Photoluminescence spectra of oligo-paraphenyllenevinylenes: a joint theoretical and experimental characterization

Cornil, Jérôme; Beljonne, David; Heller, Christian; Campbell, I. H.; Laurich, B.; Smith, D. L.; Bradley, Donal D. C.; Müllen, Kläus; Brédas, Jean‐Luc

doi:10.1016/s0009-2614(97)00986-x

Cited by 158 publications

(146 citation statements)

References 28 publications

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“…Experimental linear absorption spectrum has well-pronounced vibronic progression that is not accounted for in the present calculations but may be computed using optimal ground and excited-state geometries and a set of normal modes. 62,63 In contrast, distinct peaks in TPA spectra usually reflect involvement of different excited states. 61 Experimental and calculated cross section magnitudes at the absolute maxima of TPA spectra are summarized in Table 5, and plotted in Figure 4.…”

Section: Resultsmentioning

confidence: 99%

Prediction of Two-Photon Absorption Properties for Organic Chromophores Using Time-Dependent Density-Functional Theory

2003

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In this benchmark study, time-dependent density-functional theory (TDDFT) is applied to calculate one-and two-photon absorption spectra (related to linear and third-order optical responses, respectively) in a series of large donor-acceptor substituted conjugated molecules. Calculated excitation energies corresponding to oneand two-photon-absorption maxima are found to be in excellent agreement with experiment. The evaluated two-photon-absorption cross sections agree with experimental data as well. We conclude that the TDDFT approach is a numerically efficient method for quantitative calculations of resonant nonlinear polarizabilities in large organic chromophores.

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Section: Resultsmentioning

confidence: 99%

Prediction of Two-Photon Absorption Properties for Organic Chromophores Using Time-Dependent Density-Functional Theory

2003

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“…In MOPV4, 2 is approximately unity, a value which, in conjunction with the cubic frequency dependence in the emission rate yields roughly equal single molecule 0-0 and 0-1 emission peak intensities, as is found for OPV4 molecules in solution. 36 The aggregate Hamiltonian including all of the aforementioned contributions written in the subspace in which one chromophore is excited ͑one-exciton͒ is…”

Section: Model Aggregates Hamiltonian and Observablesmentioning

confidence: 99%

Using circularly polarized luminescence to probe exciton coherence in disordered helical aggregates

Spano

Meskers

Hennebicq

et al. 2008

The Journal of Chemical Physics

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Circularly polarized emission from helical MOPV4 aggregates is studied theoretically based on a Hamiltonian including excitonic coupling, exciton phonon coupling, and site disorder. The latter is modeled via a Gaussian distribution of site energies. The frequency dependence of the circularly polarized luminescence dissymmetry g lum ͑͒ contains structural information about the low-energy-neutral ͑excitonic͒ polaron from which emission originates. Near the 0-0 emission frequency, g lum ͑͒ provides a measure of the exciton coherence length, while at lower energies, in the vicinity of the sideband frequencies, g lum ͑͒ probes the polaron radius. The present work focuses on how the 0-0 dissymmetry, g lum 0-0 , relates to the emitting exciton's coherence function, from which the coherence length is deduced. In the strong disorder limit where the exciton is localized on a single chromophore, g lum 0-0 is zero. As disorder is reduced and the coherence function expands, ͉g lum 0-0 ͉ increases more rapidly than the sideband dissymmetries, resulting in a pronounced surge in g lum ͑͒ near the 0-0 transition frequency. The resulting spectral shape of g lum ͑͒ is in excellent agreement with recent experiments on MOPV4 aggregates. In the limit of very weak disorder, corresponding to the motional narrowing regime, the coherence function extends over the entire helix. In this region, g lum 0-0 undergoes a surprising sign reversal but only for helices which are between n + 1 2 and n + 1 complete turns ͑n =0,1, ...͒. This unusual sign change is due to the dependence of the rotational line strength on long-range exciton coherences which are also responsible for a heightened sensitivity of g lum ͑͒ to long-range excitonic coupling.

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“…for PA [27], PTA, [28] PPV [29], PTh [30,31], PPy [32±35], and PAn [36]. Each panel represents the oligomer shown in the inset, whereas groups of points correspond to the oligomers of dierent sizes.…”

Section: Conjugated Oligomersmentioning

confidence: 99%

CEO/semiempirical calculations of UV–visible spectra in conjugated molecules

Tretiak

Saxena

Martin

et al. 2000

Chemical Physics Letters

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The collective electronic oscillators (CEO) approach based on the TDHF approximation is combined with INDO/S, MNDO, AM1, and PM3 semiempirical Hamiltonians. This technique is applied to compute and analyze the electronic structure of acceptor-substituted oligomers and conjugated polymers. Calculated excited-state energies and oscillator strengths agree well with the experimental data and with each other. In particular, the results using the Hamiltonians parameterized for ground-state calculations such as AM1 and PM3 agree well with the INDO/S results. In addition, a two-dimensional analysis of the corresponding transition density matrices provides an ecient way for tracing the origin of various optical transitions by identifying the underlying changes in charge densities and bond-orders. Ó

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Photoluminescence spectra of oligo-paraphenyllenevinylenes: a joint theoretical and experimental characterization

Cited by 158 publications

References 28 publications

Prediction of Two-Photon Absorption Properties for Organic Chromophores Using Time-Dependent Density-Functional Theory

Prediction of Two-Photon Absorption Properties for Organic Chromophores Using Time-Dependent Density-Functional Theory

Using circularly polarized luminescence to probe exciton coherence in disordered helical aggregates

CEO/semiempirical calculations of UV–visible spectra in conjugated molecules

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