Article
Chemistry, Physical
Jumi Park, Jooyoung Sung, Dongho Kim
Summary: In this study, the charge transfer (CT) processes in donor-pyreneacceptor (DPA) molecules were deciphered using various time-resolved spectroscopic measurements. The ultrafast CT rate of approximately 200 fs in DPA molecules was observed, indicating isoenergetic potential surfaces for LE and CT states. Strong electronic coupling between the LE and CT states was found upon the introduction of the acceptor to the pyrene moiety in DPA systems.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Applied
Fang-Zhou Li, Xing-Yu Li, Wenjun Ni, Zhi-Wei Wu, Changwei Lin, Gagik G. Gurzadyan, Gui-Chao Kuang
Summary: By finely tuning various parameters, the novel donor-acceptor-donor (D-A-D') type of BODIPY derivative BDP-1 exhibited single component white light emission (WLE), achieved through the balance between aggregation and energy transfer (ET) and intramolecular charge transfer (CT).
Article
Optics
Ines G. Tavares, Erki Enkvist, Joosep Kaimre, Asko Uri, Fernando B. Dias
Summary: This work investigates the intramolecular energy transfer between two thiophene donors and a perylene bisimide acceptor, demonstrating the transfer of energy from the thiophene donor's excited triplet state to the perylene bisimide acceptor's singlet state. The designed organic luminophore, ARC-1467, shows delayed fluorescence of perylene bisimide upon excitation of the donor unit, indicating the occurrence of energy transfer from the triplet state of the donor unit to the perylene bisimide acceptor.
JOURNAL OF LUMINESCENCE
(2021)
Article
Chemistry, Analytical
Roberto F. Delgadillo, Katie A. Carnes, Kathia Zaleta-Rivera, Omar Olmos, Lawrence J. Parkhurst
Summary: The time-resolved donor-detected Forster resonance energy transfer (trDDFRET) allows observation of molecular interactions within 10-100 angstrom region, while the time-resolved acceptor-detected FRET (trADFRET) can observe longer-range interactions. A new methodology based on trADFRET, namely FLIM-trADFRET, has been proposed to observe biological machinery in the range of 100-300 A in vivo. Proof of concept was demonstrated with a set of well-defined DNA scaffolds to evaluate this new methodology.
ANALYTICAL CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Chen Lu, Eunkyung Cho, Zhiyuan Cui, Yuhang Gao, Wenjuan Cao, Jean-Luc Bredas, Veaceslav Coropceanu, Feng Li
Summary: In contrast to closed-shell luminescent molecules, organic luminescent radicals have both spin doublet electronic states, resulting in spin-allowed radiative transitions. The efficiency and stability of donor-acceptor (D-A center dot) type luminescent radicals, which have a donor group covalently attached to an electron-withdrawing radical core, remain challenging to define. Experimental and theoretical results suggest that the luminescence efficiency and stability of the radicals are determined by the degree of conjugation and the number of imine nitrogen atoms in the substituents, with higher conjugation and lower number of imine nitrogen atoms leading to higher efficiency and stability.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Wenqi Xu, Lei Wei, Zhengxin Wang, Ruixue Zhu, Jiaming Jiang, Huiyan Liu, Juan Du, Tsu-Chien Weng, Yue-Biao Zhang, Yifan Huang, Weimin Liu
Summary: Understanding the excited state structural dynamics of conjugated molecules with A-D-A architecture is crucial for determining their performance in organic electronic devices. In this study, utilizing various spectroscopic methods and quantum chemical calculations, the unique fluorescence and charge transfer characteristics of AnDA molecule were observed, while removing the aldehyde group from TMDPAn resulted in loss of charge transfer properties.
JOURNAL OF PHYSICAL CHEMISTRY B
(2021)
Article
Chemistry, Physical
Chengxi Li, Xue Jin, Jianlei Han, Tonghan Zhao, Pengfei Duan
Summary: This article discusses the circularly polarized luminescence (CPL) activity of chiroptical materials, emphasizing the importance of increasing the dissymmetry factor glum value. Recent studies have shown that amplification of glum value can be achieved in hybrid donor-acceptor systems, providing new insights for the development of highly efficient CPL materials.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Multidisciplinary Sciences
Jianwei Shen, Ajay Jha, Meng Lv, Guanyu Jiang, Qixu Zhao, Zihui Liu, Jinquan Chen, Yan Yang, Haitao Sun, Hong-Guang Duan, Zhenrong Sun
Summary: Merocyanine dyes are of great interest due to their nonlinear optical properties and solvatochromism. In this study, the excited state dynamics of a merocyanine dye known as HB194 were investigated, revealing solvent-dependent charge transfer dynamics. The excited state decays in different solvents showed multi-exponential components, with polar solvents inducing conformationally relaxed intramolecular charge transfer states and nonpolar solvents exhibiting solvent-stabilized ICT states. An anomalously red-shifted emission was observed in ethylene glycol, which was attributed to the presence of molecular dimers. This work emphasizes the importance of gaining molecular-level insight into system-solvent interactions for designing next-generation merocyanine-based solvatochromic dyes.
SCIENTIFIC REPORTS
(2022)
Article
Chemistry, Multidisciplinary
Chao Wu, Weiqiang Liu, Kai Li, Gang Cheng, Jinfan Xiong, Teng Teng, Chi-Ming Che, Chuluo Yang
Summary: Intramolecular through-space charge-transfer (TSCT) excited states are utilized for developing thermally activated delayed fluorescence (TADF) emitters, with a series of precisely controlled TSCT emitters designed through alignment optimization of donor and acceptor segments. By increasing intramolecular pi-pi interactions, radiative decay rate of the lowest singlet excited state (S-1) is progressively enhanced with suppression of nonradiative decay, leading to significantly improved photoluminescence quantum yields of up to 0.99 in doped thin films. A high-efficiency electroluminescence device achieves a maximum external quantum efficiency (EQE) of 23.96% and maintains >20% at a brightness of 1000 cd m(-2), highlighting the importance of conformation control for high-efficiency intramolecular exciplex emitters.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Courtney A. DelPo, Saeed-Uz-Zaman Khan, Kyu Hyung Park, Bryan Kudisch, Barry P. Rand, Gregory D. Scholes
Summary: Enhanced delocalization is beneficial for absorbing molecules in organic solar cells, and polaritons offer exceptional delocalization that can improve the efficiency of bilayer organic photovoltaics by aiding in exciton delivery to the donor-acceptor interface. The decay of polaritons in bilayer cavities shows an additional pathway through charge transfer, indicating that the charge transfer from the polariton is fast enough to outcompete decay to the ground state.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Puja Agarwala, Enrique D. Gomez, Scott T. Milner
Summary: This study presents a coarse-graining method for simulating conjugated polymers, allowing for faster and more accurate investigation of their structure and properties. The method is validated through simulations of donor and acceptor polymers, which reveal the influence of interface width and slow cooling on polymer morphology.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Chemistry, Physical
Thomas P. P. Fay, David T. T. Limmer
Summary: In this paper, a physically motivated framework is proposed to describe spin-selective recombination processes in chiral systems. Spin-selective reaction operators for recombination reactions of donor-bridge-acceptor molecules are derived based on chirality and spin-orbit coupling. It is found that spin polarization selectivity only arises in hopping-mediated electron transfer. The framework presented here can be extended to describe spin-selective recombination processes in more complex systems.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
David Guzman, Ilias Papadopoulos, Giulia Lavarda, Parisa R. Rami, Rik R. Tykwinski, M. Salome Rodriguez-Morgade, Dirk M. Guldi, Tomas Torres
Summary: The study demonstrates the efficient energy transfer between a subporphyrazine and a pentacene dimer through intramolecular Forster resonance energy transfer and intramolecular singlet fission. The polarity of the solvent plays a crucial role in adjusting spectral overlap, ensuring a significant Forster rate constant, and maximizing triplet quantum yields.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Qing Ma, Zhen Cheng, Lei Yang, Wei Du, Yilin Yin, Wenqiang Ma, Guijuan Fan, Jinshan Li
Summary: By conducting domain-related data search and using combinatorial design, we have successfully developed a novel energetic material with excellent energy performance, safety performance, and thermal stability. This research may have significant implications for searching other high-performing energetic materials.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Haoyu Jing, Nikki Cecil M. Magdaong, James R. Diers, Christine Kirmaier, David F. Bocian, Dewey Holten, Jonathan S. Lindsey
Summary: Researchers have investigated energy transfer processes similar to those in photosynthetic systems by preparing synthetic bacteriochlorin-bacteriochlorin dyads. The use of a phenylethyne linker resulted in differential shifts in excited-state energies and efficient energy transfer. This study provides valuable insights for artificial photosynthesis and other processes requiring ultrafast energy transfer.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Luo Yan, Jiaojiao Zhu, Bao-Tian Wang, Junjie He, Hai-Zhi Song, Weibin Chu, Sergei Tretiak, Liujiang Zhou
Summary: The study reports the discovery of two-dimensional transition metal oxide materials beyond the MXene family, which exhibit superconducting, semiconducting, and light-harvesting properties. This expands the understanding of emerging phenomena in this field and provides a new platform for optoelectronic and photovoltaic applications.
Article
Multidisciplinary Sciences
Yu Zheng, Yulun Han, Braden M. Weight, Zhiwei Lin, Brendan J. Gifford, Ming Zheng, Dmitri Kilin, Svetlana Kilina, Stephen K. Doorn, Han Htoon, Sergei Tretiak
Summary: By controlling the morphology of the emitting sites, spin-selective photochemistry diversifies the tunability of carbon nanotube emission.
NATURE COMMUNICATIONS
(2022)
Article
Quantum Science & Technology
Yu Zhang, Lukasz Cincio, Christian F. A. Negre, Piotr Czarnik, Patrick J. Coles, Petr M. Anisimov, Susan M. Mniszewski, Sergei Tretiak, Pavel A. Dub
Summary: This study presents an approach to reduce quantum circuit complexity for electronic structure calculations. The method divides the qubit space into clusters and connects them using a new dressed Hamiltonian, enabling accurate simulation with fewer resources.
NPJ QUANTUM INFORMATION
(2022)
Article
Chemistry, Multidisciplinary
Hsinhan Tsai, Dibyajyoti Ghosh, Eli Kinigstein, Bogdan Dryzhakov, Honora Driscoll, Magdalena Owczarek, Bin Hu, Xiaoyi Zhang, Sergei Tretiak, Wanyi Nie
Summary: The dynamic structure changes in metal halide perovskite lattice upon photoexcitation and its impact on carrier transport properties in Ruddlesden-Popper phase perovskite thin films are reported in this study. Time-resolved X-ray scattering technique reveals rapid lattice expansion and slow relaxation over 100 ns after photoexcitation. The expansion is attributed to lattice thermal fluctuations caused by photon energy deposition. High laser powers induce strong local structural disorder, increasing the charge dissociation activation energy and leading to localized transport.
Article
Chemistry, Multidisciplinary
Hossein Goudarzi, Loukas Koutsokeras, Ahmed H. Balawi, Chen Sun, Giorgos K. Manolis, Nicola Gasparini, Yuan Peisen, Giannis Antoniou, Stavros Athanasopoulos, Charalampos C. Tselios, Polycarpos Falaras, Constantinos Varotsis, Frederic Laquai, Juan Cabanillas-Gonzalez, Panagiotis E. Keivanidis
Summary: This study investigates a solution-processed model green-to-blue triplet-triplet annihilation induced photon energy up-conversion (TTA-UC) binary composite. The solid-state microstructure of the composite is examined by a set of complementary characterization techniques. The results reveal the correlation between the composition of the composite and its photophysical properties, providing insights for the effective integration of functional TTA-UC interlayers.
Article
Chemistry, Multidisciplinary
Daniel Kroh, Stavros Athanasopoulos, Vojtech Nadazdy, Frank-Julian Kahle, Heinz Bassler, Anna Kohler
Summary: By measuring energy-resolved impedance and intrinsic photoconduction, this study investigates the dissociation of charge-transfer (CT) states in a PM6:Y6 solar cell. It finds that the Coulomb binding energy of the CT state is lower than expected due to hole delocalization and electron sharing among Y6 molecules. The temperature dependence of the photocurrent is not reflective of the CT state's binding energy because the dissociation process has a different activation energy and the saturation of dissociation yield occurs when the rate of dissociation exceeds the rate of intrinsic decay.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Mechanics
M. Serrano, K. Larkin, M. Ghommem, S. Tretiak, A. Abdelkefi
Summary: A multi-purpose energy harvesting microgyroscope system based on piezoelectric materials is proposed for small devices in remote areas. Numerical analysis shows that a system with a non-symmetric beam design is suitable for broadband energy harvesting. The nonlinear softening effects create a broadband frequency response with high voltage output, but careful selection of DC and AC voltages is necessary to avoid dynamic pull-in.
EUROPEAN JOURNAL OF MECHANICS A-SOLIDS
(2023)
Article
Mechanics
M. Serrano, K. Larkin, S. Tretiak, A. Abdelkefi
Summary: Most microelectromechanical systems (MEMS) are made from brittle materials that are prone to cracking. Understanding the potential influences cracks in MEMS is necessary for the longevity of these systems. This study developed an electromechanical model to capture the impacts of cracks on the performance of a damaged energy harvesting microgyroscope, and numerical methods were used to approximate the damage associated with distributed crack networks. The study revealed that cracks can significantly affect the static and dynamic behaviors of the microgyroscope energy harvester.
EUROPEAN JOURNAL OF MECHANICS A-SOLIDS
(2023)
Article
Chemistry, Physical
Hassiel Negrin-Yuvero, Victor M. Freixas, Dianelys Ondarse-Alvarez, Ana E. Ledesma, Sergei Tretiak, Sebastian Fernandez-Alberti
Summary: The photoexcitation, energy relaxation, and redistribution of a recently synthesized zigzag carbon nanobelt were studied using molecular dynamics simulations. The transition dipole moments and electronic transition density were found to gradually change during the internal conversion process. The electronic relaxation involved long-lived states with large energy gaps and changes in symmetry. These results provide insights into the excited-state properties of the zigzag nanobelt and can inspire the design of tailored nanobelts for specific nanoelectronic and photonic applications.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Chintam Hanmandlu, Rohan Paste, Hsinhan Tsai, Shyam Narayan Singh Yadav, Kuan-Wen Lai, Yen-Yu Wang, Chandra Shekar Gantepogu, Chen-Hung Hou, Jing-Jong Shyue, Yu-Jung Lu, Tushar Sanjay Jadhav, Jian-Ming Liao, Hsien-Hsin Chou, Hui Qi Wong, Chao-Sung Lai, Dibyajyoti Ghosh, Sergei Tretiak, Ta-Jen Yen, Hung-Ju Yen, Chih-Wei Chu
Summary: This study used a holistic interface strategy to enhance the efficiency and stability of perovskite solar cells by decreasing the number of interfacial defect states. The researchers utilized three-dimensional triphenylamine-based nanographene precursors to form a bridge between the perovskite film and the hole transport layer, resulting in improved performance characteristics.
Article
Chemistry, Physical
Hassiel Negrin-Yuvero, Victor M. Freixas, Dianelys Ondarse-Alvarez, Ana E. Ledesma, Sergei Tretiak, Sebastian Fernandez-Alberti
Summary: Progress in the synthesis of new carbon nanorings and nanobelts broadens the library of materials with unique structural and optical properties that can be attractive for further potential applications in host-guest chemistry, nanoelectronics, and photonics. In this study, we investigate the photoexcitation and subsequent energy relaxation and redistribution of a recently synthesized zigzag carbon nanobelt using nonadiabatic excited state molecular dynamics simulations. Our results reveal the excited-state dynamical properties of the zigzag-type nanobelt that differentiate this molecule from other nanobelts, providing insights for further designs tailored for specific nanoelectronic and photonic applications.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Multidisciplinary Sciences
Guoqing Zhou, Nicholas Lubbers, Kipton Barros, Sergei Tretiak, Benjamin Nebgen
Summary: Conventional machine learning models in computational chemistry predict molecular properties using quantum chemistry, but their accuracy degrades on larger or newer chemical systems. Incorporating quantum chemistry frameworks into machine learning models improves accuracy. This study demonstrates accurate prediction of various molecular properties on larger chemical systems by using machine-learned dynamic values in semiempirical quantum mechanics.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Physical
Laura Alfonso Hernandez, Victor M. Freixas, Beatriz Rodriguez-Hernandez, Sergei Tretiak, Sebastian Fernandez-Alberti, Nicolas Oldani
Summary: The effect of introducing a satellite tetraphenyl substitution on the structural and dynamical properties of cycloparaphenylene is studied. The results show that the substitution accelerates the electronic relaxation and induces efficient inter-band energy transfer and exciton self-trapping.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Aaron Forde, Victor M. Freixas, Sebastian Fernandez-Alberti, Amanda J. Neukirch, Sergei Tretiak
Summary: This article investigates a novel donor-acceptor molecular complex with dual fluorescence properties for charge transfer. Using time-dependent density functional theory, the alignment of excitonic and charge-transfer states is characterized, and the results are in agreement with experimental observations. This work is important for understanding and utilizing charge transfer processes.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Materials Science, Multidisciplinary
Dibyajyoti Ghosh, Carlos Mora Perez, Oleg Prezhdo, Wanyi Nie, Sergei Tretiak, Amanda J. Neukirch
Summary: Mixed A-cation halide perovskites have shown great potential for next-generation optoelectronic applications due to their attractive charge carrier transport properties and enhanced stability. In this study, we investigate the influence of A-cation mixing on the relaxation processes of hot charge carriers in FA(1-x)Cs(x)PbI(3) materials using nonadiabatic molecular dynamics and time-domain density functional theory methods. Our results demonstrate that the partial substitution of organic FA species with inorganic Cs cations significantly extends the relaxation times of hot electrons and hot holes. The understanding of the relationship between the dynamic structure and carrier relaxation allows us to propose rational design principles for enhancing the hot carrier lifetimes in photoactive materials.
JOURNAL OF MATERIALS CHEMISTRY C
(2022)