Article
Chemistry, Physical
Tetsuyuki Takayama, Kota Kishi, Takuhiro Otosu, Takuma Yagasaki, Shoichi Yamaguchi
Summary: This study presents an experimental and theoretical analysis of the Raman spectra of ice VI at high pressure, demonstrating the applicability and accuracy of molecular dynamics simulations and spectroscopic maps. The results show that the theoretical Raman spectra match well with the experimental data, providing insights into the site dependence of the OH-stretch frequency in ice VI.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Shoichi Yamaguchi, Tetsuyuki Takayama, Yuki Goto, Takuhiro Otosu, Takuma Yagasaki
Summary: The chi(2) spectrum of the water surface has been measured experimentally and theoretically reproduced, shedding light on the effects of intramolecular, intermolecular, and Fermi resonance couplings on the OH-stretch vibrational spectra of water at both the surface and in the bulk.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Spectroscopy
Senri Ishihara, Tetsuyuki Takayama, Miyuki Sakaguchi, Takuhiro Otosu, Takuma Yagasaki, Yoshiharu Suzuki, Shoichi Yamaguchi
Summary: This study presents an investigation of Raman spectroscopy of isotopically pure and diluted amorphous and crystalline ices at 30 K, using both experimental and theoretical approaches. The comparison between experimental and calculated spectra confirms the reliability of the molecular dynamics simulation method and allows for detailed spectral assignments and analysis.
JOURNAL OF RAMAN SPECTROSCOPY
(2022)
Article
Chemistry, Physical
Romain Botella, Andrey A. Kistanov
Summary: To date, vibrational simulation results have been mainly used as experimental support rather than predictive tools due to the discreteness of the simulated vibrational modes caused by quantization. In this study, we propose a method to combine outputs from ab initio simulations, such as the phonon density of states surrogate and peak intensities, to enable comparison with experimental data using machine learning. This work opens up possibilities for using simulated vibrational spectra to identify materials with defined stoichiometry, allowing for the separation of genuine vibrational features from morphological and defect-induced signals.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Engineering, Chemical
Wenzhu Xia, Xuewen Cao, Yongqi Xu, Jiang Bian
Summary: This study summarizes the limitations of Gibbs' formula in describing interfacial adsorption and proposes a new isothermal adsorption formula based on thermodynamic equilibrium. Through this approach, a quantitative description of interface adsorption can be achieved, and the relationship between surface concentration and surface tension can be elucidated. The accuracy of the model is validated through the study of the numerical curve of anionic surfactant sodium dodecyl sulfate, and an algorithm for calculating the surface area of the fluctuating interface is established.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Chemistry, Physical
Tongwei Zhang, Jie Wu, Xingjian Lin
Summary: In this study, numerical simulations and theoretical analyses were conducted to investigate the dynamic behaviors of droplets impacting on a wettability-patterned surface. The results showed that arc-shaped hydrophilic patterns are more suitable for droplet lateral motion. The study established general rules between patterns and droplet lateral motion, and proposed design principles for hydrophilic patterns.
Article
Chemistry, Multidisciplinary
Alexandre Poirier, Antonio Stocco, Romain Kapel, Martin In, Laurence Ramos, Amelie Banc
Summary: The study investigated the adsorption process of sunflower protein extract at two air-water and oil-water interfaces, revealing a three-step mechanism. Initially, a diffusion-limited adsorption of proteins at interfaces occurs, followed by the formation of a three-dimensional saturated monolayer of proteins, and finally a thick layer expanding in the aqueous phase. The study also found that the adsorption mechanisms of proteins exhibit significant divergences at longer adsorption times.
Article
Chemistry, Physical
Subhadip Roy, Jahur Alam Mondal
Summary: Research shows that ions have a strong correlation with the structure of hydrogen bonding at the air/water interface and in bulk water. Specifically, structure-breaking anions decrease hydrogen bonding at the interface, while structure-making anions have the opposite effect. None of the electrolytes studied significantly affect the orientation of water molecules at the interface.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Multidisciplinary
Ryoji Kusaka, Satoshi Nihonyanagi, Tahei Tahara
Summary: The study directly observed a photochemical reaction occurring at the air-water interface using ultrafast phase-sensitive interface-selective nonlinear vibrational spectroscopy. The results showed that the reaction rate at the water surface is 10^4 times faster than in the bulk aqueous phase, indicating significant differences in photochemical reactions between water interfaces and bulk water.
Article
Multidisciplinary Sciences
Hongxia Hao, Itai Leven, Teresa Head-Gordon
Summary: Reaction rates of common organic reactions can significantly increase by several orders of magnitude in aqueous microdroplets compared to bulk solution. However, the reasons for this rate acceleration are still poorly understood. By studying the electric field distributions at the air-water interface, it has been found that the electric field alignments along free O-H bonds at the surface are on average around 16 MV/cm larger than those in the interior of the water droplet. This difference in electric field distribution may contribute to the enhanced surface reactivity observed in microdroplets.
NATURE COMMUNICATIONS
(2022)
Article
Environmental Sciences
Wenjing Zhang, Shengyu Wu, Yunqi Qin, Shuo Li, Liancheng Lei, Simiao Sun, Yuesuo Yang
Summary: This study investigated the transport and retention of viruses in the vadose zone, focusing on the effects of moisture content and ionic strength on virus behavior at different interfaces. Results showed that solid-water interfaces (SWIs) and air-water interfaces (AWIs) play a significant role in virus retention, with moisture content and ionic strength influencing the mechanisms of virus straining and attachment. The findings have important implications for modeling and predicting virus transport in soil under various environmental conditions.
ENVIRONMENTAL POLLUTION
(2021)
Article
Chemistry, Multidisciplinary
Jacopo Vialetto, Sergii Rudiuk, Mathieu Morel, Damien Baigl
Summary: This study presents a generic method for optically reconfigurable colloidal crystals at the air/water interface and reveals a new mechanism for controlling lattice properties using light. The photoreversible melting process is driven by thermocapillary stress and increased particle diffusivity, allowing for dynamic patterns and multiresponsive assembly to be achieved with light and magnetic stimuli.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Environmental Sciences
Leslie J. Saunders, Jose L. Rodriguez-Gil, Sawyer S. Stoyanovich, Linda E. Kimpe, Mark L. Hanson, Bruce P. Hollebone, Diane M. Orihel, Jules M. Blais
Summary: Petroleum oil spills in water can impede the volatilization process and increase the persistence of chemicals in water. This study assesses the impact of diluted bitumen spills on the volatilization of sulfur hexafluoride (SF6) in a lake, and finds that the volatilization rate of SF6 significantly decreases with increasing spill cover.
Article
Engineering, Environmental
Wenzhang Tian, Jun Yang, Wen-Qing Xu, Lin Lian, Xia-Wen Qiu, Xiao Liang, Chen-Chou Wu, Xiangjun Gong, Guangzhao Zhang, Lian-Jun Bao, Eddy Y. Zeng
Summary: Quantifying chemical transfer across the air-water interface is crucial for understanding global geochemical processes. This study presents a fluorescence optical system that visualizes the formation of the air-water microlayer and quantifies the diffusion flux using pyrene. The results show that the air-water microlayer consists of a surface microlayer in water and a diffusion layer in air.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2023)
Article
Engineering, Environmental
Kejian Li, Wenbo You, Wei Wang, Kedong Gong, Yangyang Liu, Longqian Wang, Qiuyue Ge, Xuejun Ruan, Jianpeng Ao, Minbiao Ji, Liwu Zhang
Summary: This study demonstrates that the photodecomposition of perfluorooctanoic acid (PFOA) can be significantly accelerated by carrying out the process in microdroplets. The abundance of the air-water interface in microdroplets promotes the decomposition of PFOA, resulting in higher removal rates. The method shows high performance and universality in actual water matrices.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2023)
Editorial Material
Chemistry, Physical
Sobhan Sen, Anindya Datta, Tahei Tahara
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Physical
Munetaka Iwamura, Rina Urayama, Airi Fukui, Koichi Nozaki, Li Liu, Hikaru Kuramochi, Satoshi Takeuchi, Tahei Tahara
Summary: The excited-state dynamics of [Au(CN)(2)(-)] oligomers were investigated using femtosecond time-resolved absorption and emission measurements. The oscillations in the temporal profiles of the absorption signals were observed, indicating the coherent wavepacket motion of the excited-state oligomers. Fourier transforms of the oscillations provided 2D plots, allowing for determination of the peak wavelength of the excited-state absorption of different oligomers.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Harison Rozak, Satoshi Nihonyanagi, Anton Myalitsin, Subhadip Roy, Mohammed Ahmed, Tahei Tahara, Izabela I. Rzeznicka
Summary: The receptor binding domain (RBD) of spike proteins plays a crucial role in the attachment of SARS-CoV-2 to ACE2. Mutations in the spike RBD, such as N501Y, result in higher transmissibility by enhancing the binding with negatively charged ACE2. This study investigates the adsorption of ACE2 and spike (N501Y) RBD at a lipid/water interface and provides insights into their interaction in a lipid matrix.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Physical
Achintya Kundu, Shoichi Yamaguchi, Tahei Tahara
Summary: The local pH at the interfaces between neutral and charged lipids in biomembranes is crucial for their structure and function. Previous studies have shown that the local pH at charged lipid interfaces is determined by the charge of the lipid. This study uses HD-ESFG spectroscopy to investigate the local pH at neutral lipid interfaces and finds that it is higher than in bulk water for nonionic lipids, and lower for zwitterionic lipids.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Physical
Atsushi Sayama, Satoshi Nihonyanagi, Yasuhiro Ohshima, Tahei Tahara
Summary: Superconcentrated electrolyte solutions can stabilize solvent molecules in high-voltage rechargeable batteries, but the mechanism behind this stabilization is not fully understood. This study investigated the interfaces of platinum electrodes and acetonitrile solutions containing dilute and superconcentrated lithium bis-(trifluoromethanesulfonyl)-imide (LiTFSI) using in situ and ex situ vibrational spectroscopy techniques. The results showed that the electrode interfaces have different structures in the two solutions, with acetonitrile decomposing in the dilute solution and the TFSI- anion decomposing in the superconcentrated solution.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Tahei Tahara, Pardeep Kumar, Hikaru Kuramochi, Satoshi Takeuchi
Summary: Metal nanoparticles can transfer absorbed photon energy to adsorbates, making them highly potential in light-harvesting applications. However, the ultrafast plasmon-driven dynamics of adsorbates on metal nanoparticles are not well understood. In this study, we used TR-SE-ISRS to investigate the ultrafast plasmon-driven processes of trans-1,2-bis(4-pyridyl)ethylene (BPE) adsorbed on gold nanoparticle assemblies (GNAs). Our results revealed that photoexcitation of the localized surface plasmon resonance (LSPR) band of GNAs altered the chemical interaction between BPE and GNAs on an ultrafast timescale.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Feng Wei, Shu-hei Urashima, Satoshi Nihonyanagi, Tahei Tahara
Summary: In this study, the vibrational spectra of the silica/water interface were measured in a wide pH range. The spectra were decomposed into the diffuse Gouy-Chapman layer and the compact Stern layer, allowing for quantitative analysis of each layer. The surface charge density and pKa value of the silica/water interface were evaluated, providing a molecular-level understanding of the electric double layer at the interface.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Pankaj Seliya, Mischa Bonn, Maksim Grechko
Summary: This study focuses on the interaction between quantum-mechanical systems and fluctuating thermal environments, providing insights into their coupling through a combined experimental and theoretical approach. The experimental part involves spectroscopy measurements to directly observe the coupling between quantum oscillators and low-frequency modes. The theoretical part introduces a mixed quantum-classical formalism to describe the sample response. This approach enables the quantitative and mode-specific analysis of coupled quantum and classical dynamics in complex chemical systems.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Meeting Abstract
Biophysics
Arpan Dey, Aditi Verma, Bidyut Sarkar, Uchit Bhaskar, Mamata Kallianpur, Vicky Visvakarma, Kanchan Garai, Odity Mukherjee, Kunihiko Ishii, Tahei Tahara, Sudipta Maiti
EUROPEAN BIOPHYSICS JOURNAL WITH BIOPHYSICS LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Feng Wei, Shu-hei Urashima, Satoshi Nihonyanagi, Tahei Tahara
Summary: The investigation of the water structure at the silica/water interface is crucial, and in this study, the interface-selective vibrational spectra were measured using vibrational sum-frequency generation spectroscopy. Through analysis, the spectra were separated into the diffuse Gouy-Chapman layer and the compact Stern layer, allowing for a quantitative understanding of each spectral component. The salt concentration dependence of the spectra and the pH-dependent changes were also analyzed, providing valuable insights into the electric double layer at the silica/water interface.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Pardeep Kumar, Hikaru Kuramochi, Satoshi Takeuchi, Tahei Tahara
Summary: Metal nanoparticles have the potential to transfer absorbed photon energy to adsorbates in light-harvesting applications. However, the ultrafast plasmon-driven dynamics of adsorbates on metal nanoparticles are not well understood. In this study, we investigated the ultrafast plasmon-driven processes of trans-1,2-bis(4-pyridyl)ethylene (BPE) adsorbed on gold nanoparticle assemblies (GNAs) using time-resolved surface-enhanced impulsive stimulated Raman spectroscopy (TR-SE-ISRS). Our results show that photoexcitation of the localized surface plasmon resonance (LSPR) band of GNAs alters the chemical interaction between BPE and GNAs on an ultrafast time scale.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Nathaniel. P. Gallop, Dmitry R. Maslennikov, Navendu Mondal, Katelyn P. Goetz, Zhenbang Dai, Aaron M. Schankler, Woongmo Sung, Satoshi Nihonyanagi, Tahei Tahara, Maryna I. Bodnarchuk, Maksym V. Kovalenko, Yana Vaynzof, Andrew M. Rappe, Artem A. Bakulin
Summary: Vibrational control through optical stimulation of structural dynamics can effectively reduce non-radiative recombination and voltage losses in perovskite solar cells.
Article
Chemistry, Physical
Yongkang Wang, Yuki Nagata, Mischa Bonn
Summary: Graphene, as a transparent two-dimensional conductive electrode, has brought new perspectives to electrochemical systems. The substrate plays a crucial role in determining the water organization and wetting behavior of graphene. Surface-specific spectroscopy study reveals that the charging of graphene is decoupled from the charging of its substrate.
FARADAY DISCUSSIONS
(2023)