Article
Chemistry, Physical
Chelsea Liekhus-Schmaltz, Zachary W. Fox, Amity Andersen, Kasper S. Kjaer, Roberto Alonso-Mori, Elisa Biasin, Julia Carlstad, Matthieu Chollet, James D. Gaynor, James M. Glownia, Kiryong Hong, Thomas Kroll, Jae Hyuk Lee, Benjamin Poulter, Marco Reinhard, Dimosthenis Sokaras, Yu Zhang, Gilles Doumy, Anne Marie March, Stephen H. Southworth, Shaul Mukamel, Amy A. Cordones, Robert W. Schoenlein, Niranjan Govind, Munira Khalil
Summary: In this study, we successfully quantified the evolving valence hole charge distribution in the photoexcited charge transfer state of a prototypical mixed valence bimetallic iron-ruthenium complex in solution, providing a spectroscopic ruler for quantifying excited-state valency in solvated complexes.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Biochemistry & Molecular Biology
Cheng Chen, J. Nathan Henderson, Dmitry A. Ruchkin, Jacob M. Kirsh, Mikhail S. Baranov, Alexey M. Bogdanov, Jeremy H. Mills, Steven G. Boxer, Chong Fang
Summary: This study systematically analyzed the vibrational properties of FP chromophores by using FSRS and quantum calculations. A bond-stretching mode characteristic of the quinoidal resonance structure was found to be present in most FPs and model chromophores, which can serve as a vibrational marker for interpreting chromophore-environment interactions and structural effects on the electronic properties of the chromophore.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Article
Chemistry, Analytical
Steven A. Diaz, David W. Mccamant
Summary: By improving the collection optics, we have developed two new diffuse reflectance-based femtosecond stimulated Raman spectroscopy (drFSRS) techniques for collecting Raman spectra of opaque systems. The experimental results demonstrate the current capabilities of collecting high-quality Raman spectra using drFSRS.
ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Piotr Kabacinski, Pietro Marabotti, Daniele Fazzi, Vasilis Petropoulos, Andrea Iudica, Patrick Serafini, Giulio Cerullo, Carlo S. S. Casari, Margherita Zavelani-Rossi
Summary: Investigated the photophysics of one-dimensional linear nanostructures and revealed their excellent mechanical, thermal, and electronic properties. Studied the excited state relaxation processes using experimental and computational methods, providing important insights into photoinduced events in low-dimensional carbon-based materials.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Physics, Multidisciplinary
Rebecca Boll, Julia M. Schaefer, Benoit Richard, Kilian Fehre, Gregor Kastirke, Zoltan Jurek, Markus S. Schoeffler, Malik M. Abdullah, Nils Anders, Thomas M. Baumann, Sebastian Eckart, Benjamin Erk, Alberto De Fanis, Reinhard Doerner, Sven Grundmann, Patrik Grychtol, Alexander Hartung, Max Hofmann, Markus Ilchen, Ludger Inhester, Christian Janke, Rui Jin, Max Kircher, Katharina Kubicek, Maksim Kunitski, Xiang Li, Tommaso Mazza, Severin Meister, Niklas Melzer, Jacobo Montano, Valerija Music, Giammarco Nalin, Yevheniy Ovcharenko, Christopher Passow, Andreas Pier, Nils Rennhack, Jonas Rist, Daniel E. Rivas, Daniel Rolles, Ilme Schlichting, Lothar Ph H. Schmidt, Philipp Schmidt, Juliane Siebert, Nico Strenger, Daniel Trabert, Florian Trinter, Isabel Vela-Perez, Rene Wagner, Peter Walter, Miriam Weller, Pawel Ziolkowski, Sang-Kil Son, Artem Rudenko, Michael Meyer, Robin Santra, Till Jahnke
Summary: Intense femtosecond X-ray pulses can visualize the structural dynamics of exploding photoionized molecules, providing important insights into chemical reactions.
Article
Chemistry, Multidisciplinary
Diana Bregenholt Zederkof, Klaus B. Moller, Martin M. Nielsen, Kristoffer Haldrup, Leticia Gonzalez, Sebastian Mai
Summary: This study investigates the nonadiabatic dynamics of the iron complex [Fe(CN)4(bpy)]2- in aqueous solution and reveals the significant role of solute-solvent interactions in solvent reorganization and complex behavior. The simulations uncover the ultrafast intersystem crossing and the effect of nuclear motion on this process. Additionally, a branched decay mechanism from singlet metal-to-ligand charge transfer states to triplet states is observed. The findings also suggest the potential application of time-resolved X-ray solution scattering experiments in observing solvent reorganization.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Basanta Kumar Rajbongshi, Shahnawaz Rafiq, Suman Bhowmik, Pratik Sen
Summary: In this study, the excited state dynamics of a GFP chromophore analogue, DPI, was investigated using femtosecond spectroscopy and quantum chemical calculations. It was found that the dynamics of DPI involves the formation of an intramolecular charge transfer state mediated by a twisting motion. Quantum chemical computations further predicted the formation of a conical intersection between the S1 and S0 states, which is the main nonradiative deactivation pathway. This study highlights the importance of restricting twisting motion for GFP analogues to exhibit GFP-like excited state properties.
JOURNAL OF MOLECULAR STRUCTURE
(2023)
Article
Chemistry, Physical
A. L. Dobryakov, O. A. Krohn, M. Quick, I. N. Ioffe, S. A. Kovalenko
Summary: This study analytically evaluates the resonance stimulated Raman signal and line shape, and applies the results to spectroscopic measurements of different compounds. The results show that the resonance stimulated Raman signal is more complex compared to spontaneous Raman, with contributions from higher and lower electronic states.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Yujin Kim, Rory Ma, Junho Lee, Jessica Harich, Daewoong Nam, Sangsoo Kim, Minseok Kim, Miguel Ochmann, Intae Eom, Nils Huse, Jae Hyuk Lee, Tae Kyu Kim
Summary: This study employs femtosecond X-ray absorption spectroscopy to investigate the time evolution of spin and charge density in [Ru(m-bpy)(3)](2+) upon metal-to-ligand charge transfer excitation. The results reveal a short MLCT lifetime and a longer lifetime of (MC)-M-3 state, along with the influence of ligand methylation on the stabilization of these states. The study also highlights the potential of femtosecond L-edge spectroscopy as a probe of valence charge density and spin-state in 4d transition metals.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Multidisciplinary
Qiaozhi Yu, Zhengjian Yao, Haolin Zhang, Zhibin Li, Zhixing Chen, Hanqing Xiong
Summary: Researchers have developed a new ultrafast time-domain spectroscopy technique called transient stimulated Raman excited fluorescence (T-SREF), which enables background-free Raman spectra of electronic-coupled vibrational modes. By exciting the sample with two successive broadband femtosecond pulse pairs and performing Fourier transform on the resulting time-domain fluorescence trace, T-SREF achieves high sensitivity at the level of a few molecules, paving the way for supermultiplexed fluorescence detection and molecular dynamics sensing.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Ruihua Pu, Ziyu Wang, Ruixue Zhu, Jiaming Jiang, Tsu-Chien Weng, Yifan Huang, Weimin Liu
Summary: Phototherapy is an effective and safe method for reducing high levels of ZZ-BR in the serum of newborns. This study used various spectroscopic techniques and quantum chemical calculations to investigate the primary configurational isomerization dynamics of ZZ-BR in organic solvents. The results showed that upon photoexcitation, ultrafast configurational isomerization occurred, followed by intramolecular hydrogen-bond distortion and large-scale rotation of the two dipyrrinone halves of the ZZ-BR isomer in a few picoseconds. Most of the population returned back to ZZ-BR, while a small amount converted into stable BR isomers via structural isomerization.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Ruihua Pu, Ziyu Wang, Ruixue Zhu, Jiaming Jiang, Tsu-Chien Weng, Yifan Huang, Weimin Liu
Summary: Phototherapy is an effective and safe method for reducing high levels of ZZ-BR in newborns' serum. The process involves photoinduced configurational and structural isomerization, which generates excretable isomers. However, the exact mechanism of ZZ-BR photoinduced isomerization is still not well understood.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Review
Materials Science, Multidisciplinary
Qian Cheng, Yupeng Miao, Joseph Wild, Wei Min, Yuan Yang
Summary: Stimulated Raman scattering (SRS) is a powerful chemical imaging technique with high chemical, spatial, and temporal resolution, suitable for applications in materials science and biomedicine. The high-speed and high-chemical sensitivity of SRS have attracted attention from the materials science community and have been successfully applied in various areas, such as 2D materials, energy storage, and polymer chemistry.
Article
Chemistry, Inorganic & Nuclear
A. I. Zvyagina, E. A. Gusarova, A. A. Averin, M. A. Kalinina
Summary: The study elucidated the role of substituents in a perylene molecule in energy transfer between a chromophore and reduced graphene oxide, showing that interactions between the unsubstituted chromophore and reduced GO cause surface-enhanced Raman scattering while interactions between the substituted chromophore and the carbon framework are weak due to steric hindrances.
RUSSIAN JOURNAL OF INORGANIC CHEMISTRY
(2021)
Article
Biochemistry & Molecular Biology
Aristides Marcano Olaizola, Robinson Kuis, Anthony Johnson, David Kingsley
Summary: This study investigates the generation of singlet oxygen from dissolved oxygen in water and heavy water using Raman stimulation. Without singlet oxygen photosensitizers, nanosecond-pulsed visible blue laser light can produce a red Stokes peak that is oxygen-dependent. This peak is absent in the presence of an oxygen quencher, and the temporal photodepletion of uric acid absorbance peak supports singlet oxygen generation. The authors suggest a two-photon stimulated Raman process as the mechanism behind singlet oxygen production from dissolved O2 in the solvents.
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY B-BIOLOGY
(2022)