Article
Chemistry, Physical
Yi Zhao, Yang Liu, Yuying Wang, Shulan Li, Yi Liu, Zhong Lin Wang, Peng Jiang
Summary: Solid-liquid interfaces are widely present in nature and have various applications. Electron transfer at the interface has been discovered, and a two-step theory for the formation of solid-liquid electric double layer (EDL) has been proposed. Hydroxyl radical (.OH) is generated at the interface without external interference, and its concentration increases with pH, indicating that it is generated from hydroxide ions (OH-) through electron transfer during contact electrification. The generation of reactive oxygen species (.OH and .O2-) at the interface has potential applications in pollutant degradation.
Article
Chemistry, Multidisciplinary
Shuai Zhang, Jiajun Chen, Jianli Liu, Harley Pyles, David Baker, Chun-Long Chen, James J. De Yoreo
Summary: Biomolecular self-assembly is a fundamental process used by life to create functional materials, but progress in engineering self-assembly at solid-liquid interfaces lags behind that in bulk solutions. Recent research has focused on programming self-assembly of peptides, proteins, and peptoids at solid-liquid interfaces, as well as advancing physical understandings of self-assembly pathways using in situ atomic force microscopy. These developments are leading to novel strategies for designing biomaterials organized at and interfaced with inorganic surfaces.
ADVANCED MATERIALS
(2021)
Article
Chemistry, Physical
Zhilong Zhang, Jooyoung Sung, Daniel T. W. Toolan, Sanyang Han, Raj Pandya, Michael P. Weir, James Xiao, Simon Dowland, Mengxia Liu, Anthony J. Ryan, Richard A. L. Jones, Shujuan Huang, Akshay Rao
Summary: This study reveals the exciton dynamics in quantum dot solids using transient absorption microscopy and observes the changes and transitions in initial exciton diffusion. The spacing between quantum dots, packing density, and heterogeneity all have an impact on exciton dynamics. These findings contribute to the control of optoelectronic properties in quantum dot solids.
Article
Chemistry, Multidisciplinary
Fan Wang, Peng Yang, Xinglin Tao, Yuxiang Shi, Shuyao Li, Zhaoqi Liu, Xiangyu Chen, Zhong Lin Wang
Summary: The study investigates the electrification mechanism at liquid-gas interfaces by using an acoustic levitation method. Positive charges are generated on water droplets due to the tribomotion induced by ultrasound wave, with the charge amount reaching saturation within 30s. The presence of solid particles in droplets increases the transferred charge amount, while higher ion concentration suppresses charge generation.
Article
Multidisciplinary Sciences
Mingzi Sun, Qiuyang Lu, Zhong Lin Wang, Bolong Huang
Summary: Through analysis of electronic structures, this study investigated the contact charge transfer mechanism at the liquid-solid interface, confirming that the surface electrostatic charge perturbation-induced outer shell charge transfer is more significant than inter-bonding-orbital charge transfer, revealing multiple factors involved in charge transfer. The pinning factor provides a more direct visualization of charge transfer, offering critical guidance for future exploration of contact electrification induced charge transfer systems.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Physical
Yusen Su, Andy Berbille, Zhong Lin Wang, Wei Tang
Summary: Chemical functional groups on solid surfaces play a vital role in contact electrification at water-solid interfaces. In this study, ion coupled plasma etching was used to modify a high-density polyethylene (HDPE) film and generate fluoride (HDPE-F) and hydroxyl (HDPE-OH) functional groups, which endowed HDPE with charge withdrawing ability. HDPE-F withdrew 2.5-2.7 times more charges than HDPE-OH, and the accumulated surface charges altered the motion of droplets. This study provides an alternative approach to study contact electrification and evaluate the contribution of electrons to solid-liquid CE, and also demonstrates the superior activity of HDPE-F in contact-electro-catalysis compared to commercial fluorinated films.
Article
Materials Science, Multidisciplinary
Changzheng Li, Hongrui Zhang, Yaofeng Wang, Xuyang Liu, Asad Ali, Zhi Qun Tian
Summary: A bubble driven triboelectric nanogenerator (BD-TENG) is explored to efficiently scavenge energy directly from rising air bubbles in a PTFE tube filled with deionized water. The BD-TENG can generate sustained voltages of up to -120 V and has been demonstrated to illuminate blue LEDs. The innovative research work provides a roadmap for bubble energy harvesting in liquid media.
ADVANCED MATERIALS TECHNOLOGIES
(2023)
Article
Materials Science, Multidisciplinary
Yancheng Meng, Cong Hu, Luxian Li, Yuyang Long, Jun Yin, Jianxin Zhou, Wanlin Guo
Summary: Buckling patterns are common in living organisms and play a key role in the functionality of organs, often dependent on the deformation of these buckling structures and the interfacial interaction between liquid and solid surfaces. Experimental simulation of buckling behavior at the liquid-solid interface can result in various ordered buckling patterns, providing insights into the effects of interfacial interaction between liquid and solid surfaces.
ADVANCED ENGINEERING MATERIALS
(2022)
Review
Chemistry, Physical
Gengnan Li, Bin Wang, Daniel E. Resasco
Summary: Catalytic reactions involve direct interactions between reactants, intermediates, and products with the catalyst surface. The effects of solvents in liquid-phase catalysis play a crucial role in altering binding and reactivity of surface species. Controlling solvent structures can lead to changes in molecular binding and reactions at solid-liquid interfaces.
SURFACE SCIENCE REPORTS
(2021)
Article
Chemistry, Multidisciplinary
Bogdan Dereka, Nicholas H. C. Lewis, Yong Zhang, Nathan T. Hahn, Jonathan H. Keim, Scott A. Snyder, Edward J. Maginn, Andrei Tokmakoff
Summary: Understanding charge transport mechanisms in batteries is crucial for designing new electrolyte formulations. This study used ultrafast two-dimensional infrared (2D IR) spectroscopy to investigate exchange processes in Li+, Mg2+, Zn2+, Ca2+, and Ba2+ electrolytes. The results showed that the observed spectral dynamics mainly originated from intermolecular energy transfer, with no solvent exchange phenomena observed.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Multidisciplinary Sciences
Joshua Vogwell, Laura Rego, Olga Smirnova, David Ayuso
Summary: We present an ultrafast all-optical approach for efficient chiral recognition based on the interference between sum-frequency generation and third-harmonic generation. Our method encodes the handedness of the medium in the intensity of the emitted harmonic signal, enabling full control over the enantiosensitive response. By manipulating the sub-optical-cycle oscillations of the driving laser field, we achieve high efficiency in chiral sensitivity via low-order nonlinear light-matter interactions, paving the way for ultrafast and highly efficient imaging and control of chiral molecules.
Review
Chemistry, Multidisciplinary
Yang Dong, Nannan Wang, Di Yang, Jian Wang, Wenlong Lu, Daoai Wang
Summary: Solid-liquid triboelectric nanogenerators (SL-TENGs) are a new technology that combines contact electrification and electrostatic induction to collect clean energy stored in natural water. They have attracted increasing attention in recent years due to their high energy density, material versatility, and potential for large-scale applications. Matching SL-TENGs with different applications is critical for stable output and long-cycle life.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Ruiqi Wu, Xiankun Li, Lijuan Wang, Dongping Zhong
Summary: By using femtosecond spectroscopy, we have characterized the dynamic evolution of fatty acid photodecarboxylase and identified key steps in its reaction mechanism. These results are crucial for understanding the catalytic cycle of the enzyme and for the design of flavin-based artificial photoenzymes.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Mohammad Ali Khazaei, Dariush Bastani, Aliasghar Mohammadi, Azadeh Kordzadeh
Summary: Understanding the adsorption dynamics of surface-modified silica nanoparticles at solid-liquid interfaces is crucial for their engineering in various applications. This study experimentally examined the adsorption behavior of round-shaped silica nanoparticles with hydrophobic and/or hydrophilic agents, and found that nanoparticles with both types of agents showed higher adsorption. Kinetic models were used to simulate the adsorption dynamics, and it was found that mixed diffusion kinetics models predicted the dynamics better.
Review
Chemistry, Physical
Ben Jagger, Mauro Pasta
Summary: Lithium metal batteries (LMBs) have attracted great interest as a higher energy density alternative to conventional lithium-ion batteries (LIBs). However, the poor cycle life of LMBs due to inhomogeneous lithium deposition and active lithium loss impedes their commercialization. The solid electrolyte interphase (SEI) that forms on the anode surface plays a crucial role in controlling these issues, and current strategies are insufficient for achieving the necessary high cycling stabilities. Further research is needed to understand the SEI and guide future electrolyte design for safe and stable LMBs.
Article
Chemistry, Physical
A. Shalit, S. J. Mousavi, P. Hamm
Summary: Hybrid 2D Raman-terahertz spectroscopy was utilized to investigate the interactions between two solvents in a binary CHBr3-MeOH mixture, revealing a coupling to a new set of low-frequency modes formed due to hydrogen bond interactions between the solvents.
JOURNAL OF PHYSICAL CHEMISTRY B
(2021)
Article
Chemistry, Physical
Gokcen Tek, Peter Hamm
Summary: Resonant and off-resonant mid-infrared pump-probe spectroscopy were used to study the vibrational dynamics of CO adsorbed to different thicknesses of Pt layers. The mechanism of CO desorption was found to be thermal, with desorption yield depending on the fluence of absorbed light rather than its wavelength. Thin Pt layers facilitated CO desorption by concentrating absorbed energy in a small volume.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Peter Hamm
Summary: A new application of high-repetition rate, femtosecond Yb-laser/amplifier systems is introduced for transient 2D IR spectroscopy covering the time range from micro- to milliseconds. This approach combines the measurement of 2D IR spectra with the time separation from an actinic pump pulse, utilizing the high repetition rate of these lasers systems to offer high time resolution and enable the measurement of multiple 2D IR spectra. The well-studied photocycle of bacteriorhodopsin is used as a demonstration object in this proof-of-principle experiment.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Biochemistry & Molecular Biology
Philipp J. Heckmeier, Jeannette Ruf, David Buhrke, Brankica G. Jankovic, Peter Hamm
Summary: The protein MCL-1 is essential in regulating apoptosis in various cancers by binding to BIM according to an induced fit mechanism, leading to a cascade of structural rearrangements across a wide range of time scales.
JOURNAL OF MOLECULAR BIOLOGY
(2022)
Review
Chemistry, Multidisciplinary
Olga Bozovic, Brankica Jankovic, Peter Hamm
Summary: Controlling protein activity with azobenzene photoswitches is a powerful tool to manipulate biological function, allowing changes in binding affinities, control of allostery, and initiation of out-of-equilibrium processes. By combining the potency of azobenzene photoswitching with transient spectroscopic techniques, researchers can reveal the order of events and experimentally observe biomolecular interactions in real time, providing insights into the dynamic nature of proteins.
NATURE REVIEWS CHEMISTRY
(2022)
Article
Chemistry, Physical
Seyyed Jabbar Mousavi, Arian Berger, Peter Hamm, Andrey Shalit
Summary: In this study, two-dimensional Raman-THz spectroscopy was used to investigate the crystalline structure of bromoform. The results showed that the cross peaks in the crystalline sample were sharper and could be assigned to specific vibrational modes. The frequency positions of these cross peaks corresponded to the intramolecular bending modes in the Raman dimension and the lattice modes in the THz dimension. This work expands the applicability of this spectroscopic technique to solid samples and provides new experimental evidence for the coupling between intra- and intermolecular vibrational modes.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Kai Toepfer, Andrea Pasti, Anuradha Das, Seyedeh Maryam Salehi, Luis Itza Vazquez-Salazar, David Rohrbach, Thomas Feurer, Peter Hamm, Markus Meuwly
Summary: This study investigates the spectroscopy and structural dynamics of a deep eutectic mixture with varying water content using 2D IR and THz spectroscopy. Molecular dynamics simulations accurately describe the dependence of spectroscopic signatures on water content. The results demonstrate that the combination of structure-sensitive spectroscopies and molecular dynamics simulations provides molecular-level insights into the heterogeneity of such mixtures.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Multidisciplinary Sciences
David Buhrke, Norbert Michael, Peter Hamm
Summary: Phytochromes are commonly found photoreceptor proteins that undergo secondary structure refolding in response to chromophoric group photoisomerization. Two-dimensional infrared absorption spectroscopy is used to study the photoreaction of bacterial phytochrome Agp1, showing that dipole coupling between the chromophore and the tongue region plays a role in stabilizing the protein in the light-activated state.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Physical
Beliz Sertcan, Seyyed Jabbar Mousavi, Marcella Iannuzzi, Peter Hamm
Summary: Theoretical calculations of low-frequency anharmonic couplings in the beta-phase of crystalline bromoform were conducted based on density functional theory quantum chemistry calculations. The dominant role of electrical anharmonicity in the 2D Raman-THz response of both crystalline and liquid bromoform was revealed. The difference in relative cross-peak intensities between intramolecular and intermolecular modes in bromoform can be explained by the C-3v symmetry of bromoform along with orientational averaging.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Philipp J. J. Heckmeier, Jeannette Ruf, Brankica G. G. Jankovic, Peter Hamm
Summary: The study investigates the interaction between the allosteric protein MCL-1 and its natural inhibitors PUMA, BIM, and NOXA. Photoswitchable versions of MCL-1/PUMA and MCL-1/NOXA were designed, and the protein response was studied using transient infrared spectroscopy. Partial alpha-helical unfolding was observed in all cases, with varying timescales, suggesting a BH3-only-specific structural resilience in MCL-1's binding pocket.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Multidisciplinary Sciences
Brankica Jankovic, Olga Bozovic, Peter Hamm
NATURE COMMUNICATIONS
(2023)
Review
Chemistry, Multidisciplinary
Paul M. Donaldson, Greg M. Greetham, Chris T. Middleton, Bradley M. Luther, Martin T. Zanni, Peter Hamm, Amber T. Krummel
Summary: Ultrafast spectroscopy and imaging have become essential tools for scientists in various fields. The commercialization of advanced spectrometers, such as transient absorption spectrometers and vibrational sum frequency generation spectrometers, has made these measurements available to non-experts in ultrafast spectroscopy. The shift to new Yb-based lasers offers exciting new possibilities in the chemical and physical sciences, with higher efficiency and improved noise characteristics.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Chemistry, Physical
Jan Helbing, Peter Hamm
Summary: This article introduces several ways to electronically synchronize different types of amplified femtosecond laser systems using a single freely programmable electronics hardware. These methods allow for rapid probing of a wide range of timescales in a single transient absorption experiment without the need to move any delay stage. The approach is versatile and can synchronize different lasers, such as a Ti:Sa amplifier and a 100 kHz Yb-laser system. The time-resolution in the transient experiment ranges from 1 to 3 ps, depending on the method.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
David Buhrke, Yigal Lahav, Aditya Rao, Jeannette Ruf, Igor Schapiro, Peter Hamm
Summary: In this study, the researchers explored a cyanobacteriochrome called Slr1393-g3, which can switch between red-absorbing and green-absorbing forms. They used advanced IR spectroscopic methods to track the intermediates during the photocycle and discovered a new intermediate with distinct spectroscopic features. Additionally, they measured the vibrational couplings and structural disorder in these intermediate states using stationary and transient 2D IR experiments. Anharmonic QM/MM calculations were also performed to predict the spectra and suggest structural changes of the intermediates.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Seyedeh Maryam Salehi, Silvan Kaeser, Kai Toepfer, Polydefkis Diamantis, Rolf Pfister, Peter Hamm, Ursula Rothlisberger, Markus Meuwly
Summary: In this work, the structural dynamics and infrared spectroscopy of para-fluorophenol and phenol in the gas phase and in water were investigated using a combination of experiment and molecular dynamics simulations. The study found that the CF group of para-fluorophenol is highly hydrophobic, which is particularly relevant for applications in pharmaceutical chemistry.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)