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In some molecular systems, such as nucleobases, polyenes or the active ingredients of sunscreens, substantial amounts of photo-excitation energy are dissipated on a sub-picosecond time scale, raising questions such as: where does this energy go or among which degrees of freedom it is being distributed at such early times? Here we use transient absorption spectroscopy to track excitation energy dispersing from the optically accessible vibronic subsystem into the remaining vibrational subsystem of the solute and solvent. Monitoring the flow of energy during vibrational redistribution enables quantification of local molecular heating. Subsequent heat dissipation away from the solute molecule is characterized by classical thermodynamics and molecular dynamics simulations. Hence, we present a holistic approach that tracks the internal temperature and vibronic distribution from the act of photo-excitation to the restoration of the global equilibrium. Within this framework internal vibrational redistribution and vibrational cooling are emergent phenomena. We demonstrate the validity of the framework by examining a highly controversial example, carotenoids. We show that correctly accounting for the local temperature unambiguously explains their energetically and temporally congested spectral dynamics without the postulation of additional 'dark' states. An immediate further application of this approach would be to monitor the excitation and thermal dynamics of pigment-protein systems.
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http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6521204 | PMC |
http://dx.doi.org/10.1039/c9sc00410f | DOI Listing |
Chem Soc Rev
December 2024
Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, and National Synchrotron Radiation Laboratory, School of Nuclear Science and Technology, University of Science and Technology of China, Hefei, Anhui 230026, China.
The ultimate goal of catalysis is to control the cleavage and formation of chemical bonds at the molecular or even atomic level, enabling the customization of catalytic products. The essence of chemical bonding is the electromagnetic interaction between atoms, which makes it possible to directly manipulate the dynamic behavior of molecules and electrons in catalytic processes using external electric, magnetic and electromagnetic fields. In this tutorial review, we first introduce the feasibility and importance of field effects in regulating catalytic reaction processes and then outline the basic principles of electric-/magnetic-/electromagnetic-field interaction with matter, respectively.
View Article and Find Full Text PDFAnn Bot
December 2024
Instituto de Biologia, Universidade Federal de Uberlândia. Uberlândia, Brazil.
Background: Floral adaptations supposedly favour pollen grains to cross the numerous barriers faced during their journey to stigmas. Stamen dimorphism and specialized petals, like the cucculus in the Cassieae tribe (Fabaceae), are commonly observed in flowers that offer only pollen as a resource for bee pollinators. Here, we experimentally investigated whether the stamen dimorphism and cucculus enhance pollen placement on the bee's body.
View Article and Find Full Text PDFInt J Biol Macromol
December 2024
Key Laboratory for Forest Resources Conservation and Utilization in the Southwest Mountains of China, Ministry of Education, Southwest Forestry University, Kunming 650224, China; Key Laboratory of State Forestry and Grassland Administration on Highly-Efficient Utilization of Forestry Biomass Resources in Southwest China, Southwest Forestry University, Kunming 650224, China. Electronic address:
Composites derived from plant fibers are promising reinforcing materials for engineering because of their renewable and easily available characteristics. In this study, a simple pretreatment method was developed to fabricate structurally intact bamboo cellulose scaffolds. Water-stable, flexible, impact-resistant, and high damping ratio bamboo-based rubber composites were synthesized using carboxylated styrene-butadiene latex-impregnated 3D bamboo scaffolds.
View Article and Find Full Text PDFChemphyschem
December 2024
Clausius-Institut für Physikalische und Theoretische Chemie, Rheinische Friedrich-Wilhelms-Universität Bonn, Wegelerstrasse 12, 53115, Bonn.
Infrared probes are chemical moieties whose vibrational modes are used to obtain spectroscopic information about structural dynamics of complex systems; in particular, of biomacromolecules. Here, we explore the vibrational spectroscopy and dynamics of a reagent, 3-(4-azidophenyl)propiolonitrile (AzPPN), for selectively tagging thiols in protein environments with a multifunctional infrared probe containing both, an azide and a nitrile chromophore. The linear infrared spectrum of AzPPN is heavily perturbed in the antisymmetric azide stretching region as a result of accidental Fermi resonances.
View Article and Find Full Text PDFNanophotonics
May 2024
Department of Chemistry and Biochemistry, University of California San Diego, La Jolla, CA 92093, USA.
Vibrational polaritons have shown potential in influencing chemical reactions, but the exact mechanism by which they impact vibrational energy redistribution, crucial for rational polariton chemistry design, remains unclear. In this work, we shed light on this aspect by revealing the role of solvent phonon modes in facilitating the energy relaxation process from the polaritons formed of a mode of W(CO) to an IR inactive mode. Ultrafast dynamic measurements indicate that along with the direct relaxation to the dark modes, lower polaritons also transition to an intermediate state, which then subsequently relaxes to the mode.
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