Article
Chemistry, Organic
Yaping Li, Ming Wang, Xuefeng Jiang
Summary: The study successfully achieved a multicomponent reaction involving sodium dithionite for constructing alkyl and alkenyl tertiary sulfones. By utilizing sodium dithionite as a substitute and single-electron reductant, the decarboxylation of redox-active esters was initiated. Mechanistic studies revealed a proton trapping process in the transformation, distinct from the traditional radical trapping pathway.
Article
Chemistry, Multidisciplinary
Sven A. Donges, R. Peyton Cline, Steven E. Zeltmann, Jun Nishida, Bernd Metzger, Andrew M. Minor, Joel D. Eaves, Markus B. Raschke
Summary: The study utilizes vibrational exciton nanoimaging technology and density functional theory to uncover the link between microscopic molecular interactions and the structure-function relationship in molecular materials. By applying this approach to poly(tetrafluoroethylene), it reveals the connection between local crystallinity and disorder, as well as the potential role of local disorder in molecular coupling as a missing link between nanoscale morphology and functional properties.
Article
Chemistry, Organic
Kai-Yi Zhang, Fang Long, Chuan-Chong Peng, Jin-Hui Liu, Li-Jun Wu
Summary: A Pd-catalyzed multicomponent cross-coupling reaction using K2S2O5 as a connector is reported for the first time to synthesize allylic sulfones from allyl esters and alkyl bromides. The reaction shows broad substrate generality, excellent functional group compatibility, and high regioselectivity (only E). Biologically active molecules including aspirin, menthol, borneol, and estrone are also highly compatible with this multicomponent cross-coupling reaction. Mechanistic studies suggest that the process of SO2 insertion into the C-Pd bond is involved in this transformation.
Article
Chemistry, Physical
Paul Cavanaugh, Haochen Sun, Ilan Jen-La Plante, Maria J. Bautista, Christian Ippen, Ruiqing Ma, Anne Myers Kelley, David F. Kelley
Summary: In this study, time-correlated single photon counting was used to investigate the radiative dynamics of InP/ZnSe/ZnS core/shell/shell quantum dots with varying amounts of excess indium. The results show that QDs with excess indium exhibit different luminescence kinetics, attributed to the transient population of indium-based hole traps in the ZnSe shell. This indicates a complex interplay between shell thickness, core/shell interfaces, and the distribution of indium-based hole traps within the QDs.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
Ze Wu, Yiqiong Zhang, Li Zhang, Bo Zhou, Zengxi Wei, Dongdong Wang, Wenbo Lu, Jianfeng Jia, Li Tao, Tehua Wang, Shuangyin Wang
Summary: This work proposes a Fe(II)/Fe(III) redox mediated SO2 conversion method for simultaneous hydrogen production and sulfur dioxide capture at low voltage. Experiments show that SO2 in the electrolyte can reduce Fe(III) to Fe(II), completing the Fe(II)/Fe(III) redox cycle and the conversion of SO2 to sulfuric acid. The assembled flow cell electrolyzer exhibits good performance under low voltage.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Engineering, Environmental
Xingyu Pang, Wei Liu, Haomiao Xu, Qinyuan Hong, Peng Cui, Wenjun Huang, Zan Qu, Naiqiang Yan
Summary: The use of ZnO-CuS composite materials has proven effective in capturing gaseous SO3 and Hg-0, especially at high temperatures with high feasibility and performance. Additionally, ZnO and CuS demonstrate unique advantages in the adsorption of SO3 and Hg-0, making gaseous mercury easier to capture.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Physics, Applied
J. M. Benoit, K. Chevrier, C. Symonds, J. Bellessa
Summary: In this paper, we achieve strong light-matter coupling between a surface plasmon and two organic emitters, resulting in hybrid materials with bifunctionality properties. The optical properties of the materials are drastically modified between activated and deactivated forms of a photochromic material coupled to a cyanine dye, allowing for a tunable emission system. Light-matter interaction is shown to have the potential for modifying the fluorescence of photochromes without the need for covalent bonding.
APPLIED PHYSICS LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Mengqi Zhu, Zhineng Zhang, Tao Zhang, Dongdong Liu, Hao Zhang, Zhenxiao Zhang, Zhuolun Li, Yingchun Cheng, Wei Huang
Summary: This study reveals the influence of high pressure and tensile strain on interlayer and intralayer excitons in the WSe2/WS2 heterostructure. High pressure can transform intralayer excitons to interlayer excitons, while tensile strain leads to the transformation of interlayer excitons to intralayer excitons.
Article
Materials Science, Multidisciplinary
M. Balasubrahmaniyam, Cyriaque Genet, Tal Schwartz
Summary: We reveal a transition within the strong coupling regime and below the crossover to ultrastrong coupling, which alters the coupling mechanism in multimode cavities. This transition drastically modifies the Hamiltonian describing the polaritons, such that different cavity modes are either entangled via the material or completely decoupled.
Article
Chemistry, Physical
Xinbo Wang, Li Li, Kai Li, Ruyue Su, Yue Zhao, Song Gao, Wenhan Guo, Zhiqiang Luan, Guojie Liang, Hailing Xi, Ruqiang Zou
Summary: The hierarchically porous metal hydroxide/metal-organic framework composite nanoarchitectures show broad-spectrum removal activity for three chemically distinct toxic gases. The inclusion of M(OH)4 enhances the material's ability for toxic chemical mitigation, with high breakthrough uptake for SO2, NH3, and NO2. Post-breakthrough characterization reveals abundant M-OH groups and unsaturated M (IV) centers, providing extra adsorption sites for irreversible toxic chemical capture.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2022)
Article
Chemistry, Physical
Xiaoyu Liu, Linjing Yang, Man Huang, Qiang Li, Lili Zhao, Yuanhua Sang, Xiaoli Zhang, Zhenhuan Zhao, Hong Liu, Weijia Zhou
Summary: This study demonstrates the promising photocatalytic CO2 reduction performance of metallic MoO2_x nanobelts in pure water. The wide-bandgap and unique surface properties of MoO2 nanobelts enable efficient CO2 reduction through the self-coupling of intrinsic excited photoelectrons and plasmonic hot electrons. The presence of oxygen vacancies enhances CO2 adsorption and chemical activation.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Organic
Chuan-Chong Peng, Fang Long, Kai-Yi Zhang, Yun-Chu Hu, Li-Jun Wu
Summary: A copper-catalyzed cross-coupling reaction between arylsulfonyl radicals and diazo compounds has been developed for the synthesis of various arylsulfones under mild conditions. The reaction utilizes inexpensive and readily available K2S2O5 as the sulfur dioxide source to generate arylsulfonyl radicals. A radical mechanism involving the insertion of sulfur dioxide with aryl radicals followed by the coupling of arylsulfonyl radicals with copper carbenes is proposed.
JOURNAL OF ORGANIC CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Keisuke Shinokita, Yuhei Miyauchi, Kenji Watanabe, Takashi Taniguchi, Kazunari Matsuda
Summary: The moire patterns in van der Waals heterostructures can be used to engineer optically generated excitonic properties, offering the possibility for coherent quantum emitters and quantum simulation. The interaction between moire excitons and phonons can be tuned by adjusting the excitation energy, leading to selective excitation at phonon resonances and relaxation between different potential minima. This resonant coupling of moire excitons to phonons highlights a new way to explore novel quantum phenomena.
Article
Crystallography
Jing Zhou, Peng Chen, Zili Xie, Xiangqian Xiu, Dunjun Chen, Ping Han, Yi Shi, Rong Zhang, Youdou Zheng
Summary: This paper investigates the behavior of exciton radiative recombination in a GaN-based triangular-like ridge cavity at room temperature. The results show a clear modulation of the spontaneous emission and the presence of a new transition channel in the microcavity, with the effect depending on the angle. Furthermore, changing the tilt angle reveals that the coupling between excitons and photons is strongest at a tilt angle of 10 degrees.
Article
Chemistry, Multidisciplinary
Niclas S. Mueller, Rakesh Arul, Lukas A. Jakob, Matthew Oliver Blunt, Tamas Foeldes, Edina Rosta, Jeremy J. Baumberg
Summary: This article investigates the impact of collective vibrations on SERS spectra and proposes a method to measure intermolecular distance and disorder using collective vibrations.
Review
Engineering, Chemical
Chenxi Li, Ruth Signorell
Summary: Gas phase nucleation is a universal phenomenon that plays a crucial role in both natural settings and industrial processes. Despite more than 100 years' work to decipher this highly dynamic process, our understanding of nucleation remains incomplete. Techniques offering molecular level insight into nucleation have limitations in terms of applicable scope and measurement uncertainties.
JOURNAL OF AEROSOL SCIENCE
(2021)
Article
Engineering, Chemical
Evelyne A. Parmentier, Gregory David, Pablo Corral Arroyo, Simone Bibawi, Kivanc Esat, Ruth Signorell
Summary: The photodegradation of optically trapped oleic acid droplets by visible light was studied, showing that the oxygen amount and droplet size have minimal influence on the reaction rate. However, higher laser power and shorter wavelength significantly increased the reaction rate, suggesting that mechanisms involving the photoexcitation of oleic acid are dominant pathways. This study highlights the importance of considering direct photodegradation when using optical traps or spectroscopic methods to study aerosol particles containing fatty acids.
JOURNAL OF AEROSOL SCIENCE
(2021)
Article
Multidisciplinary Sciences
Chenxi Li, Jan Krohn, Martina Lippe, Ruth Signorell
Summary: This research used a specially designed experiment to directly measure the chemical composition and concentration of nucleating clusters in various binary CO2-containing vapors, finding that CO2 can catalyze nucleation of the low vapor pressure component by forming transient heteromolecular clusters, providing alternative pathways for more efficient nucleation. This work opens up new avenues for quantitatively assessing nucleation mechanisms involving transient species in multicomponent vapors.
Correction
Engineering, Chemical
Evelyne A. Parmentier, Gregory David, Pablo Corral Arroyo, Simone Bibawi, Kivanc Esat, Ruth Signorell
JOURNAL OF AEROSOL SCIENCE
(2021)
Article
Chemistry, Physical
Matus E. Diveky, Michael J. Gleichweit, Sandra Roy, Ruth Signorell
Summary: The uptake of water vapor by various organic aerosols plays a crucial role in applications such as medical delivery of pharmaceutical aerosols and cloud formation in the atmosphere. The mass accommodation coefficient, alpha(M), defines the probability of gas-phase molecules sticking to a surface, but accurate values are lacking for many systems. Experimental techniques, including photothermal single-particle spectroscopy (PSPS), have been used to study interfacial water transport and evaluate alpha(M) values for different organics.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Chemistry, Physical
John W. Niman, Benjamin S. Kamerin, Vitaly V. Kresin, Jan Krohn, Ruth Signorell, Roope Halonen, Klavs Hansen
Summary: The abundance spectra of (CO2)(N) clusters were analyzed under a wide range of adiabatic expansion conditions, revealing a universal pattern in cluster stability functions. Individual cluster properties, size-dependent cluster binding energies, shell and subshell closing sizes, and cuboctahedral packing ordering for larger sizes were identified through the analysis. The study demonstrates that even a small variation in dissociation energies can lead to significant abundance variations, especially for larger clusters.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Multidisciplinary Sciences
Pablo Corral Arroyo, Gregory David, Peter A. Alpert, Evelyne A. Parmentier, Markus Ammann, Ruth Signorell
Summary: Direct evidence of optical confinement-induced patterning inside aerosol particles is provided using x-ray spectromicroscopic imaging and modeling. The study found that photochemical reactions in most aerosol particles are accelerated by optical confinement effects, with rotation of free aerosol particles and intraparticle molecular transport further enhancing the photochemistry. Atmospheric models should consider the influence of optical confinement effects on aerosol particle photochemistry.
Article
Chemistry, Physical
Evelyne A. Parmentier, Pablo Corral Arroyo, Richard Gruseck, Loren Ban, Gregory David, Ruth Signorell
Summary: The influence of electric charges on the photodegradation of oleic acid droplets was investigated, and it was found that the charge did not affect the chemical composition or kinetics.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Chemistry, Physical
Stefan Feusi, Jan Krohn, Chenxi Li, Ruth Signorell
Summary: The interaction of water with different substances in the earth's atmosphere and its contribution to the water vapor phase transition is still unclear. This study provides the first measurements of water-nonane binary nucleation and unary nucleation data in the 50-110 K temperature range. The experiments show that hetero-molecular clusters do not play a role during nucleation, and the nucleation rates of water and nonane are not significantly affected by the presence of the other species.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Multidisciplinary Sciences
Sebastian Hartweg, Jonathan Barnes, Bruce L. Yoder, Gustavo A. Garcia, Laurent Nahon, Evangelos Miliordos, Ruth Signorell
Summary: Low-energy electrons dissolved in liquid ammonia or aqueous media can serve as powerful reducing agents but can also cause radiation damage to biological tissue. The mechanistic processes underlying electron transfer steps are still not fully understood. This study demonstrates how ultraviolet (UV) photoexcitation of metal-ammonia clusters can be used to generate tunable low-energy electrons. The UV light-induced generation of spin-paired solvated dielectrons and their subsequent relaxation through unconventional electron transfer-mediated decay offer an efficient source of low-energy electrons. This process has the potential to improve our understanding of radiation damage and facilitate mechanistic studies of solvated electron reduction reactions.
Article
Chemistry, Physical
Jonathan V. Barnes, Dominique P. Borgeaud Dit Avocat, Edith Simmen, Huanyu Yang, Bruce L. Yoder, Ruth Signorell
Summary: Using experimental and simulation methods, this study compares the magnetic properties of different neutral sodium-doped solvent clusters. It is found that clusters with longer spin transition times exhibit better deflection, while other clusters show reduced deflection. The observed magnetic deflection behavior is correlated to the number of excited rotational states in the clusters.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Environmental Sciences
Oliver Reich, Michael J. J. Gleichweit, Gregory David, Nicole Leemann, Ruth Signorell
Summary: Sea salt aerosol is abundant in the atmosphere and its hygroscopicity plays a crucial role in its interaction with solar radiation. Conflicting values for its hygroscopic growth have been reported, impacting the accuracy of climate modeling. We present new values of hygroscopic growth for atmospheric sea salt, obtained through optical trapping and single particle mass measurement. Our findings reconcile discrepancies in previous studies and also reveal the crystallization of gypsum at higher relative humidity.
ENVIRONMENTAL SCIENCE-ATMOSPHERES
(2023)
Article
Environmental Sciences
Xiangrui Kong, Suyun Zhu, Andrey Shavorskiy, Jun Li, Wanyu Liu, Pablo Corral Arroyo, Ruth Signorell, Sen Wang, Jan B. C. Pettersson
Summary: Salt aerosols play important roles in atmospheric chemistry and climate systems. This study used ambient pressure X-ray photoelectron spectroscopy to characterize Martian salt analogues and their responses to varying relative humidities. The results showed that the surface chemical environment of the salts is similar to ion chromatography results, but differences exist for species that preferentially partition to the surface or the bulk. The study also found that changes in relative humidity do not have a major impact on the surface chemical environment.
ENVIRONMENTAL SCIENCE-ATMOSPHERES
(2022)
Article
Chemistry, Physical
Ruth Signorell, Bernd Winter
Summary: This perspective article reviews the specific challenges of photoemission spectroscopy in studying bulk liquid water, aqueous solutions, water droplets, and water clusters. The focus is on accurately retrieving energetics and photoelectron angular information from measured spectra and understanding the differences in different aqueous environments. Various phenomena, such as multiple energy-dependent electron scattering and different energy referencing methods, are discussed. Recommendations on accounting for or minimizing the influence of electron scattering are provided.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Loren Ban, Hanchao Tang, Bruce L. Yoder, Ruth Signorell
Summary: In this study, photoemission from submicrometer droplets containing a mixture of dioctyl phthalate and dioctyl sebacate was investigated using femtosecond and nanosecond photoionization techniques. The results showed significant differences in the photoelectron spectra between ionization with nanosecond and femtosecond laser pulses, attributed to ionization of long-lived states within the duration of the nanosecond pulse. The decay dynamics of these long-lived states were investigated using a nanosecond-femtosecond pump-probe scheme, and an accelerated decay rate was observed at higher dioctyl phthalate concentrations. Additionally, the decay dynamics were found to be faster in smaller droplets and neutral droplets compared to charged droplets, suggesting the influence of droplet size and charge.
FARADAY DISCUSSIONS
(2022)
