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Doubly resonant three-wave-mixing spectroscopy of a chiral coupled-chromophore system in solution: Coherent two-dimensional optical activity spectroscopy
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10.1063/1.2431806
/content/aip/journal/jcp/126/5/10.1063/1.2431806
http://aip.metastore.ingenta.com/content/aip/journal/jcp/126/5/10.1063/1.2431806

Figures

Image of FIG. 1.
FIG. 1.

Energy levels of coupled two-electronic-state system. The electronic coupling constant is and the delocalized one-exciton states are denoted as and , respectively, and is the single two-exciton state. Depending on the exciton-exciton binding energy, the energy of the two-exciton state can be slightly different from the value of .

Image of FIG. 2.
FIG. 2.

Molecular structure of alanine dipeptide and first and second derivatives, denoted as and , respectively, of the dipole moment with respect to the amide I local coordinate of the -methylacetamide.

Image of FIG. 3.
FIG. 3.

Amide I IR absorption spectra for the eight representative secondary structure dipeptides.

Image of FIG. 4.
FIG. 4.

(Color) The 2D IR-IR-SFG spectra, , are plotted in (a)–(h): (a) RHH, (b) LHH, (c) , (d) , (e) APB, (f) PB, (g) PII, and (h) FEB conformations, respectively. Frequencies are in .

Image of FIG. 5.
FIG. 5.

(Color) spectrum of and five spectra (see the main context for detailed descriptions).

Tables

Generic image for table
Table I.

Amide I local mode frequencies, mixing angles (in deg), two amide I normal mode frequencies, doubly excited state frequencies, and interpeptide amide I coupling constants (in ).

Generic image for table
Table II.

Magnitudes of the second-order dipole derivatives with respect to amide I local coordinates. values obtained by using the finite-difference calculation method are compared with approximate values [Eq. (41)]. Here, the dimensions of and are and , respectively, where and are the electron charge and mass and is the Bohr radius, respectively.

Generic image for table
Table III.

components of the rotationally averaged transition dipole products in Eq. (37) and the three angles in Eq. (47). The dimension of the transition dipole products is .

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/content/aip/journal/jcp/126/5/10.1063/1.2431806
2007-02-01
2014-04-24
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Doubly resonant three-wave-mixing spectroscopy of a chiral coupled-chromophore system in solution: Coherent two-dimensional optical activity spectroscopy
http://aip.metastore.ingenta.com/content/aip/journal/jcp/126/5/10.1063/1.2431806
10.1063/1.2431806
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