Article
Chemistry, Multidisciplinary
Sunil Kumar Kandappa, Lakshmy Kannadi Valloli, Steffen Jockusch, Jayaraman Sivaguru
Summary: An unprecedented photochemical reactivity of 1,3-dicarbonyl compounds with amino-alkenes has been discovered, leading to the formation of dihydropyrans. This novel reaction has changed the established paradigm related to the De Mayo reaction between 1,3-dicarbonyl compounds and alkenes and allows for convenient access to the Marmycin core from commercially available reactants in a single step. Detailed origin and scope of this new photoreaction have been investigated with preliminary photophysical and mechanistic studies.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Junyi Liu, Xu Zhang, Gang Lu
Summary: In this work, the excited state dynamics in a WS2/graphene heterostructure are investigated through first-principles calculations, providing insights into the charge and energy transfer mechanisms. It is found that charge transfer is primarily driven by interlayer Auger-like processes due to strong electron-hole interactions, rather than direct interlayer excitations. The electron-phonon coupling is unable to compete with Auger processes due to phonon bottleneck. Additionally, the asymmetrical dynamics are attributed to the difference in density of states of the heterostructure.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Inorganic & Nuclear
Lu-Lu Liu, Li-Xin Wang, Min Peng, Jing Xiang, Huan Yang, Shek-Man Yiu, Tai-Chu Lau
Summary: The reactivity of electrophilic OsVI and RuVI nitrides with amines has been reported before. In this study, a luminescent osmium(VI) nitrido complex was found to undergo ring nitrogenation of aromatic amines under visible light irradiation. The reaction proceeds through nucleophilic addition of the amine nitrogen to the excited state complex. The products were characterized using spectroscopic techniques and X-ray crystallography. The reaction mechanism involves electron transfer and proton transfer steps.
INORGANIC CHEMISTRY
(2023)
Article
Spectroscopy
Guijie Zhao, Wei Shi, Xin Xin, Yunfan Yang, Fengcai Ma, Yongqing Li
Summary: This study theoretically analyzed the influence of different alkyl chain lengths on excited state intramolecular proton transfer (ESIPT) using phenothiazine derivatives as models. The results showed an inverse relationship between alkyl chain length and the shift value of the fluorescence spectrum. Density functional theory (DFT) and time-dependent density functional theory (TD-DFT) were used to simulate the molecular dynamics in the ground state and excited state. The analysis revealed stronger hydrogen bonding in the excited state molecules, favoring the ESIPT process. Frontier molecular orbitals (FMOs) indicated that electron density rearrangement was the driving force of the ESIPT process. Scanning potential energy curves qualitatively analyzed the data and concluded that longer alkyl chains weakened the hydrogen bonding effect and made the ESIPT process more unfavorable.
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
(2023)
Article
Chemistry, Multidisciplinary
Gibu George, Olga. A. Stasyuk, Alexander A. Voityuk, Anton J. Stasyuk, Miquel Sola
Summary: The incorporation of pyrrolo[3,2-b]pyrrole units into carbon nanorings allows for modulation of their properties, due to the combined effect of heteroatom and antiaromatic character on electronic properties. Different units lead to the formation of stereoisomers. This computational study investigates how the spatial orientation of monomeric units in the ring affects the properties of cyclic dibenzopyrrolo[3,2-b]pyrroles and their complexes with C-60 fullerene.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Xingmao Chang, Zhaolong Wang, Gang Wang, Taihong Liu, Simin Lin, Yu Fang
Summary: By manipulating the geometrical arrangement of perylene bisimide (PBI) moieties within supramolecular coordination complexes (SCCs), the photophysical properties of PBI can be effectively tuned, providing another effective way to construct high-performance optical molecular materials.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Jia-Xiong Chen, Ya-Fang Xiao, Kai Wang, Dianming Sun, Xiao-Chun Fan, Xiang Zhang, Ming Zhang, Yi-Zhong Shi, Jia Yu, Feng-Xia Geng, Chun-Sing Lee, Xiao-Hong Zhang
Summary: Developing red thermally activated delayed fluorescence (TADF) emitters for high-performance OLEDs is a challenge, but the newly designed and synthesized red TADF emitters in this study show promising results with significant efficiency enhancements. Among them, oDTBPZ-DPXZ demonstrates efficient TADF feature and high exciton utilization, achieving excellent external quantum efficiency in both vacuum-processed and solution-processed OLEDs. This work provides an effective strategy for designing red TADF molecules by managing energy level alignments to enhance exciton harvesting.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Svetlana Shostak, Woojin Park, Juwon Oh, Jinseok Kim, Seunghoon Lee, Hyeongwoo Nam, Michael Filatov, Dongho Kim, Cheol Ho Choi
Summary: The excited-state aromatization dynamics in the photochemical ring opening of DHA was investigated using nonadiabatic molecular dynamics simulations and the mixed-reference spin-flip (MRSF)-TDDFT method. It was found that the ring opening occurs in the excited state through a series of steps with increasing aromaticity. The competition between Baird and anti-Baird channels suggests that the quantum yield of the photochemical products can be controlled by tipping their balance.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Engineering, Environmental
Jialiang Liang, Jingke Wu, Pengfei Gan, Yudan Liu, Peng Zhen, Yunyi Li, Zhiwei Zhao, Wen Liu, Meiping Tong
Summary: This study investigates the dephosphorization of dimethoate (DMT), a representative organophosphorus pesticide, using a vacuum ultraviolet system. It finds that non-radical processes, such as photoexcitation and singlet oxygen atoms (O(1D)), have a significant effect on DMT dephosphorization. The study highlights the significant contribution of non-radical pathways in DMT dephosphorization by VUV.
Article
Chemistry, Physical
Li Zhao, Xuehui Geng, Guoxia Han, Yahui Guo, Runze Liu, Junsheng Chen
Summary: This study investigates the excited state decay mechanism of cytidine in both gas phase and aqueous solution using high-level electronic structure calculations and non-adiabatic dynamic simulations. It is found that cytidine undergoes barrierless decay driven by ring-puckering motion and relaxation channel with a small energy barrier driven by elongation motion of C=O bond. The presence of water molecules significantly reduces the energy barrier, suggesting that the long-lived decay channel in aqueous solution is likely attributed to the cytidine-water intermolecular hydrogen/proton transfer process. These findings contribute to a better understanding of the photostability of DNAs and RNAs and resolve the debate on the cytidine excited-state decay mechanism.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Yiwen Wang, Zehua Chen, Yang Yang
Summary: Modeling and interpreting vibrational spectra are important for studying reaction dynamics. This study presents a new method using excited state constrained minimized energy surfaces (CMESs) to describe vibrational excited state absorptions. Results from various model systems show that this method provides good estimations of transition frequencies for vibrational excited state absorptions, surpassing conventional harmonic approximations using potential energy surfaces.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Applied
Jie Ma, Jinlong Li, Rui Yang, Weijian Xue, Qingxia Wang, Shenmiao Li
Summary: The study revealed that N-1 to N-5 exhibit significantly red-shifted UV-vis absorption and emission properties, with N-1 demonstrating dual emission, confirming their ESIPT characteristics. All compounds generated triplet excited states, with N-3 and N-4 showing longer triplet excited state lifetimes and higher photooxidative abilities than the other compounds.
Article
Chemistry, Physical
Ibanrishisha Mawa, Aditya N. Panda
Summary: In this study, the ground and excited state properties of two nitrile-substituted 2-(oxazolinyl)-phenols in the gas phase and two implicit solvents were investigated. Computational studies indicated that the implicit solvent had little influence on proton transfer timescale but affected the non-radiative decay channels, with these channels being more probable in the gas phase and cyclohexane compared to methanol.
CHEMICAL PHYSICS LETTERS
(2022)
Article
Chemistry, Physical
Souradip Dasgupta, Shrobona Banerjee, Sharmistha Das, Anindya Datta
Summary: Various strategies have been explored to enhance the fluorescence of a weakly fluorescent Schiff base, salampy. The fluorescence lifetime of salampy varies in different forms and can be further extended by forming complexes with Zn2+ or Al3+.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Aparna Shukla, Vikas Kumar Jha, Soumit Chatterjee
Summary: 5-(tert-Butyl)-2-hydroxy-1,3-isophthalaldehyde (5-tBHI) exhibits solvent-dependent single or dual emission. The photophysics of 5-tBHI were investigated in different solvents, and compared with the methyl derivative of the probe and the 5-tBHI anion. The results showed that in non-polar solvents, 5-tBHI mainly adopts an intramolecular H-bonded conformer and undergoes excited state intramolecular proton transfer (ESIPT). However, a dynamic equilibrium was observed in polar, protic solvents, except for water. The proton transfer process, whether intramolecular or intermolecular, was found to occur within 1 picosecond.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Correction
Chemistry, Physical
Chen Luo, Yan Shao, Hua Yu, Hong-zhi Ma, Yu-hao Zhang, Long Gu, Bo Yin, Ming-bo Yang
CHEMICAL PHYSICS LETTERS
(2024)
Article
Chemistry, Physical
Stefano Borocci, Armando Camerlingo, Felice Grandinetti, Maria Rutigliano, Nico Sanna
Summary: The complexes of He, Ne, Ar, Kr, and Xe with B3N3H6 were investigated using MP2, CCSD(T), and SAPT ab initio methods. The complexes can be described as mono-, di-, and tri-coordinated to the N atoms, with stability following the order N-mono < N-di < N-tri. The interactions are dominated by dispersion and the binding energies are within the range of 1 or 2 kcal mol(-1). The results were compared with a recent DFT study on larger BN sheets complexes [Phys. Chem. Chem. Phys. 24 (2022) 2554-2566.].
CHEMICAL PHYSICS LETTERS
(2024)
Article
Chemistry, Physical
V. Nagarajan, R. Bhuvaneswari, R. Chandiramouli
Summary: In this study, stable phosphoborane was used as a sensor to detect isobutane and n-propane in Liquefied Petroleum Gas (LPG). Phosphoborane demonstrated structural stability and semiconducting nature, and exhibited promising adsorption properties for the LPG molecules.
CHEMICAL PHYSICS LETTERS
(2024)
Article
Chemistry, Physical
Xiaoxi Xu, Zijiang Yang, Bayaer Buren, Maodu Chen
Summary: In this study, the time-dependent wave packet method was used to investigate the reaction channels and mechanisms of Ca+ + HD. The results show that the CaH+ + D reaction channel plays a primary role, which is consistent with experimental results. Complex forming and direct-abstraction reaction mechanisms exist in this reaction process.
CHEMICAL PHYSICS LETTERS
(2024)
Article
Chemistry, Physical
Keshab Pandey, Hae Kyung Jeong
Summary: A free-standing silicon-carbon nanofiber composite film was synthesized and investigated for supercapacitor applications. It exhibited high specific capacitance, energy density, and power density. After 5000 cycles, the film showed excellent specific capacitance retention and Coulombic efficiency.
CHEMICAL PHYSICS LETTERS
(2024)
Article
Chemistry, Physical
Xinyu Zhang, Haosong Li, Xiaoyu Cao, Jing Gao, Yong Wei, Jianzhuo Zhu
Summary: The evaporation behavior of nanosized water aggregations on two-dimensional electroneutral solid surfaces with different surface polar unit densities was investigated. The results showed that the evaporation rate changes non-monotonically with the surface polar unit density, and the minimum evaporation rate is obtained when the surface has a modest surface polar unit ratio of 66.7%.
CHEMICAL PHYSICS LETTERS
(2024)
Article
Chemistry, Physical
Yanyan Xu, Rui Dai, Xiaojie Wang, Zhijun Qiao, Haowei Wen, Dianbo Ruan, Yuzuo Wang
Summary: This article presents an innovative solvothermal sodium insertion method for synthesizing Triphylite-NaFePO4, which demonstrates optimal electrochemical performance in sodium-ion batteries.
CHEMICAL PHYSICS LETTERS
(2024)
Article
Chemistry, Physical
Meiyi Jiang, Kun Yang, Yancheng Liu, Li Yao
Summary: The geometric structure and electronic properties of transition metal M (M = Cu, Fe, Mn)-TiO2 (101) surface adsorbed by NO2 and N2O were calculated by density functional theory (DFT) and DFT + U theory. The results showed that the adsorption of NO2 and N2O on Mn and Fe atoms is more stable, and a large number of active electrons are formed around these atoms, facilitating the catalytic reactions.
CHEMICAL PHYSICS LETTERS
(2024)
Article
Chemistry, Physical
Sergey A. Vyrko, Yulia G. Polynskaya, Nikita A. Matsokin, Andrey M. Popov, Andrey A. Knizhnik, Nikolai A. Poklonski, Yurii E. Lozovik
Summary: In this study, carbon nanobracelets, which are cyclic molecules composed of alternating polycyclic regions and double carbon chains, were investigated using spin-polarized density functional theory. The results show that carbon nanobracelets with odd number of monomers exhibit distinct electronic energy levels, band gaps, and carbon chain deformation compared to those with even number of monomers.
CHEMICAL PHYSICS LETTERS
(2024)
Article
Chemistry, Physical
Chanchan Wang, Quan Yang, Yanzhi Ding, Xiaoyong Lu, Dong Tian
Summary: It has been found that the introduction of buffer layers improves the electrical performance of solid oxide fuel cells (SSOFCs). In this study, varying ratios of Gd-doped CeO2 were used as buffer layers in YSZ-based SSOFCs. The results demonstrate that the performance of SSOFCs is enhanced when a buffer layer is added, with the highest performance achieved using Ce0.8Gd0.2O2-delta (GDC20) as the buffer layer. This suggests that the use of GDC series buffer layers is an attractive strategy to optimize performance loss due to electrolyte-electrode interactions.
CHEMICAL PHYSICS LETTERS
(2024)
Article
Chemistry, Physical
Wang Li, Yi-Fan Zhang, Jia-Bin Huang, Chang-Yang Wang, Feng Zhang, Jiu-Zhong Yang, Long Zhao
Summary: The gas-phase reaction of propargyl with vinylacetylene was investigated using synchrotron photoionization and molecular-beam mass spectrometry methodologies. The formation mechanisms of the resulting cyclic structures were examined using quantum computations. Two previously unidentified isomers were detected and identified for the first time.
CHEMICAL PHYSICS LETTERS
(2024)
Article
Chemistry, Physical
Avijit Pramanik, Sanchita Kundu, Olorunsola Praise Kolawole, Kaelin Gates, Paresh Chandra Ray
Summary: This study investigates the influence of aspect ratio and quantum confinement on the single-photon and two-photon absorption cross-section of perovskite CsPbI3 nanorods. Experimental data shows that CsPbI3 nanorods have an extremely high two-photon absorption cross-section, significantly surpassing organic chromophores and other CsPbBr3 nanocrystals. Moreover, adjusting the aspect ratio can significantly enhance the absorption ability. Additionally, the study also reveals a moderate quantum confinement effect on the single-photon and two-photon absorption cross-section of the nanorods.
CHEMICAL PHYSICS LETTERS
(2024)
Article
Chemistry, Physical
Hyon-Tae Pak, Jin-A Choe, Kyong-Sik Ju, Yong -Son Rim
Summary: Drug-loaded cellulose diacetate (CDA) membranes were prepared using different compositions of mixed solvent. The microstructure and performance of the membranes were investigated, and a method to predict drug release properties was proposed. The results showed that the composition of the mixed solvent significantly affected the overall performance of CDA membranes, and the release rates of drugs were related to Δdelta and the intrinsic viscosity of CDA.
CHEMICAL PHYSICS LETTERS
(2024)
Article
Chemistry, Physical
Gabriella E. Ravin, E. Curotto
Summary: We have developed a systematic approach to optimize the training set sizes for neural networks in fitting ab initio potential energy surfaces. Using this approach, we have constructed several spectroscopic quality potential energy surfaces for [Li(H2)n]+, n = 1 - 9. The ground state properties have been computed for all the systems and selected states.
CHEMICAL PHYSICS LETTERS
(2024)
Article
Chemistry, Physical
Guohua Xu, Lei Xu, Feng Zhang, Chunling Yu, Yu Song
Summary: NiS1.03@Ni7S6/carbon composite was successfully prepared using corn stalk as a carbon source via a simple adsorption-sulphurization process. The composite exhibited a specific capacitance of 1554.6 F/g at 1 A/g as a supercapacitor electrode, with a capacitance retention rate of 80.4% after 5000 cycles. Furthermore, the NiS1.03@Ni7S6/carbon//AC asymmetric supercapacitor showed a high energy density of 41.2 Wh kg-1 at a power density of 750 W kg-1, and excellent cycling stability with 86.8% capacitance retention after 10,000 cycles.
CHEMICAL PHYSICS LETTERS
(2024)