Article
Optics
Alberto Ghezzi, Armin J. M. Lenz, Fernando Soldevila, Enrique Tajahuerce, Vito Vurro, Andrea Bassi, Gianluca Valentini, Andrea Farina, Cosimo D'Andrea
Summary: In this work, we propose a time-resolved multispectral fluorescence microscopy system based on the Single-Pixel Camera (SPC) scheme, which achieves high resolution and short measurement time using Compressive Sensing (CS) technology. Data Fusion (DF) with a high-resolution camera is used to address the low spatial resolution issue typical of SPC. By integrating hardware and algorithms, this system reduces the number of measurements while preserving the information content, allowing for a zoom feature without moving the optical system. The system is characterized in terms of spatial, spectral, and temporal properties, and is validated on a cellular sample.
Review
Chemistry, Multidisciplinary
Adam A. L. Michalchuk, Franziska Emmerling
Summary: Mechanochemical transformations offer environmentally friendly routes for synthesis, increasing reaction speed and selectivity. Time-resolved in situ (TRIS) approaches have provided new insights into mechanochemical reactions, revealing new features and advancing our understanding through the combination of complementary techniques.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Optics
Dzmitryi Ushakou
Summary: Nowadays, there is a growing scientific interest in both single and multiple excited-state intramolecular proton transfer (ESIPT) processes. These processes offer great opportunities for applications in chemical sensors, molecular switches, NIR emitting devices, and liquid crystals. One example of multiple ESIPT is stepwise excited-state intramolecular double proton transfer (ESIDPT), which occurs via intramolecular hydrogen bonding and involves sequential proton transfers in a molecule.
JOURNAL OF LUMINESCENCE
(2023)
Article
Materials Science, Multidisciplinary
G. Stefanucci, E. Perfetto
Summary: The study highlights the effects of phonon-induced decoherence and relaxation on excitations, leading to shifts and broadening of band replicas, as well as exciton formation in the bandgap. Resonant excitations generate valence-band replicas, while nonresonant excitations eventually display conduction-band replicas, both accompanied by asymmetries in photoelectron energies.
Article
Chemistry, Physical
Naoya Tajima, Katsuichi Kanemoto
Summary: We have conducted time-resolved photo-induced absorption spectroscopy to study the behavior of carriers in operating dye-sensitized solar cells (DSSCs). We discovered that the transfer of electron carriers in DSSCs is very slow and occurs in a specific order. These findings can be observed through PIA signals and photocurrents, which reach equilibrium at the same rate determined by the transfer rate of iodine ions. These operando measurements provide valuable insights into the operational mechanism of solar cells and can be applied to various types of solar cells.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Anthony V. Sica, Ash Sueh Hua, Helen H. Lin, Ellen M. Sletten, Timothy L. Atallah, Justin R. Caram
Summary: We demonstrate a method called Spectrally selective Time-resolved Emission through Fourier-filtering (STEF) for separating and resolving the dynamics of multiple emitters without using conventional filters. Our approach utilizes a fixed path-length imbalanced Mach-Zehnder interferometer to interfere and cancel (or enhance) specific spectral signatures corresponding to one emissive species. We show the range and utility of STEF by performing various procedures, including filtering laser scatter, separating fluorescence lifetimes, and resolving overlapping fluorescent stains.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Multidisciplinary Sciences
Yuichi Yokoyama, Shogo Kawaguchi, Masaichiro Mizumaki
Summary: Clarifying dynamic processes of materials is important in materials science. Time-resolved X-ray diffraction is a powerful technique for studying dynamic processes. Analyzing time-series data with appropriate time-evolution models and accurate start times is essential. In this study, a Bayesian framework including time-evolution models is established. It is applied to investigate an adsorption process, enabling information extraction about the time-evolution model and adsorption start time.
SCIENTIFIC REPORTS
(2023)
Article
Chemistry, Multidisciplinary
Luca D'Amario, Maria Bruna Stella, Tomas Edvinsson, Maurizio Persico, Johannes Messinger, Holger Dau
Summary: This study describes a transient spectro-electrochemical Raman setup that achieves sub-ms time resolution, allowing for the study of electrochemical processes. The technique was validated through experiments and confirmed to be effective in assigning spectral properties to transient species. This research provides a foundational contribution to the development of next generation electrolizers, fuel cells, and batteries.
Article
Chemistry, Physical
Paraic M. Keane, Clara Zehe, Fergus E. Poynton, Sandra A. Bright, Sandra Estayalo-Adrian, Stephen J. Devereux, Paul M. Donaldson, Igor V. Sazanovich, Michael Towrie, Stanley W. Botchway, Christine J. Cardin, D. Clive Williams, Thorfinnur Gunnlaugsson, Conor Long, John M. Kelly, Susan J. Quinn
Summary: In this study, the interactions of metal-free TMPyP4 and Pt(ii)TMPyP4 with guanine-containing nucleic acids were investigated using time-resolved infrared spectroscopy (TRIR) for the first time. The results showed that both compounds bound close to guanine, and electron transfer occurred when D(2)TMPyP4 was bound to guanine-containing systems.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Spectroscopy
Jonathan Merten, Erin Nicholas, Shealyn Chestnut, Shawnda Ethridge, Hannah Bariola, Mary Elizabeth Foster
Summary: The absolute atomized mass of a laser-induced yttrium plasma was measured under various noble and oxidizing cover gases using high resolution atomic-absorption spectroscopy mapping. The maximum spatial extent of the plasma decreased with the molar mass of the cover gas. Time-resolved masses measured under oxidizing atmospheres showed continuous net loss from the first measured delay. Plasmas under helium and argon atmospheres also exhibited net loss of atomized yttrium beyond 4 mu s, due to an unknown mechanism.
SPECTROCHIMICA ACTA PART B-ATOMIC SPECTROSCOPY
(2023)
Article
Chemistry, Physical
Runhui Liang, Wenjuan Xiong, Xueqin Bai, Lili Du, David Lee Phillips
Summary: In this study, TPE containing Pt(II) acetylide complexes were synthesized and their photophysical properties were investigated using resonance Raman and time-resolved transient absorption spectroscopies. The results revealed that TPE has a significant impact on the lifetimes of triplet excited states, possibly due to the intramolecular rotation of TPE that accelerates the nonradiative decay process.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Thermodynamics
Hongtao Zhong, Chao Yan, Chu C. Teng, Guoming Ma, Gerard Wysocki, Yiguang Ju
Summary: This study measured the rate constant and branching ratios of the reaction between ethyl and hydroperoxyl radical for the first time, using mid-IR Faraday rotation spectroscopy and UV-IR direct absorption spectroscopy. The results indicated that the formation of OH was the major channel in the reaction at 297K.
PROCEEDINGS OF THE COMBUSTION INSTITUTE
(2021)
Article
Chemistry, Multidisciplinary
C. Blake Wilson, Robert Tycko
Summary: Elucidating the detailed mechanisms of structural conversions in biological macromolecules is crucial for biophysical chemistry, and new experimental methods are needed for further understanding. The article presents a simple technique called rapid inverse temperature jump, which enables the initiation of a structural conversion process in solutions by rapidly decreasing the temperature. The technique is demonstrated using a 26-residue peptide called melittin, where the conversion from a disordered state to a helical state was studied. Time-resolved solid-state nuclear magnetic resonance (ssNMR) was used to analyze the kinetics and mechanism of the conversion.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Review
Chemistry, Physical
Angel Cuesta
Summary: This article reviews the application of surface-enhanced infrared spectroscopy in the attenuated total reflection mode (ATR-SEIRAS) for time-resolved studies of electrode-electrolyte interfaces. Different time resolutions and methodologies are used to explore the kinetics of electrochemical reactions and specific adsorption, as well as the dynamics of double layer charging, the vibrational relaxation of adsorbates, and the spectral diffusion of adsorbates.
CURRENT OPINION IN ELECTROCHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Shiny Maity, Brad D. D. Price, C. Blake Wilson, Arnab Mukherjee, Matthieu Starck, David Parker, Maxwell Z. Z. Wilson, Janet E. E. Lovett, Songi Han, Mark S. S. Sherwin
Summary: We propose a time-resolved Gd-Gd electron paramagnetic resonance (TiGGER) technique at 240 GHz to monitor inter-residue distances in proteins' mechanical cycles in solution state. TiGGER utilizes Gd-sTPATCN spin labels with favorable properties, including spin-7/2 EPR-active center, short linker, narrow intrinsic linewidth, and minimal anisotropy at high fields. By applying TiGGER, we observed that the C-terminus and N-terminus of AsLOV2 separate within 1 s upon light activation and relax back to equilibrium with a time constant of approximately 60 s. TiGGER also revealed that the light-induced long-range mechanical motion is decelerated in the Q513A variant of AsLOV2, which is correlated with the slowed relaxation of the optically excited chromophore as reported in recent literature. TiGGER has the potential to complement existing methods for studying triggered functional dynamics in proteins.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)