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
Stephanie E. Sanders, Ashley M. Stingel, Poul B. Petersen
Summary: Phase sensitive and heterodyne-detected sum-frequency generation spectroscopy provides the ability to separate the nonlinear susceptibility into real and imaginary components. It also offers information about the absolute orientation of molecules at interfaces and produces a linear absorptive spectrum that can be easily decomposed into different spectral components. However, maintaining both phase accuracy and phase stability is still a challenge. In this study, a new experimental design incorporating a wedge pair is introduced to accurately control the timing between the local oscillator and the sample signal, resulting in high phase accuracy and long-term stability in a compact and flexible configuration.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Review
Chemistry, Physical
Haoyuan Wang, Wei Xiong
Summary: This review discusses the recent developments and applications of vibrational sum-frequency generation (VSFG) microscopy, highlighting its relationship with traditional spectroscopy, microscopy, and time-resolved measurements. Crucial applications of VSFG microscopy in self-assembled materials were emphasized, revealing hidden relationships between physical properties. The review also touches upon the recent development of ultrafast transient VSFG microscopy, offering spatial measurements of the ultrafast vibrational dynamics of self-assembled materials.
ANNUAL REVIEW OF PHYSICAL CHEMISTRY, VOL 72
(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
Multidisciplinary Sciences
Werner M. J. van Weerdenburg, Anand Kamlapure, Eirik Holm Fyhn, Xiaochun Huang, Niels P. E. van Mullekom, Manuel Steinbrecher, Peter Krogstrup, Jacob Linder, Alexander Ako Khajetoorians
Summary: We observe a threefold enhancement of the superconducting critical temperature and gap size in ultrathin epitaxial Al films on Si(111) approaching the 2D limit. We characterize the vortex structure using spatially resolved spectroscopy and find evidence of a paramagnetic Meissner effect originating from odd-frequency pairing contributions. These results highlight the influences of reduced dimensionality on a BCS superconductor and provide a platform for studying BCS superconductivity in large magnetic fields.
Article
Chemistry, Multidisciplinary
Davide Mitoli, Jefferson Maul, Alessandro Erba
Summary: In the framework of density functional theory (DFT) simulations of molecules and materials, an efficient approach to calculate cubic and quartic interatomic force constants in the basis of normal modes was implemented in the CRYSTAL program. By applying group theory, the associated computational cost can be further reduced by exploiting point symmetry. The proposed group theoretical approach, implemented in the CRYSTAL program, shows significant speedup in high-symmetry molecular and periodic systems.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Chemistry, Multidisciplinary
Davide Mitoli, Jefferson Maul, Alessandro Erba
Summary: In the framework of density functional theory, a group theoretical approach was implemented to reduce computational cost and improve efficiency. The approach was assessed on six test case systems, showing significant speedup in high-symmetry molecular and periodic systems.
CRYSTAL GROWTH & DESIGN
(2023)
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
Chemistry, Multidisciplinary
Chu Wang, Yong-Hao Ma, Xiaofeng Han, Xiaolin Lu
Summary: A highly efficient antimicrobial peptide called Aur, derived from Australian frog skin secretions, can disrupt bacterial membranes and interact with negatively charged model cell membranes. This study provides molecular-level details on the interaction between Aur and cell membranes, offering support for the design and application of antimicrobial peptides.
Article
Multidisciplinary Sciences
Gang-Hua Deng, Yuqin Qian, Tong Zhang, Jian Han, Hanning Chen, Yi Rao
Summary: Interactions of electronic and vibrational degrees of freedom play a crucial role in understanding excited-state relaxation pathways of molecular systems at interfaces and surfaces. The development of interface-specific two-dimensional electronic-vibrational sum frequency generation (2D-EVSFG) spectroscopy reveals strong vibronic couplings and the relaxation process in photoexcited interface-active molecules. Time-dependent experiments show that the relaxation of the locally excited state is strongly coupled with specific high-frequency modes, leading to the transition to a lower excited state.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Physical
Max Lukas, Ellen H. G. Backus, Mischa Bonn, Maksim Grechko
Summary: SFG vibrational spectroscopy is a powerful technique to study interfaces. However, implementing this technique is challenging. In this study, a collinear PR-SFG setup using a displaced Sagnac interferometer is developed, which allows independent control of time delay and intensity and provides long-time phase stabilization for the measured signal.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Chemistry, Multidisciplinary
Takakazu Seki, Xiaoqing Yu, Peng Zhang, Chun-Chieh Yu, Kejun Liu, Lucas Gunkel, Renhao Dong, Yuki Nagata, Xinliang Feng, Mischa Bonn
Summary: The research focuses on the polymerization reaction mechanism at water surfaces and the highly crystalline materials produced through surfactant-monolayer-assisted interfacial synthesis (SMAIS). It was found that the accumulation and ordered arrangement of positively charged aniline derivatives at the water surface play a crucial role in the formation of highly crystalline, conductive polyaniline films.
Article
Chemistry, Multidisciplinary
Verena Pramhaas, Holger Unterhalt, Hans-Joachim Freund, Guenther Rupprechter
Summary: The surface structure and shape of oxide-supported metal nanoparticles can be determined using polarization-dependent sum-frequency-generation (SFG) spectroscopy. This technique reveals the average surface structure and shape of the nanoparticles and can be used to monitor particle restructuring in situ. It has the potential to be a valuable tool for operando catalysis.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Florent Goujon, Aziz Ghoufi, Patrice Malfreyt
Summary: The study reveals the presence of a two-dimensional hydrogen bond network in the layer closest to graphene, and quantifies the strengthening of intermolecular interactions in liquids by calculating interface tension with a graphene monolayer.
JOURNAL OF CHEMICAL PHYSICS
(2021)
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)
Article
Chemistry, Physical
Simerjeet K. Gill, Jiahao Huang, Julia Mausz, Ruchi Gakhar, Santanu Roy, Fernando Vila, Mehmet Topsakal, William C. Phillips, Bobby Layne, Shannon Mahurin, Phillip Halstenberg, Sheng Dai, James F. Wishart, Vyacheslav S. Bryantsev, Anatoly Frenkel
JOURNAL OF PHYSICAL CHEMISTRY B
(2020)
Article
Chemistry, Physical
Fei Wu, Shobha Sharma, Santanu Roy, Phillip Halstenberg, Leighanne C. Gallington, Shannon M. Mahurin, Sheng Dai, Vyacheslav S. Bryantsev, Alexander S. Ivanov, Claudio J. Margulis
JOURNAL OF PHYSICAL CHEMISTRY B
(2020)
Article
Chemistry, Physical
Santanu Roy, Gregory K. Schenter, Joseph A. Napoli, Marcel D. Baer, Thomas E. Markland, Christopher J. Mundy
JOURNAL OF PHYSICAL CHEMISTRY B
(2020)
Article
Chemistry, Physical
Haimeng Wang, Ryan S. DeFever, Yong Zhang, Fei Wu, Santanu Roy, Vyacheslav S. Bryantsev, Claudio J. Margulis, Edward J. Maginn
JOURNAL OF CHEMICAL PHYSICS
(2020)
Correction
Chemistry, Physical
Fei Wu, Santanu Roy, Alexander S. Ivanov, Simerjeet K. Gill, Mehmet Topsakal, Eric Dooryhee, Milinda Abeykoon, Gihan Kwon, Leighanne C. Gallington, Phillip Halstenberg, Bobby Layne, Yoshiki Ishii, Shannon M. Mahurin, Sheng Dai, Vyacheslav S. Bryantsev, Claudio J. Margulis
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Santanu Roy, Martin Brehm, Shobha Sharma, Fei Wu, Dmitry S. Maltsev, Phillip Halstenberg, Leighanne C. Gallington, Shannon M. Mahurin, Sheng Dai, Alexander S. Ivanov, Claudio J. Margulis, Vyacheslav S. Bryantsev
Summary: By employing a multimodal approach and theoretical modeling, researchers in this work successfully resolved issues concerning the local structure of molten MgCl2. They demonstrated the reliability of AIMD simulations in achieving excellent agreement between experimental and simulated spectra, providing structural insights not directly available from experiments alone.
JOURNAL OF PHYSICAL CHEMISTRY B
(2021)
Article
Chemistry, Multidisciplinary
Santanu Roy, Yang Liu, Mehmet Topsakal, Elaine Dias, Ruchi Gakhar, William C. Phillips, James F. Wishart, Denis Leshchev, Phillip Halstenberg, Sheng Dai, Simerjeet K. Gill, Anatoly Frenkel, Vyacheslav S. Bryantsev
Summary: By combining various methods, we can accurately study the solvation, exchange, and speciation of ions in molten salts, quantifying populations of different coordination states of ions and understanding their sensitivity to temperature and melt composition changes.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Nanoscience & Nanotechnology
Santanu Roy, Vera Bocharova, Andrew G. Stack, Vyacheslav S. Bryantsev
Summary: This study investigates the nucleation process of sodium sulfate in aqueous solution using coordination number as a reaction coordinate and rate theory, revealing that rate processes exhibit high sensitivity to evolving structures, providing a means to predict nucleation-related structures and dynamics.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Matthew S. Emerson, Shobha Sharma, Santanu Roy, Vyacheslav S. Bryantsev, Alexander S. Ivanov, Ruchi Gakhar, Michael E. Woods, Leighanne C. Gallington, Sheng Dai, Dmitry S. Maltsev, Claudio J. Margulis
Summary: Lanthanides are important fission products in molten salt reactors, and understanding their structure and that of their mixtures is relevant to many scientific and technological problems. However, the literature on this topic is often fragmented and contradictory, necessitating the need for a clear and unified understanding of the structure. This article aims to answer specific questions about the structure of lanthanide salts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Nanoscience & Nanotechnology
Uvinduni I. Premadasa, Dengpan Dong, Diana Stamberga, Radu Custelcean, Santanu Roy, Ying-Zhong Ma, Vera Bocharova, Vyacheslav S. Bryantsev, Benjamin Doughty
Summary: The interfacial behavior of amino acid solvents used in direct air capture (DAC) plays a crucial role in the absorption and capture of CO2, suggesting the potential for developing new DAC approaches to address climate change.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Multidisciplinary Sciences
Corey D. Pilgrim, Travis S. Grimes, Clayn Smith, Colt R. Heathman, Jopaul Mathew, Santa Jansone-Popova, Santanu Roy, Debmalya Ray, Vyacheslav S. Bryantsev, Peter R. Zalupski
Summary: This study investigated the complexation of two acyclic aminopolycarboxylate chelators with trivalent lanthanides and minor actinides. The chelators, H(4)octapa and H(4)pypa-peg, are suitable for radiometal coordination and f-element isolation. H(4)octapa forms a compact coordination packet, while H(4)pypa-peg is less constrained. The solubility of H(4)pypa-peg is increased by introducing a polyethylene glycol group, without affecting its ability to complex the lanthanides and minor actinides.
SCIENTIFIC REPORTS
(2023)
Article
Chemistry, Multidisciplinary
Rajni Chahal, Santanu Roy, Martin Brehm, Shubhojit Banerjee, Vyacheslav Bryantsev, Stephen T. Lam
Summary: LiF-NaF-ZrF4 multicomponent molten salts have desirable properties for clean energy systems, but the quantification of their complex structures and composition dependence is limited. This study utilizes machine learning potentials to accurately predict extended-range structures and shows good agreement with experimental spectra.
Article
Chemistry, Multidisciplinary
Santanu Roy, Shobha Sharma, Waruni Karunaratne, Fei Wu, Ruchi Gakhar, Dmitry S. Maltsev, Phillip Halstenberg, Milinda Abeykoon, Simerjeet K. Gill, Yuanpeng Zhang, Shannon M. Mahurin, Sheng Dai, Vyacheslav S. Bryantsev, Claudio J. Margulis, Alexander S. Ivanov
Summary: This study reveals the clustering behavior of dilute Cr3+ metal ions in molten salt and demonstrates that the dynamical processes are primarily controlled by the charge density of the constituent ions. These findings challenge assumptions about specific ionic interactions and transport in molten salts.
Article
Chemistry, Physical
Santanu Roy, Fei Wu, Haimeng Wang, Alexander S. Ivanov, Shobha Sharma, Phillip Halstenberg, Simerjeet K. Gill, A. M. Milinda Abeykoon, Gihan Kwon, Mehmet Topsakal, Bobby Layne, Kotaro Sasaki, Yong Zhang, Shannon M. Mahurin, Sheng Dai, Claudio J. Margulis, Edward J. Maginn, Vyacheslav S. Bryantsev
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2020)
Article
Chemistry, Physical
Santanu Roy, Lili Wu, Sriram Goverapet Srinivasan, Andrew G. Stack, Alexandra Navrotsky, Vyacheslav S. Bryantsev
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2020)
