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Fluorescence-detected two-dimensional electronic coherence spectroscopy by acousto-optic phase modulation
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10.1063/1.2800560
/content/aip/journal/jcp/127/21/10.1063/1.2800560
http://aip.metastore.ingenta.com/content/aip/journal/jcp/127/21/10.1063/1.2800560

Figures

Image of FIG. 1.
FIG. 1.

Energy level diagram for the D line transitions (described in text and Table I). For the purposes of our experiments, the system behaves as a three-level atom with ground state , first excited state , and second excited state .

Image of FIG. 2.
FIG. 2.

Illustration of a train of four sequential phase-modulated pulses. Each pulse sequence is labeled by the superscript ; the individual pulses are labeled by subscripts 1–4. A pulse sequence is characterized by the interpulse delays , , and and the relative temporal phases and .

Image of FIG. 3.
FIG. 3.

Wave packet pathway diagrams for the four nonlinear population terms isolated by PM-ECS (described in text). Separate panels illustrate the pathways for (a) , (b) , (c) , and (d) . The overlaps described in panels (a) and (d) contribute to our “sum signal” and the overlaps described in panels (b) and (c) contribute to our “difference signal.”

Image of FIG. 4.
FIG. 4.

Diagrams illustrating the four distinct wave packet pathways that contribute to the overlap (described in text). The pathways depicted in panels (a) and (b) are “single-mode” pathways, while those depicted in panels (c) and (d) are “coupling” pathways.

Image of FIG. 5.
FIG. 5.

(Color online) Schematic diagram of the experimental setup for phase modulation (PM)-ECS (described in text). Abbreviations have the following meanings. APD, amplified photodiode; PD, photodiode; AO, acousto-optic Bragg cell; BS, beam splitter.

Image of FIG. 6.
FIG. 6.

Grayscale contour diagrams of the calculated difference [panels (g)–(l)] and sum signals for the Rb system, obtained from PM-ECS (described in text). Real and imaginary parts of each signal are given in the top and bottom rows, respectively. In the left column [panels (a), (d), (g), and (j)] are plots of the undersampled two-dimensional interferograms. In the center column [panels (b), (e), (h), and (k)] are plots of the fully sampled interferograms. In the right column [panels (c), (f), (i), and (l)] are plots of the instrumental phase functions.

Image of FIG. 7.
FIG. 7.

Comparison between theoretical calculations [panels (a)–(d)] and experimental data [panels (e)–(h)] for the difference signal interferograms obtained by PM-ECS (described in text).

Image of FIG. 8.
FIG. 8.

Comparison between theoretical calculations [panels (a)–(d)] and experimental data [panels (e)–(h)] for the sum signal interferograms obtained by PM-ECS (described in text).

Image of FIG. 9.
FIG. 9.

Comparison between theoretical calculations [panels (a)–(d)] and experimental data [panels (e)–(h)] for the rephasing susceptibility obtained by PM-ECS (described in text).

Image of FIG. 10.
FIG. 10.

Comparison between theoretical calculations [panels (a)–(d)] and experimental data [panels (e)–(h)] for the nonrephasing susceptibility obtained by PM-ECS (described in text).

Image of FIG. 11.
FIG. 11.

Comparison between theoretical calculations [panels (a)–(d)] and experimental data [panels (e)–(h)] for the two-dimensional correlation spectra obtained by PM-ECS (described in text).

Tables

Generic image for table
Table I.

Physical constants associated with optical line transitions. is the transition index, is the transition frequency, is the transition wavelength, is the transition dipole moment (in units of Debye), is the lifetime, and is the natural line width (Ref. 41).

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/content/aip/journal/jcp/127/21/10.1063/1.2800560
2007-12-07
2014-04-25
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Fluorescence-detected two-dimensional electronic coherence spectroscopy by acousto-optic phase modulation
http://aip.metastore.ingenta.com/content/aip/journal/jcp/127/21/10.1063/1.2800560
10.1063/1.2800560
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