Article
Chemistry, Multidisciplinary
Xiaobo Yu, Liangliang Chen, Cheng Li, Chenying Gao, Xiang Xue, Xisha Zhang, Guanxin Zhang, Deqing Zhang
Summary: This paper reports terpolymers as intrinsically stretchable polymeric semiconductors with good ductility and high charge mobility by incorporating non-centrosymmetric spiro-fluorene units into the backbone of DPP-based conjugated polymers. These terpolymers exhibit high crack onset strains, reduced tensile moduli, and high charge mobilities (>1.0 cm2 V-1 s-1) at 100% strain, even after repeated stretching and releasing cycles. Among them, terpolymer P2, with cyclopropane linked to the spiro-fluorene unit, has the highest reported mobility of 3.1 cm2 V-1 s-1 at 150% strain and 1.4 cm2 V-1 s-1 after 1000 cycles of stretching and releasing.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
John McGrady, Shinichi Yamashita, Sho Kano, Huilong Yang, Hiroaki Abe
Summary: The study found that the presence of oxides affects the decay behavior of hydrated electrons, with Fe2O3 slowing down the decay rate and ZrO2 increasing it, while Cr2O3 had negligible effect. The electron yield for all oxide/water mixtures was higher compared to pure water, indicating electron transfer from the oxides to the water.
RADIATION PHYSICS AND CHEMISTRY
(2021)
Article
Chemistry, Physical
Hung H. Nguyen, Vyacheslav S. Bryantsev, Claudio J. Margulis
Summary: Recent research has shown that excess electrons in high-temperature molten salts can react with the salts and form new species, including nanoparticles. This study investigates the fate of an excess electron in molten ZnCl2 and identifies three different states in which the electron can exist. Each state can be characterized by its own electronic spectrum.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Physical
Mohammed G. Kotp, Ahmed M. Elewa, Ahmed F. M. EL-Mahdy, Ho-Hsiu Chou, Shiao-Wei Kuo
Summary: Conjugated microporous polymers (CMPs) are promising light harvesters for photocatalytic H2 evolution due to their simple preparation and various band gaps. By selecting different geometries of multibrominated monomers, four triphenylpyridine-based CMPs were synthesized with controlled electron enrichment, porosities, and optoelectronic properties. Among them, TPP-Py CMP exhibited the highest photocatalytic performance under visible light irradiation, with high surface area, thermal stability, hydrogen production rate, and quantum yield.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Yifei Jiang, Haobin Chen, Xiaoju Men, Zezhou Sun, Zhen Yuan, Xuanjun Zhang, Daniel T. Chiu, Changfeng Wu, Jason McNeill
Summary: A novel multimode superresolution method was developed to map the structure and measure the energy landscape of single carrier transport along conjugated polymer nanowires. By quenching of local emission and tracking the motion of a single photogenerated hole using blinking-assisted localization microscopy, the method successfully correlated structures with charge transport properties. The efficiency of inter- and intrachain hole transport inside the nanowires was compared, and the depth of carrier traps from torsional disorder and chemical defects was directly measured for the first time.
Article
Polymer Science
Gui-Sheng Jiao, Yuanshuo Zhang, He Cheng, Tongfei Shi, Zhi-Chao Yan
Summary: Charge transport in conjugated polymers is influenced by both static structure and dynamics of backbone segments. Molecular dynamics simulations are used to study regiorandom poly(3-alkylthiophenes) (P3ATs) with 6-12 alkyl carbons per side chain. The effect of temperature and side chain length on the static structure is investigated, revealing that the peak at q & SIM; 0.42 & ANGS;(-1) is due to edge-to-edge packing along the side-chain direction and shifts to lower q with longer side chains. The peak at q & SIM; 1.35 & ANGS;(-1) is contributed by intrachain side chain-side chain correlation and interchain correlation on the face-to-face stacking direction. Moreover, longer side chains result in faster backbone dynamics, with the carbon atoms farther from the backbone exhibiting faster motion. The last three atoms near the end of the alkyl side chain play a significant role in the faster motion of the backbone.
Article
Materials Science, Multidisciplinary
Yilin Song, Jiamin Ding, Xiaojuan Dai, Cheng Li, Chong-an Di, Deqing Zhang
Summary: In this study, a new strategy to enhance the thermoelectric performance of n-doped semiconducting polymers was demonstrated. The introduction of linear alkyl chains in a conjugated donor-acceptor polymer based on n-doped naphthalenediimide (NDI) led to films with higher electrical conductivity and power factor. These results provide a new molecular design rationale for the future development of high-performance n-type thermoelectric semiconducting polymers.
ACS MATERIALS LETTERS
(2022)
Article
Chemistry, Physical
Nan Luo, Peng Ren, Yu Feng, Xiangfeng Shao, Hao-Li Zhang, Zitong Liu
Summary: This article focuses on the side-chain modulation of conjugated polymers and evaluates their effects on the performance of OFETs. The challenges and potential applications of functional high-performance OFETs through side-chain engineering are also discussed.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Polymer Science
Chunhui Liu, Chengyi Xiao, Jing Wang, Baiqiao Liu, Yidi Hao, Jiayi Guo, Jiali Song, Zheng Tang, Yanming Sun, Weiwei Li
Summary: High-molecular-weight conjugated polymers were successfully obtained through the introduction of long-branched alkyl chains and optimization of polymerization conditions. These polymers exhibited excellent mechanical properties and high efficiencies in organic solar cells.
Article
Materials Science, Multidisciplinary
Massimiliano Comin, Vincent Lemaur, Andrea Giunchi, David Beljonne, Xavier Blase, Gabriele D'Avino
Summary: Depending on the sample preparation protocol, doped semi-crystalline polymers can have different structures, leading to different charge-transport and thermoelectric properties. In this study, accurate hybrid quantum-classical calculations were used to explore the intricate relationship between structure and properties, taking into account the effect of the environment. The findings reveal that the position of dopants in the polymer lamellae significantly affects their electron affinity, and the orbital overlap between dopants in different regions of the polymer determines the charge-transfer states. Moreover, the interaction between the charge carrier and the ionized dopants is influenced by the dopant position.
JOURNAL OF MATERIALS CHEMISTRY C
(2022)
Article
Materials Science, Multidisciplinary
Christian Kupfer, Vincent M. Le Corre, Chaohui Li, Larry Lueer, Karen Forberich, Masashi Kato, Andres Osvet, Christoph J. Brabec
Summary: To accurately assess the properties of metal halide perovskites, a combination of time-resolved photoluminescence and microwave photoconductivity measurements is used. This approach allows for a rapid extraction of material properties, such as recombination rate constants and mobility ratio, by incorporating a rate-equation model into a fitting algorithm. The inclusion of microwave photoconductivity measurements enhances the accuracy of estimation and provides valuable information about trap-assisted recombination. This method is crucial for improving the efficiency of solar devices.
JOURNAL OF MATERIALS CHEMISTRY C
(2023)
Article
Nanoscience & Nanotechnology
Artur P. Herman, Szymon J. Zelewski, Kamil Misztal, Robert Kudrawiec
Summary: In this study, long-lived free charge carriers generated from excitons in MoS2, MoSe2, WS2, and WSe2 crystals were observed using TRMC for the first time. The lifetime of these carriers depends on surface and defect states as well as surface band bending.
Article
Chemistry, Multidisciplinary
Narayanaswamy Kamatham, Olzhas A. Ibraikulov, Pablo Durand, Jing Wang, Olivier Boyron, Benoit Heinrich, Thomas Heiser, Patrick Leveque, Nicolas Leclerc, Stephane Mery
Summary: This study reports the impact of functionalizing four different semiconducting polymer structures with linear siloxane-terminated side-chains, showing that the substitution of alkyl chains with siloxane chains significantly influences the properties of the polymers. The increase in pi-stacking overlap of the polymer backbones leads to enhanced charge mobility values. Additionally, different siloxane chains have distinct effects on the polymer structure.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Nanoscience & Nanotechnology
Fang Yao, Qianqian Lin
Summary: Metal halide perovskites are promising optoelectronic materials with excellent properties and success in photovoltaics. Recent studies have shown that mixing lower-dimensional cations within perovskites can help improve their stability. However, the charge carrier transport properties in mixed 2D/3D perovskites are still not fully understood.
Article
Polymer Science
Yuchai Pan, Jianyao Huang, Dong Gao, Zhihui Chen, Weifeng Zhang, Gui Yu
Summary: Semiconducting polymers play a crucial role in both industrial and academic purposes, with ongoing research focusing on the structure-performance relationship. By improving structural engineering, new semiconducting polymers with enhanced properties can be developed. Through studying a series of diketopyrrolopyrrole-based polymers with different alkyl chain lengths, a strong correlation between electrical performance and alkyl side chain was observed, leading to a comprehensive understanding of design rules for high-performance semiconductor materials.
Article
Chemistry, Physical
Francisco Manteiga Vazquez, Qianli Yu, Lars F. Klepzig, Laurens D. A. Siebbeles, Ryan W. Crisp, Jannika Lauth
Summary: Colloidal PbS nanoplatelets (NPLs) with a cubic crystal structure were studied for their photoexcited excitons characteristics and dynamics, with their photoluminescence quantum yield significantly enhanced after CdCl2 treatment. Surface treatment and exciton-phonon interactions were utilized to control and improve the optical properties of IV-VI semiconductor NPLs.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Pieter Schiettecatte, Deepika Poonia, Ivo Tanghe, Sourav Maiti, Michele Failla, Sachin Kinge, Zeger Hens, Laurens D. A. Siebbeles, Pieter Geiregat
Summary: In this study, the nature and dynamics of charge carriers in highly crystalline liquid-phase exfoliated ReS2 were analyzed using a unique combination of experimental techniques. Two distinct time regimes were identified, both dominated by unbound charge carriers despite a high exciton binding energy. The results indicate the potential of ReS2 to produce mobile free charge carriers, which is relevant for photovoltaic applications.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Sourav Maiti, Deepika Poonia, Pieter Schiettecatte, Zeger Hens, Pieter Geiregat, Sachin Kinge, Laurens D. A. Siebbeles
Summary: The study found that in a bilayer of ReS2 and tetracene, the transfer of photoexcited states from ReS2 to triplet states in tetracene occurred within 5 ps with an efficiency near 38%. This opens up new possibilities for heterostructure design of two-dimensional materials with suitable organics to produce long-lived triplets. Triplets have potential applications in optoelectronics, photovoltaics, photocatalysis, and photon upconversion.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Deepika Poonia, Nisha Singh, Jeff J. P. M. Schulpen, Marco van der Laan, Sourav Maiti, Michele Failla, Sachin Kinge, Ageeth A. Bol, Peter Schall, Laurens D. A. Siebbeles
Summary: We studied the exciton properties of the Mo0.6W0.4S2 alloy compared to pure MoS2 and WS2. The energy and line width of the exciton peaks in optical transmission spectra were found to decrease and increase, respectively, with increasing temperature. The exciton-phonon interactions in the alloy were closer to MoS2 than WS2, suggesting a larger amplitude of exciton wave functions on Mo atoms. TDDFT calculations successfully reproduced the experimental absorption spectra and indicated that Mo and W atoms are uniformly distributed among all layers in the alloy.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Yingying Tang, Deepika Poonia, Marco van der Laan, Dolf Timmerman, Sachin Kinge, Laurens D. A. Siebbeles, Peter Schall
Summary: This study investigates the optical properties and ultrafast carrier dynamics of assembled perovskite nanocrystals (NCs) known as supercrystals (SCs). The results show that SCs exhibit a red shift in absorption and photoluminescence (PL) peak, signatures of collective band-like states, smaller Stokes shift, decreased biexciton binding energy, and increased carrier cooling rates. These findings highlight the potential of assembled perovskite NCs in optoelectronic device applications.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Indy du Fosse, Jence T. Mulder, Guilherme Almeida, Anne G. M. Spruit, Ivan Infante, Ferdinand C. Grozema, Arjan J. Houtepen
Summary: One of the most promising properties of lead halide perovskite nanocrystals is their defect tolerance. However, studies have shown that deep trap states can still be created by dangling bonds on surface bromide ions. This research uses density functional theory calculations to show that surface bromide sites experience a destabilizing local electrostatic potential, which pushes their dangling orbitals into the bandgap. The addition of ions can electrostatically passivate these deep trap states without covalently binding to the nanocrystal surface.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Editorial Material
Chemistry, Multidisciplinary
Ferdinand C. Grozema
Summary: Photoredox catalysts show promise in high energy requirement reactions, but the influence of solvent and counter ions is not fully understood. A microwave-based technique provides direct insight into their effects on charge reorganization during catalysis.
Article
Chemistry, Physical
Zimu Wei, Abbey M. Philip, Wolter F. . Jager, Ferdinand C. Grozema
Summary: This study investigates the photodynamics of perylenemonoimide-p-oligophenylene-dimethylaniline molecular dyads, revealing anomalous distance dependence of charge separation rate as a function of donor-acceptor distance.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Luca Ornago, Jerry Kamer, Maria El Abbassi, Ferdinand C. Grozema, Herre S. J. van der Zant
Summary: Switching effects play a crucial role in the design and characterization of nanoscale molecular electronics systems. This study investigates the presence of switching events in reference molecular systems and highlights the importance of proper anchoring group selection and comparison with reference compounds in understanding the origin of switching in molecular break junctions.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Michele Failla, Fransisco Garcia Florez, Bastiaan B. V. Salzmann, Daniel Vanmaekelbergh, Henk T. C. Stoof, Laurens D. A. Siebbeles
Summary: In this study, the initial nature and relaxation of photoexcited electronic states in CdSe nanoplatelets were investigated using ultrafast transient optical absorption measurements and theoretical analysis. It was found that the initial quantum yields of excitons and charge carriers vary with photon energy, and thermal relaxation occurs within 1 ps. No signatures of biexcitons or larger complexes were observed up to the highest average number of absorbed photons per NPL in the experiments.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Jorrit Bleeker, Aron P. Kahn, Lorenz M. Baumgartner, Ferdinand C. Grozema, David A. Vermaas, Wolter F. Jager
Summary: Spatiotemporal pH imaging using fluorescence lifetime imaging microscopy (FLIM) is an excellent technique for investigating dynamic (electro)chemical processes. However, current probes for FLIM are not suitable for high pH values. In this study, we developed dedicated pH probes based on 1-methyl-7-amino-quinolinium fluorophore, which possesses high fluorescence lifetime and quantum yield, (photo)stability, and water solubility. The flexible fluorophore-spacer-receptor architecture allows tunable probe lifetimes in the pH range of 5.5-11, and deprotonation of the aromatic amine at the quinolinium core enables additional fluorescence lifetime response at pH values of 11-13.
Article
Chemistry, Physical
Zimu Wei, Jence T. Mulder, Rajeev K. Dubey, Wiel H. Evers, Wolter F. Jager, Arjan J. Houtepen, Ferdinand C. Grozema
Summary: Understanding the kinetics and energetics of photophysical processes in perovskite-chromophore hybrid systems is crucial for their applications in optoelectronics, photocatalysis, and light-harvesting. By investigating the charge transfer mechanism between CsPbBr3 nanoplatelets and surface-anchored perylene derivatives, we have shown that the CT rate can be controlled by tuning the CT driving force. Our findings provide insights into the photophysics of perovskite-molecule systems and offer guidelines for tailoring these hybrid systems for specific applications.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Nanoscience & Nanotechnology
Marco van der Laan, Edwin Heemskerk, Floris Kienhuis, Nella Diepeveen, Deepika Poonia, Sachin Kinge, Minh Triet Dang, Van An Dinh, Laurens D. A. Siebbeles, Anna Isaeva, Jorik van de Groep, Peter Schall
Summary: Rhenium disulfide is a unique 2D van der Waals material with anisotropy and weak interlayer interactions, confining excitons within single atomic layers. The influence of different interlayer coupling on excitonic properties in AA and AB-stacked rhenium disulfide is explored using polarization-dependent optical measurements. The results show that while the excitonic properties are largely determined by in-plane interactions, they are strongly modified by interlayer coupling, making ReS2 an excellent platform for studying stacking as a tuning parameter for 2D materials. Additionally, its optical anisotropy makes it an interesting candidate for polarization-sensitive applications.
Article
Chemistry, Physical
Michele Failla, Fransisco Garcia Florez, Bastiaan B. V. Salzmann, Daniel Vanmaekelbergh, Henk T. C. Stoof, Laurens D. A. Siebbeles
Summary: We studied the initial nature and relaxation of photoexcited electronic states in CdSe nanoplatelets (NPLs) using ultrafast transient optical absorption measurements and theoretical analysis. The quantum yields of heavy-hole (HH) excitons, light-hole (LH) excitons, and charge carriers vary strongly with photon energy, while thermal relaxation occurs within 1 ps. We observed no signs of biexcitons or larger complexes, except when a probe-generated exciton interacted with a previously produced exciton.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Sourav Maiti, Laurens D. A. Siebbeles
Summary: In this Perspective, recent advances in harvesting triplets for photovoltaic and photon upconversion applications are overviewed. The two angles discussed are singlet fission-sensitized solar cells and triplet-triplet annihilation upconversion using transition metal dichalcogenides (TMDCs) and organic semiconductors.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
