
Journal cover image

Published In

Journal of Physical Chemistry A

DOI

ISSN

1089-5639

Publication Date

December 9, 1999

Volume

103

Issue

49

Start / End Page

10369 / 10380

Related Subject Headings

  • 5102 Atomic, molecular and optical physics
  • 3407 Theoretical and computational chemistry
  • 3406 Physical chemistry
  • 0307 Theoretical and Computational Chemistry
  • 0306 Physical Chemistry (incl. Structural)
  • 0202 Atomic, Molecular, Nuclear, Particle and Plasma Physics