Electron relaxation is studied in endofullerene Mg@C_{60} after an initial localized photoexcitation in Mg by nonadiabatic molecular dynamics simulations. Two approaches to the electronic structure of the excited electronic states are used: (i) an independent particle approximation based on a density-functional theory description of molecular orbitals and (ii) a configuration-interaction description of the many-body effects. Both methods exhibit similar relaxation times, leading to an ultrafast decay and charge transfer from Mg to C_{60} within tens of femtoseconds. Method (i) further elicits a transient trap of the transferred electron that can delay the electron-hole recombination. Results shall motivate experiments to probe these ultrafast processes by two-photon transient absorption or photoelectron spectroscopy in gas phase, in solution, or as thin films.
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http://dx.doi.org/10.1103/PhysRevLett.126.183002 | DOI Listing |
J Phys Chem Lett
January 2025
Key Laboratory of Materials Physics, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei 230031, China.
Unveiling the nonlinear interactions between terahertz (THz) electromagnetic waves and free carriers in two-dimensional materials is crucial for the development of high-field and high-frequency electronic devices. Herein, we investigate THz nonlinear transport dynamics in a monolayer graphene/MoS heterostructure using time-resolved THz spectroscopy with intense THz pulses as the probe. Following ultrafast photoexcitation, the interfacial charge transfer establishes a nonequilibrium carrier redistribution, leaving free holes in the graphene and trapping electrons in the MoS.
View Article and Find Full Text PDFNanomicro Lett
January 2025
College of Materials Science and Engineering, Ocean University of China, Qingdao, 266100, People's Republic of China.
Solar-driven interfacial evaporation is one of the most attractive approaches to addressing the global freshwater shortage. However, achieving an integrated high evaporation rate, salt harvesting, and multifunctionality in evaporator is still a crucial challenge. Here, a novel composite membrane with biomimetic micro-nanostructured superhydrophobic surface is designed via ultrafast laser etching technology.
View Article and Find Full Text PDFACS Nano
January 2025
Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem 9190401, Israel.
Semiconductor-metal hybrid nanoparticles (HNPs) are promising materials for photocatalytic applications, such as water splitting for green hydrogen generation. While most studies have focused on Cd containing HNPs, the realization of actual applications will require environmentally compatible systems. Using heavy-metal free ZnSe-Au HNPs as a model, we investigate the dependence of their functionality and efficiency on the cocatalyst metal domain characteristics ranging from the single-atom catalyst (SAC) regime to metal-tipped systems.
View Article and Find Full Text PDFChem Sci
December 2024
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences Zhongshan Road 457 Dalian 116023 China
In solid-state NMR, dipolar-based heteronuclear polarization transfer has been extensively used for sensitivity enhancement and multidimensional correlations, but its efficiency often suffers from undesired spin interactions and hardware limitations. Herein, we propose a novel dipolar-echo edited R-symmetry (DEER) sequence, which is further incorporated into the INEPT-type scheme, dubbed DEER-INEPT, for achieving highly efficient heteronuclear polarization transfer. Numerical simulations and NMR experiments demonstrate that DEER-INEPT offers significantly improved robustness, enabling efficient polarization transfer under a wide range of MAS conditions, from slow to ultrafast rates, outperforming existing methods.
View Article and Find Full Text PDFJ Chem Theory Comput
January 2025
HUN-REN Wigner Research Centre for Physics, P.O. Box 49, H-1525 Budapest, Hungary.
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