Article
Chemistry, Physical
Ruth Chau-Ting Chan, Chris Tsz-Leung Chan, Chensheng Ma, Kang-Yi Gu, Han-Xin Xie, Allen Ka-Wa Wong, Qing-Wu Xiong, Ming-Liang Wang, Wai-Ming Kwok
Summary: This study investigates the excited state dynamics of protonated Adenosine (AdoH(+)) using ultrafast time-resolved fluorescence spectroscopy and theoretical calculation, revealing different conformers leading to distinct excited states and decay dynamics. Protonation and solvent environment play a crucial role in dramatically altering the excited states of Ado, providing valuable insights for understanding the nonradiative dynamics of both monomeric bases and oligomeric or polymeric DNAs.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
Patryk Rybczynski, Manon H. E. Bousquet, Anna Kaczmarek-Kedziera, Beata Jedrzejewska, Denis Jacquemin, Borys Osmialowski
Summary: Precisely tuning the fluorescence quantum yield is crucial for numerous applications of fluorophores, but remains exceptionally challenging due to the complex relationship between Franck-Condon excited state and conical intersection position. In this study, a series of nine fluorophores with peripheral substitution of two relatively mild electron donating and withdrawing groups were reported, leading to a wide range of fluorescence quantum yields from dark to ultra-bright, with extreme values obtained for isomeric molecules. Experimental findings were rationalized by advanced quantum chemical calculations showing good correlation between measured emission parameters and theoretical radiative and internal conversion rate constants. Therefore, the described substituent exchange provides a method to rigorously adjust the properties of molecular probes structurally similar to thioflavin T.
Article
Chemistry, Physical
Leila Shahrokh, Reza Omidyan, Gholamhassan Azimi
Summary: The non-radiative relaxation mechanism of protonated adenine was investigated using quantum chemical computational methods and dynamics simulations. It was found that the out-of-plane deformation of the six-member ring plays a significant role in the deactivation of the excited state to the ground state, which is important for the photostability of protonated DNA/RNA bases.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Lu-ran Fei, Jian Wang, Fu-quan Bai, Shi-ping Wang, Bin Hu, Chui-peng Kong, Hong-xing Zhang
Summary: In this study, the photoluminescence properties of TTM-based radicals were evaluated using DFT and TD-DFT methods. The calculated results matched well with previous experimental results, and it was found that the conjugated structures and solvent polarity can influence kr and knr.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Leila Shahrokh, Reza Omidyan, Gholamhassan Azimi
Summary: The study utilizes ab initio and surface-hopping nonadiabatic dynamics simulation methods to investigate relaxation mechanisms in protonated thymine (TH+) and cytosine (CH+). Multiple conical intersections were located between (1)pi pi* and S-0 states for each system, with particular focus on the barrier-free out-of-plane deformation governing relaxation from the (1)pi pi* state to the ground state. The ring puckering coordinate from the C-6 position of the heterocycle ring was found to play a prominent role in the deactivation mechanism of the considered systems, supported by excited-state nonadiabatic dynamics simulations.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Biology
Michael F. Roberts, Stephen E. Bricher
Summary: This article proposes a theoretical basis for analyzing genetic diseases caused by dominant alleles, including disease prevalence, genotype penetrance, and the relationship between causal genotype frequency and disease frequency. In addition, it provides a theoretical framework for accurate diagnosis and clinical approaches for disease study, including examples that highlight the impact of inaccurate and incomplete diagnoses on disease prevalence estimates. The article also discusses the aggregation of genetic diseases and suggests alternative measures that address deficiencies associated with the sibling recurrence-risk ratio.
Article
Spectroscopy
Francesca Macii, Lorenzo Cupellini, Mariassunta Stifano, Javier Santolaya, Cristina Perez-Arnaiz, Andrea Pucci, Giampaolo Barone, Begona Garcia, Natalia Busto, Tarita Biver
Summary: In this study, a combined spectroscopic and theoretical analysis was conducted to investigate the binding of PZPERY to various biosubstrates. The results showed distinct binding modes of PZPERY to DNA and RNA, with intercalation observed for DNA and groove binding for RNAs. PZPERY exhibited the highest affinity towards DNA G-quadruplexes, particularly human telomeric G4s, with both sitting-atop and lateral binding modes considered concurrently for hybrid G4 forms.
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
(2021)
Article
Chemistry, Physical
Panwang Zhou, Zhe Tang, Peng Li, Jianyong Liu
Summary: The fluorescence tuning mechanisms of fluorescein derivatives involve a dark n pi* state and minimal energy conical intersection (MECI). MECI formation includes significant rotation of the benzene ring and flip-flop motion of the xanthene moiety, which are restricted by intermolecular hydrogen bonding and lower temperature. The energy barrier to reach MECI depends on the substituents in the benzene moiety, as observed in experimental substituent effects.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Xue-fang Yu, Ting-he Fu, Bo Xiao, Hong-yuan Yu, Qingzhong Li
Summary: The study reveals that the deformation of double bonds in A and 5FU can affect the excited-state decay paths of the A-5FU dimer, competing with proton transfer paths and influencing the photostability of DNA base pairs.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
Maxime Hodee, Augustin Lenne, Julian Rodriguez-Lopez, Francoise Robin-le Guen, Claudine Katan, Sylvain Achelle, Arnaud Fihey
Summary: In this study, seven new push-pull systems were designed by combining a protonable diazine heterocycle with a deprotonable phenol unit through various pi-conjugated linkers. (De)protonation in solution resulted in a systematic bathochromic shift in both absorption and emission maxima. Computational analysis revealed that (de)protonation affects the energy and nature of vertical transitions, increasing the Intramolecular Charge Transfer (ICT) character of the excitations. Some compounds remained luminescent after (de)protonation, allowing for white light emission.
NEW JOURNAL OF CHEMISTRY
(2021)
Article
Crystallography
N. P. Yadav, A. K. Vishwkarma, K. Kumar, A. Vats, A. Pathak, R. Kumar, V Mukerjee, S. Moharana, T. Yadav, C. Mahapatra, S. Srivastava
Summary: The present work focuses on the vibrational spectroscopic properties of synephrine molecule and its radical in gas phase. The study involves optimizing the ground state structures of synephrine and synephrine(-), and comparing their vibrational frequencies with experimental data. The effects of hydrogen removal from the oxygen site on the geometrical parameters and vibrational frequencies of synephrine are reported. Thermodynamic parameters of synephrine and its radical at room temperature are calculated and discussed. The stability of the electronic structure of the radical form is analyzed using NBO analysis, and the HOMO-LUMO energy gap suggests greater reactivity of synephrine in its radical form.
Article
Chemistry, Physical
Nivedita Pan, Tuhin Kumar Maji, Sayantika Bandyopadhyay, Pritam Biswas, Arka Chatterjee, Mala Mitra, Arpita Chatterjee, Samir Kumar Pal
Summary: Plasmonic nanoparticles, particularly citrate functionalized silver nanoparticles, self-assemble into linear chains in the presence of lead ions, leading to the generation of new LSPR modes. This unique self-assembled geometry, driven by the high interaction affinity between citrate and Pb2+, allows for the development of low cost, highly selective and sensitive lead ion sensors for industrial lead pollution monitoring.
Review
Chemistry, Multidisciplinary
Qian Peng, Zhigang Shuai
Summary: Understanding the luminescence mechanism is crucial for the development of AIE materials. Weak intermolecular excitonic coupling in AIEgens challenges conventional models, leading to new theoretical proposals. Multiscale computational approaches provide insights into radiative and nonradiative decay processes, offering potential for predicting molecular design.
Article
Engineering, Electrical & Electronic
Nivedita Pan, Ria Ghosh, Debdatta Mukherjee, Neha Bhattacharyya, Lopamudra Roy, Amrita Banerjee, Soumendra Singh, Radha Tamal Goswami, Mala Mitra, Arpita Chattopadhyay, Samir Kumar Pal
Summary: With the advancement of technology, nanosensors have become an integral tool for sustainable monitoring of environmental pollution. In this study, we present a spectroscopic method using citrate functionalized gold nanoparticles (Au NPs) to detect lead (Pb), a toxic heavy metal pollutant, followed by the development of a low-cost prototype device. The self-aggregation of citrate functionalized Au NPs in the presence of Pb was observed spectroscopically, allowing for the determination of Pb concentration and the development of a prototype for monitoring Pb pollution.
IEEE SENSORS LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Yishen Liu, Meijia Gu, Qihang Ding, Zhiyun Zhang, Wanxia Gong, Yuncong Yuan, Xiaofei Miao, Huili Ma, Xuechuan Hong, Wenbo Hu, Yuling Xiao
Summary: We developed efficient heavy-atom-free photosensitizers in the near-infrared (NIR) range using a facile approach. By modifying the thiopyrylium-based NIR-II dyads, our study showed that a sterically bulky and electron-rich moiety enhanced the intersystem crossing and electron excitation characteristics, resulting in significantly elevated reactive oxygen species (ROS) quantum yield. Our optimized lung-targeting nanoparticles enabled real-time NIR-II lung imaging and guided effective pulmonary coronavirus inactivation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Engineering, Environmental
Zuping Xiong, Wenqi Gong, Pengfei Xu, Mengyi Jiang, Xuting Cai, Yuqing Zhu, Xinni Ping, Hui Feng, Huili Ma, Zhaosheng Qian
Summary: This study re-examined the classic heavy-atom effect from a completely fresh perspective and proposed a universal heavy-atom-induced fluorescence enhancement principle suited for most AIEgens.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Applied
Jia Gao, Shenyu Shi, Qiuying Li, Huili Ma
Summary: Room temperature phosphorescence (RTP) in organic aggregates depends on molecular conformation and packing, which pose challenges in understanding the mechanism of polymorphism-dependent RTP. In this study, different RTP lifetimes were observed in organic polymorphs of DOS compounds (DOS-O and DOS-S). By analyzing molecular and electronic structures, and decay dynamics of T(1) states, it was found that the decreased energy gap of T-1 states due to conformational variation is responsible for the shortened RTP lifetime from DOS-O to DOS-S. This was further supported by the good agreement between theory and experiment in RTP lifetime.
Article
Chemistry, Multidisciplinary
Xuan Zeng, Lu Wang, Hengyi Dai, Tianyu Huang, Mingxu Du, Dong Wang, Dongdong Zhang, Lian Duan
Summary: Green multiresonance (MR) emitters with narrow full widths at half maximum (FWHMs) of 13 nm and 14 nm have been synthesized by fusing indolo(3,2,1-jk)carbazole and naphthalene moieties. These emitters exhibit high photoluminescence quantum yields (>95%) and have the smallest FWHMs among all green MR emitters. The molecular architecture with extended conjugation length and small FWHM is achieved by orbital interactions between antisymmetric segments.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Shi Tang, Zhi Wang, Yanzi Xu, Huili Ma, Jia Wang, Christian Larsen, Dongfeng Dang, Ergang Wang, Ludvig Edman
Summary: The emission efficiency of organic semiconductors (OSCs) often suffers from aggregation caused quenching (ACQ). An elegant solution is aggregation-induced emission (AIE), which inhibits quenching pi-pi interactions and non-radiative motional deactivation by designing the morphology of the OSC. This study investigates the retention of AIE morphology during the operation of light-emitting electrochemical cells (LECs) and finds that AIE-LECs outperform ACQ-LECs due to intact AIE morphology and appropriate free-volume voids for ion transport and suppressed non-radiative excitonic deactivation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Ze Yu, Qiuying Li, Qian Ma, Wenpeng Ye, Zhongfu An, Huili Ma
Summary: Electro-fluorescent materials with 100% internal quantum efficiency and short fluorescence lifetimes can be achieved by harvesting high-lying triplet excitons. In this study, two excited-state descriptors, triplet-triplet energy gap ΔETT and oscillator strength f, were established to characterize exciton utilization efficiency, photoluminescence quantum yield, and fluorescence lifetime. High-throughput screening of over 5000 fluorophores predicted 19 candidate molecules with a high IQE (>90%), guided by these descriptors.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Tianhao Tan, Dong Wang
Summary: Transfer integral, a crucial parameter determining the charge mobility of organic semiconductors, can be efficiently predicted using machine learning models based on artificial neural networks. This study successfully developed such models for four typical organic semiconductor molecules and achieved high accuracy in predicting transfer integrals. By applying these models to study charge transport in organic crystals, the obtained results are in perfect agreement with quantum chemical calculations. Moreover, with the supplementation of more molecular packings representing the amorphous phase, these models can be refined to investigate charge transport in organic thin films with polymorphs and static disorders.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Thermodynamics
Yan Chen, Xinhua Wang, Huili Ma
Summary: This article introduces the tooth surface of dual-lead helical gear enveloping hourglass worm, which is a complex space enveloped surface with difference tooth profile, unequal pitch, and variable tooth thickness. To understand its geometry characteristics and precision manufacturing method, an analytical method for toroidal helix is presented. The mathematical model of toroidal helix is developed, and the geometry characteristics of helix angle, axial tooth thickness, and tooth surface undercutting are analyzed. The manufacturing and measuring method of toroidal helix is found to be effective and feasible through the manufacturing and testing of an hourglass worm sample.
ADVANCES IN MECHANICAL ENGINEERING
(2023)
Article
Materials Science, Multidisciplinary
Yixiao He, Jing Wang, Qiuying Li, Shuli Qu, Chifeng Zhou, Chengzhu Yin, Huili Ma, Huifang Shi, Zhengong Meng, Zhongfu An
Summary: A series of novel organic room-temperature phosphorescence (RTP) materials are developed based on indole luminophore, and the structure isomerism is regulated to enhance the intramolecular-space heavy-atom effect and promote high RTP efficiency. The fully occupied chlorine atoms at the positions 2 and 6 effectively favor the intramolecular effect, and the anti-parallel stacking in 26CIM further boosts RTP emission. The findings provide insights into the structure-performance relationship and a general strategy for constructing high-efficiency RTP materials.
ADVANCED OPTICAL MATERIALS
(2023)
Article
Optics
He Wang, Yuan Zhang, Chifeng Zhou, Xiao Wang, Huili Ma, Jun Yin, Huifang Shi, Zhongfu An, Wei Huang
Summary: Here, we present a concise and universal strategy for achieving photoactivated ultralong phosphorescence at room temperature through stereo-hindrance engineering. The dynamic photoactivated phosphorescence behavior is attributed to the suppression of non-radiative transitions and improvement of spin-orbit coupling (SOC) through the variation of molecular conformation. This study not only outlines a principle for designing dynamic phosphorescent materials, but also extends their utility in intelligent sensors and robotics.
LIGHT-SCIENCE & APPLICATIONS
(2023)
Article
Chemistry, Applied
Ze Yu, Yufeng Mao, Anqi Lv, Zhongfu An, Huili Ma
Summary: Organic fluorophores are crucial for organic optoelectronic and bioelectronic applications. The enhancement of fluorescence in bromo-organic aggregates, which breaks the traditional belief of heavy-atom effect leading to fluorescence quenching, is achieved by the limited acceleration of intersystem crossing process and the large reduction of vibronic coupling of singlet excitons caused by bromine atoms. The excited-state dynamics further demonstrate that bromine substituents decelerate the internal conversion process and result in slow ISC rates, leading to abnormal fluorescence enhancement.
Article
Chemistry, Inorganic & Nuclear
Xianwang Tao, Zhichao Yao, Aihua Zhou, Kaiqi Lv, Xuyu Gao, Jian Ye, Huili Ma, Youtian Tao
Summary: In this study, two octahedral cyclometalated Ir(III) complexes were designed and their coordination with DPPTBz resulted in increased optical absorption. When used as electron donor materials in organic solar cells, the complexes showed improved power conversion efficiency.
JOURNAL OF ORGANOMETALLIC CHEMISTRY
(2023)
Article
Multidisciplinary Sciences
Xiao Wang, Guowei Niu, Zixing Zhou, Zhicheng Song, Ke Qin, Xiaokang Yao, Zhijian Yang, Xiaoze Wang, He Wang, Zhuang Liu, Chengzhu Yin, Huili Ma, Kang Shen, Huifang Shi, Jun Yin, Qiushui Chen, Zhongfu An, Wei Huang
Summary: Organic scintillators, materials that emit luminescence when exposed to X-rays, have been gaining attention. However, improving both radioluminescence and X-ray absorption in organic scintillators has been challenging due to the waste of triplet excitons and weak X-ray absorption. In this study, halogenated thermally activated delayed fluorescence materials were used to simultaneously enhance triplet exciton utilization and X-ray absorption, resulting in efficient scintillation with a low detection limit. Experimental and theoretical analysis revealed the positive role of X-ray absorption, quantum yields of prompt fluorescence, and intersystem crossing in promoting radioluminescence intensity, offering opportunities for designing diverse organic scintillators and expanding the applications of thermally activated delayed fluorescence.
Article
Materials Science, Multidisciplinary
Jun-Cheng Yang, Zhiyuan Fu, Huili Ma, Tao Wang, Qiuying Li, Kai Wang, Lin Wu, Pu Chen, Hai-Tao Feng, Ben Zhong Tang
Summary: A novel emitter (DCzPy) was synthesized and its stimuli-responsive luminescence was studied. The emitter showed bluegreen fluorescence in the crystalline state, with dramatically enhanced and hypsochromic-shifted fluorescence upon gentle grinding. The emission wavelength returned to the original state after further heavy grinding. Under isotropic compression, the emitter exhibited a large bathochromic-shifted and weakened fluorescence. In addition, in the film state, the emission color of the emitter changed from green to blue as the temperature increased.
ACS MATERIALS LETTERS
(2023)
Article
Nanoscience & Nanotechnology
Jie Zhou, Yiwen Sun, Jin Zhang, Fusui Luo, Huili Ma, Min Guan, Junfen Feng, Xiaomeng Dong
Summary: In this study, a detection system based on the entropy-driven strand displacement reaction (ESDR) principle was developed for the sensitive detection of miR-193b and AflO42, biomarkers for early stage AD. The system consisted of a dumbbell detection probe (H), an indicator probe (R), and graphene oxide (GO). GO adsorbed free R and quenched fluorescence, enhancing the sensitivity of the system. The detection limits for miR-193b and AflO42 were 77 pM and 53 pM, respectively.
ACS APPLIED MATERIALS & INTERFACES
(2023)