TDDFT Study of One- and Two-Photon Absorption Properties:  Donor−π−Acceptor Chromophores

Day, Paul N.; Nguyen, Kiet A.; Pachter, Ruth

doi:10.1021/jp047511i

Cited by 101 publications

(126 citation statements)

References 95 publications

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“…More recently, Frediani et al 13 calculated a value of 765 GM for the higher energy transition of DIAMINO in vacuo. In spite of the energy difference ͑about 0.4 eV͒, we believe that the S 0 → S 3 transition determined in this work accesses the same 3 1 Ag state reported by Frediani et al 13 For DO3, a value of 84 GM was reported by Day et al 11 through a TDDFT/B3LYP study applying the two-state approximation and a Lorentzian line-shape for the S 0 → S 2 transition. Frediani et al 13 also studied this compound using the B3LYP functional and reported values of 327 and 247 GM for S 0 → S 2 and S 0 → S 4 transitions in vacuo, respectively.…”

Section: -7supporting

confidence: 85%

“…The calculated oscillator strength is related to the experimental integrated intensity by the relation 11 f gf = 4.32 ϫ 10 −9…”

Section: B 1pamentioning

confidence: 99%

“…It is common practice to assume a single Gaussian ͑or Lorentzian͒ function to represent an experimental spectral band, which gives rise to an approximate measure of the corresponding band intensity. For a Gaussian line-shape one gets 11 f gf = 4.32 ϫ 10 −9 2͑ln 2͒ 1/2 ͱ max ⌫ gf ,…”

Section: ͑2͒mentioning

confidence: 99%

“…͑4͔͒. In this work the two-photon transition matrix element is defined considering single beam 2PA measurements, and therefore it is one fourth of the Birge's formula, 41 defined considering double-beam 2PA measurements and which was used by Day et al 11 and Frediani et al 13 On the other hand, while in these works the 2PA cross-section was defined dividing the transition rate by the square of photon flux, here it is defined dividing the dissipation rate of the photons of the incident light single beam by the square of photon flux, what make consistent the comparison of our theoretical results with the experimental data obtained by De Boni et al 6 using the Z-scan technique. 19 Therefore, our definition for 2PA cross-section ͓Eq.…”

Section: -7mentioning

confidence: 99%

“…[7][8][9] More recently, theoretical methods have been employed to support the understanding of experimental 2PA spectrum of several compounds, 8,[10][11][12] including azoaromatic compounds, which have also been the target of theoretical studies. [11][12][13] Among several theoretical methods used to study electronic transitions of compounds, the density functional theory ͑DFT͒ combined with linear response function formalism 14 has been shown to provide accurate excitation energies particularly when employing hybrid exchange-correlation functionals. Likewise, application of quadratic response function can be used to study the 2PA process.…”

Section: Introductionmentioning

confidence: 99%

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Theoretical study of one- and two-photon absorption spectra of azoaromatic compounds

Silva

Krawczyk

Bartkowiak

et al. 2009

The Journal of Chemical Physics

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Following the excited state relaxation dynamics of indole and 5-hydroxyindole using time-resolved photoelectron spectroscopy J. Chem. Phys. 135, 194307 (2011) Population inversion of molecular nitrogen in an Ar: N2 mixture by selective resonance-enhanced multiphoton ionization J. Appl. Phys. 110, 083112 (2011) Control of vibronic excitation using quantum-correlated photons J. Chem. Phys. 135, 164304 (2011) Resonant two-photon ionization spectroscopy of jet-cooled PdSi J. Chem. Phys. 135, 134308 (2011) Optical purification of a mixture of chiral forms by dimer formation J. Chem. Phys. 135, 124304 (2011) Additional information on J. Chem. Phys. In this study, the one-and two-photon absorption spectra of seven azoaromatic compounds ͑five pseudostilbenes-type and two aminoazobenzenes͒ were theoretically investigated using the density functional theory combined with the response functions formalism. The equilibrium molecular structure of each compound was obtained at three different levels of theory: Hartree-Fock, density functional theory ͑DFT͒, and Møller-Plesset 2. The effect of solvent on the equilibrium structure and the electronic transitions of the compounds were investigated using the polarizable continuum model. For the one-photon absorption, the allowed → ‫ء‬ transition energy showed to be dependent on the molecular structures and the effect of solvent, while the n → ‫ء‬ and → ‫ء‬ ͑n͒ transition energies exhibited only a slight dependence. An inversion between the bands corresponding to the → ‫ء‬ and n → ‫ء‬ states due to the effect of solvent was observed for the pseudostilbene-type compounds. To characterize the allowed two-photon absorption transitions for azoaromatic compounds, the response functions formalism combined with DFT using the hybrid B3LYP and PBE0 functionals and the long-range corrected CAM-B3LYP functional was employed. The theoretical results support the previous findings based on the three-state model. The model takes into account the ground and two electronic excited states and has already been used to describe and interpret the two-photon absorption spectrum of azoaromatic compounds. The highest energy two-photon allowed transition for the pseudostilbene-type compounds shows to be more effectively affected ͑ϳ20%͒ by the torsion of the molecular structure than the lowest allowed transition ͑ϳ10%͒. In order to elucidate the effect of the solvent on the two-photon absorption spectra, the lowest allowed two-photon transition ͑dipolar transition͒ for each compound was analyzed using a two-state approximation and the polarizable continuum model. The results obtained reveal that the effect of solvent increases drastically the two-photon cross-section of the dipolar transition of the pseudostilbene-type compounds. In general, the features of both one-and two-photon absorption spectra of the azoaromatic compounds are well reproduced by the theoretical calculations.

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Section: -7supporting

confidence: 85%

“…The calculated oscillator strength is related to the experimental integrated intensity by the relation 11 f gf = 4.32 ϫ 10 −9…”

Section: B 1pamentioning

confidence: 99%

Section: ͑2͒mentioning

confidence: 99%

Section: -7mentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Theoretical study of one- and two-photon absorption spectra of azoaromatic compounds

Silva

Krawczyk

Bartkowiak

et al. 2009

The Journal of Chemical Physics

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Excited States from Time‐Dependent Density Functional Theory

Elliott¹,

Furche²,

Burke³

2008

Reviews in Computational Chemistry

219

195

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Time-dependent density functional theory (TDDFT) is presently enjoying enormous popularity in quantum chemistry, as a useful tool for extracting electronic excited state energies. This article explains what TDDFT is, and how it differs from ground-state DFT. We show the basic formalism, and illustrate with simple examples. We discuss its implementation and possible sources of error. We discuss many of the major successes and challenges of the theory, including weak fields, strong fields, continuum states, double excitations, charge transfer, high harmonic generation, multiphoton ionization, electronic quantum control, van der Waals interactions, transport through single molecules, currents, quantum defects, and, elastic electron-atom scattering. ContentsVII. Beyond standard functionals 22 A. Double excitations 22 B. Polymers 23 C. Solids 23 D. Charge transfer 23 VIII. Other topics 23 A. Ground-state XC energy 23 B. Strong fields 24 C. Transport 25

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The index of microcirculatory resistance (IMR) in takotsubo cardiomyopathy

Daniels¹,

Fearon²

2010

Cathet Cardio Intervent

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We report a patient who presents with acute chest pain and positive cardiac enzymes clinically consistent with an acute coronary syndrome (ACS). Coronary angiography revealed normal epicardial arteries and the left ventriculogram was notable for apical ballooning. This was strongly suggestive of takotsubo cardiomyopathy. Pressure wire measurements of Fractional flow reserve (FFR) and IMR demonstrated a normal FFR, but significant microcirculatory dysfunction. This is the first such case that documents this abnormality invasively using the IMR, which unlike CFR is specific for the microcirculation and reproducible through a range of hemodynamic states.

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TDDFT Study of One- and Two-Photon Absorption Properties: Donor−π−Acceptor Chromophores

Cited by 101 publications

References 95 publications

Theoretical study of one- and two-photon absorption spectra of azoaromatic compounds

Theoretical study of one- and two-photon absorption spectra of azoaromatic compounds

Excited States from Time‐Dependent Density Functional Theory

The index of microcirculatory resistance (IMR) in takotsubo cardiomyopathy

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