Article
Chemistry, Organic
Emily P. Bacher, Kevin J. Koh, Antonio J. Lepore, Allen G. Oliver, Olaf Wiest, Brandon L. Ashfeld
Summary: A phosphorus(III)-mediated dearomatization of ortho-substituted dianiline squaraine dyes led to the formation of exotic benzofuranone and oxindole scaffolds with a linear side chain comprised of an enol, a phosphorus ylide, and 2,4-disubstituted aniline. Mechanistic evaluation revealed a significant dependence on the acidity of the aniline ortho substituent, with the rearrangement adducts reverting back to the parent squaraine in the presence of a Bronsted acid.
Article
Chemistry, Multidisciplinary
Frederik Unger, Luca Moretti, Julian Hausch, Jona Bredehoeft, Clemens Zeiser, Sara Haug, Roel Tempelaar, Nicholas J. Hestand, Giulio Cerullo, Katharina Broch
Summary: In this study, we investigated a blend of the prototypical SF chromophore pentacene by engineering the polarizability of the molecular environment. We found that vibrational modes near 1150 cm-1 play a key role in facilitating ultrafast SF in pentacene.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Materials Science, Multidisciplinary
Bao-Ning Li, Jia-Jun Wang, Peng-Yan Fu, Shi-Cheng Wang, Mei Pan
Summary: Platinum(ii) complexes with controllable color emission exhibit highly emissive properties and interesting fluorescence characteristics under different conditions, making them suitable for barcode modules and logo design. Furthermore, these complexes can achieve high brightness and quantum efficiency when used as emitting materials in solid-state lighting applications.
JOURNAL OF MATERIALS CHEMISTRY C
(2021)
Article
Chemistry, Multidisciplinary
James H. May, Jeff M. Van Raden, Ruth L. Maust, Lev N. Zakharov, Ramesh Jasti
Summary: In this study, a series of mechanically interlocked carbon nanostructures were synthesized using an active-template method. By catalyzing the reactions between a [n]cycloparaphenylene precursor macrocycle and metal ions, fully pi-conjugated catenanes and a [3]rotaxane were obtained. The developed synthetic method of mechanically interlocked carbon nanostructures can contribute to the understanding of the implications of mechanical bonding and provide insights into the structure-property relationships.
Article
Chemistry, Multidisciplinary
Rishi Shivhare, Gareth John Moore, Andreas Hofacker, Sebastian Hutsch, Yufei Zhong, Mike Hambsch, Tim Erdmann, Anton Kiriy, Stefan C. B. Mannsfeld, Frank Ortmann, Natalie Banerji
Summary: A study of a blend of low-optical-gap diketopyrrolopyrrole polymer and a fullerene derivative with near-zero driving force for electron transfer was conducted using femtosecond transient absorption and electroabsorption spectroscopy. Ultrafast electron transfer was observed, along with significant charge recombination and short excited and CT state lifetimes. Density functional theory calculations confirmed the effects of back-transfer and CT hybridization on charge recombination, while simulations showed potential strategies to increase free charge yield despite short lifetimes.
ADVANCED MATERIALS
(2022)
Editorial Material
Chemistry, Multidisciplinary
Daehyun Ahn, Nowshin Kabir, Thirumurugan Prakasam, Ali Trabolsi
Summary: The development of analytical tools over the past three decades has enabled the study of increasingly complex mechanically inter-locked molecules. The first synthesis of a [2]catenane by Edel Wasserman in 1960 was controversial due to the lack of experimental evidence. Recently, Leigh et al. re-examined this pioneering synthesis using modern techniques, confirming its structure in the Journal of the American Chemical Society.
Article
Chemistry, Inorganic & Nuclear
Caiyun Liu, Chang Gao, Amir Said, Huihui Niu, Dexin Wang, Chen-Ho Tung, Yifeng Wang
Summary: Catenane, rotaxane, and pseudorotaxane molecules based on a cyclic titanium oxide cluster and cyclic/linear alkylammonium cations were synthesized and shown to remain intact in acidic water, promising for assembling inorganic-organic hybrid supramolecular structures in water.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Physical
Hehe Zhang, Jan Mischke, Wolfgang Mertin, Gerd Bacher
Summary: This paper provides an overview of the current status of graphene-based transparent conductive electrodes in GaN-based LEDs. It focuses on manufacturing progress and the resulting properties of the fabricated devices, discussing the impact of graphene-based transparent conductive electrodes on current spreading and contact resistance, as well as future challenges and perspectives on the use of graphene in GaN-based LEDs.
Article
Chemistry, Inorganic & Nuclear
Grace Turner, Andrew Docker, Paul D. Beer
Summary: A novel halogen bonding (XB) motif has been successfully incorporated into a [2]rotaxane using a discrete chloride anion template directed clipping methodology. Anion titration experiments show that the interlocked host can strongly bind halide and sulfate oxoanions in competitive aqueous-organic solvent mixtures. Compared to a hydrogen bonding rotaxane analogue, the XB rotaxane exhibits a preference towards lighter halides Cl- ≈ Br- > SO42- > I-.
DALTON TRANSACTIONS
(2021)
Article
Chemistry, Multidisciplinary
Ruben Canton-Vitoria, Ajyal Z. Alsaleh, Georgios Rotas, Yusuke Nakanishi, Hisanori Shinohara, Francis D'Souza, Nikos Tagmatarchis
Summary: In this article, the versatility of free-base and zinc-metallated porphyrin to combine with boron azadipyrromethene NIR absorbing species and anchor onto graphene was introduced. The results showed that the zinc-metallated porphyrin confirmed additional charge separation between the chromophores, while graphene acted as an electron donor in the hybrids, forming charge-separated states at an ultrafast timescale. These donor-acceptor systems featuring graphene as an electron donor have potential applications in optoelectronics.
Article
Chemistry, Multidisciplinary
Jamie T. T. Wilmore, Yuen Cheong Tse, Andrew Docker, Caspar Whitehead, Charlotte K. K. Williams, Paul D. D. Beer
Summary: A series of dynamic metalloporphyrin [2]rotaxane molecular shuttles were synthesized with high yield using active metal template synthetic methodology. The dynamic macrocycle translocation is controlled by an inter-component co-ordination interaction between the macrocycle pyridyl and axle Zn(II) metalloporphyrin. The shuttling behavior can be inhibited by a neutral Lewis base, but can be tuned through rotaxane demetallation or subsequent metallation.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Dong Li, Xiaoxiao He, Litao Zhao, Haoyang Li, Xiaolei Zhang, Jinquan Chen, Qingyuan Jin, Jianhua Xu
Summary: Graphene and its derivatives can be assembled with organic dyes to create composite materials for photovoltaic and photocatalytic assemblies. The quenching mechanisms of fluorescence in RdB-GO and RdB-RGO were investigated, revealing that the electron transfer process was more effective in RdB-RGO due to a change in energy levels caused by GO reduction. This suggests that RdB-RGO composite materials may have higher application values for dye-sensitized solar cells.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Materials Science, Multidisciplinary
Marvin T. Unruh, Ullrich Scherf, Hilke Bahmann, Ana Clara B. Rodrigues, Carla Cunha, J. Sergio Seixas de Melo, Jakob Schedlbauer, John M. Lupton
Summary: A new conjugated ladder polymer PAL with a polyacene skeleton was synthesized via an Aldol-type condensation protocol, showing differences in photophysical properties compared to MeLPPP. The behavior of PAL was found to be influenced by solvent mixtures, displaying remarkable molecular shape heterogeneity as revealed by single molecule spectroscopy.
JOURNAL OF MATERIALS CHEMISTRY C
(2021)
Article
Chemistry, Physical
Aloke Bapli, Aninda Chatterjee, Rajesh Kumar Gautam, Souvik Pandit, Rabindranath Jana, Debabrata Seth
Summary: This report studied the binding interaction between 7-(N, N'-diethylamino)coumarin-3-carboxylic add (7-DCCA) and bovine serum albumin (BSA), and investigated the impact of graphene oxide (GO) on this interaction. Various spectroscopic, microscopic, and isothermal titration calorimetric (ITC) methods, as well as molecular docking studies, were employed to probe the binding interaction. The results showed a strong complexation between 7-DCCA and BSA, with changes in absorption and emission intensity indicating the binding effect.
JOURNAL OF MOLECULAR LIQUIDS
(2021)
Article
Engineering, Electrical & Electronic
H. M. Abd El-daim, F. A. Taher, N. S. Morsy, G. M. Turky, A. A. Ali
Summary: Through surface modification with reduced graphene oxide (rGO), pure and blend fabrics showed enhanced electrical conductivity, making them suitable for various potential applications in smart textiles, such as sensing, energy storage, and conversion devices.
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
(2021)
Article
Materials Science, Multidisciplinary
Haidong Liang, Yuan Chen, Chengyuan Yang, Kenji Watanabe, Takashi Taniguchi, Goki Eda, Andrew A. Bettiol
Summary: This study demonstrates the generation of spin defects with high PL intensity and ODMR contrast using high-energy helium ion beams, while maintaining a small linewidth, thereby achieving good sensitivity. By comparing different fluences of helium irradiations, an optimal fluence is determined that can create spin defects without damaging the overall crystal lattice structure. Furthermore, with a focused beam, such spin defects can be created deterministically with nanometer precision.
ADVANCED OPTICAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Chaofei Liu, Xiuying Zhang, Xinyun Wang, Ziying Wang, Ibrahim Abdelwahab, Ivan Verzhbitskiy, Yan Shao, Goki Eda, Wanxin Sun, Lei Shen, Kian Ping Loh
Summary: A systematic study of the ferroelectric properties in 2D materials NbOX2 (X = Cl, I) reveals that NbOCl2 exhibits stronger ferroelectricity than NbOI2. The presence of 1D collinear ferroelectric strips is observed in NbOCl2. Scanning tunneling microscopy (STM) imaging provides insights into the unreconstructed atomic structures of NbOX2 surfaces, while scanning tunneling spectroscopy probes the electronic states induced at defect (vacancy) sites.
Article
Chemistry, Multidisciplinary
He Zhu, Qiang Chen, Igor Roncevic, Kirsten E. Christensen, Harry L. Anderson
Summary: In this study, a series of fully edge-fused porphyrin-anthracene oligomeric ribbons (dimer and trimer) were synthesized, and the corresponding infinite polymer was computationally studied. The porphyrin dimer and trimer were synthesized in high yield via oxidative cyclodehydrogenation of singly linked precursors using DDQ and TfOH. The crystal structure of the dimer showed a flat central π-system with a slight S-shaped wave distortion at each porphyrin terminal. The results demonstrate the potential for longer π-conjugated nanoribbons with integrated metalloporphyrin units.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Marcin A. Majewski, Wojciech Stawski, Jeff M. Van Raden, Michael Clarke, Jack Hart, James N. O'Shea, Alex Saywell, Harry L. Anderson
Summary: We demonstrate the synthesis of a macrocycle composed entirely of 5,15-linked porphyrins, providing insights into electronic delocalization and motivation for creating larger nanorings with closely spaced porphyrin units. The nanoring was constructed using a covalent six-armed template and consists of six edge-fused zinc(II) porphyrin dimer units and six un-fused nickel(II) porphyrins. STM imaging confirmed the size and shape of the spoked 18-porphyrin nanoring on a gold surface.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Andrew T. Frawley, Kathryn G. Leslie, Virginia Wycisk, Silvia Galiani, Dilip Shrestha, Christian Eggeling, Harry L. Anderson
Summary: A switchable solvatochromic fluorescent dyad enables the mapping of lipid ordering in vesicle membranes with higher resolution than the diffraction limit. By combining a Nile Red fluorophore with a photochromic spironaphthoxazine quencher, fluorescence can be controlled using visible light via photoswitching and FRET quenching. Synthetic lipid vesicles of different compositions were imaged with an average 2.5-fold resolution enhancement compared to confocal images. Ratiometric detection was used to probe membrane polarity and distinguish domains of different lipid ordering within the same membrane.
Article
Chemistry, Multidisciplinary
Yuan Chen, Haidong Liang, Leyi Loh, Yiwei Ho, Ivan Verzhbitskiy, Kenji Watanabe, Takashi Taniguchi, Michel Bosman, Andrew A. Bettiol, Goki Eda
Summary: We observe bound exciton (BX) complex manifolds in monolayer MoSe2 with intentionally created monoselenium vacancies (VSe) using proton beam irradiation. The emission intensity of different BX peaks exhibits contrasting dependence on electrostatic doping near the onset of free electron injection. These complexes, which are more strongly bound than trions and biexcitons, survive up to around 180 K and show moderate valley polarization memory, indicating partial free exciton character.
Article
Multidisciplinary Sciences
Maya Khela, Maciej Dabrowski, Safe Khan, Paul S. Keatley, Ivan Verzhbitskiy, Goki Eda, Robert J. Hicken, Hidekazu Kurebayashi, Elton J. G. Santos
Summary: In this study, the ability to generate different types of spin textures in the 2D van der Waals magnet CrGeTe3 and achieve reversible transformation between them using ultrafast laser excitation is demonstrated. Atomistic spin dynamics simulations and wide-field Kerr microscopy measurements show that high-intense laser pulses can generate different spin textures within the picosecond regime. The phase transformation between the different spin textures can be controlled by external magnetic fields through additional laser pulses. These results indicate the potential of laser-driven spin textures as a pathway to reconfigurable topological architectures at the atomistic level.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Anatol Prudnikau, Hossein Roshan, Fabian Paulus, Beatriz Martin-Garcia, Rene Huebner, Houman Bahmani Jalali, Manuela De Franco, Mirko Prato, Francesco Di Stasio, Vladimir Lesnyak
Summary: Cadmium mercury selenide (CdHgSe) nanocrystals with controlled shape and heterostructure design show improved optical properties. A colloidal synthesis method is developed to synthesize CdHgSe/ZnCdS core/shell nanoplatelets with tunable emission wavelength. These nanoplatelets exhibit low turn-on voltage and high external quantum efficiency in light-emitting diodes.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Polymer Science
Xiangyan Yu, Pietro Steiner, Qichen Zhou, Coskun Kocabas, Han Zhang, Dimitrios G. Papageorgiou, Oliver Fenwick, Haixue Yan, Michael John Reece, Emiliano Bilotti
Summary: In order to enhance the thermal conductivity of polymer dielectrics, we have developed a composite film with high thermal conductivity and high breakdown strength by introducing thermally conductive and electrically insulating fillers. Through finite element simulation, we have demonstrated that our material can significantly reduce the operating temperature of devices while maintaining other properties.
Article
Chemistry, Multidisciplinary
Gabriel Merino, Miquel Sola, Israel Fernandez, Cina Foroutan-Nejad, Paolo Lazzeretti, Gernot Frenking, Harry L. Anderson, Dage Sundholm, Fernando P. Cossio, Marina A. Petrukhina, Jishan Wu, Judy I. Wu, Albeiro Restrepo
Summary: Aromaticity is a deeply rooted concept in chemistry, but there is no consensus on its definition due to the many attributes associated with it. This perspective aims to reflect the current state and future direction of the aromaticity research community.
Article
Chemistry, Multidisciplinary
Sili Qiu, Andrew T. T. Frawley, Kathryn G. G. Leslie, Harry L. L. Anderson
Summary: In this study, the photophysical and photochemical properties of eight dithienylethenes with different substitution patterns were investigated. The electron-donor or -acceptor substituents in push-pull dithienylethenes caused a shift in their absorption spectra to the near-infrared region. The pull-pull systems exhibited the highest quantum yields for both ring-closure and ring-opening, and a water-soluble dithienylethene showed excellent fatigue resistance and potential for biological applications.
Article
Materials Science, Multidisciplinary
Erica Sutcliffe, Xingjian Sun, Ivan Verzhbitskiy, Theodor Griepe, Unai Atxitia, Goki Eda, Elton J. G. Santos, J. Olof Johansson
Summary: Femtosecond optical control of magnetic materials shows promise for future ultrafast data storage devices. Broadband probing in the visible spectrum enables the extraction of the magneto-optical spectrum of electrons in the conduction band in the two-dimensional van der Waals ferromagnet Cr2Ge2Te6 (CGT). The magneto-optical signal in CGT is a sum of contributions from electrons in the conduction and valence bands, which can lead to an erroneous interpretation regarding the magnetization direction after excitation.
Article
Chemistry, Multidisciplinary
Dongxu Zhu, Houman Bahmani Jalali, Gabriele Saleh, Francesco Di Stasio, Mirko Prato, Nefeli Polykarpou, Andreas Othonos, Sotirios Christodoulou, Yurii P. Ivanov, Giorgio Divitini, Ivan Infante, Luca De Trizio, Liberato Manna
Summary: The synthesis of InAs@ZnSe core@shell nanocrystals with adjustable shell thickness was optimized, resulting in improved emission efficiency. A high quantum yield was achieved when the shell thickness was at least 3ML. Moreover, the photoluminescence lifetime remained stable, while the Auger recombination time increased with increasing shell thickness.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Zilu Liu, Md Azimul Haque, Chris N. Savory, Tianjun Liu, Satoru Matsuishi, Oliver Fenwick, David O. Scanlon, Martijn A. Zwijnenburg, Derya Baran, Bob C. Schroeder
Summary: Poly(nickel-benzene-1,2,4,5-tetrakis(thiolate)) (Ni-btt) and poly(nickel-benzene-1,2,3,4-tetrakis(thiolate)) (Ni-ibtt) are isomers with different backbone geometries. Ni-ibtt exhibits slightly higher solubility and an increased bandgap compared to Ni-btt. The most significant difference lies in their thermoelectric properties, with Ni-btt showing p-type behavior and Ni-ibtt demonstrating n-type carrier characteristics.
FARADAY DISCUSSIONS
(2023)
Article
Chemistry, Organic
Wojciech Stawski, Jeff M. Van Raden, Connor W. Patrick, Peter N. Horton, Simon J. Coles, Harry L. Anderson
Summary: V-shaped porphyrin dimers undergo efficient oxidative coupling to form cyclic porphyrin oligomers, with curved walls. The strain in the macrocycle bends the p-phenylene and fused porphyrin dimer units, but does not significantly alter the electronic structure of the fused porphyrins.
