doi:10.1016/j.cplett.2004.01.027 
Copyright © 2004 Elsevier B.V. All rights reserved.
Two-dimensional spectroscopy using diffractive optics based phased-locked photon echoes
Departments of Physics and Chemistry, University of Toronto, 80 St. George Street, Toronto, ON, Canada M5S3H6
Received 8 October 2003;
Revised 11 January 2004.
Available online 19 February 2004.
References and further reading may be available for this article. To view references and further reading you must
purchase this article.
Abstract
A novel technique has been developed to passively phase-lock heterodyne-detected three-pulse photon echo experiments for two-dimensional optical spectroscopy. By using a diffractive optic to generate the pulses required, and with careful introduction of the time delays between the pulses, we achieve excellent passive phase-locking, approaching λ/100 at a wavelength of 540 nm. The ability to generate phase-locked pulse pairs with independent time delays solves a long standing impediment for stable phase sensitive detection in true optical analogues of multi-dimensional nuclear magnetic resonance (NMR) techniques, and should be equally valuable in executing related multi-dimensional spectroscopies in the infrared.
Fig. 1. Experimental setup and definition of the pulse sequence. Glass slides CB1 and CB2 compensate for the beam splitter BS and neutral density filter ND. The τ1 delay is implemented using either (a) two vertically stacked roof mirror retroreflectors, one of which is on a motorized translation stage or (b) rotating glass slides. (c) Two positions of the glass slides and beam paths are drawn (solid and dashed lines), showing how lateral beam shifts due to refraction are geometrically cancelled. (d) The boxcar geometry of the beams. (e) The timing of the 3 pulse echo pulse sequence.
Fig. 2. (a) Phase stability of the heterodyne-detected signal with the τ1 delay implemented using stacked retroreflectors. (b) The phase stability of the individual beam pairs, φ2−φ1 (solid) and φ3−φR (dashed), showing the strong anti-correlations that lead to the cancellation of fluctuations in the heterodyne-detected signal in their sum (dotted).
Fig. 3. Fit of the projection of the 2D data (points) to the spectrally resolved pump–probe data (line), at τ2=10 ps. This sets the phase of the 2D spectrum.
Fig. 4. (a) Amplitude, |S(ν3,ν1,τ2)|, of the 2D heterodyne-detected signal in R6G-ethanol at τ2=10 ps, (b) the absorptive (real) part, and (c) dispersive (imaginary) part. Contours are at intervals of 
5% of the peak, in arbitrary units, as shown in the upper (a and b) and lower (c) legends.
Abstract
Purchase PDF (269 K)
E-mail Article
Add to my Quick Links
Cited By in Scopus (46)
Purchase PDF (460 K)
