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Dive into the research topics where Rodrigo Q. Albuquerque is active.

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Featured researches published by Rodrigo Q. Albuquerque.


Inorganic Chemistry | 2008

Essential role of the ancillary ligand in the color tuning of iridium tetrazolate complexes.

Stefano Stagni; Silvia Colella; Antonio Palazzi; Giovanni Valenti; Stefano Zacchini; Francesco Paolucci; Massimo Marcaccio; Rodrigo Q. Albuquerque; Luisa De Cola

We report on the synthesis and physical chemical characterization of a class of heteroleptic mononuclear cyclometalated bis(phenylpyridine)iridium(III) complexes with tetrazolate chelate ligands, such as the deprotonated form of 2-(1 H-tetrazol-5-yl)pyridine ( PyTzH), 2-(1 H-tetrazol-5-yl)pyrazine ( PzTzH), and 5-bromo-2-(1 H-tetrazol-5-yl)pyridine ( BrPyTzH). The electrochemical and photophysical investigations of the resulting iridium(III) complexes revealed a rather wide span of redox and emission properties as a consequence of the nature of the ancillary tetrazolate ligand. In particular, within a series of the three neutral species, the emission observed changes from the blue-green of the pyridyltetrazolate complex to the red of that containing the pyrazinyltetrazolate ligand. The bromo-containing species, despite it displaying poor photophysical performances, is a synthetically attractive building block for the construction of polymetallic architectures. Moreover, the investigation of the reactivity toward electrophiles of one of the neutral mononuclear complexes, by methylation of the coordinated tetrazolate ligand, has also allowed further tuning of the electronic properties. In the latter case, the emission color tuning is also associated with a simple method for the conversion of a neutral species, a potentially triplet emitter for organic light-emitting devices, into the corresponding methylated cation, which might be used as a dopant for light-emitting electrochemical cell type devices or as a marker for biological labeling.


Journal of the American Chemical Society | 2013

Cooperative supramolecular polymerization driven by metallophilic Pd···Pd interactions.

María Mayoral; Christina Rest; Vladimir Stepanenko; Jennifer Schellheimer; Rodrigo Q. Albuquerque; Gustavo Fernández

A new oligophenyleneethynylene (OPE)-based Pd(II) pyridyl complex has been synthesized, and its self-assembly has been investigated in solution, in the bulk state, and on surfaces. Detailed analysis of concentration- and temperature-dependent UV-vis studies in methylcyclohexane supported by DFT calculations demonstrate for the first time that cooperative supramolecular polymerization processes can be driven by metallophilic interactions.


Journal of Materials Chemistry | 2008

1,2,3-Triazolyl-pyridine derivatives as chelating ligands for blue iridium(III) complexes. Photophysics and electroluminescent devices

Enrico Orselli; Rodrigo Q. Albuquerque; P. Michel Fransen; Roland Fröhlich; Henk M. Janssen; Luisa De Cola

We report on the study of a new family of neutral heteroleptic Ir(F2ppy)2L (F2ppy = 2-(2,4-difluorophenyl)pyridine) complexes bearing different triazole derivatives (L = 2-(1,2,3-triazol-5-yl)pyridine) as the third ligand. Two of these ligands were used for the first time as ancillary ligands in iridium(III) complexes. A full photophysical and electrochemical study of these complexes is reported here, together with theoretical investigations at the density functional theory (DFT) level. The complexes were also obtained as single crystals and their structures were determined by X-ray crystallography. The newly reported complexes exhibit blue emission with high quantum yields in solution. Photophysical results are also compared to those reported for their 1,2,4-triazole isomer analogues. The emitting state is a mixture between the triplet metal-to-ligand charge transfer (3MLCT) and triplet inter-ligand charge transfer (3ILCT) states, and it is more localized on the F2ppy ligand as supported by DFT calculations. In addition, this paper reports some preliminary tests of polymer light-emitting diodes (PLEDs) doped with these iridium complexes. The results indicate that such molecules are good candidates as blue- and green-emitting dopants in LED devices.


Molecular Physics | 2003

Highly luminescent europium(III) complexes with naphtoiltrifluoroacetone and dimethyl sulphoxide

Luís D. Carlos; C. De Mello Donegá; Rodrigo Q. Albuquerque; Severino Alves; J. F. S. Menezes; Oscar L. Malta

The synthesis, luminescence properties, experimental determination and theoretical calculation of the emission quantum yield of Eu(NTA)3.2L complexes, where NTA is naphtoiltri-fluroacetone and L denotes H2O or DMSO (dimethyl sulphoxide), were reported. The compounds were characterized by elemental analysis (carbon, hydrogen and europium), thermal analysis, UV-visible absorption and photoluminescence spectroscopies. The experimental quantum yields were determined based on a method previously proposed by Bril and collaborators. The Eu(NTA)3.2DMSO compound shows a high value for the Ω2 intensity parameter (35.8 × 10−20 cm2), reflecting the hypersensitive nature of the 5D0 → 7F2 transition and indicating that the lanthanide ion is in a highly polarizable chemical environment. The experimental quantum yield measured for that compound, 0.75, is one of the highest so far reported for solid-state europium complexes. The theoretical calculations of the quantum yield were carried out by solving an appropriate set of rate equations and by using empirical spectroscopic parameters and energy transfer rates. The theoretical results agree well with the experimental data for both complexes. The photostability of Eu(NTA)3.2DMSO at 358K was evaluated in order to verify whether this complex can be applied as a phosphor for blue light emitting devices.


Inorganic Chemistry | 2008

Tuning emission properties of iridium and ruthenium metallosurfactants in micellar systems.

Andrés Guerrero-Martínez; Yolanda Vida; David Domínguez-Gutiérrez; Rodrigo Q. Albuquerque; Luisa De Cola

Ruthenium metallosurfactant forms micelles that show efficient electronic energy-transfer processes in the presence of an analogous iridium complex. Modulation of the process is achieved upon incorporation of these amphiphiles into cetyltrimethylammonium bromide micelles, allowing a tuning of the two emissions.


Soft Matter | 2012

Formation of a supramolecular chromophore : a spectroscopic and theoretical study

Andreas Bernet; Rodrigo Q. Albuquerque; Marina Behr; Sebastian T. Hoffmann; Hans-Werner Schmidt

Spectroscopic and theoretical investigations of the self-assembly of a particular 1,3,5-benzene trisamide-based low molecular weight hydrogelator are described. This trisamide is pH-sensitive, and surprisingly forms a photoluminescent supramolecular hydrogel. Controlled gel formation in combination with the luminescence properties allows studying the self-assembly process in detail. The experimental results are confirmed by Density Functional Theory (DFT) calculations, revealing that the photoluminescence originates from the formation of a supramolecular chromophore.


Chemistry: A European Journal | 2013

Theoretical Investigation of Macrodipoles in Supramolecular Columnar Stackings

Rodrigo Q. Albuquerque; Andreas Timme; Roman Kress; Jürgen Senker; Hans-Werner Schmidt

Supramolecular columnar assemblies are known to form intrinsic macrodipoles, which play an important role in intercolumnar interactions and govern the self-assembly on the mesoscale. A prominent class that provides this feature are trisamide derivatives, namely, 1,3,5-benzenetrisamides and 1,3,5-cyclohexanetrisamides. The understanding of how subtle changes in the chemical structure influence the columnar order and consequently the macrodipole formation is of fundamental interest. Here we report on the theoretical investigation of trisamide derivatives and how the formed macrodipole is related to the properties of the columnar aggregates. Calculations were carried out on a semiempirical level using the PM6 approximation, which is able to treat weak interactions like hydrogen bonding and dispersion forces with a sufficient accuracy. We have compared the influence of a benzene core with a cyclohexane core on the macrodipole formation. It was revealed that columnar aggregates based on 1,3,5-cyclohexanetrisamides have much higher dipole moments than those formed with aromatic cores. A cooperative effect was found during aggregation, as longer aggregates show stronger hydrogen bonding, thereby facilitating the addition of the next molecule. We have also investigated the influence of the amide connection on the strength of the formed macrodipole. The trends observed for the macrodipole strength correlate with the calculated heat of formation. If the amide groups are inverted, the strength of the macrodipole is reduced and the negative heat of formation is increased. HOMO-LUMO gaps were correlated with the inverse of the dipole moment per monomer unit, thus indicating that the macrodipole might act as a perturbation to the supramolecular assemblies.


Chemistry: A European Journal | 2012

Phase Behavior and Mesophase Structures of 1,3,5‐Benzene‐ and 1,3,5‐Cyclohexanetricarboxamides: Towards an Understanding of the Losing Order at the Transition into the Isotropic Phase

Andreas Timme; Roman Kress; Rodrigo Q. Albuquerque; Hans-Werner Schmidt

One of the simplest and most-versatile motifs in supramolecular chemistry is based on 1,3,5-benzenetricarboxamides. Variation of the core structure and subtle changes in the structures of the lateral substituents govern the self-assembly and determine the phase behavior. Herein, we provide a comprehensive comparison between the phase behavior and mesophase structure of a series of 1,3,5-benzene- and 1,3,5-cyclohexanetricarboxamides that contain linear and branched alkyl substituents. Depending on the substituent, different crystalline, plastic crystalline, and liquid crystalline phases were formed. The relatively rare columnar nematic (N(C)) phase was only observed in cyclohexane-based trisamides that contained linear alkyl substituents. Of fundamental interest in liquid crystalline supramolecular systems is the transition from the mesomorphic state into the isotropic state and, in particular, the question of how the order decreases. Temperature-dependent IR spectroscopy and XRD measurements revealed that columnar H-bonded aggregates were still present in the isotropic phase. At the clearing transition, mainly the lateral order was lost, whilst shorter columnar aggregates still remained. A thorough understanding of the phase behavior and the mesophase structure is relevant for selecting processing conditions that use supramolecular structures in devices or as fibrillar nanomaterials.


Chemical Physics Letters | 2000

On the charge factors of the simple overlap model for the ligand field in lanthanide coordination compounds

Rodrigo Q. Albuquerque; Gerd B. Rocha; Oscar L. Malta; Pierre Porcher

Abstract In this Letter, we propose a semi-empirical procedure through which the charge factors, appearing in the simple overlap model (SOM) for the ligand field in lanthanide compounds, can be obtained. The idea is based on the concept of bond valence and bond strength introduced by Pauling in the 1920s. The charge factors thus obtained are used in the calculation of the so-called ligand field parameters, B q k s, and, subsequently, in the prediction of the Stark levels of the 7 F J manifolds ( J =1,2,3 and 4) of the Eu 3+ ion in coordination compounds with mixed ligands. Comparison with experiment shows that the results are quite satisfactory.


ChemPhysChem | 2010

On the Reversible Photoisomerization of Spiropyran-Modified Zeolite L Single Crystals

Rodrigo Q. Albuquerque; Joël Kühni; Peter Belser; L. De Cola

Photoisomerization of spiropyrans has been the subject of many interesting studies in a wide number of fields, such as sensors for cations, sensors of pH, switchable surfaces, lasing effect, among many others. This molecule can be photoisomerized upon UV irradiation, giving rise to the zwitterionic merocyanine (MC) form, which dramatically changes its hydrophilicity and photophysical properties (see Scheme 1). Irra-

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Luisa De Cola

University of Strasbourg

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Gustavo Fernández

Complutense University of Madrid

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Gerd B. Rocha

Federal University of Paraíba

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Oscar L. Malta

Federal University of Pernambuco

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