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Light-Harvesting Spin Hyperpolarization of Organic Radicals in a Metal-Organic Framework.
J Am Chem Soc
January 2025
Department of Chemistry, Graduate School of Science, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, Japan.
Light-driven spin hyperpolarization of organic molecules is a crucial technique for spin-based applications such as quantum information science (QIS) and dynamic nuclear polarization (DNP). Synthetic chemistry provides the design of spins with atomic precision and enables the scale-up of individual spins to hierarchical structures. The high designability and extended pore structure of metal-organic frameworks (MOFs) can control interactions between spins and guest molecules.
View Article and Find Full Text PDFSulfur isotope engineering in heterostructures of transition metal dichalcogenides.
Nanoscale Adv
January 2025
Department of Condensed Matter Physics, Faculty of Mathematics and Physics, Charles University Ke Karlovu 5, 12116, Prague 2 Czech Republic
Heterostructuring of two-dimensional materials offers a robust platform to precisely tune optoelectronic properties through interlayer interactions. Here we achieved a strong interlayer coupling in a double-layered heterostructure of sulfur isotope-modified adjacent MoS monolayers two-step chemical vapor deposition growth. The strong interlayer coupling in the MoS(S)/MoS(S) was affirmed by low-frequency shear and breathing modes in the Raman spectra.
View Article and Find Full Text PDFBroad-Temperature Optical Thermometry via Dual Sensitivity of Self-Trapped Excitons Lifetime and Higher-Order Phonon Anharmonicity in Lead-Free Perovskites.
Angew Chem Int Ed Engl
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DICP: Chinese Academy of Sciences Dalian Institute of Chemical Physics, State Key Laboratory of Molecular Reaction Dynamics and Dalian Coherent Light Source, CHINA.
Broad-temperature optical thermometry necessitates materials with exceptional sensitivity and stability across varied thermal conditions, presenting challenges for conventional systems. Here, we report a lead-free, vacancy-ordered perovskite Cs2TeCl6, that achieves precise temperature sensing through a novel combination of self-trapped excitons (STEs) photoluminescence (PL) lifetime modulation and unprecedented fifth-order phonon anharmonicity. The STEs PL lifetime demonstrates a highly temperature-sensitive response from 200 to 300 K, ideal for low-to-intermediate thermal sensing.
View Article and Find Full Text PDFVariational Quantum Algorithm for Non-Markovian Quantum Dynamics Using an Ensemble of Ehrenfest Trajectories.
J Phys Chem Lett
January 2025
Department of Chemistry and Biochemistry, George Mason University, Fairfax, Virginia 22030, United States.
The simulation of non-Markovian quantum dynamics plays an important role in the understanding of charge and exciton dynamics in the condensed phase environment, yet such a simulation remains computationally expensive on classical computers. In this work, we develop a variational quantum algorithm that is capable of simulating non-Markovian quantum dynamics on quantum computers. The algorithm captures the non-Markovian effect by employing the Ehrenfest trajectories and Monte Carlo sampling of their thermal distribution.
View Article and Find Full Text PDFDesign Rule of Tetradentate Ligand-Based Pt(II) Complex for Efficient Singlet Exciton Harvesting in Fluorescent Organic Light-Emitting Diodes.
J Phys Chem Lett
January 2025
School of Chemical Engineering, Sungkyunkwan University, 2066, Seobu-ro, Jangan-gu, Suwon-si, Gyeonggi-do 16419, Republic of Korea.
Controlling intermolecular interactions, such as triplet-triplet annihilation (TTA) and triplet-polaron annihilation (TPA), is crucial for achieving high quantum efficiency in organic light-emitting diodes (OLEDs) by suppressing exciton loss. This study investigates the molecular design of tetradentate Pt(II) complexes used for singlet exciton harvesting in fluorescent OLEDs to elucidate the relationship between the chemical structure of the ligands and exciton quenching mechanisms. It was discovered that the bulkiness of substituents is pivotal for maximizing quantum efficiency in these devices.
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