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2. Ultrafast two-colour X-ray emission spectroscopy reveals excited state landscape in a base metal dyad

Author

Nowakowski, Michal, Huber-Gedert, Marina, Elgabarty, Hossam, Kubicki, Jacek, Kertem, Ahmet, Lindner, Natalia, Khakhulin, Dmitry, Lima, Frederico Alves, Choi, Tae-Kyu, Biednov, Mykola, Piergies, Natalia, Zalden, Peter, Kubicek, Katerina, Rodriguez-Fernandez, Angel, Salem, Mohammad Alaraby, Kühne, Thomas, Gawelda, Wojciech, and Bauer, Matthias

Subjects
Physics - Chemical Physics
Abstract

Effective photoinduced charge transfer makes molecular bimetallic assemblies attractive for applications as active light induced proton reduction systems. For a more sustainable future, development of competitive base metal dyads is mandatory. However, the electron transfer mechanisms from the photosensitizer to the proton reduction catalyst in base metal dyads remain so far unexplored. We study a Fe-Co dyad that exhibits photocatalytic H2 production activity using femtosecond X-ray emission spectroscopy, complemented by ultrafast optical spectroscopy and theoretical time-dependent DFT calculations, to understand the electronic and structural dynamics after photoexcitation and during the subsequent charge transfer process from the FeII photosensitizer to the cobaloxime catalyst. Using this novel approach, the simultaneous measurement of the transient Kalpha X-ray emission at the iron and cobalt K-edges in a two-colour experiment is enabled making it possible to correlate the excited state dynamics to the electron transfer processes. The methodology, therefore, provides a clear and direct spectroscopic evidence of the Fe->Co electron transfer responsible for the proton reduction activity.

Published
2023

3. Classical, semi-classical and quantum optical models for x-ray planar cavity with electronic resonance

Author

Huang, Xin-Chao, Li, Tian-Jun, Lima, Frederico Alves, and Zhu, Lin-Fan

Subjects
Quantum Physics
Abstract

Here two theoretical models of semi-classical matrix and quantum Green's function are developed for the system of x-ray thin-film planar cavity with inner-shell electronic resonances. The semi-classical model is based on the matrix formalism to treat each layer as the propagating matrix. The crucial idea is to expand the propagating matrix of the resonant atomic layer under ultrathin-film approximation, then derive the analytical expression of the spectral observation, i.e, the cavity reflectance. The typical cavity effects of cavity enhanced decay rate, cavity induced energy shift and the Fano interference which were observed in the recent experiments could be phenomenologically interpreted. The second quantum model employs the analytical Green's function to solve the cavity system. The system Hamiltonian and the effective energy-level are derived. The effective energy-level scheme indicates that the cavity effect acts on the regulation of the intermediated core-hole state. To test the validity of the semi-classical matrix and quantum Green's function models, the classical Parratt's formalism and the dispersion correction of the atomic refractive index are also recalled. Very good agreements in reflectivity spectra between semi-classical and quantum models with the Parratt's results are observed. The present semi-classical matrix and quantum Green's function models will be useful to predict the new phenomena and optimize the cavity structures for future experiments and promote the emerging of quantum optical effects with modern x-ray spectroscopy techniques., Comment: 16 pages, 14 figures

Published
2022

6. Investigation of the Thermal Cooling Load of a Multifamily Residential Building by Different Algorithms of Heat Transfer

Author

Silva, Wesley Cecilio, de A. Duarte, Matheus, Lima, Frederico Romagnoli Silveira, Oliveira, Raquel Diniz, Förstner, Ulrich, Series Editor, Rulkens, Wim H., Series Editor, Wang, Liangzhu Leon, editor, Ge, Hua, editor, Zhai, Zhiqiang John, editor, Qi, Dahai, editor, Ouf, Mohamed, editor, Sun, Chanjuan, editor, and Wang, Dengjia, editor

Published
2023
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7. Doming and spin cascade in Ferric Haems: Femtosecond X-ray Absorption and X-ray Emission Studies

Author

Bacellar, Camila, Kinschel, Dominik, Mancini, Giulia F., Ingle, Rebecca A., Rouxel, Jérémy, Cannelli, Oliviero, Cirelli, Claudio, Knopp, Gregor, Szlachetko, Jakub, Lima, Frederico A., Menzi, Samuel, Pamfilidis, Georgios, Kubicek, Katharina, Khakhulin, Dmitry, Gawelda, Wojciech, Rodriguez-Fernandez, Angel, Biednov, Mykola, Bressler, Christian, Arrell, Christopher A., Johnson, Philip J. M., Milne, Christopher, and Chergui, Majed

Subjects
Physics - Chemical Physics
Abstract

The structure-function relationship is at the heart of biology and major protein deformations are correlated to specific functions. In the case of heme proteins, doming is associated with the respiratory function in hemoglobin and myoglobin, while ruffling has been correlated with electron transfer processes, such as in the case of Cytochrome c (Cyt c). The latter has indeed evolved to become an important electron transfer protein in humans. In its ferrous form, it undergoes ligand release and doming upon photoexcitation, but its ferric form does not release the distal ligand, while the return to the ground state has been attributed to thermal relaxation. Here, by combining femtosecond Fe K-edge X-ray absorption near-edge structure (XANES) studies and femtosecond Fe Kalpha and Kbeta X-ray emission spectroscopy (XES), we demonstrate that the photocycle of ferric Cyt c is entirely due to a cascade among excited spin states of the Iron ion, causing the ferric heme to undergo doming, which we identify for the first time. We also argue that this pattern is common to all ferric haems, raising the question of the biological relevance of doming in such proteins.

Published
2020

8. Femtosecond X-ray emission study of the spin cross-over dynamics in haem proteins

Author

Kinschel, Dominik, Bacellar, Camila, Cannelli, Oliviero, Sorokin, Boris, Katayama, Tetsuo, Mancini, Giulia F., Rouxel, Jeremy R., Obara, Yuki, Nishitani, Junichi, Ito, Hironori, Ito, Terumasa, Kurahashi, Naoya, Higashimura, Chika, Kudo, Shotaro, Keane, Theo, Lima, Frederico A., Gawelda, Wojciech, Zalden, Peter, Schulz, Sebastian, Budarz, James, Khakhulin, Dmitry, Galler, Andreas, Bressler, Christian, Milne, Christopher J., Penfold, Thomas, Yabashi, Makina, Suzuki, Toshinori, Misawa, Kazuhiko, and Chergui, Majed

Subjects
Physics - Chemical Physics, Condensed Matter - Soft Condensed Matter, Physics - Biological Physics
Abstract

In haemoglobin (consisting of four globular myoglobin-like subunits), the change from the low-spin (LS) hexacoordinated haem to the high spin (HS) pentacoordinated domed form upon ligand detachment and the reverse process upon ligand binding, represent the transition states that ultimately drive the respiratory function. Visible-ultraviolet light has long been used to mimic the ligand release from the haem by photodissociation, while its recombination was monitored using time-resolved infrared to ultraviolet spectroscopic tools. However, these are neither element- nor spin-sensitive. Here we investigate the transition state in the case of Myoglobin-NO (MbNO) using femtosecond Fe Kalpha and Kbeta non-resonant X-ray emission spectroscopy (XES) at an X-ray free-electron laser upon photolysis of the Fe-NO bond. We find that the photoinduced change from the LS (S = 1/2) MbNO to the HS (S = 2) deoxy-myoglobin (deoxyMb) haem occurs in ca. 800 fs, and that it proceeds via an intermediate (S = 1) spin state. The XES observables also show that upon NO recombination to deoxyMb, the return to the planar MbNO ground state is an electronic relaxation from HS to LS taking place in ca. 30 ps. Thus, the entire ligand dissociation-recombination cycle in MbNO is a spin cross-over followed by a reverse spin cross-over process.

Published
2020
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11. ESTUDO COMPARATIVO DE MÉTODOS DE FIXAÇÃO DA OSTEOTOMIA DE CHEVRON NA CIRURGIA PERCUTÂNEA DO HÁLUX VALGO

Author

Xavier, Nívea Ribeiro, primary, Lara, Luiz Carlos Ribeiro, additional, Vaz, Gabriela Abrahão Rosa, additional, Lima, Frederico Pinheiro de, additional, Bordignon, Glaucia, additional, Lancia, Lara Furtado, additional, Carvalho, Matheus Maciel Dornelles de, additional, Gonçalves, Antonio Henrique Santos, additional, Silva, Matheus Frade da, additional, and Costa, Letícia Tondato da Silva, additional

Published
2024
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14. Structural Evolution of Photoexcited Methylcobalamin toward a CarH-like Metastable State: Evidence from Time-Resolved X‑ray Absorption and X‑ray Emission.

Author

Sension, Roseanne J., McClain, Taylor P., Michocki, Lindsay B., Miller, Nicholas A., Alonso-Mori, Roberto, Lima, Frederico Alves, Ardana-Lamas, Fernando, Biednov, Mykola, Chung, Taewon, Deb, Aniruddha, Jiang, Yifeng, Kaneshiro, April K., Khakhulin, Dmitry, Kubarych, Kevin J., Lamb, Ryan M., Meadows, Joseph H., Otte, Florian, Sofferman, Danielle L., Song, Sanghoon, and Uemura, Yohei

Published
2024
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15. Transient X‐Ray Absorption Near Edge Structure Spectroscopy Using Broadband Free‐Electron Laser Pulses.

Author

Juranić, Pavle, Cirelli, Claudio, Mamyrbayev, Talgat, Uemura, Yohei, Vila‐Comamala, Joan, Lima, Frederico Alves, Bacellar, Camila, Johnson, Philip J. M., Prat, Eduard, Reiche, Sven, Wach, Anna, Bykova, Iuliia, Kahraman, Abdullah, Kabanova, Victoria, Milne, Christopher, and David, Christian

Subjects
OXALATES, X-ray absorption near edge structure, ACQUISITION of data, SPECTROMETRY, BANDWIDTHS, FREE electron lasers, ABSORPTION, LASER pulses
Abstract

A new method for time‐resolved X‐ray absorption near edge structure (XANES) spectroscopy that enables faster data acquisition and requires smaller sample quantities for high‐quality data, thus allowing the analysis of more samples in a shorter time is introduced. The method uses large bandwidth free electron laser pulses to measure laser‐excited XANES spectra in transmission mode. A beam‐splitting grating configuration allows simultaneous measurements of the spectra of the incoming X‐ray Free Electron Laser (XFEL) pulses and transmission XANES, which is crucial for compensating the pulse‐dependent intensity and spectrum fluctuations due to the self‐amplified spontaneous emission operation. The implementation of this new methodology is applied on a liquid solution of ammonium iron(III) oxalate jet and is compared to previous results, showing great improvements in the speed of acquisition and spectral resolution, and the ability to measure a large 2‐D spectral‐time map quickly. [ABSTRACT FROM AUTHOR]

Published
2024
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18. Nonadiabatic Charge Transfer within Photoexcited Nickel Porphyrins

Author

Naumova, Maria A., primary, Paveliuc, Gheorghe, additional, Biednov, Mykola, additional, Kubicek, Katharina, additional, Kalinko, Aleksandr, additional, Meng, Jie, additional, Liang, Mingli, additional, Rahaman, Ahibur, additional, Abdellah, Mohamed, additional, Checchia, Stefano, additional, Alves Lima, Frederico, additional, Zalden, Peter, additional, Gawelda, Wojciech, additional, Bressler, Christian, additional, Geng, Huifang, additional, Lin, Weihua, additional, Liu, Yan, additional, Zhao, Qian, additional, Pan, Qinying, additional, Akter, Marufa, additional, Kong, Qingyu, additional, Retegan, Marius, additional, Gosztola, David J., additional, Pápai, Mátyás, additional, Khakhulin, Dmitry, additional, Lawson Daku, Max, additional, Zheng, Kaibo, additional, and Canton, Sophie E., additional

Published
2024
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21. Spin cascade and doming in ferric hemes : Femtosecond X-ray absorption and X-ray emission studies

Author

Bacellar, Camila, Kinschel, Dominik, Mancini, Giulia F., Ingle, Rebecca A., Rouxel, Jérémy, Cannelli, Oliviero, Cirelli, Claudio, Knopp, Gregor, Szlachetko, Jakub, Lima, Frederico A., Menzi, Samuel, Pamfilidis, Georgios, Kubicek, Katharina, Khakhulin, Dmitry, Gawelda, Wojciech, Rodriguez-Fernandez, Angel, Biednov, Mykola, Bressler, Christian, Arrell, Christopher A., Johnson, Philip J. M., Milne, Christopher J., and Chergui, Majed

Published
2020

23. Nonadiabatic Charge Transfer within Photoexcited Nickel Porphyrins

Author

Naumova, Maria A., Paveliuc, Gheorghe, Biednov, Mykola, Kubicek, Katharina, Kalinko, Aleksandr, Meng, Jie, Liang, Mingli, Rahaman, Ahibur, Abdellah, Mohamed, Checchia, Stefano, Alves Lima, Frederico, Zalden, Peter, Gawelda, Wojciech, Bressler, Christian, Geng, Huifang, Lin, Weihua, Liu, Yan, Zhao, Qian, Pan, Qinying, Akter, Marufa, Kong, Qingyu, Retegan, Marius, Gosztola, David J., Pápai, Mátyás, Khakhulin, Dmitry, Lawson Daku, Max, Zheng, Kaibo, Canton, Sophie E., Naumova, Maria A., Paveliuc, Gheorghe, Biednov, Mykola, Kubicek, Katharina, Kalinko, Aleksandr, Meng, Jie, Liang, Mingli, Rahaman, Ahibur, Abdellah, Mohamed, Checchia, Stefano, Alves Lima, Frederico, Zalden, Peter, Gawelda, Wojciech, Bressler, Christian, Geng, Huifang, Lin, Weihua, Liu, Yan, Zhao, Qian, Pan, Qinying, Akter, Marufa, Kong, Qingyu, Retegan, Marius, Gosztola, David J., Pápai, Mátyás, Khakhulin, Dmitry, Lawson Daku, Max, Zheng, Kaibo, and Canton, Sophie E.

Abstract

Metalloporphyrins with open d-shell ions can drive biochemical energy cycles. However, their utilization in photoconversion is hampered by rapid deactivation. Mapping the relaxation pathways is essential for elaborating strategies that can favorably alter the charge dynamics through chemical design and photoexcitation conditions. Here, we combine transient optical absorption spectroscopy and transient X-ray emission spectroscopy with femtosecond resolution to probe directly the coupled electronic and spin dynamics within a photoexcited nickel porphyrin in solution. Measurements and calculations reveal that a state with charge-transfer character mediates the formation of the thermalized excited state, thereby advancing the description of the photocycle for this important representative molecule. More generally, establishing that intramolecular charge-transfer steps play a role in the photoinduced dynamics of metalloporphyrins with open d-shell sets a conceptual ground for their development as building blocks capable of boosting nonadiabatic photoconversion in functional architectures through “hot” charge transfer down to the attosecond time scale.

Published
2024

24. Experimental and theoretical correlations between vanadium K-edge X-ray absorption and Kβ emission spectra

Author

Rees, Julian A, Wandzilak, Aleksandra, Maganas, Dimitrios, Wurster, Nicole IC, Hugenbruch, Stefan, Kowalska, Joanna K, Pollock, Christopher J, Lima, Frederico A, Finkelstein, Kenneth D, and DeBeer, Serena

Subjects
Quantum Theory, Spectrometry, X-Ray Emission, Vanadium Compounds, X-Ray Absorption Spectroscopy, Vanadium, X-ray spectroscopy, Density functional theory DFT, XES, XAS, Inorganic Chemistry, Medicinal and Biomolecular Chemistry, Biochemistry and Cell Biology, Biophysics
Abstract

A series of vanadium compounds was studied by K-edge X-ray absorption (XAS) and K[Formula: see text] X-ray emission spectroscopies (XES). Qualitative trends within the datasets, as well as comparisons between the XAS and XES data, illustrate the information content of both methods. The complementary nature of the chemical insight highlights the success of this dual-technique approach in characterizing both the structural and electronic properties of vanadium sites. In particular, and in contrast to XAS or extended X-ray absorption fine structure (EXAFS), we demonstrate that valence-to-core XES is capable of differentiating between ligating atoms with the same identity but different bonding character. Finally, density functional theory (DFT) and time-dependent DFT calculations enable a more detailed, quantitative interpretation of the data. We also establish correction factors for the computational protocols through calibration to experiment. These hard X-ray methods can probe vanadium ions in any oxidation or spin state, and can readily be applied to sample environments ranging from solid-phase catalysts to biological samples in frozen solution. Thus, the combined XAS and XES approach, coupled with DFT calculations, provides a robust tool for the study of vanadium atoms in bioinorganic chemistry.

Published
2016

25. Soluble Silicon Source via Foliar Application Improve Plant Physiology and Fruit Quality of Solanum lycopersicum L.

Author

Flores, Rilner Alves, primary, de Lima, Frederico Simões Raimundo, additional, Xavier, Maxuel Fellipe Nunes, additional, Bueno, Amanda Magalhães, additional, de Andrade, Aline Franciel, additional, de Souza Júnior, Jonas Pereira, additional, Campos, Cid Naudi Silva, additional, Cunha Júnior, Luís Carlos, additional, Oliveira Abdala, Klaus de, additional, and de Mello Prado, Renato, additional

Published
2023
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33. XFEL Microcrystallography of Self-Assembling Silver n-Alkanethiolates

Author

Aleksich, Mariya, primary, Paley, Daniel W., additional, Schriber, Elyse A., additional, Linthicum, Will, additional, Oklejas, Vanessa, additional, Mittan-Moreau, David W., additional, Kelly, Ryan P., additional, Kotei, Patience A., additional, Ghodsi, Anita, additional, Sierra, Raymond G., additional, Aquila, Andrew, additional, Poitevin, Frédéric, additional, Blaschke, Johannes P., additional, Vakili, Mohammad, additional, Milne, Christopher J., additional, Dall’Antonia, Fabio, additional, Khakhulin, Dmitry, additional, Ardana-Lamas, Fernando, additional, Lima, Frederico, additional, Valerio, Joana, additional, Han, Huijong, additional, Gallo, Tamires, additional, Yousef, Hazem, additional, Turkot, Oleksii, additional, Bermudez Macias, Ivette J., additional, Kluyver, Thomas, additional, Schmidt, Philipp, additional, Gelisio, Luca, additional, Round, Adam R., additional, Jiang, Yifeng, additional, Vinci, Doriana, additional, Uemura, Yohei, additional, Kloos, Marco, additional, Hunter, Mark, additional, Mancuso, Adrian P., additional, Huey, Bryan D., additional, Parent, Lucas R., additional, Sauter, Nicholas K., additional, Brewster, Aaron S., additional, and Hohman, J. Nathan, additional

Published
2023
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34. Watching Excited State Dynamics with Optical and X-ray Probes: The Excited State Dynamics of Aquocobalamin and Hydroxocobalamin

Author

Sension, Roseanne J., primary, McClain, Taylor P., additional, Lamb, Ryan M., additional, Alonso-Mori, Roberto, additional, Lima, Frederico Alves, additional, Ardana-Lamas, Fernando, additional, Biednov, Mykola, additional, Chollet, Matthieu, additional, Chung, Taewon, additional, Deb, Aniruddha, additional, Dewan, Paul A., additional, Gee, Leland B., additional, Huang Ze En, Joel, additional, Jiang, Yifeng, additional, Khakhulin, Dmitry, additional, Li, Jianhao, additional, Michocki, Lindsay B., additional, Miller, Nicholas A., additional, Otte, Florian, additional, Uemura, Yohei, additional, van Driel, Tim B., additional, and Penner-Hahn, James E., additional

Published
2023
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35. Ultrafast Jahn‐Teller Photoswitching in Cobalt Single‐Ion Magnets

Author

Canton, Sophie E., primary, Biednov, Mykola, additional, Pápai, Mátyás, additional, Lima, Frederico A., additional, Choi, Tae‐Kyu, additional, Otte, Florian, additional, Jiang, Yifeng, additional, Frankenberger, Paul, additional, Knoll, Martin, additional, Zalden, Peter, additional, Gawelda, Wojciech, additional, Rahaman, Ahibur, additional, Møller, Klaus B., additional, Milne, Christopher, additional, Gosztola, David J., additional, Zheng, Kaibo, additional, Retegan, Marius, additional, and Khakhulin, Dmitry, additional

Published
2023
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37. ANÁLISE DA ADMINISTRAÇÃO DO CAPITAL DE GIRO E SUA INFLUÊNCIA NA RENTABILIDADE: UM ESTUDO DE EMPRESAS DE CAPITAL ABERTO NA BOLSA DE VALORES BRASILEIRA.

Author

BORGES DE LIMA, FREDERICO NUNES, PEREIRA BASTOS, SÉRGIO AUGUSTO, and SOARES DE OLIVEIRA, EDVAN

Subjects
INDUSTRIAL management, FINANCIAL leverage, WORKING capital, RATE of return, PUBLIC companies
Abstract

Copyright of Revista de Administração FACES Journal is the property of Revista de Administracao FACES Journal and its content may not be copied or emailed to multiple sites or posted to a listserv without the copyright holder's express written permission. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)

Published
2024

39. Ultrafast Energy Transfer from Photoexcited Tryptophan to the Haem in Cytochrome c

Author

Bacellar, Camila, primary, Rouxel, Jérémy R., additional, Ingle, Rebecca A., additional, Mancini, Giulia F., additional, Kinschel, Dominik, additional, Cannelli, Oliviero, additional, Zhao, Yang, additional, Cirelli, Claudio, additional, Knopp, Gregor, additional, Szlachetko, Jakub, additional, Lima, Frederico A., additional, Menzi, Samuel, additional, Ozerov, Dmitry, additional, Pamfilidis, Georgios, additional, Kubicek, Katharina, additional, Khakhulin, Dmitry, additional, Gawelda, Wojciech, additional, Rodriguez-Fernandez, Angel, additional, Biednov, Mykola, additional, Bressler, Christian, additional, Arrell, Christopher A., additional, Johnson, Philip J. M., additional, Milne, Christopher J., additional, and Chergui, Majed, additional

Published
2023
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40. Ultrafast Jahn-Teller Photoswitching in Cobalt Single-Ion Magnets

Author

Canton, Sophie E., Biednov, Mykola, Pápai, Mátyás, Lima, Frederico A., Choi, Tae Kyu, Otte, Florian, Jiang, Yifeng, Frankenberger, Paul, Knoll, Martin, Zalden, Peter, Gawelda, Wojciech, Rahaman, Ahibur, Møller, Klaus B., Milne, Christopher, Gosztola, David J., Zheng, Kaibo, Retegan, Marius, Khakhulin, Dmitry, Canton, Sophie E., Biednov, Mykola, Pápai, Mátyás, Lima, Frederico A., Choi, Tae Kyu, Otte, Florian, Jiang, Yifeng, Frankenberger, Paul, Knoll, Martin, Zalden, Peter, Gawelda, Wojciech, Rahaman, Ahibur, Møller, Klaus B., Milne, Christopher, Gosztola, David J., Zheng, Kaibo, Retegan, Marius, and Khakhulin, Dmitry

Abstract

Single-ion magnets (SIMs) constitute the ultimate size limit in the quest for miniaturizing magnetic materials. Several bottlenecks currently hindering breakthroughs in quantum information and communication technologies could be alleviated by new generations of SIMs displaying multifunctionality. Here, ultrafast optical absorption spectroscopy and X-ray emission spectroscopy are employed to track the photoinduced spin-state switching of the prototypical complex [Co(terpy)2]2+ (terpy = 2,2′:6′,2″-terpyridine) in solution phase. The combined measurements and their analysis supported by density functional theory (DFT), time-dependent-DFT (TD-DFT) and multireference quantum chemistry calculations reveal that the complex undergoes a spin-state transition from a tetragonally elongated doublet state to a tetragonally compressed quartet state on the femtosecond timescale, i.e., it sustains ultrafast Jahn-Teller (JT) photoswitching between two different spin multiplicities. Adding new Co-based complexes as possible contenders in the search for JT photoswitching SIMs will greatly widen the possibilities for implementing magnetic multifunctionality and eventually controlling ultrafast magnetization with optical photons.

Published
2023

41. Atomic-scale observation of solvent reorganization influencing photoinduced structural dynamics in a copper complex photosensitizer

Author

Katayama, Tetsuo, Choi, Tae Kyu, Khakhulin, Dmitry, Dohn, Asmus O., Milne, Christopher J., Vankó, György, Németh, Zoltán, Lima, Frederico A., Szlachetko, Jakub, Sato, Tokushi, Nozawa, Shunsuke, Adachi, Shin Ichi, Yabashi, Makina, Penfold, Thomas J., Gawelda, Wojciech, Levi, Gianluca, Katayama, Tetsuo, Choi, Tae Kyu, Khakhulin, Dmitry, Dohn, Asmus O., Milne, Christopher J., Vankó, György, Németh, Zoltán, Lima, Frederico A., Szlachetko, Jakub, Sato, Tokushi, Nozawa, Shunsuke, Adachi, Shin Ichi, Yabashi, Makina, Penfold, Thomas J., Gawelda, Wojciech, and Levi, Gianluca

Abstract

Photochemical reactions in solution are governed by a complex interplay between transient intramolecular electronic and nuclear structural changes and accompanying solvent rearrangements. State-of-the-art time-resolved X-ray solution scattering has emerged in the last decade as a powerful technique to observe solute and solvent motions in real time. However, disentangling solute and solvent dynamics and how they mutually influence each other remains challenging. Here, we simultaneously measure femtosecond X-ray emission and scattering to track both the intramolecular and solvation structural dynamics following photoexcitation of a solvated copper photosensitizer. Quantitative analysis assisted by molecular dynamics simulations reveals a two-step ligand flattening strongly coupled to the solvent reorganization, which conventional optical methods could not discern. First, a ballistic flattening triggers coherent motions of surrounding acetonitrile molecules. In turn, the approach of acetonitrile molecules to the copper atom mediates the decay of intramolecular coherent vibrations and induces a further ligand flattening. These direct structural insights reveal that photoinduced solute and solvent motions can be intimately intertwined, explaining how the key initial steps of light harvesting are affected by the solvent on the atomic time and length scale. Ultimately, this work takes a step forward in understanding the microscopic mechanisms of the bidirectional influence between transient solvent reorganization and photoinduced solute structural dynamics.

Published
2023

43. ESOFAGITE E ÚLCERA PÉPTICA: PREVALÊNCIA EM PESSOAS COM DISPEPSIA

Author

Horley Soares Britto Neto, Lima, Elaine Oliveira, De Jesus, Pedro Henrique Santos, De Melo, Alexandre Magno Teixeira, Cesar, Alan Silva, Campos, Andrey Melo, Menezes, Icaro Celso Gomes, Assis, João Marcos Ferreira, Alves, Mathias Luca Melo, Rocha, Yan Alves, Trindade, Leda Maria Delmondes Freitas, and De Lima, Frederico Santana

Subjects
Dispepsia, DRG, Refluxo, Úlcera, Dyspepsia, GERD, Reflux, Ulcer, ERGE, Reflujo
Abstract

Objetivo: avaliar a prevalência de esofagite e úlcera péptica em pacientes com dispepsia. Metodologia: estudo prospectivo e transversal realizado em duas clínicas privadas em Aracaju, capital do estado de Sergipe, de 2018 a 2019. A amostra foi composta por 860 pacientes, com diagnóstico clínico de dispepsia, que foram submetidos à Endoscopia Digestiva Alta (EDA) e ao estudo histopatológico de mucosa esofagogastroduodenal. Foram aplicados questionários sociodemográficos e clínicos, além de questões que abordaram os Critérios de ROMA III. Resultados: 845 (98,2%) dos laudos foram considerados válidos, desses 195 (23,07%) tiveram o diagnóstico endoscópico e histopatológico de esofagite, sendo mais comum em homens com idade média de 39 anos, casados 105 (54,7%), pardos 95 (51,1%) e com ensino médio completo 102 (53,4%). Além disso, das lesões associadas à esofagite, hérnia hiatal foi estatisticamente significativa (p

Published
2023
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44. Estudantes com necessidades educacionais específicas: possibilidades e desafios para implementação do Napnee no Campus Santo Antônio de Pádua do IFFluminense

Author

Santiago Lima, Frederico and Pimentel Martins, Rosângela

Abstract

Resumen: Este artículo surge de inquietudes en el Campus Santo Antônio de Pádua, recientemente implementado, del Instituto Federal Fluminense (IFFLUMINENSE), en el interior del Estado de Río de Janeiro, en relación al Centro de Apoyo a Personas con Necesidades Educativas Específicas ( NAPNEE). El objetivo es analizar informaciones sobre el campo de actuación, posibilidades y desafíos del NAPNEE en el IFFluminense y su implementación en el Campus Santo Antônio de Pádua, además de la formación y familiarización de los docentes en el área de inclusión. La metodología consiste en investigación documental y bibliográfica, encuesta a los alumnos atendidos y aplicación de un cuestionario a los docentes. Identificamos que el campo de acción, las posibilidades y las necesidades del seguimiento de los estudiantes son enormes, sin embargo, los desafíos son mucho mayores, ya sea por la falta de formación docente, prioridad e incentivo institucional, la precariedad en el seguimiento de los estudiantes y la falta de personal y espacio físico apropiado en la escuela para NAPNEE. Palabras clave: Napnee. Desafíos. Implementación., Este artigo surge das inquietações no recém-implantado Campus Santo Antônio de Pádua, do Instituto Federal Fluminense (IFFLUMINENSE), localizado no interior do Estado do Rio de Janeiro em relação ao Núcleo de Apoio às Pessoas com Necessidades Educacionais Específicas (NAPNEE). O referido campus fica a aproximadamente trezentos quilômetros de distância da capital fluminense. O objetivo é analisar informações sobre o campo de atuação, possibilidades e desafios do NAPNEE no IFFluminense e sua implementação no Campus Santo Antônio de Pádua, além da capacitação e familiaridade dos professores na área de inclusão. A metodologia utilizada consiste em pesquisa documental e bibliográfica, levantamento dos alunos atendidos e aplicação de questionário para os docentes. Identificamos que o campo de atuação, as possibilidades e as necessidades de acompanhamento dos alunos são enormes, porém, os desafios são bem maiores, seja pela falta de formação docente, incentivo institucional, a precariedade no acompanhamento dos discentes e a falta de equipe e espaço físico apropriado na escola destinado ao NAPNEE., Resumo: Este artigo surge das inquietações no recém-implantado Campus Santo Antônio de Pádua, do Instituto Federal Fluminense (IFFLUMINENSE), no interior do Estado do Rio de Janeiro em relação ao Núcleo de Apoio às Pessoas com Necessidades Educacionais Específicas (NAPNEE). O objetivo é analisar informações sobre o campo de atuação, possibilidades e desafios do NAPNEE no IFFluminense e sua implementação no Campus Santo Antônio de Pádua, além da capacitação e familiaridade dos professores na área de inclusão. A metodologia consiste em pesquisa documental e bibliográfica, levantamento dos alunos atendidos e aplicação de questionário para os docentes. Identificamos que o campo de atuação, as possibilidades e as necessidades de acompanhamento dos alunos são enormes, porém, os desafios são bem maiores, seja pela falta de formação docente, prioridade e incentivo institucional, a precariedade no acompanhamento dos discentes e a falta de equipe e espaço físico apropriado na escola destinado ao NAPNEE. Palavras-chave: Napnee. Desafios. Implementação.

Published
2023

45. Tracking multiple components of a nuclear wavepacket in photoexcited Cu(I)-phenanthroline complex using ultrafast X-ray spectroscopy

Author

Katayama, Tetsuo, Northey, Thomas, Gawelda, Wojciech, Milne, Christopher J., Vankó, György, Lima, Frederico A., Bohinc, Rok, Németh, Zoltán, Nozawa, Shunsuke, Sato, Tokushi, Khakhulin, Dmitry, Szlachetko, Jakub, Togashi, Tadashi, Owada, Shigeki, Adachi, Shin-ichi, Bressler, Christian, Yabashi, Makina, and Penfold, Thomas J.

Published
2019
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47. Atomic-scale observation of solvent reorganization influencing photoinduced structural dynamics in a copper complex photosensitizer

Author

Katayama, Tetsuo, primary, Choi, Tae-Kyu, additional, Khakhulin, Dmitry, additional, Dohn, Asmus O., additional, Milne, Christopher J., additional, Vankó, György, additional, Németh, Zoltán, additional, Lima, Frederico A., additional, Szlachetko, Jakub, additional, Sato, Tokushi, additional, Nozawa, Shunsuke, additional, Adachi, Shin-ichi, additional, Yabashi, Makina, additional, Penfold, Thomas J., additional, Gawelda, Wojciech, additional, and Levi, Gianluca, additional

Published
2023
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48. Atomic-scale observation of solvent reorganization influencing photoinduced structural dynamics in a copper complex photosensitizer

Author

Katayama, Tetsuo, primary, Choi, Tae-Kyu, additional, Khakhulin, Dmitry, additional, Dohn, Asmus, additional, Milne, Christopher, additional, Vankó, György, additional, Németh, Zoltán, additional, Lima, Frederico, additional, Szlachetko, Jakub, additional, Sato, Tokushi, additional, Nozawa, Shunsuke, additional, Adachi, Shin-ichi, additional, Yabashi, Makina, additional, Penfold, Thomas, additional, Gawelda, Wojciech, additional, and Levi, Gianluca, additional

Published
2022
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