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Alternative selection rules for one- and two-photon transitions in tribenzotetraazachlorin: Quasi-centrosymmetrical π-conjugation pathway of formally non-centrosymmetrical molecule
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10.1063/1.4807594
/content/aip/journal/jcp/138/21/10.1063/1.4807594
http://aip.metastore.ingenta.com/content/aip/journal/jcp/138/21/10.1063/1.4807594

Figures

Image of FIG. 1.
FIG. 1.

Schematic of the femtosecond pump-probe setup. QPD1, QPD2 are quad photo-detectors used for the alignment of the beam overlap; SPD1, SPD2 are sandwich photo-detectors; NDFW1, NDFW2 are neutral density filter wheels; M1, M2, M3 are computer-controlled mirrors; BS1 is a computer-controlled beam splitter. SM1 is a spherical focusing mirror; SH1, SH2 are computer-controlled shutters; SHG BBO is a frequency doubling BBO crystal.

Image of FIG. 2.
FIG. 2.

1PA (blue solid line), 2PA (red symbols) spectra, and fluorescence anisotropy as a function of one-photon excitation wavelength (solid line, upper panels) of HTBTAC (left panel) and HTtBuPc (right panel). Vertical dashed lines indicate locations of the quasi and transitions (see text for details).

Image of FIG. 3.
FIG. 3.

Prevalent theoretical π-conjugation pathway (thick lines) in HTBTAC (a) and HTtBuPc (b). Numbers shown next to the bonds symbols in HTtBuPc depict relative induced current density calculated in Ref. .

Image of FIG. 4.
FIG. 4.

ESA spectra (symbols) of HTBTAC (a) and HTtBuPc (b). Linear absorption spectra are shown for comparison (blue line). Vertical arrows indicate the positions of the tentative transitions relevant to the 2PA spectra.

Image of FIG. 5.
FIG. 5.

Experimental 2PA spectra (red symbols) and 2PA spectra simulated as a stepwise GS + ESA absorption (solid line) of HTBTAC (a) and HTtBuPc (b) using the parameters summarized in Table I . Insets show the energy level diagrams with the corresponding degenerate 2PA (red arrows) and singlet-singlet ESA with the pump photon shown by a blue arrow and the probe photon shown by a maroon arrow. Two states labeled as S and S in the case of HTtBuPc correspond to two different final states of the 2PA transition, as described in the text. The solid brown curve in panel (b) shows the result obtained by assuming that both the 1st and 2nd peak having A → A symmetry; whereas the dashed brown line corresponds to the A → B character of the 2nd peak.

Tables

Generic image for table
Table I.

Transition frequencies calculated as a sum of GS and ESA peaks ( ) and 2PA ( ), dipole moments, symmetry factor A with the symmetry of the final state shown in parentheses, and calculated and measured peak 2PA cross sections of the transition.

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/content/aip/journal/jcp/138/21/10.1063/1.4807594
2013-06-07
2014-04-23
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Alternative selection rules for one- and two-photon transitions in tribenzotetraazachlorin: Quasi-centrosymmetrical π-conjugation pathway of formally non-centrosymmetrical molecule
http://aip.metastore.ingenta.com/content/aip/journal/jcp/138/21/10.1063/1.4807594
10.1063/1.4807594
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