Archive for the ‘Hot Articles’ Category

How can cooling rate define the nature of nano-structures formed using block copolymers?

Block copolymers (BCPs) consist of amphiphilic molecules that can self-assemble in selective solvents and generate various types of nano- and micro-dimensional structures. The unique self-assembly process is low-cost and relatively straight forward in solution phase.  The final structures have morphological diversity and complexity.  These self-assembled structures have been widely used in various applications such as drug delivery, catalysis, and water purification. The self-assembly process follows a heating step for dissolution of all the components and a subsequent cooling step. Both the steps and the parameters are vital for final structural characteristics of the assembled structures. A group of scientists from two esteemed universities in Canada recently studied the effects of rate of cooling in the self-assembly process.

Schematic representation of how cooling rate can change the morphology of formed micellar structures using PFS BCP and homopolymers

The authors used a systematic approach to explain the influence of cooling rate on micelle morphologies for a series of PFS based BCPs. The cooling rate greatly influences the size and the shape of colloidal structures. Rapid cooling increases branching and opens a new avenue to manipulate micelle morphologies. The study finds that rapid cooling reduces crystallinity, as polymer chains do not have enough time to pack in ordered structures.

The authors standardized sample preparation protocol and then varied the cooling times, with quick cooling of 2.5 min producing flower like structures and median cooling time of 50 mins leading to the same structural features with larger size. Co-self-assembly of homopolymer BCP mixtures with variable cooling rate also shows that quick cooling generates uniform sized branched micellar structures with elongated central platelets whereas slow cooling led to a long single fiber with a dark circle platelet in the centre.

With several examples and optimization conditions, the effect of cooling in the formation of self-assembled micellar structures has been evaluated. The main outcome of this study is that the cooling rate is another parameter to manipulate crystallization-driven self-assembly and to control micelle morphologies. There exists a lot of possibilities to use the findings and apply them to generate BCPs with a crystallizable block with important optical or electronic properties.

For details, please visit the entire article at https://doi.org/10.1039/D1SC05937H

About the author:

Dr Damayanti Bagchi is a postdoctoral researcher in Irene Chen’s lab at University of California, Los Angeles, United States. She obtained her PhD in Physical Chemistry from Satyendra Nath Bose National Centre for Basic Sciences, India. Her research is focused on spectroscopic studies of nano-biomaterials. She is interested in exploring light enabled therapeutics. She enjoys food and experimenting with various cuisines, which she found resembles products/ side products of chemical reactions!

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Chemical Science HOT Articles: October 2021

New month, new HOT articles!

We are pleased to share a selection of our referee-recommended HOT articles for October 2021. We hope you enjoy reading these articles, congratulations to all the authors whose articles are featured! As always, Chemical Science is free to read & download.

You can explore our full 2021 Chemical Science HOT Article Collection here!

Browse a selection of our October HOT articles below:

Quantification of the charge transport processes inside carbon nanopipettes
Rujia Liu, Yingfei Ma, Xiaoyue Shena and Dengchao Wang
Chem. Sci., 2021,12, 14752-14757

Artificial transmembrane signal transduction mediated by dynamic covalent chemistry
Carlo Bravin, Nol Duindama and Christopher A. Hunter
Chem. Sci., 2021,12, 14059-14064

Pair distribution function and 71Ga NMR study of aqueous Ga3+ complexes
Ida Gjerlevsen Nielsen, Sanna Sommer, Ann-Christin Dippel, Jørgen Skibsted and Bo Brummerstedt Iversen
Chem. Sci., 2021,12, 14420-14431

General stereoretentive preparation of chiral secondary mixed alkylmagnesium reagents and their use for enantioselective electrophilic aminations
Alexander Kremsmair, Henrik R. Wilke, Matthias M. Simon, Quirin Schmidt, Konstantin Karaghiosoff and Paul Knochel
Chem. Sci., 2022, Advance Article

Inhibition of (dppf)nickel-catalysed Suzuki–Miyaura cross-coupling reactions by α-halo-N-heterocycles
Alasdair K. Cooper, Megan E. Greaves, William Donohoe, Paul M. Burton, Thomas O. Ronson, Alan R. Kennedy and David J. Nelson
Chem. Sci., 2021,12, 14074-14082

Impact of symmetry-breaking of non-fullerene acceptors for efficient and stable organic solar cells
Peddaboodi Gopikrishna, Huijeong Choi, Do Hui Kim, Jun Ho Hwang, Youngwan Lee, Hyeonwoo Jung, Gyeonghwa Yu, Telugu Bhim Raju, Eunji Lee, Youngu Lee, Shinuk Cho and BongSoo Kim
Chem. Sci., 2021,12, 14083-14097

 

Chemical Science, Royal Society of Chemistry

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A new class of bioluminescent substrate-enzyme pair for deep tissue multi-colour imaging

Bioluminescent enzymes (luciferases) generate light via the oxidation of small molecule luciferins. The process is highly specific and accurate even at heterogeneous environment. Luciferin-luciferases based imaging technique is highly appreciated for specificity in tracking cell movements, cell proliferation, and numerous other features in living organisms.

Imaging of in-depth organ tissues requires emission at NIR region for effective penetration through tissue layer. There existed a big gap in successful synthesis followed by appropriate multiplexed imaging application of bioluminescent pairs. Researchers from University of California, Irvine recently developed a unique class of orthogonal, NIR emitting luciferins that could promise more accessible, long-wavelength bioluminescent pairs for in-vivo imaging.

Fig. 1 Red-emitting orthogonal bioluminescent probes designed from fluorophores. (a) D-Luciferin is oxidized by firefly luciferase (Fluc) to produce oxyluciferin and a photon of light. (b) Coumarin fluorophores were used as templates for red-shifted luciferins. (c) Retrosynthetic analysis of the CouLuc-1 analogs.

The authors focused on a new class of luciferins (CouLuc-1s) comprising both an elongated pi-system and a 4-tri-fluoromethylcoumarin unit (Fig 1). The synthesis follows two-step route to bridge the fluorescent coumarin heterocycle with the key thiazoline unit necessary for luciferin bioluminescence. The small size of the coumarin core require only minimal enzyme engineering to identify complementary luciferases that were identified via a parallel engineering approach.

Fig. 2 Multi-component imaging with three NIR-emitting probes.

The brightest luciferase-CouLuc-1 pair exhibited higher luminescent signals compared to native bioluminescent probes and can be immediately adopted for biological imaging. Multiplexed NIR imaging could also be attained using three different analogues of the newly prepared luciferins (Fig 2). In a broader sense, synthesis of novel luminophores from simple fluorophores pave a step forward in the bioluminescent imaging field.

For details: please visit https://pubs.rsc.org/en/content/articlelanding/2021/sc/d1sc03114g

About the blogger:

Dr. Damayanti Bagchi is a postdoctoral researcher in Irene Chen’s lab at University of California, Los Angeles, United States. She has obtained her PhD in Physical Chemistry from Satyendra Nath Bose National Centre for Basic Sciences, India. Her research is focused on spectroscopic studies of nano-biomaterials. She is interested in exploring light enabled therapeutics. She enjoys travelling and experimenting with various cuisines.

You can find her on Twitter at @DamayantiBagchi.

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Chemical Science HOT Articles: August 2021

New month, new HOT articles!

We are pleased to share a selection of our referee-recommended HOT articles for August 2021. We hope you enjoy reading these articles, congratulations to all the authors whose articles are featured! As always, Chemical Science is free to read & download.

You can explore our full 2021 Chemical Science HOT Article Collection here!

Browse a selection of our August HOT articles below:

Nickel-catalyzed reductive coupling of unactivated alkyl bromides and aliphatic aldehydes
Cole L. Cruz and John Montgomery
Chem. Sci., 2021, Advance Article

Single-crystal-to-single-crystal synthesis of a pseudostarch via topochemical azide–alkyne cycloaddition polymerization
Arthi Ravi, Amina Shijad and Kana M. Sureshan
Chem. Sci., 2021, Advance Article

Catalytic enantioselective synthesis of 1,4-dihydropyridines via the addition of C(1)-ammonium enolates to pyridinium salts
Calum McLaughlin, Jacqueline Bitai, Lydia J. Barber, Alexandra M. Z. Slawin and Andrew D. Smith
Chem. Sci., 2021, Advance Article

Albumin-targeting of an oxaliplatin-releasing platinum(iv) prodrug results in pronounced anticancer activity due to endocytotic drug uptake in vivo
Hemma Schueffl, Sarah Theiner, Gerrit Hermann, Josef Mayr, Philipp Fronik, Diana Groza, Sushilla van Schonhooven, Luis Galvez, Nadine S. Sommerfeld, Arno Schintlmeister, Siegfried Reipert, Michael Wagner, Robert M. Mader, Gunda Koellensperger, Bernhard K. Keppler, Walter Berger, Christian R. Kowol, Anton Legin and Petra Heffeter
Chem. Sci., 2021, Advance Article

Two-step anti-cooperative self-assembly process into defined π-stacked dye oligomers: insights into aggregation-induced enhanced emission
Yvonne Vonhausen, Andreas Lohr, Matthias Stolte and Frank Würthner
Chem. Sci., 2021, Advance Article

β-Trioxopyrrocorphins: pyrrocorphins of graded aromaticity
Nivedita Chaudhri, Matthew J. Guberman-Pfeffer, Ruoshi Li, Matthias Zeller and Christian Brückner
Chem. Sci., 2021, Advance Article

 

Chemical Science, Royal Society of Chemistry

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Chemical Science HOT Articles: July 2021

New month, new HOT articles!

We are pleased to share a selection of our referee-recommended HOT articles for July 2021. We hope you enjoy reading these articles, congratulations to all the authors whose articles are featured! As always, Chemical Science is free to read & download.

You can explore our full 2021 Chemical Science HOT Article Collection here!

Browse a selection of our July HOT articles below:

Physically inspired deep learning of molecular excitations and photoemission spectra
Julia Westermayr and Reinhard J. Maurer
Chem. Sci., 2021, Advance Article

Synthesis and enantioseparation of chiral Au13 nanoclusters protected by bis-N-heterocyclic carbene ligands
Hong Yi, Kimberly M. Osten, Tetyana I. Levchenko, Alex J. Veinot, Yoshitaka Aramaki, Takashi Ooi, Masakazu Nambo and Cathleen M. Crudden
Chem. Sci., 2021, Advance Article

A copper-free and enzyme-free click chemistry-mediated single quantum dot nanosensor for accurate detection of microRNAs in cancer cells and tissues
Zi-yue Wang, Dong-ling Li, Xiaorui Tian and Chun-yang Zhang
Chem. Sci., 2021, Advance Article

Azanone (HNO): generation, stabilization and detection
Cecilia Mariel Gallego, Agostina Mazzeo, Paola Vargas, Sebastián Suárez, Juan Pellegrino and Fabio Doctorovich
Chem. Sci., 2021, Advance Article

Coumarin luciferins and mutant luciferases for robust multi-component bioluminescence imaging
Zi Yao, Donald R. Caldwell, Anna C. Love, Bethany Kolbaba-Kartchner, Jeremy H. Mills, Martin J. Schnermann and Jennifer A. Prescher
Chem. Sci., 2021, Advance Article

Conformational interplay in hybrid peptide–helical aromatic foldamer macrocycles
Sebastian Dengler, Pradeep K. Mandal, Lars Allmendinger, Céline Douat and Ivan Huc
Chem. Sci., 2021, Advance Article

Chemical Science, Royal Society of Chemistry

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Watch out for artifacts in your next multi-colour fluorescence imaging experiment

The discovery of super resolution microscopy, followed by the announcement of 2014 Chemistry Nobel prize, facilitated a great expansion in the use of multi colour fluorescence imaging to study cellular or sub-cellular systems. Super resolution localization microscopy requires highly photostable, sufficiently bright fluorophores to achieve the blinking which is necessary to distinguish individual fluorophores within the diffraction limit. To validate all these criteria, organic dyes are a most obvious choice as fluorophores. However, chemical conversion of organic dyes upon prolonged laser exposure exhibit multicolour image artifacts leading to false-positive colocalization. Researchers from Pohang University, South Korea demonstrate a detailed protocol to understand and avoid such artifacts.

The researchers labelled cell membrane using far-IR dye (A647) which shows a red photoluminescence. But surprisingly, upon photobleaching of the A647 dye, which is blue in colour, it turned to red. This photobleached product also emits at red region, coinciding with the original emission of A647. This phenomenon is called blue-conversion. A range of commonly used organic dyes are evaluated for blue-conversion occurrences which indicates cyanine dyes show multiple blue-converted species. Interestingly, among all the dye groups there is not a single group that exhibit no blue-conversion at all.

Blue-conversion of far-red organic dyes upon photobleaching. A647 dissolved in DMSO before (left) and after (right) photobleaching using direct laser illumination. (a) TIRF images of A647-EGFR on COS7 cells in the far-red (upper panels) channel excited at 642 nm and the red (lower panels) channel excited at 561 nm before (left panels) and after (right panels) photobleaching of A647-EGFR.

The researchers also study multicolour fluorescence imaging by colocalization of two well-known dyes. They have observed that the single-molecule brightness of the blue-converted species contributed to the production of the artifact in the reconstructed images. Finally, they concluded sufficient care must be taken in multicolour imaging applications, including colocalization, and other fluorescence-based multi-well plate format assays, to prevent false positives produced by blue-conversion of organic dyes.

Although they primarily discussed the negative effect of the blue-conversion of organic dyes, they are also hopeful to use this new photoconversion pathway of cyanine dyes for advantages of fluorescence imaging applications. They propose that super-resolution techniques require the photoactivation of organic dyes, which might exert some undesirable effects in live cells. However, the photoactivation of the blue-converted species occurs without any external stimuli and can be inferred as an advantage for super resolution techniques.

For details please read: https://doi.org/10.1039/D1SC00612F

About the blogger:

Dr. Damayanti Bagchi is a postdoctoral researcher in Irene Chen’s lab at University of California, Los Angeles, United States. She has obtained her PhD in Physical Chemistry from Satyendra Nath Bose National Centre for Basic Sciences, India. Her research is focused on spectroscopic studies of nano-biomaterials. She is interested in exploring light enabled therapeutics. She enjoys travelling and experimenting with various cuisines.

You can find her on Twitter at @DamayantiBagchi.

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Chemical Science HOT Articles: June 2021

New month, new HOT articles!

We are pleased to share a selection of our referee-recommended HOT articles for June 2021. We hope you enjoy reading these articles, congratulations to all the authors whose articles are featured! As always, Chemical Science is free to read & download.

You can explore our full 2021 Chemical Science HOT Article Collection here!

Browse a selection of our June HOT articles below:

[GaF(H2O)][IO3F]: a promising NLO material obtained by anisotropic polycation substitution
Qian-Ming Huang, Chun-Li Hu, Bing-Ping Yang, Zhi Fang, Yuan Lin, Jin Chen, Bing-Xuan Li and Jiang-Gao Mao
Chem. Sci., 2021, Advance Article

Photocleavable proteins that undergo fast and efficient dissociation
Xiaocen Lu, Yurong Wen, Shuce Zhang, Wei Zhang, Yilun Chen, Yi Shen, M. Joanne Lemieux and Robert E. Campbell
Chem. Sci., 2021, Advance Article

Electrochemically switchable polymerization from surface-anchored molecular catalysts
Miao Qi, Haochuan Zhang, Qi Dong, Jingyi Li, Rebecca A. Musgrave, Yanyan Zhao, Nicholas Dulock, Dunwei Wang and Jeffery A. Byers
Chem. Sci., 2021, Advance Article

Flow electrochemistry: a safe tool for fluorine chemistry
Bethan Winterson, Tim Rennigholtz and Thomas Wirth
Chem. Sci., 2021, Advance Article

Biomimetic enterobactin analogue mediates iron-uptake and cargo transport into E. coli and P. aeruginosa
Robert Zscherp, Janetta Coetzee, Johannes Vornweg, Jörg Grunenberg, Jennifer Herrmann, Rolf Müller and Philipp Klahn
Chem. Sci., 2021, Advance Article

Sensitization-initiated electron transfer via upconversion: mechanism and photocatalytic applications
Felix Glaser, Christoph Kerzig and Oliver S. Wenger
Chem. Sci., 2021, Advance Article
Chemical Science, Royal Society of Chemistry

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Chemical Science HOT Articles: May 2021

New month, new HOT articles!

We are pleased to share a selection of our referee-recommended HOT articles for May 2021. We hope you enjoy reading these articles, congratulations to all the authors whose articles are featured! As always, Chemical Science is free to read & download.

You can explore our full 2021 Chemical Science HOT Article Collection here!

Browse a selection of our May HOT articles below:

Aromatic side-chain flips orchestrate the conformational sampling of functional loops in human histone deacetylase 8
Vaibhav Kumar Shukla, Lucas Siemons, Francesco L. Gervasio and D. Flemming Hansen
Chem. Sci., 2021, Advance Article

Blue-conversion of organic dyes produces artifacts in multicolor fluorescence imaging
Do-Hyeon Kim, Yeonho Chang, Soyeon Park, Min Gyu Jeong, Yonghoon Kwon, Kai Zhou, Jungeun Noh, Yun-Kyu Choi, Triet Minh Hong, Young-Tae Chang and Sung Ho Ryu
Chem. Sci., 2021, Advance Article

Controllable DNA strand displacement by independent metal–ligand complexation
Liang-Liang Wang, Qiu-Long Zhang, Yang Wang, Yan Liu, Jiao Lin, Fan Xie and Liang Xu
Chem. Sci., 2021, Advance Article

Spatial-confinement induced electroreduction of CO and CO2 to diols on densely-arrayed Cu nanopyramids
Ling Chen, Cheng Tang, Kenneth Davey, Yao Zheng, Yan Jiao and Shi-Zhang Qiao
Chem. Sci., 2021, Advance Article

Manipulating valence and core electronic excitations of a transition-metal complex using UV/Vis and X-ray cavities
Bing Gu, Stefano M. Cavaletto, Daniel R. Nascimento, Munira Khalil, Niranjan Govind and Shaul Mukamel
Chem. Sci., 2021, Advance Article

Chemical Science, Royal Society of Chemistry

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Chemical domain image recognition using autocatalysis

A reaction in which one of the products speeds up further product formation is called an autocatalytic reaction. Autocatalysis plays an important role in living systems including DNA replication, apoptosis, and even in the origin of life, due to self-sustaining growth and oscillation. Researchers from Brown University employ this nature of autocatalytic click chemistry to generate an artificial neural network that can be used for image classification.

Autocatalytic reaction rate depends on the concentration of product and shows a non-linear dependency of product formation with progress in reaction time. In this view, a network of autocatalytic reactions is analogous to an artificial neural network. An artificial neuron is a basic learning unit, inspired by biological neurons, which multiplies it’s inputs by a set of weights and transforms their sum through a nonlinear operator. Researchers used this resemblance to formulate a winner-take-all neural network.

Fig 1: Kinetics of autocatalysis. (a) Reagent and autocatalytic product evolution over time (b) Rate of product concentration change over time for the reaction simulated in a, showing the accelerated production typical of an autocatalytic process.

Copper-catalyzed azide–alkyne cycloaddition (CuAAC) reaction was chosen for autocatalysis as it is fast, can occur under mild conditions and produce high yield. Also, CuAAC reaction involves colored copper–ligand complexes and can be quantitatively monitored using UV-vis spectroscopy.

In a winner-take-all neural network, winner is determined by it’s achievement to reach to a particular condition. Here, they have used the reaction half-way point (t1/2) as the condition of image classification. Experiment wise, they have used automated liquid handling equipment to remove a certain volume and then added it together into individual pools for potential image class. The pool that reaches the transition time first is determined as the winner.

Fig 2: An overview of the copper (C) catalyzed azide–alkyne cycloaddition reaction, showing the buildup of triazole branches on the amine backbone of (A) after each azide (B) incorporation. The threebranched product (D) catalyzes its own generation by promoting the reduction of Cu(II). Experimental setup for evaluating a chemical WTA network (Right: upper panel). (Right lower panel) Network training and in silico simulation. (a) Example images from each of the considered classes. (b) Trained weights for each class.  

This study shows an interesting adaptation of autocatalysis as a platform for non-linear activation function necessary for artificial neural network classification. The findings are expected to improve future development of chemical-domain computing systems.

 

For further details, please go through:

Leveraging autocatalytic reactions for chemical domain image classification

Christopher E. Arcadia, Amanda Dombroski, Kady Oakley, Shui Ling Chen, Hokchhay Tann, Christopher Rose, Eunsuk Kim, Sherief Reda, Brenda M. Rubensteinb and Jacob K. Rosenstein*

Chem. Sci., 2021, 12, 5464

 

About the blogger

Dr Damayanti Bagchi is a postdoctoral researcher in Irene Chen’s lab at University of California, Los Angeles, United States. She has obtained her PhD in Physical Chemistry from Satyendra Nath Bose National Centre for Basic Sciences, India. Her research is focused on spectroscopic studies of nano-biomaterials. She is interested in exploring light enabled therapeutics. She enjoys travelling and experimenting with various cuisines, which she found resembles with products/ side products of chemical reactions!

You can find her on Twitter at @DamayantiBagchi.

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Chemical Science HOT Articles: April 2021

New month, new HOT articles!

We are pleased to share a selection of our referee-recommended HOT articles for April 2021. We hope you enjoy reading these articles, congratulations to all the authors whose articles are featured! As always, Chemical Science is free to read & download.

You can explore our full 2021 Chemical Science HOT Article Collection here!

 

Browse a selection of our April HOT articles below:

Reaction-based machine learning representations for predicting the enantioselectivity of organocatalysts
Simone Gallarati, Raimon Fabregat, Rubén Laplaza, Sinjini Bhattacharjee, Matthew D. Wodrich and Clemence Corminboeuf
Chem. Sci., 2021, Advance Article

Deaminative meta-C–H alkylation by ruthenium(ii) catalysis
Wen Wei, Hao Yu, Agnese Zangarelli and Lutz Ackermann
Chem. Sci., 2021, Advance Article

Prediction and mitigation of mutation threats to COVID-19 vaccines and antibody therapies
Jiahui Chen, Kaifu Gao, Rui Wang and Guo-Wei Wei
Chem. Sci., 2021, Advance Article

Recent advances in single atom catalysts for the electrochemical carbon dioxide reduction reaction
Jincheng Zhang, Weizheng Cai, Fang Xin Hu, Hongbin Yang and Bin Liu
Chem. Sci., 2021, Advance Article

Wavy graphene sheets from electrochemical sewing of corannulene
Carlo Bruno, Eleonora Ussano, Gianni Barucca, Davide Vanossi, Giovanni Valenti, Edward A. Jackson, Andrea Goldoni, Lucio Litti, Simona Fermani, Luca Pasquali, Moreno Meneghetti, Claudio Fontanesi, Lawrence T. Scott, Francesco Paolucci and Massimo Marcaccio
Chem. Sci., 2021, Advance Article

Oxidative additions of alkynyl/vinyl iodides to gold and gold-catalyzed vinylation reactions triggered by the MeDalphos ligand
Jessica Rodriguez, Alexis Tabey, Sonia Mallet-Ladeira and Didier Bourissou
Chem. Sci., 2021, Advance Article

 

Chemical Science, Royal Society of Chemistry

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