Electronic excitations in the liquid phase are surprisingly rich and considerably more complex than either gas-phase or solid-state systems. While the majority of physical and biological processes take place in solvent, our understanding of nonequilibrium excited-state processes in these condensed phase environments remains far from complete. A central and long-standing issue in these solvated environments is the assessment of many-body interactions, particularly when the entire system is out of equilibrium and many quantum states participate in the overall process. Here we present a microscopic picture of solute-solvent electron dynamics and solvatochromic effects, which we uncover using a new real-time quantum dynamics approach for extremely large solvated nanodroplets. In particular, we find that a complex interplay of quantum interactions underlies our observations of solute-solvent effects, and simple macroscopic solvatochromic shifts can even be qualitatively different at the microscopic molecular level in these systems. By treating both the solvent and the solute on the same footing at a quantum-mechanical level, we demonstrate that the electron dynamics in these systems are surprisingly complex, and the emergence of many-body interactions underlies the dynamics in these solvated systems.
Download full-text PDF |
Source |
---|---|
http://dx.doi.org/10.1021/acs.jctc.5b01019 | DOI Listing |
Nanomaterials (Basel)
January 2025
Hunan Key Laboratory of Super-Microstructure and Ultrafast Process, School of Physics, Central South University, Changsha 410083, China.
Two-dimensional (2D) layered materials have received much attention due to the unique properties stemming from their van der Waals (vdW) interactions, quantum confinement, and many-body interactions of quasi-particles, which drive their exotic optical and electronic properties, making them critical in many applications. Here, we review our past years' findings, focusing on many-body interactions in 2D layered materials, including phonon anharmonicity, electron-phonon coupling (), exciton dynamics, and phonon anisotropy based on temperature (polarization)-dependent Raman spectroscopy and Photoluminescence (PL). Our review sheds light on the role of quasi-particles in tuning the material properties, which could help optimize 2D materials for future applications in electronic and optoelectronic devices.
View Article and Find Full Text PDFEntropy (Basel)
January 2025
Chula Intelligent and Complex Systems Lab, Department of Physics, Faculty of Science, Chulalongkorn University, Bangkok 10330, Thailand.
Quantum reservoir computing (QRC) has emerged as a promising paradigm for harnessing near-term quantum devices to tackle temporal machine learning tasks. Yet, identifying the mechanisms that underlie enhanced performance remains challenging, particularly in many-body open systems where nonlinear interactions and dissipation intertwine in complex ways. Here, we investigate a minimal model of a driven-dissipative quantum reservoir described by two coupled Kerr-nonlinear oscillators, an experimentally realizable platform that features controllable coupling, intrinsic nonlinearity, and tunable photon loss.
View Article and Find Full Text PDFEntropy (Basel)
January 2025
CeBio-Departamento de Ciencias Básicas, Universidad Nacional del Noroeste Provincia de Buenos Aires (UNNOBA), CONICET, Junin 6000, Argentina.
In this study, we utilize information theory tools to investigate notable features of the quantum degree of mixedness (Cf) in a finite model of interacting fermions. This model serves as a simplified proxy for an atomic nucleus, capturing its essential features in a more manageable form compared to a realistic nuclear model, which would require the diagonalization of matrices with millions of elements, making the extraction of qualitative features a significant challenge. Specifically, we aim to correlate Cf with particle number fluctuations and temperature, using the paradigmatic Lipkin model.
View Article and Find Full Text PDFJ Chem Phys
January 2025
Department of Chemistry, Chicago Center for Theoretical Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, Chicago, Illinois 60637, USA.
Bottom-up coarse-grained (CG) modeling is an effective means of bypassing the limited spatiotemporal scales of conventional atomistic molecular dynamics while retaining essential information from the atomistic model. A central challenge in CG modeling is the trade-off between accuracy and efficiency, as the inclusion of often pivotal many-body interaction terms in the CG force-field renders simulation markedly slower than simple pairwise models. The Ultra Coarse-Graining (UCG) method incorporates many-body terms through discrete internal state variables that modulate the CG force-field according to, e.
View Article and Find Full Text PDFJ Phys Chem Lett
January 2025
Kenneth S. Pitzer Theory Center and Department of Chemistry, University of California, Berkeley, California 94720, United States.
This work constructs an advanced force field, the Completely Multipolar Model (CMM), to quantitatively reproduce each term of an energy decomposition analysis (EDA) for aqueous solvated alkali metal cations and halide anions and their ion pairings. We find that all individual EDA terms remain well-approximated in the CMM for ion-water and ion-ion interactions, except for polarization, which shows errors due to the partial covalency of ion interactions near their equilibrium. We quantify the onset of the dative bonding regime by examining the change in molecular polarizability and Mayer bond indices as a function of distance, showing that partial covalency manifests by breaking the symmetry of atomic polarizabilities while strongly damping them at short-range.
View Article and Find Full Text PDFEnter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!