Nonlocal Electron-Phonon Coupling in Prototypical Molecular Semiconductors from First Principles

A substantial amount of evidence indicates a relevant role played by the nonlocal electron–phonon couplings in the mechanism of charge transport in organic semiconductors. In this work, we compute the nonlocal electron–phonon coupling for the prototypical molecular semiconductors rubrene and tetracene using the phonon modes obtained from <i>ab initio</i> methods. We do not make the rigid molecular approximation allowing a mixing of intra- and intermolecular modes, and we use a supercell approach to sample the momentum space. Indeed, we find that some low-frequency intramolecular modes are mixed with the rigid-molecule translations and rotations in the modes with the strongest electron–phonon coupling. To rationalize the results we propose a convenient decomposition of the delocalized lattice modes into molecular-based modes

Exciton-Phonon Interaction Model for Singlet Fission in Prototypical Molecular Crystals

In singlet fission (SF), a spin-conserving splitting of one singlet exciton into two triplet excitation states, the transition between localized electronic states can be controlled and modulated by delocalized lattice phonons. In this work, we built an exciton–phonon (ex–ph) interaction model accounting local electronic states coupled with both local molecular vibrations and low frequency intermolecular phonon modes for SF in crystalline tetracene and rubrene. On the basis of the calculated electronic couplings at the equilibrium structure of the molecular dimer, a superexchange path for SF was found for tetracene while couplings between the triplet pair (TT) state and other diabatic states are zero for rubrene due to the high symmetry. Our further ex–ph spectral density analysis and quantum dynamics simulation based on our ex–ph interaction model suggested a thermal-activated mechanism for SF in rubrene crystal via symmetry breaking by nuclear vibration, which is in agreement with recent experiments. It is also shown that thermal fluctuations of electronic couplings in both tetracene and rubrene are mostly in the same order of magnitude at room temperature, and this could be one of the reasons for both tetracene and rubrene to exhibit SF time scales within a close range (hundreds to thousands of femtoseconds) in experiments

Guanosine-based hydrogen-bonded 2D scaffolds: Metal-free formation of G-quartet and G-ribbon architectures at the solid/liquid interface

We report on the synthesis and self-assembly of three novel lipophilic guanosine derivatives exposing a ferrocene moiety in the C(50) position of the sugar unit. Their self-association in solution, and at the solid/ liquid interface, can be tuned by varying the size and nature of the C(8)-substituent, leading to the generation of either G-ribbons, lamellar G-dimer based arrays or the G4 cation-free architecture

Congreso Internacional de Responsabilidad Social Apuestas para el desarrollo regional.

Congreso Internacional de Responsabilidad Social: apuestas para el desarrollo regional [Edición 1 / Nov. 6 - 7: 2019 Bogotá D.C.]El Congreso Internacional de Responsabilidad Social “Apuestas para el Desarrollo Regional”, se llevó a cabo los días 6 y 7 de noviembre de 2019 en la ciudad de Bogotá D.C. como un evento académico e investigativo liderado por la Corporación Universitaria Minuto de Dios -UNIMINUTO – Rectoría Cundinamarca cuya pretensión fue el fomento de nuevos paradigmas, la divulgación de conocimiento renovado en torno a la Responsabilidad Social; finalidad adoptada institucionalmente como postura ética y política que impacta la docencia, la investigación y la proyección social, y cuyo propósito central es la promoción de una “sensibilización consciente y crítica ante las situaciones problemáticas, tanto de las comunidades como del país, al igual que la adquisición de unas competencias orientadas a la promoción y al compromiso con el desarrollo humano y social integral”. (UNIMINUTO, 2014). Dicha postura, de conciencia crítica y sensibilización social, sumada a la experiencia adquirida mediante el trabajo articulado con otras instituciones de índole académico y de forma directa con las comunidades, permitió establecer como objetivo central del evento la reflexión de los diferentes grupos de interés, la gestión de sus impactos como elementos puntuales que contribuyeron en la audiencia a la toma de conciencia frente al papel que se debe asumir a favor de la responsabilidad social como aporte seguro al desarrollo regional y a su vez al fortalecimiento de los Objetivos de Desarrollo Sostenible

Congreso Internacional de Responsabilidad Social Apuestas para el desarrollo regional.

Congreso Internacional de Responsabilidad Social: apuestas para el desarrollo regional [Edición 1 / Nov. 6 - 7: 2019 Bogotá D.C.]El Congreso Internacional de Responsabilidad Social “Apuestas para el Desarrollo Regional”, se llevó a cabo los días 6 y 7 de noviembre de 2019 en la ciudad de Bogotá D.C. como un evento académico e investigativo liderado por la Corporación Universitaria Minuto de Dios -UNIMINUTO – Rectoría Cundinamarca cuya pretensión fue el fomento de nuevos paradigmas, la divulgación de conocimiento renovado en torno a la Responsabilidad Social; finalidad adoptada institucionalmente como postura ética y política que impacta la docencia, la investigación y la proyección social, y cuyo propósito central es la promoción de una “sensibilización consciente y crítica ante las situaciones problemáticas, tanto de las comunidades como del país, al igual que la adquisición de unas competencias orientadas a la promoción y al compromiso con el desarrollo humano y social integral”. (UNIMINUTO, 2014). Dicha postura, de conciencia crítica y sensibilización social, sumada a la experiencia adquirida mediante el trabajo articulado con otras instituciones de índole académico y de forma directa con las comunidades, permitió establecer como objetivo central del evento la reflexión de los diferentes grupos de interés, la gestión de sus impactos como elementos puntuales que contribuyeron en la audiencia a la toma de conciencia frente al papel que se debe asumir a favor de la responsabilidad social como aporte seguro al desarrollo regional y a su vez al fortalecimiento de los Objetivos de Desarrollo Sostenible

Density functional theory and model-based studies of charge transfer and molecular self-organization on surfaces:: implications for molecular-based Quantum Cellular Automata

Molecular-based quantum cellular automata (m-QCA), as an extension of quantum-dot QCAs, offer a novel alternative in which binary information can be encoded in the molecular charge configuration of a cell and propagated via nearest-neighbor Coulombic cell-cell interactions. Appropriate functionality of m-QCAs involves a complex relationship between quantum mechanical effects, such as electron transfer processes within the molecular building blocks, and electrostatic interactions between cells. In the first part of this document, the influence of structural distortions in single m-QCA is addressed within a minimal model using an diabatic-to-adiabatic transformation. Thus, it is shown that even small changes of the classical square geometry between driver and target cells, such as those induced by distance variations or shape distortions, can make cells respond to interactions in a far less symmetric fashion, modifying and potentially impairing the expected computational behavior of the m-QCA. The model has been further extended to consider time-dependent external electric fields in which a special emphasis is given to the profiles in which this external parameter can interact with the associated molecular complex. The results of the model have been validated by a direct comparison with first-principle calculations allowing to conclude the plausibility to induce the intra-molecular charge transfer process in a controllable manner via the interaction with the external electric field. The influence played by the electric field profile in the response of the molecular complex is also investigated. The results suggests a major role played by this variable in terms of the time length in which the intra-molecular charge transfer can be observed. In the second part, first-principle theoretical calculations of the self-assembly properties and electronic structure of Ferrocene-functionalized complexes have been carried out. Hence, five different molecular complexes which offer a potential playground to realistic implement the m-QCA paradigm have been investigated. The main emphasis is given to study the interaction between localized charge-carrier molecular states and the delocalized surface states. The results of these calculations demonstrate the possibility to obtain real systems in which intra-molecular charge localization can be combined with self-assembly scaffolding and absorbed on either Highly oriented pyrolytic graphite (HOPG) or metallic-surfaces. Finally, the validation of these findings is carried out via comparison with accesible experimental results and opening the gate to plausible strategies where the paradigm can be implemented

Density functional theory and model-based studies of charge transfer and molecular self-organization on surfaces:: implications for molecular-based Quantum Cellular Automata

Molecular-based quantum cellular automata (m-QCA), as an extension of quantum-dot QCAs, offer a novel alternative in which binary information can be encoded in the molecular charge configuration of a cell and propagated via nearest-neighbor Coulombic cell-cell interactions. Appropriate functionality of m-QCAs involves a complex relationship between quantum mechanical effects, such as electron transfer processes within the molecular building blocks, and electrostatic interactions between cells. In the first part of this document, the influence of structural distortions in single m-QCA is addressed within a minimal model using an diabatic-to-adiabatic transformation. Thus, it is shown that even small changes of the classical square geometry between driver and target cells, such as those induced by distance variations or shape distortions, can make cells respond to interactions in a far less symmetric fashion, modifying and potentially impairing the expected computational behavior of the m-QCA. The model has been further extended to consider time-dependent external electric fields in which a special emphasis is given to the profiles in which this external parameter can interact with the associated molecular complex. The results of the model have been validated by a direct comparison with first-principle calculations allowing to conclude the plausibility to induce the intra-molecular charge transfer process in a controllable manner via the interaction with the external electric field. The influence played by the electric field profile in the response of the molecular complex is also investigated. The results suggests a major role played by this variable in terms of the time length in which the intra-molecular charge transfer can be observed. In the second part, first-principle theoretical calculations of the self-assembly properties and electronic structure of Ferrocene-functionalized complexes have been carried out. Hence, five different molecular complexes which offer a potential playground to realistic implement the m-QCA paradigm have been investigated. The main emphasis is given to study the interaction between localized charge-carrier molecular states and the delocalized surface states. The results of these calculations demonstrate the possibility to obtain real systems in which intra-molecular charge localization can be combined with self-assembly scaffolding and absorbed on either Highly oriented pyrolytic graphite (HOPG) or metallic-surfaces. Finally, the validation of these findings is carried out via comparison with accesible experimental results and opening the gate to plausible strategies where the paradigm can be implemented

Efecto del suero autólogo en la reparación de la superficie ocular asociada a ojo seco

The ocular surface damage associated with the alteration of the tear film causes multiple symptoms, and autologous serum is used as treatment. Objectives: To compare the effect of autologous serum on the ocular surface repair, prepared with two different concentrations (80 y 20 %). Materials and methods: A quasi-experimental prospective study was carried out in 25 patients diagnosed with dry eye through the Schirmer test, tbut and Rose Bengal staining. Autologous serum eye drops wereadministered to 80% in the right eye and 20% in the left eye, and after 30 days of application, tests were once again performed. For the preparation of autologous serum, ethical procedures were performed and the standardized protocol at the University of Lübeck, Germany, was followed according to the Bundesärztekammer guide and the Paul Ehrlich Institute. Results: The application of autologous serum to 80% and 20% showed a significant increase in both tear volume (Schirmer)and tear stability and quality (tbut) and, additionally, ocular surface repair is achieved. No significant differences were found with the two concentrations but with higher concentrations a greater effect on production and time of rupture of the tear film is achieved (p<0.080). Conclusions: The administration of autologous serum as a treatment for dry eye presents repair on the ocular surface in both concentrations of 80% and 20%.El daño de la superficie ocular asociado a la alteración de la película lagrimal causa múltiples síntomas y como tratamiento se usa el suero autólogo. Objetivos: comparar el efecto del suero autólogo sobre la reparación de la superficie ocular, preparado con dos concentraciones diferentes (80 y 20 %). Materiales y métodos: se realizó un estudio prospectivo cuasiexperimental en 25 pacientes diagnosticados con ojo seco, mediante el test de Schirmer, tbut y tinción con rosa de Bengala. Se administró colirio de suero autólogo al 80 % en el ojo derecho y al 20 % en el ojo izquierdo, y después de 30 días de utilización se realizaron nuevamente los tests. Para la preparación del suero autólogo se realizaron los procedimientos éticos y se siguió con el protocolo estandarizado de la Universidad de Lübeck, Alemania, de acuerdo con la guía Bundesärztekammer y del Instituto Paul Ehrlich. Resultados: la aplicación de suero autólogo al 80 % y al 20 % presenta un aumento significativo tanto en el volumen lagrimal (Schirmer) como en la estabilidad y calidad lagrimal (tbut) y se logra, además, reparación sobre la superficie ocular. No se encontraron diferencias significativas con las dos concentraciones, pero con mayores concentraciones se logra un mayor efecto sobre la producción y tiempo de ruptura de la película lagrimal (p<0,080). Conclusiones: la administración de suero autólogo como tratamiento para el ojo seco presenta reparación sobre la superficie ocular en concentraciones tanto del 20 % como del 80 %