Two-photon absorption and optical-limiting properties of novel organic compounds: erratum

He, Guang S.; Reinhardt, Bruce A.; Bhatt, J.; Dillard, Ann G.; McKellar, Robert; Xu, Chunxiang; Prasad, Paras N.

doi:10.1364/ol.20.001930

Cited by 29 publications

(31 citation statements)

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“…In the quest of improving NLO properties, attention has been essentially focused on dipolar molecules for several decades. [1][2][3] More recently, quadrupolar systems have been designed and investigated [4][5][6][7][8][9][10][11][12][13][14][15][16][17][18][19][20][21] and have shown improved properties, in particular with respect to the trade-off between optical transparency and NLO performance. Lately, attention has turned toward multipolar [22][23][24][25][26][27][28][29][30][31][32][33] and branched structures including dendrimers.…”

Section: Introductionmentioning

confidence: 99%

“…Depending on the nature of this coupling, the ground state or the excited state may be either localized or delocalized, and specific optical properties may be either enhanced or suppressed. 44 Among the many NLO effects, two-photon absorption (TPA) has become very popular during the past decade owing to its wide-ranging applications such as two-photon laser scanning microscopy, [45][46][47] photodynamic therapy, 48 optical power limitation, 4,5 microfabrication, [49][50][51][52] or 3D optical data storage. [53][54][55][56] Depending on the applications, two-photon chromophores have to satisfy different kinds of requirements.…”

Section: Introductionmentioning

confidence: 99%

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Effects of (Multi)branching of Dipolar Chromophores on Photophysical Properties and Two-Photon Absorption

et al. 2005

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To investigate the effect of branching on linear and nonlinear optical properties, a specific series of chromophores, epitome of (multi)branched dipoles, has been thoroughly explored by a combined theoretical and experimental approach. Excited-state structure calculations based on quantum-chemical techniques (timedependent density functional theory) as well as a Frenkel exciton model nicely complement experimental photoluminescence and one-and two-photon absorption findings and contribute to their interpretation. This allowed us to get a deep insight into the nature of fundamental excited-state dynamics and the nonlinear optical (NLO) response involved. Both experiment and theory reveal that a multidimensional intramolecular charge transfer takes place from the donating moiety to the periphery of the branched molecules upon excitation, while fluorescence stems from an excited state localized on one of the dipolar branches. Branching is also observed to lead to cooperative enhancement of two-photon absorption (TPA) while maintaining high fluorescence quantum yield, thanks to localization of the emitting state. The comparison between results obtained in the Frenkel exciton scheme and ab initio results suggests the coherent coupling between branches as one of the possible mechanisms for the observed enhancement. New strategies for the rational design of NLO molecular assemblies are thus inferred on the basis of the acquired insights.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Effects of (Multi)branching of Dipolar Chromophores on Photophysical Properties and Two-Photon Absorption

et al. 2005

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“…Multiphoton absorption has also attracted considerable attention for optical limiting [27][28][29][30][31][32][33][34][35][36][37][38][39] mainly focusing on optical limiting in the visible region aiming at eye-protection. [37][38][39] Whereas a number of multiphoton chromophores have been designed and studied in that context, only scarce effort has been dedicated to the protection of NIR detectors typically working in the 700-900 nm region.…”

Section: Introductionmentioning

confidence: 99%

“…[40,[43][44][45] Indeed quadrupolar systems [27,30,35, have been found to be more efficient than push-pull systems [13,28,46,47,56,64,68,[80][81][82][83][84][85][86][87][88] in terms of TPA in particular for multiphoton-based optical limiting applications. [27,30,39] Such derivatives can display very high TPA cross sections in connection with a quadrupolar intramolecular charge transfer taking place between the ends and the center of the molecules. [42] Very large σ 2 values have been obtained with DAAD, ADDA, DADAD, DDADD… systems having strong D and A moieties but often at the cost of reduced fluorescence quantum yield and/or pronounced red-shift of the one-photon absorption band.…”

Section: Introductionmentioning

confidence: 99%

Synthesis, Fluorescence, and Two‐Photon Absorption of a Series of Elongated Rodlike and Banana‐Shaped Quadrupolar Fluorophores: A Comprehensive Study of Structure–Property Relationships

Mongin

Porrès

Charlot

et al. 2007

Chemistry A European J

240

204

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An extensive series of push-push and pull-pull derivatives was prepared from the symmetrical functionalization of an ambivalent core with conjugated rods made from arylenevinylene or arylene-ethynylene building blocks, bearing different acceptor or donor endgroups. Their absorption and photoluminescence as well as their two-photon absorption (TPA) properties in the near infrared (NIR) region have been systematically investigated in order to derive structure-property relationships and lay the guidelines for both spectral tuning and amplification of molecular TPA in the target region. Whatever the nature of the core or of the connectors, push-push systems were found to be more efficient than pull-pull systems and planarization of the core (fluorene vs biphenyl) always leads to an increase of the TPA crosssections. At contrary, increasing the conjugation length as well as replacement of a phenylene moiety by a thienylene moiety in the conjugated rods did not necessarily lead to increased TPA responses. The present study also demonstrated that the topology of the conjugated rods can dramatically influence the TPA properties. This is of particular interest in terms of molecular engineering for specific applications since both TPA properties and photoluminescence characteristics can be considerably affected. It thus becomes possible to optimize the transparency/TPA and fluorescence/TPA efficiency trade-offs, for optical limiting in the red-NIR region (700-900 nm) and TPEF microscopy applications, respectively.

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“…[6][7][8] In the search for adequate materials for the various applications, organic molecular systems are of particularly interest due to their inherent modularity and the potentially high TPA response of conjugated systems. Indeed, over the past decade, an increasing effort has been devoted to the design of chromophores with enhanced TPA responses progressively moving from monomeric chromophores such as dipoles [9][10][11][12][13][14][15] and quadrupoles 4,5,11, toward multimeric complex molecular architectures. Given the effort required to synthesize such compounds, thorough understanding of the various factors influencing the TPA response is highly desirable for the achievement of optimized TPA figures of merit.…”

Section: Introductionmentioning

confidence: 99%

Two-Photon Transitions in Quadrupolar and Branched Chromophores: Experiment and Theory

et al. 2007

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A combined experimental and theoretical study is conducted on a series of model compounds in order to assess the combined role of branching and charge symmetry on absorption, photoluminescence, and twophoton absorption (TPA) properties. The main issue of this study is to examine how branching of quadrupolar chomophores can lead to different consequences as compared to branching of dipolar chromophores. Hence, three structurally related π-conjugated quadrupolar chromophores symmetrically substituted with donor end groups and one branched structure built from the assembly of three quadrupolar branches via a common donor moiety are used as model compounds. Their photophysical properties are studied using UV-vis spectroscopy, and the TPA spectra are determined through two-photon excited fluorescence experiments using femtosecond pulses in the 500-1000 nm range. Experimental studies are complemented by theoretical calculations. The applied theoretical methodology is based on time-dependent density functional theory, the Frenkel exciton model, and analysis in terms of the natural transition orbitals of relevant electronic states. Theory reveals that a symmetrical intramolecular charge transfer from the terminal donating groups to the middle of the molecule takes place in all quadrupolar chromophores upon photoexcitation. In contrast, branching via a central electron-donating triphenylamine moiety breaks the quadrupolar symmetry of the branches. Consequently, all Frank-Condon excited states have significant asymmetric multidimensional charge-transfer character upon excitation. Subsequent vibrational relaxation of the branched chromophore in the excited state leads to a localization of the excitation and fluorescence stemming from a single branch. As opposed to what was earlier observed when dipolar chromophores are branched via the same common electron-donating moiety, we find only a slight enhancement of the maximum TPA response of the branched compound with respect to an additive contribution of its quadrupolar branches. In contrast, substantial modifications of the spectral shape are observed. This is attributed to the subtle interplay of interbranch electronic coupling and asymmetry caused by branching.

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Two-photon absorption and optical-limiting properties of novel organic compounds: erratum

Cited by 29 publications

References 1 publication

Effects of (Multi)branching of Dipolar Chromophores on Photophysical Properties and Two-Photon Absorption

Effects of (Multi)branching of Dipolar Chromophores on Photophysical Properties and Two-Photon Absorption

Synthesis, Fluorescence, and Two‐Photon Absorption of a Series of Elongated Rodlike and Banana‐Shaped Quadrupolar Fluorophores: A Comprehensive Study of Structure–Property Relationships

Two-Photon Transitions in Quadrupolar and Branched Chromophores: Experiment and Theory

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