Bulletin of the American Physical Society
2024 APS March Meeting
Monday–Friday, March 4–8, 2024; Minneapolis & Virtual
Session S25: Hydrogen Bonding Interactions and Dynamics: Water and Aqueous SystemsFocus
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Sponsoring Units: DCP Chair: Santanu Roy, Oak Ridge National Laboratory Room: 101F |
Thursday, March 7, 2024 8:00AM - 8:36AM |
S25.00001: Probing the Primary Solvation Shell of Hydroxide and Observing Spin-Orbit Excited Dipole-Bound Resonances Using Cryogenic Photoelectron Spectroscopy Xue-Bin Wang Invited Speaker: Xue-Bin Wang Size-selective cryogenic photoelectron spectroscopy (cryoPES) coupled with electrospray ionization (ESI) is a powerful experimental technique to investigate electronic structures, energetics, and proton transfers of a wide variety of hydrogen bound clusters. Our latest research includes probing the primary hydration shell of hydroxide and electronic Feshbach resonances of arginine-iodide anion clusters. A key property associated with the behavior of hydroxide, one of the most important ions in aqueous chemistry, is the binding motif in its primary hydration shell. We carried out a joint experimental – theoretical study for hydrated hydroxide clusters OH–(H2O)n (n = 0-6). Our study, based on the first reported photoelectron spectra and high-level ab-initio calculations, determined the primary gas phase hydration shell of hydroxide containing four water molecules, and reconciled a long-standing debate on hydroxide solvation shell between previous IR action spectroscopic data and theory. We demonstrated ‘iodide-tagging’ PES is a sensitive probe for identifying distinct anion binding sites for polar molecules. We spectroscopically distinguished and characterized a plethora of isomers and tautomers of arginine-iodide clusters. We observed the relaxation of spin-orbit excited dipole bound states, known as an electronic Feshbach resonance, for the first time and confirmed the mechanism by which the electrons relax. The Feshbach resonance has a distinct signature directly related to the dipole of the cluster. This has enabled us to differentiate between arginine-iodide cluster isomers that are too large with too many conformers for traditional vibrational spectroscopy approaches. |
Thursday, March 7, 2024 8:36AM - 8:48AM |
S25.00002: Solvation Species of Hydrated Excess Protons in Liquid Water Benjamin P Fingerhut, Sai Vamsikrishna Isukapalli Solvation structures of excess protons in water are highly relevant to electric properties and for an understanding of proton transport in liquids and membranes. We present unprecedented long-time ab-initio molecular dynamics simulations using a state-of-the-art hybrid-meta GGA exchange-correlation functional to simulate the temporal evolution of an excess proton in liquid water. The functional yields excellent results for bulk water and results are compared to the state-of-the-art hybrid GGA functional rev-PBE0-D3. Our simulations suggest that protons in water are predominantly solvated within dimeric water structures and how the dimeric water solvation structure interacts with its closest water neighbor in a H7O3+ unit without persistent proton localization on a single water molecule. The findings are in close agreement with previous reports on water-ACN solvent mixtures [1,2] and unravel microscopic aspects of the asymmetric potential along the proton transfer coordinate observed in nonlinear two-dimensional infrared spectroscopy [3]. |
Thursday, March 7, 2024 8:48AM - 9:00AM |
S25.00003: Hydrogen-bonding structure and dynamics in metal-organic frameworks for water harvesting Francesco Paesani, Ching-Hwa Ho, Hilliary O Frank In the quest to address water scarcity issues, the harvesting of atmospheric water using metal-organic frameworks (MOFs) presents a promising solution. We will present our work on the characterization of hydrogen bonding interactions and dynamics of water in various metal-organic frameworks (MOFs) that exhibit exceptional reversible water uptake capabilities as a function of relative humidity. Integrating molecular dynamics simulations carried out with data-driven many-body potentials and infrared spectroscopy, we unravel the molecular mechanisms that govern the adsorption and pore filling steps. The distinct hydrogen bonding network of confined water within MOFs, contrasting with that of bulk water, plays a crucial role in the water harvesting process. Our findings not only shed light on the fundamental understanding of hydrogen bonding dynamics in confined environments but also pave the way for enhancing water harvesting technologies employing MOFs. |
Thursday, March 7, 2024 9:00AM - 9:12AM |
S25.00004: Abstract Withdrawn
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Thursday, March 7, 2024 9:12AM - 9:24AM |
S25.00005: Combined Classical and AIMD Simulations for Understanding the Extraction Mechanism of Li/Na/K Ions Using p-toluene Sulfonate/4-(trifluoromethyl) Benzene Sulfonate in Aqueous Medium Akshay Malik, Arun Yethiraj The demand for environmentally sustainable and easily transportable energy sources in various industries, such as electrical, automotive, and aerospace, has driven continuous attention of the research communities towards lithium (Li) ion-operated batteries. The conventional industrial method used for Li-ion extraction involves pumping mechanisms to bring Li brine to the surface, which is subjected to chemical treatment, facilitating the segregation of the metallic component from the liquid phase. This process suffers many disadvantages, such as groundwater contamination due to chemicals, and can potentially result in decreased water availability. Therefore, to overcome these drawbacks, scientists have recently discovered that para-toluene sulfonate (PTS) can be used for Li recovery and can be potentially exploited for Li-ion extraction. In the present study, we have carried out combined classical and ab-initio molecular dynamics simulations focusing on the interactions of various ions (Li, Na, K) with PTS and 4-(trifluoromethyl) Benzene Sulfonate (TBS) in water. From the analysis of radial distribution functions and potential of mean force, we found that the sulfur group present on both PTS and TBS actively interacts with Li-ion followed by Na and then K. The ion-sulfur interaction can be attributed to the efficient extraction of Li from the Li-PTS and Li-TBS aqueous solutions. We believe that tuning the side groups on the benzene ring may result in increasing the extraction efficiency. |
Thursday, March 7, 2024 9:24AM - 10:00AM |
S25.00006: Sub-picosecond hydrogen-bond anticorrelations of water Invited Speaker: Johannes Hunger Liquid water is traditionally viewed to form a distorted tetrahedral hydrogen-bond (H-bond) network. Yet, this rather symmetric structure has been challenged by x-ray [1] and computer simulation [2] studies. These studies have revealed a highly asymmetric H-bond geometry resulting in chain- or ring-like configurations, relevant to understanding the various anomalies of water [2]. Here, we characterize the inherent H-bond symmetry of water by studying water diluted in dimethylformamide with two-dimensional infrared (2D-IR) spectroscopy. We characterize the distribution of local H-bonds via coupling and broadening of the OD stretching vibrations of HOD and D2O. Experiments on the coupled OD stretch oscillators of D2O – the asymmetric and symmetric stretching modes – reveal a markedly narrower inhomogeneous linewidth for the coupled modes as compared to the uncoupled vibration of HOD. Frequency maps obtained from density functional theory calculations show that these differing linewidths can be explained by anti-correlated H-bond strengths of water. This anti-correlation is confirmed by the cross-peaks in the 2D-IR spectra. Yet, our results indicate that this anti-correlation is rather short-lived (few 100s of fs) and a mere results of the H-bond potential energy landscape. In fact, experiments on urea dissolved in dimethylsulfoxide provide evidence for a similar asymmetry of urea’s N-H H-bonds. As such, our results suggest that asymmetric H-bonding is an inherent feature of XH2 groups (X=N,O) and the structural consequences are rapidly smeared out at ambient conditions. |
Thursday, March 7, 2024 10:00AM - 10:12AM |
S25.00007: Photomolecular Effect: Visible Light Interaction with Air-Water Interface Guangxin Lv, Yaodong Tu, James H Zhang, Gang Chen Despite that water is nearly transparent to visible light, we hypothesize that visible light can directly cleave off water molecular clusters at the air-water interface via a process we call photomolecular effect. We had used this hypothesis to explain why some of the past experiments on solar-interfacial evaporation from porous materials can exceed the apparent thermodynamic limit, calculated based on the energy of the incident light and latent and sensible heat required for water evaporation. In this work, we show that this process happens at the air-water interface by measuring the dependence of photomolecular effect on the wavelength, the angle of incidence, and the polarization of the incident light. We further support the photomolecular effect by measuring the temperature response in water and the vapor phases, Raman and infrared spectroscopy, and multiple pump-probe measurements. |
Thursday, March 7, 2024 10:12AM - 10:24AM |
S25.00008: Tensor Sensitivity and long-range Coulomb interactions improve the accuracy and extensibility of Machine Learning Potentials Sakib Matin, Bowen Han, Justin Smith, Alice Allen, Nicholas E Lubbers, Adela Habib, Nikita Fedik, Xinyang Li, Richard A Messerly, Ben T Nebgen, Ying Wai Li, Sergei Tretiak, Kipton Barros Large-scale atomistic simulations using fully ab initio forces remains an open problem due to the high costs of quantum chemistry solvers. Machine learning potentials offer an efficient alternative to direct quantum molecular dynamics. Many neural network architectures for machine learning potentials have relied only on short range interatomic distances. To overcome this simplification, we present the Hierarchically Interacting Particle Neural Network with Tensor Sensitivity, which processes geometric information via the full pairwise displacement vectors between nearby atoms, and Coulomb interaction extensions, which allow for physically constrained long-range interactions between atoms. We refer to this model as HIP-NN-TS-Coulomb. We trained on a data set of small water clusters, containing up to 14 molecules, and computed at the second order Møller–Plesset level of theory. When applied to the large scale simulation of liquid water, the model accurately reproduces properties such as radial distribution functions, diffusion constants, and density over a wide range of temperatures. |
Thursday, March 7, 2024 10:24AM - 10:36AM |
S25.00009: Structure and Dynamics of Water Ice Ih Tianran Chen, David A Tennant Water ice Ih is a non-periodic system with proton disorder due to the large number of possible configurations of hydrogen atoms that follow the ice rule. Understanding the structure and dynamics of water ice Ih is important for various scientific and technological applications. In this work, we measured the static and dynamic structure factors of a single crystal ice Ih at different temperatures using elastic and inelastic neutron scattering techniques. We showed that our static structure factors could be well explained by the Fourier transform of the simulated spatial configurations of water ice. |
Thursday, March 7, 2024 10:36AM - 10:48AM |
S25.00010: What is medium-density amorphous ice? Ingrid de Almeida Ribeiro, Debdas Dhabal, Suvo Banik, Arnab Neogi, Subramanian K Sankaranarayanan, Valeria Molinero Polyamorphism in water, characterized by the coexistence of two primary amorphous forms, low-density amorphous (LDA) and high-density amorphous (HDA), each associated with distinct liquid states, low-density liquid (LDL) and high-density liquid (HDL), has long been an intriguing phenomenon. Recent research has unveiled a new dimension of complexity with the discovery of medium density amorphous (MDA) ice, raising questions about its relationship with LDA, HDA, and its connection to the liquid state (Rosu-Finsen et al., Science 2023, 379, 474-478). In this study, we employ molecular dynamics simulations to investigate the formation of MDA. Our analysis reveals that MDA exhibits properties that bridge the characteristics of both the liquid phase and HDA, yet it possesses distinct attributes and a unique formation mechanism. These observations firmly establish MDA as another distinct phase of water. |
Thursday, March 7, 2024 10:48AM - 11:00AM |
S25.00011: A Continuum of Amorphous Ices between Low- and High-Density Amorphous Ice Nicolas Giovambattista, Ali H Eltareb, Gustavo Lopez Amorphous ices at approximately P<1 GPa are usually classified as low-density or high-density amorphous ice (LDA and HDA) with densities ρ~0.94 g/cc and ρ~1.15 g/cc, respectively. However, a recent experiment crushing hexagonal ice (ball-milling) produced a medium-density amorphous ice (MDA, ρ~1.06 g/cc) adding complexity to our understanding of amorphous ice and supercooled water. Motivated by the discovery of MDA, we perform computer simulations where amorphous ices are produced by isobaric cooling and isothermal compression/decompression. We show that, depending on the pressure employed, isobaric cooling can generate a continuum of amorphous ices with densities that expand in between those of LDA and HDA (briefly, intermediate amorphous ices, IA). In particular, the IA generated at P ≈ 125 MPa has a remarkably similar density and average structure as MDA. Our results imply that MDA is not unique, and that it is not impossible that MDA may be related to liquid water. By using the potential energy landscape (PEL) formalism, we provide an intuitive understanding of the nature of LDA, HDA, and the IA generated at different pressures. In this view, LDA and HDA occupy specific and well-separated regions of the PEL; the IA prepared at P = 125 MPa is located in the intermediate region of the PEL that separates LDA and HDA. |
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