Article
Chemistry, Physical
Schuyler P. Lockwood, Ricardo B. Metz
Summary: The bond strength and photodissociation dynamics of MgI+ are studied using theory, photodissociation spectroscopy, and photofragment velocity map imaging. The photodissociation spectrum of MgI+ shows a broad and unstructured profile from 17,000 to 21,500 cm(-1), with perpendicular anisotropy observed in the photofragment images. Bond dissociation energy is determined to be 203.0 +/- 1.8 kJ/mol (2.10 +/- 0.02 eV) at 17,000 +/- 150 cm(-1). Resonance enhanced two-photon dissociation is observed at photon energies of 33,000-41,000 cm(-1), leading to the formation of exclusively I+ fragments.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Nicholas J. Shuber, Daniel P. Tabor, Simon W. North
Summary: We performed theoretical calculations on the ground state dissociation pathways of the nitromethyl radical (CH2NO2). Three dissociation pathways were identified, and the transition state associated with the formation of NO + CH2O was characterized. Thermal rate constants were calculated to model the dissociations at temperatures relevant to nitromethane combustion. Comparison with experimental data revealed a disparity in the branching fraction, suggesting the possibility of an excited state dissociation pathway.
Article
Chemistry, Physical
M. Martins, S. Reinwardt, J. O. Schunck, J. Schwarz, K. Baev, A. Mueller, T. Buhr, A. Perry-Sassmannshausen, S. Klumpp, S. Schippers
Summary: The core level photoionization of the ionic molecular radical HF+ was studied using the photon-ion merged-beams technique, revealing complex ultrafast dissociation dynamics of the F is core hole excited sigma* state. Electronic structure calculations attributed this complex process to a spin-dependent dissociation of the excited sigma* biradical state.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Peerapat Wangchingchai, Katsuyoshi Yamasaki, Hiroshi Kohguchi
Summary: State-resolved ion-imaging of the CH3 product of dimethylamine photolysis in the 3s and 3p Rydberg bands reveals bimodal velocity distributions, with a fast component attributed to direct dissociation and a slow component attributed to indirect dissociation. The study also suggests an increasing contribution of direct dissociation at shorter photolysis wavelengths.
CHEMICAL PHYSICS LETTERS
(2022)
Article
Multidisciplinary Sciences
Travis Severt, Zachary L. Streeter, Wael Iskandar, Kirk A. Larsen, Averell Gatton, Daniel Trabert, Bethany Jochim, Brandon Griffin, Elio G. Champenois, Matthew M. Brister, Dylan Reedy, Demitri Call, Richard Strom, Allen L. Landers, Reinhard Doerner, Joshua B. Williams, Daniel S. Slaughter, Robert R. Lucchese, Thorsten Weber, C. William McCurdy, Itzik Ben-Itzhak
Summary: In this study, the authors successfully separate the sequential breakup pathways in the double ionization of water molecules and experimentally identify, separate, and sequentially track the two fragmentation paths of the intermediate OD+ ion. Determining the time evolution of reactions at the quantum mechanical level is crucial for understanding molecular dynamics.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Vikas D. Trivedi, Todd C. Chappell, Naveen B. Krishna, Anuj Shetty, Gladstone G. Sigamani, Karishma Mohan, Athreya Ramesh, Pravin R. Kumar, Nikhil U. Nair
Summary: This study utilized deep mutational scanning (DMS) to explore methods for improving phenylalanine ammonia-lyase, identifying and optimizing key mutation sites that impact enzyme activity, and investigating the mechanisms behind these mutations through quantum mechanics/molecular mechanics (QM/MM) and molecular dynamics (MD) studies.
Article
Chemistry, Physical
Marc Rico-Pasto, Anna Alemany, Felix Ritort
Summary: In this study, the Kramers kinetic diffusive model and nonequilibrium pulling experiments were used to investigate the folding kinetics and force-dependent kinetic barriers of DNA hairpins. The force-dependent kinetic rates and equilibrium folding energies were successfully derived. Furthermore, this method allows for the characterization of kinetic and thermodynamic properties of intermediate states that cannot be obtained from equilibrium hopping experiments.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Daniele Catone, Mauro Satta, Mattea Carmen Castrovilli, Paola Bolognesi, Lorenzo Avaldi, Antonella Cartoni
Summary: This study investigates the reaction of labelled methanol CD3OH?+ radical cation with neutral CD3OH, shedding light on the dynamics of main reaction channels through theoretical calculations. The results suggest these processes can be potential pathways for the formation of fundamental species, which are precursors to prebiotic molecules.
CHEMICAL PHYSICS LETTERS
(2021)
Article
Chemistry, Multidisciplinary
Daniel Keefer, Jeremy R. Rouxel, Flavia Aleotti, Francesco Segatta, Marco Garavelli, Shaul Mukamel
Summary: Research demonstrates that using a resonant infrared field at conical intersections can enhance coherence features of photoisomerization reactions and bring signals of conical intersections above the detection threshold.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Instruments & Instrumentation
Tongpo Yu, Xinlang Yang, Zhi Gao, Baokun Shan, Lei Xu, Xiaoguo Zhou, Shilin Liu
Summary: Time-sliced velocity map imaging (VMI) is commonly used in studies of photodissociation dynamics. However, its time resolution is often not sufficient to distinguish adjacent m/z ions with the same kinetic energy. In this study, a novel switch design for common ion optics in three-dimensional (3D) VMI was introduced, allowing a convenient switch between 2D and 3D VMI without breaking the vacuum or replacing the electrostatic plates, resulting in improved time resolution while maintaining high energy resolution.
REVIEW OF SCIENTIFIC INSTRUMENTS
(2023)
Article
Instruments & Instrumentation
E. Scott Goudreau, Andrey E. Boguslavskiy, Douglas J. Moffatt, Varun Makhija, Michael Hemsworth, Rune Lausten, Claude Marceau, Iain Wilkinson, Albert Stolow
Summary: The 2D VMI technique is widely used in gas-phase molecular spectroscopy and dynamics investigations. However, it is limited to specific light-source polarization geometries. Therefore, a novel 3D VMI technique has been developed to measure individual electron positions and arrival times without the need for complex reconstructions.
REVIEW OF SCIENTIFIC INSTRUMENTS
(2023)
Article
Chemistry, Physical
Atilay Ayasli, Arnab Khan, Tim Michaelsen, Thomas Gstir, Milan Oncak, Roland Wester
Summary: We investigate the reactive scattering of methyl iodide (CH3I) with atomic oxygen anions (O-) and identify different ionic products depending on the attack angle. By combining crossed-beam velocity map imaging and quantum chemical calculations, we reveal the reaction dynamics. Our experiments show that three different reaction pathways can lead to the predominant product, I-. Backside attack involves a hydrogen-bonded complex and results in indirectly, forwards, and sideways scattered iodide products, while frontside attack produces IO- through halide abstraction, with mainly isotropic and backward scattered products at low energies. At a certain energy threshold, IO- dissociates further to form I- + O, showing more direct dynamics at higher collision energies.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Thermodynamics
David E. Couch, Goutham Kukkadapu, Angie J. Zhang, Ahren W. Jasper, Craig A. Taatjes, Nils Hansen
Summary: This study investigates the radical-radical reaction of phenyl (C6H5) and propargyl (C3H3) and finds that the propargyl radical reaction can contribute to the formation of polycyclic radicals related to soot inception. By conducting experiments and simulations, it is observed that the radical concentration is positively correlated with temperature under the conditions of 800-1600 K and 25 Torr pressure, and eliminating the radical reactions leads to a discrepancy between simulation and experiment.
PROCEEDINGS OF THE COMBUSTION INSTITUTE
(2023)
Article
Chemistry, Multidisciplinary
Yu Harabuchi, Hiroki Hayashi, Hideaki Takano, Tsuyoshi Mita, Satoshi Maeda
Summary: Systematic reaction path exploration revealed the entire mechanism of Knowles's light-promoted catalytic intramolecular hydroamination. This study found that bond formation/cleavage competes with single electron transfer and that reduction and proton shuttle processes proceed concertedly.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Satoru Muramatsu, Keijiro Ohshimo, Yuan Shi, Motoki Kida, Rong Shang, Yohsuke Yamamoto, Fuminori Misaizu, Yoshiya Inokuchi
Summary: In this study, the electronic and geometrical structures of hypervalent penta-coordinate carbon compounds were characterized using gas-phase techniques. The coexistence of tetra- and penta-coordinate isomers was confirmed for a compound with moderately electron-donating ligands, consistent with solution characterizations. This difference depends on the environment and reflects the lower activation barrier of the S(N)2 reaction found in neutral solvent or gas-phase reactions.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
C. E. Gunthardt, C. J. Wallace, G. E. Hall, R. W. Field, S. W. North
JOURNAL OF PHYSICAL CHEMISTRY A
(2019)
Article
Optics
Joshua D. Winner, Feng Pan, Madison H. McIlvoy, Rodney D. W. Bowersox, Simon W. North
Article
Chemistry, Physical
Colin J. Wallace, Carolyn E. Gunthardt, George C. McBane, Simon W. North
Article
Chemistry, Physical
Carolyn E. Gunthardt, Megan N. Aardema, Gregory E. Hall, Simon W. North
JOURNAL OF CHEMICAL PHYSICS
(2019)
Article
Chemistry, Physical
Alex J. Fairhall, Mia M. Orlando, Jeffrey A. Bartz
JOURNAL OF PHYSICAL CHEMISTRY A
(2020)
Article
Multidisciplinary Sciences
Shanyu Han, Carolyn E. Gunthardt, Richard Dawes, Daiqian Xie, Simon W. North, Hua Guo
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2020)
Article
Chemistry, Physical
Sk Samir Ahamed, Hyunsik Kim, Amit K. Paul, Niclas A. West, Joshua D. Winner, Diego A. Donzis, Simon W. North, William L. Hase
JOURNAL OF CHEMICAL PHYSICS
(2020)
Article
Mechanics
B. McManamen, D. A. Donzis, S. W. North, R. D. W. Bowersox
Summary: Experimental examination was conducted to study the impact of a normal shock wave on velocity and temperature fluctuations, with results showing a closer alignment with classical linear interaction analyses (LIA) rather than contemporary theory.
JOURNAL OF FLUID MECHANICS
(2021)
Article
Chemistry, Physical
Evangelia Sakkoula, Gautam Sharma, Xingan Wang, Simon W. North, David H. Parker, Wei Wei
Summary: In this study, the CO2 VUV photodissociation dynamics near 155 nm were investigated using VMI technique. Vector correlations extracted from anisotropic angular distributions indicated photodissociation mainly via the excited 2(1)A' (A) state. A trend was observed where an increase in the CO rotational state j led to a decrease in the spatial anisotropy parameter.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Megan N. Aardema, George C. McBane, Simon W. North
Summary: The rotational state distribution and vector correlations of the O-2(a (1)delta(g), v = 0) fragments from photodissociation are investigated, showing a shift to higher rotational states with decreasing wavelength and highly suppressed odd rotational state populations. Measurements agree with classical trajectory calculations but with a slightly narrower distribution. Spatial anisotropy decreases with increasing photon energy, and the v-j correlation is consistent with v perpendicular to j.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Chemistry, Physical
Aaron C. Martinez, Oliver J. Tye, Caelan M. Frazier, Jeffrey A. Bartz
Summary: Metal nitrosyls are interesting due to their significant geometrical changes in the excited state. Co(CO)3NO is a volatile compound used as a model to study excited-state behavior. In this experiment, Co(CO)3NO was photodissociated and ion images were collected to determine the vector correlations in the photodissociation. The results showed that the fastest NO products came from an excitation parallel to the dissociating Co-NO bond.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Meeting Abstract
Chemistry, Multidisciplinary
Colin Wallace, Carolyn Gunthardt, Simon North
ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY
(2018)
Meeting Abstract
Chemistry, Multidisciplinary
Michelle Warter, Carolyn Gunthardt, Wei Wei, George McBane, Simon North
ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY
(2018)
Meeting Abstract
Chemistry, Multidisciplinary
Alex Prophet, Josh Winner, Simon North, Rodrigo Sanchez-Gonzalez
ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY
(2018)
Meeting Abstract
Chemistry, Multidisciplinary
Jason Kuszynski, Niclas West, Joshua Winner, Zachary Buen, Rodney Bowersox, Simon North
ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY
(2018)