Article
Chemistry, Physical
Konstantin S. Smirnov
Summary: Classical molecular dynamics simulations were used to investigate the structural organization and vibrational sum-frequency generation spectra of water on crystalline and amorphous neutral silica surfaces. The simulations revealed that the structure of the interfacial layer was influenced by the surface morphology and density of surface OH groups. The presence of ions in the liquid phase did not significantly affect the water-silanol H-bond network and interfacial layer structure.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Review
Chemistry, Physical
Jia-Bo Le, Jun Cheng
Summary: In this article, recent progress in modeling electrified metal/water interfaces using ab initio molecular dynamics (AIMD) is reviewed, focusing on the relationship between the structure of electric double layers (EDLs) and the dielectric property of interface water, as well as the variations in the structure of interface water on metal electrodes under different potential conditions. The potential-dependent behavior of chemisorbed water on Pt(111) surface and its correlation with the differential Helmholtz capacitance peak observed by experiment are also elucidated, providing insights for future development in ab initio modeling of electrochemical interfaces.
CURRENT OPINION IN ELECTROCHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Yongkang Wang, Takakazu Seki, Xuan Liu, Xiaoqing Yu, Chun-Chieh Yu, Katrin F. Domke, Johannes Hunger, Marc T. M. Koper, Yunfei Chen, Yuki Nagata, Mischa Bonn
Summary: We used HD-SFG spectroscopy to directly probe the interfacial water at the graphene electrode supported on CaF2. The observed phase transition-like variations in the HD-SFG spectra were not due to the charging/discharging of graphene, but rather the CaF2 substrate through pseudocapacitive process. The potential-dependent spectra were similar to the pH-dependent spectra, indicating that the pseudocapacitive behavior was associated with a local pH change induced by water dissociation between CaF2 and graphene.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Multidisciplinary Sciences
Zifan Ye, Aleksander Prominski, Bozhi Tian, Giulia Galli
Summary: This study focuses on investigating the behavior of hydrogenated Si surfaces in contact with water, with applications in transient electronics and photoelectrochemical modulation of biological cells and tissues. By using first principles molecular dynamics simulations and experimental measurements, they found that voltage-dependent capacitive currents are present at the Si/water interface, while Faradaic currents are weakly dependent on the applied bias due to surface defects in newly prepared samples.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Physical
Alexander P. Fellows, Vasileios Balos, Ben John, Alvaro Diaz Duque, Martin Wolf, Martin Thaemer
Summary: Second-order nonlinear spectroscopy is an important technique for studying interfacial systems due to its ability to analyze molecular structures and interactions. This study demonstrates that information about depth distributions, molecular orientation, and local dielectric properties can be extracted from the phase of the measured signal using multiple nonlinear pathways. This novel information can be correlated to characteristic vibrational spectra, enabling advanced sample characterization and analysis of interfacial molecular structures.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Shyam Parshotam, Wentong Zhang, Benjamin Rehl, Akemi Darlington, Md. Delwar H. Sikder, Alex Brown, Julianne M. Gibbs
Summary: Isolating the contribution of silica in second harmonic generation (SHG) studies at the silica/water interface remains a challenge. Here, we compare SHG intensities with zeta potentials and vibrational sum frequency generation (SFG) intensities to understand the silica contribution in SHG measurements. The results suggest a significant pH-dependent increase in the silica contribution, which can interfere constructively or destructively with water. The study also demonstrates the direct sensitivity of SHG to surface charging, indicating its potential as a powerful tool in studying other mineral oxides.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Huda S. AlSalem, Sven P. K. Koehler
Summary: The ultrafast dephasing times of vibrational quanta in functional groups bound to graphene were measured using time-resolved sum-frequency generation spectroscopy. Decays times of 0.8 and 1.4 ps were observed for vibrational stretches in phenyl groups attached to graphene or gold, respectively, while much faster decay times of 0.3 ps were measured for vibrations of the bond connecting H atoms to graphene in hydrogenated graphene. This difference in decay times may be due to coupling between the C-H stretch and either the two-dimensional mode of graphene or nonadiabatic coupling to electrons excited by the upconversion laser pulse.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Shoichi Yamaguchi, Tetsuyuki Takayama, Takuhiro Otosu
Summary: In this study, we evaluated the performance of TIP4P-type models at the liquid water surface using HD-SFG spectroscopy. The results showed that these models were able to better reproduce certain key features at the water surface compared to some polarizable models in the literature.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Review
Chemistry, Multidisciplinary
Ricardo Garcia
Summary: The properties of graphite, few layer, and 2D materials have led to various applications in biosensing, energy storage, and water desalination. This review discusses the recent experimental and theoretical advancements in understanding the structure of water on these materials' surfaces, revealing different layer structures under different conditions and the absence of water molecules near aged material surfaces.
Article
Multidisciplinary Sciences
Deepak Ojha, Thomas D. Kuehne
Summary: In this study, a simple recipe based on narrowband IR pump and broadband vSFG probe technique was used to computationally obtain the two-dimensional vSFG spectrum of water molecules at the air-water interface. The study demonstrated that the vibrational spectral dynamics of the free OH bond is faster than that of the bonded OH mode at the interface.
SCIENTIFIC REPORTS
(2021)
Article
Chemistry, Physical
Thaddeus W. Golbek, Kris Strunge, Adam S. Chatterley, Tobias Weidner
Summary: The adsorption of proteins on nanoparticles differs from that on planar surfaces due to the Coulombic forces between peptides inside the particles.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Daria Maltseva, Ragnheidur Gudbrandsdottir, Goenuel Kizilsavas, Dominik Horinek, Grazia Gonella
Summary: The study investigates the behavior of the LK alpha 14 peptide in water/ethanol mixtures using a combination of experimental techniques and molecular dynamics simulations. It is found that ethanol significantly impacts both the conformation and location of the peptide. At low ethanol content, the peptide tends to reside at the air-solution interface, while at higher ethanol content, it adopts a stable alpha-helical conformation in the bulk solution.
Article
Chemistry, Physical
Chih-Kai Lin, Qian-Rui Huang, Michitoshi Hayashi, Jer-Lai Kuo
Summary: The study focused on the vibrational spectra of methylammonium ion in organic-inorganic halide perovskites, showing its sensitive and complex features in the 3 μm region. The simulated results were consistent with experimental observations, aiding in interpretation and analysis of experimental data, expanding the research methodology.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Carolyn J. Moll, Jan Versluis, Huib J. Bakker
Summary: Urea molecules at charged aqueous interfaces exhibit unique solvation properties, with the ability to serve as a probe for local electric fields. The addition of ionic surfactants induces specific vibrational bands in HD-VSFG spectra, providing insights into the orientation of urea molecules at the interface.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Daniel Konstantinovsky, Elsa C. Y. Yan, Sharon Hammes-Schiffer
Summary: The chemistry of interfaces is different from that of the bulk. Calculation of interfacial properties depends on the definition of the interface, which can yield ambiguous results. Voronoi tessellation provides a method to explicitly define interfaces and boundaries in molecular systems. This method has broad applications in spectroscopy and can provide insights into various systems.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Optics
Antoine Boniface, Mickael Mounaix, Baptiste Blochet, Hilton B. De Aguiar, Fabien Quere, Sylvain Gigan
Summary: This study demonstrates the manipulation of ultrashort light pulses through strongly scattering media using a multi-spectral transmission matrix (MSTM), showing how to engineer the spatial and spectral characteristics of the focused beam's point-spread function. Experimental results showcase the versatility of the technique as an alternative to simultaneous spatial and temporal focusing, with potential applications in multiphoton microscopy.
Article
Chemistry, Physical
Jean-Francois Olivieri, Damien Laage, James T. Hynes
Summary: The study found that electron transfer reactions in aqueous solutions confined between graphene sheets can occur faster than in bulk due to a reduction in solvent reorganization energy at the interface. However, this reduction is attributed to the partial desolvation of ions involved in the electron transfer by the graphene sheet, rather than a reduction in local dielectric constant.
Article
Optics
Joseph Rosen, Hilton B. de Aguiar, Vijayakumar Anand, YoonSeok Baek, Sylvain Gigan, Ryoichi Horisaki, Herve Hugonnet, Saulius Juodkazis, KyeoReh Lee, Haowen Liang, Yikun Liu, Stephan Ludwig, Wolfgang Osten, YongKeun Park, Giancarlo Pedrini, Tushar Sarkar, Johannes Schindler, Alok Kumar Singh, Rakesh Kumar Singh, Guohai Situ, Mitsuo Takeda, Xiangsheng Xie, Wanqin Yang, Jianying Zhou
Summary: In recent years, the rapid development of chaos-inspired imaging technologies, consisting of non-invasive and invasive directions, has led to faster and smarter imaging capabilities. Non-invasive imaging through scattering layers has achieved significant progress, while invasive imaging exploits chaos to achieve special imaging characteristics and increase dimensionalities beyond the limits of conventional imagers. This roadmap presents the current and future challenges in both invasive and non-invasive imaging technologies.
APPLIED PHYSICS B-LASERS AND OPTICS
(2022)
Article
Chemistry, Physical
Zeke A. Piskulich, Damien Laage, Ward H. Thompson
Summary: Recent advancements in the calculation of activation energies have provided new insights into the dynamical time scales of liquid water. This Perspective examines the central role of hydrogen-bond exchanges in the rearrangement of water's hydrogen-bond network, while also discussing the contributions of other motions to dynamical time scales and activation energies. Progress on outstanding challenges such as non-Arrhenius effects and activation volumes is detailed, along with directions for future investigations.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Chemistry, Physical
Axel Gomez, Zeke A. Piskulich, Ward H. Thompson, Damien Laage
Summary: This study investigates the molecular mechanism of water diffusion through molecular dynamics simulations and analytic modeling. The researchers establish a quantitative connection between the water diffusion coefficient and hydrogen-bond jump exchanges, and provide an explanation for the coupling between translational, rotational, and hydrogen-bond dynamics in liquid water.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Optics
Bingxin Tian, Bernhard Rauer, Antoine Boniface, Jun Han, Sylvain Gigan, Hilton B. de Aguiar
Summary: In this study, we demonstrate chemically selective energy deposition behind a scattering medium by combining prior information on the chemical's spectrum with the measurement of a spectrally resolved Raman speckle as a feedback mechanism for wavefront shaping. We achieve unprecedented sixfold signal enhancement in an epi-geometry, realizing targeted energy deposition and focusing on individual Raman active particles.
Article
Multidisciplinary Sciences
Lei Zhu, Fernando Soldevila, Claudio Moretti, Alexandra d'Arco, Antoine Boniface, Xiaopeng Shao, Hilton B. de Aguiar, Sylvain Gigan
Summary: The authors demonstrate a method for non-invasive fluorescence imaging behind scattering layers that extends beyond the optical memory effect. By demixing speckle patterns emitted by a fluorescent object using matrix factorization and fingerprint-based reconstruction, they achieve imaging with a larger field of view. Experimental validation confirms the efficiency and robustness of the method across various fluorescent samples.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Miguel de la Puente, Rolf David, Axel Gomez, Damien Laage
Summary: The acidity at the air-water interface decreases compared to the bulk, but is higher below the interface. This has important implications for environmental and biochemical processes.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Optics
Sylvain Gigan, Ori Katz, Hilton B. de Aguiar, Esben Ravn Andresen, Alexandre Aubry, Jacopo Bertolotti, Emmanuel Bossy, Dorian Bouchet, Joshua Brake, Sophie Brasselet, Yaron Bromberg, Hui Cao, Thomas Chaigne, Zhongtao Cheng, Wonshik Choi, Tomas Cizmar, Meng Cui, Vincent R. Curtis, Hugo Defienne, Matthias Hofer, Ryoichi Horisaki, Roarke Horstmeyer, Na Ji, Aaron K. LaViolette, Jerome Mertz, Christophe Moser, Allard P. Mosk, Nicolas C. Pegard, Rafael Piestun, Sebastien Popoff, David B. Phillips, Demetri Psaltis, Babak Rahmani, Herve Rigneault, Stefan Rotter, Lei Tian, Ivo M. Vellekoop, Laura Waller, Lihong Wang, Timothy Weber, Sheng Xiao, Chris Xu, Alexey Yamilov, Changhuei Yang, Hasan Yilmaz
Summary: In the last decade, various tools such as wavefront shaping and computational methods have been developed to understand and control the propagation of light in complex mediums. This field has revolutionized the possibility of diffraction-limited imaging at depth in tissues, and a vibrant community is actively working on it.
JOURNAL OF PHYSICS-PHOTONICS
(2022)
Article
Optics
Bernhard Rauer, Hilton B. de Aguiar, Laurent Bourdieu, Sylvain Gigan
Summary: This study demonstrates scattering correcting wavefront shaping using a simple continuous optimization algorithm to improve the performance of three-photon microscopy in deep tissue imaging. The research shows the ability to focus and image behind scattering layers and explores convergence trajectories for different sample geometries and feedback non-linearities. Additionally, a novel fast phase estimation scheme is presented for imaging through a mouse skull.
Article
Physics, Multidisciplinary
Nicolas Bolik-Coulon, Olivier Languin-Cattoen, Diego Carnevale, Milan Zachrdla, Damien Laage, Fabio Sterpone, Guillaume Stirnemann, Fabien Ferrage
Summary: Nuclear magnetic relaxation is commonly used for studying protein dynamics, but the model-free approach falls short when it comes to describing large carbon-13 relaxation datasets in protein side chains. To overcome this limitation, molecular dynamics simulations are employed to design explicit models of motion and solve Fokker-Planck diffusion equations, resulting in improved agreement with relaxation data, mechanistic insight, and a direct linkage to configuration entropy.
PHYSICAL REVIEW LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Miguel de la Puente, Damien Laage
Summary: Acidity is a crucial factor in determining the chemical reactivity of atmospheric aqueous aerosols and water microdroplets used for catalysis. This study combines density functional theory-based molecular simulations with neural networks and analytic models to investigate the acidity of droplets and thin films in the size range from nanometers to micrometers. The results reveal that the acidity is controlled by the properties of the air-water interface as well as the surface-to-volume ratio, and that there are concentration gradients of hydronium and hydroxide ions at the interface. These findings have implications for understanding chemical reactivity in atmospheric aerosols and catalysis in aqueous microdroplets.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Jean-Francois Olivieri, James T. Hynes, Damien Laage
Summary: The dynamics of water at interfaces between an electrode and an electrolyte play a crucial role in the transportation of redox species and the kinetics of charge transfer reactions. In this study, molecular dynamics simulations were used to investigate the water dynamics at the interface between aqueous NaCl solutions and graphene electrodes, and the effects of ion concentration and electrode potential were examined. The results showed that water dynamics exhibited asymmetric behavior, slowing down at positively charged electrodes and accelerating at negatively charged electrodes. The behavior was mainly determined by the electrode potential at negative potentials, while it was influenced by both ion-water and electrode-water interactions at positive potentials.
FARADAY DISCUSSIONS
(2023)
Article
Chemistry, Physical
Axel Gomez, Zeke A. Piskulich, Ward H. Thompson, Damien Laage
Summary: This study uses molecular dynamics simulations and analytical modeling to determine the molecular mechanism of water diffusion, establishing a quantitative relationship between the water diffusion coefficient and hydrogen-bond jump exchanges. It explains the different temperature dependences of dynamics and discusses the implications for water diffusion in supercooled conditions and water transport in complex aqueous systems.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)