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Electronic optical response of molecules in intense fields: Comparison of TD-HF, TD-CIS, and TD-CIS(D) approaches
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10.1063/1.2743982
/content/aip/journal/jcp/126/24/10.1063/1.2743982
http://aip.metastore.ingenta.com/content/aip/journal/jcp/126/24/10.1063/1.2743982

Figures

Image of FIG. 1.
FIG. 1.

Simulation of in an oscillating electric field (energies and time in a.u., and ) with the basis. Top row: (a) electric field, (b) the instantaneous dipole calculated by TD-HF, and (c) the Fourier transform of the residual dipole after the field has returned to zero calculated by TD-HF. Second row: the Fourier transform of the residual dipole calculated by (d) TD-CIS, (e) TD-CIS(D), and (f) TD-CISD. Third row: contributions to the oscillation of the residual dipole computed from the wavefunction at the end of the simulation by (g) TD-CIS, (h) TD-CIS(D), and (i) TD-CISD. Bottom row: magnitude of the excited state coefficients in the wave function at the end of the simulation by (j) TD-CIS, (k) TD-CIS(D), and (l) TD-CISD.

Image of FIG. 2.
FIG. 2.

Simulation of in an oscillating electric field (energies and time in a.u., and ) with the aug-pVTZ basis plus three additional sets of diffuse functions. Top row: instantaneous dipole calculated by (a) TD-CIS, (b) TD-CISD, and (c) TD-HF. Second row: Fourier transform of the residual dipole after the field has returned to zero calculated by (d) TD-CIS, (e) TD-CISD, and (f) TD-HF. Third row: contributions to the oscillation of the residual dipole computed from the wave function at the end of the simulation by (g) TD-CIS and (h) TD-CISD. Bottom row: magnitude of the excited state coefficients in the wave function at the end of the simulation by (i) TD-CIS and (j) TD-CISD.

Image of FIG. 3.
FIG. 3.

Simulation of in an oscillating electric field (energies and time in a.u., and ) with the aug-pVTZ basis plus three additional sets of diffuse functions. Top row: instantaneous dipole calculated by (a) TD-CIS, (b) TD-CISD, and (c) TD-HF. Second row: Fourier transform of the residual dipole after the field has returned to zero calculated by (d) TD-CIS, (e) TD-CISD, and (f) TD-HF. Third row: contributions to the oscillation of the residual dipole computed from the wave function at the end of the simulation by (g) TD-CIS and (h) TD-CISD. Bottom row: magnitude of the excited state coefficients in the wave function at the end of the simulation by (i) TD-CIS and (j) TD-CISD.

Image of FIG. 4.
FIG. 4.

Response of the hydrogen molecule to increasing field strength: Fourier transform of the residual dipole obtained by (a) TD-HF, (b) TD-CIS, and (c) TD-CISD, and the squares of the wave function coefficients obtained by (d) TD-CIS and (e) TD-CISD (, aug-pVTZ basis plus three additional sets of diffuse functions).

Image of FIG. 5.
FIG. 5.

Comparison of excitation spectra for butadiene calculated with the basis set: (a) CIS excitation energies vs RPA or linear response TD-HF and (b) CIS(D) energies vs RPA . (c) The CIS spectrum polarized along the long axis of the molecule and (d) the corresponding RPA spectrum.

Image of FIG. 6.
FIG. 6.

Wave function coefficients as a function of the number of states included in the TD-CIS simulation. The magnitudes of the ten largest states are shown after the pulse has returned to zero: (a) neutral butadiene with a field strength of and (b) neutral hexatriene with a field strength of

Image of FIG. 7.
FIG. 7.

Fourier transform of the residual dipole after the field has returned to zero for butadiene calculated with the basis set: neutral (top row), monocation (middle two rows), and dication (bottom row) for TD-CIS (left column), TD-CIS(D) (middle column), and TD-HF (right column). Energies in a.u.: first two rows were calculated with and , and the last two rows were calculated with and

Image of FIG. 8.
FIG. 8.

Response of butadiene to increasing field strength: Fourier transform of the residual dipole obtained by (a) TD-HF, (b) TD-CIS, and (c) TD-CIS(D) and the squares of the wave function coefficients obtained by (d) TD-CIS and (e) TD-CIS(D) [, basis].

Image of FIG. 9.
FIG. 9.

Fourier transform of the residual dipole after the field has returned to zero for hexatriene [, basis]: neutral (top row, ), monocation (middle row, ), and dication (bottom row, ) for TD-CIS (left column), TD-CIS(D) (middle column), and TD-HF (right column).

Image of FIG. 10.
FIG. 10.

Response of hexatriene to increasing field strength: Fourier transform of the residual dipole obtained by (a) TD-HF, (b) TD-CIS, and (c) TD-CIS(D) and the squares of the wave function coefficients obtained by (d) TD-CIS and (e) TD-CIS(D) [ basis].

Tables

Generic image for table
Table I.

Comparison of static polarizabilities for butadiene calculated by Hartree-Fock and CCSD, and by second order perturbation theory using the CIS, CIS(D), and TD-HF excited states [ basis set].

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/content/aip/journal/jcp/126/24/10.1063/1.2743982
2007-06-28
2014-04-23
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Electronic optical response of molecules in intense fields: Comparison of TD-HF, TD-CIS, and TD-CIS(D) approaches
http://aip.metastore.ingenta.com/content/aip/journal/jcp/126/24/10.1063/1.2743982
10.1063/1.2743982
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