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2 results on '"Wasielewski M"'

1. Many-Body Models for Chirality-Induced Spin Selectivity in Electron Transfer

Author

Chiesa, A., Garlatti, E., Mezzadri, M., Celada, L., Sessoli, R., Wasielewski, M. R., Bittl, R., Santini, P., and Carretta, S.

Subjects
Condensed Matter - Mesoscale and Nanoscale Physics
Abstract

We present the first microscopic model for chirality-induced spin selectivity effect in electron-transfer, in which the internal degrees of freedom of the chiral bridge are explicitly included. By exactly solving this model on short chiral chains we demonstrate that a sizable polarization on the acceptor arises from the interplay of coherent and incoherent dynamics, with strong electron-electron correlations yielding many-body states on the bridge as crucial ingredients. Moreover, we include the coherent and incoherent interactions with vibrational modes and show that they can play an important role in determining the long-time polarized state probed in experiments.

Published
2024
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2. Differentiating Thermal Conductances at Semiconductor Nanocrystal/Ligand and Ligand/Solvent Interfaces in Colloidal Suspensions.

Author

Liang Y, Diroll BT, Wong KL, Harvey SM, Wasielewski M, Ong WL, Schaller RD, and Malen JA

Abstract

Infrared-pump, electronic-probe (IPEP) spectroscopy is used to measure heat flow into and out of CdSe nanocrystals suspended in an organic solvent, where the surface ligands are initially excited with an infrared pump pulse. Subsequently, the heat is transferred from the excited ligands to the nanocrystals and in parallel to the solvent. Parallel heat transfer in opposite directions uniquely enables us to differentiate the thermal conductances at the nanocrystal/ligand and ligand/solvent interfaces. Using a novel solution to the heat diffusion equation, we fit the IPEP data to find that the nanocrystal/ligand conductances range from 88 to 135 MW m -2 K -1 and are approximately 1 order of magnitude higher than the ligand/solvent conductances, which range from 7 to 26 MW m -2 K -1 . Transient nonequilibrium molecular dynamics (MD) simulations of nanocrystal suspensions agree with IPEP data and show that ligands bound to the nanocrystal by bidentate bonds have more than twice the per-ligand conductance as those bound by monodentate bonds.

Published
2023
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