the detection wavelength increases (i.e., the peaks move further off-diagonal at
longer detection wavelengths) [23].
The measurement displayed in Fig. 10c is distinct from the other two in that
resonances with equal intensities appear in all four quadrants of the 2DRR
spectrum. The model calculations presented below the corresponding measurements
in Fig. 10 suggest that this pattern of resonances originates in the sequences of fieldmatter interactions discussed in Sect. 2.1. Consider that the third and fourth fieldmatter interactions occur on the same sides of the Feynman diagrams in terms 1–8.
Therefore, as discussed in Sect. 2.1, either the bra or ket must have the same
vibrational state index in both s 1 and s 2 . This constraint causes intensity to
accumulate in the upper-right and lower-left quadrants of the spectrum [22, 23]. In
contrast, the third and fourth field-matter interactions occur on opposite sides of the
Feynman diagrams in terms 9–12; vibronic coherence transfer from triiodide to
diiodide produces a coherence in s 2 that is fully independent from that in s 1 .
Consequently, peaks with equal intensities appear in all four quadrants. This
unambiguous signature of vibronic coherence transfer should generalize to other
Fig. 10 Summary of 2DRR experiments conducted on triiodide: a the response of triiodide is detected in
both dimensions (terms 1–4 in Fig. 3); b the response of the diiodide photoproduct is detected in both
dimensions (terms 5–8 in Fig. 3); c the response of triiodide and diiodide are detected in separate
dimensions (terms 9–12 in Fig. 3). Experimental and theoretical 2DRR spectra are presented in the
second and third rows, respectively. Calculations in panels (a), (b), and (c) employ Eqs. (22), (23), and
(24). Blue and red laser pulses represent wavelengths that are electronically resonant with triiodide and
diiodide, respectively Adapted from Guo et al. [23], with the permission of AIP Publishing
Top Curr Chem (Z) (2017) 375:87
123
263
Reprinted from the journal
longer detection wavelengths) [23].
The measurement displayed in Fig. 10c is distinct from the other two in that
resonances with equal intensities appear in all four quadrants of the 2DRR
spectrum. The model calculations presented below the corresponding measurements
in Fig. 10 suggest that this pattern of resonances originates in the sequences of fieldmatter interactions discussed in Sect. 2.1. Consider that the third and fourth fieldmatter interactions occur on the same sides of the Feynman diagrams in terms 1–8.
Therefore, as discussed in Sect. 2.1, either the bra or ket must have the same
vibrational state index in both s 1 and s 2 . This constraint causes intensity to
accumulate in the upper-right and lower-left quadrants of the spectrum [22, 23]. In
contrast, the third and fourth field-matter interactions occur on opposite sides of the
Feynman diagrams in terms 9–12; vibronic coherence transfer from triiodide to
diiodide produces a coherence in s 2 that is fully independent from that in s 1 .
Consequently, peaks with equal intensities appear in all four quadrants. This
unambiguous signature of vibronic coherence transfer should generalize to other
Fig. 10 Summary of 2DRR experiments conducted on triiodide: a the response of triiodide is detected in
both dimensions (terms 1–4 in Fig. 3); b the response of the diiodide photoproduct is detected in both
dimensions (terms 5–8 in Fig. 3); c the response of triiodide and diiodide are detected in separate
dimensions (terms 9–12 in Fig. 3). Experimental and theoretical 2DRR spectra are presented in the
second and third rows, respectively. Calculations in panels (a), (b), and (c) employ Eqs. (22), (23), and
(24). Blue and red laser pulses represent wavelengths that are electronically resonant with triiodide and
diiodide, respectively Adapted from Guo et al. [23], with the permission of AIP Publishing
Top Curr Chem (Z) (2017) 375:87
123
263
Reprinted from the journal