Thalappil Pradeep

Bio: Thalappil Pradeep is an academic researcher from Indian Institute of Technology Madras. The author has contributed to research in topics: Cluster (physics) & Mass spectrometry. The author has an hindex of 76, co-authored 581 publications receiving 24664 citations. Previous affiliations of Thalappil Pradeep include DST Systems & Lawrence Berkeley National Laboratory.

Facile Crystallization of Ice Ih via Formaldehyde Hydrate in Ultrahigh Vacuum under Cryogenic Conditions

Abstract: Although hexagonal ice (ice Ih) is the most common and highly studied crystalline form of ice, its nucleation from clathrate hydrates is poorly understood. Here, we report the formation of ice Ih t...

A Covalently Integrated Reduced Graphene Oxide–Ion-Exchange Resin Electrode for Efficient Capacitive Deionization

Abstract: DOI: 10.1002/admi.202001998 terms of equipment and energy consumption.[6,8–11] Capacitive deionization (CDI) is an emerging technology which involves adsorption and desorption of ions on the electrode surface by application of low potential difference (≈1.2–1.8 V) across a pair of porous carbon electrodes, thereby making it both energy and cost-efficient compared to other existing desalination methods. When a flowing water stream is passed across a CDI system, cations and anions move toward oppositely charged electrodes and get adsorbed on them, thereby generating deionized and ‘drinkable’ water, starting from brackish water. Subsequently, adsorbed ions can be removed from the electrode by reversing the polarity, thereby regenerating the electrode surface, ready for reuse for next adsorption cycle.[5] Thus, clean water can be produced continuously by repeating the adsorption and desorption cycles. CDI is a cost-effective, point-of-use method with a high theoretical desalination efficiency.[5] However, its practical applications for desalination are yet to be recognized at a large scale, and research is being carried out to synthesize new materials with improved adsorption capacities.[5,12–14] Related technologies such as Faradaic deionization and the use of different 2D materials in CDI are also explored intensely.[15–17] Various carbonaceous materials and their composites are being used as CDI electrodes because of their high salt adsorption capacities in the range of several mg g−1.[18–25] Graphene, and graphene-derivatized materials, such as, graphene-like nanoflakes,[26] activated carbon,[27] activated carbon nanofiber (ACF),[28] reduced graphene oxide (rGO),[27,29] carbon nanotubes (CNT),[29] graphene–CNT composites,[29,30] rGO–ACF,[28] 3D macroporous graphene architectures,[31] sponge-templated graphene,[14] graphene–Fe3O4, graphene chitosan–Mn3O4, rGO–activated carbon composites,[27] and functionalized graphene nanocomposite,[34] have been used as CDI electrodes. The adsorption capacities of graphenic composites, such as graphene/carbon nanotube, CO2 activated rGO, sulfonic functional graphite nanosheets, SO3H/NH2 graphene/activated carbon, MgAl-Ox/G nanohybrids, 3D-graphene architecture, and graphene sponge measured were 1.4, 6.26, 8.6, 10.3, 13.6, Capacitive deionization (CDI) is an emerging, cost-effective alternative for energy-efficient desalination technology. Efficient electrode materials based on individual reduced graphene oxide (rGO) nanosheets are produced by functionalizing them with polystyrene (rGO–PS) through an in situ polymerization process involving rGO, styrene monomer, and divinylbenzene. The rGO–PS-integrated composite nanostructures are subsequently functionalized with sulfonate and quaternary amine functionalities to achieve positively and negatively charged electro-adsorbent ion-exchange resins (EAIERs), respectively. These EAIERs ‘molecular constructs’ are used to fabricate CDI electrodes, and deionization is performed to remove various ions. These molecular constructs promote faster charge transfer at the electrode–electrolyte interface and maintained the electrical conductivity of the active rGO. This leads to a high electroadsorption capacity of 15.93 mg g−1 of Cl− using NaCl solution with a conductivity of 802 μS in laboratory batch experiments, which is approximately five times higher than the adsorption capacity of rGO electrodes reported earlier (≈2–3 mg g−1) in comparable experimental conditions. No significant Faradaic redox reactions or chemical changes are observed on the electrode surface, which make these electrodes exhibit excellent electrochemical stability even after multiple adsorption/desorption cycles.

A facile method to fabricate carbon nanostructures via the self-assembly of polyacrylonitrile/poly(methyl methacrylate-b-polyacrylonitrile) AB/B′ type block copolymer/homopolymer blends

Abstract: The self-assembly and high temperature behavior of AB/B′ type block copolymer/homopolymer blends containing polyacrylonitrile (PAN) polymers were studied for the first time. Here, microphase separated nanostructures were formed in the poly(methyl methacrylate-b-polyacrylonitrile) (PMMAN) block copolymer and their blends with homopolymer PAN at various blend ratios. Additionally, these nanostructures were transformed into porous carbon nanostructures by sacrificing PMMA blocks via pyrolysis. Spherical and worm like morphologies were observed in both TEM and AFM images at different compositions. The thermal and phase behavior examinations showed good compatibility between the blend components in all studied compositions. The PAN homopolymer (B′) with a comparatively higher molecular weight than the corresponding block (B) of the block copolymer is expected to exhibit ‘dry brush’ behavior in this AB/B′ type system. This study provides a basic understanding of the miscibility and phase separation in the PMMAN/PAN system, which is important in the nanostructure formation of bulk PAN based materials with the help of block copolymers to develop advanced functional materials.

Interaction of Carboxylic Acids and Water Ice Probed by Argon Ion Induced Chemical Sputtering

Abstract: In this paper, we investigated the interaction of simple carboxylic acids, formic acid (FA), acetic acid (AA), and propionic acid (PA) with thin layers of water ice in the temperature range of 110-190 K in ultrahigh vacuum. The focus, however, is on the AA-ice system. Molecularly thin layers of these systems were prepared on a pre-cooled polycrystalline copper substrate. The interactions and phase changes in the system were monitored with chemical sputtering using low-energy (≤30 eV) Ar + , which probes the topmost surface layers. At 110 K, the deposited AA exists as dimers in its amorphous solid form. At the same temperature, in the presence of water ice, this dimeric form gets converted to chainlike oligomers. Chemical sputtering spectra show distinct features for these two surface species. The data suggest that ion formation reflects the surface structure, implying a unique mechanism for its formation. Detailed studies have been made with amorphous solid water (ASW) and crystalline water (CW) to get a complete understanding of the system. Experiments carried out with AA-D 2 O ice confirmed the proton-transfer mechanism during chemical sputtering. Other studies were conducted with AA-CH 3 OH and AA-CCl 4 systems. Detailed investigations performed to understand the effect of thickness of AA and ice overlayers suggest that the extent of water molecules required to effect the structural transformation in the acid is dependent on the amount of the latter. Dimeric-to-oligomeric transformation does not occur for the PA-ice system. Detection of a structural transition at the very top of ice in molecularly thin films adds additional capabilities to the low-energy ion scattering technique.

I and i

Abstract: There is, I think, something ethereal about i —the square root of minus one. I remember first hearing about it at school. It seemed an odd beast at that time—an intruder hovering on the edge of reality. Usually familiarity dulls this sense of the bizarre, but in the case of i it was the reverse: over the years the sense of its surreal nature intensified. It seemed that it was impossible to write mathematics that described the real world in …

Fast parallel algorithms for short-range molecular dynamics

Abstract: Three parallel algorithms for classical molecular dynamics are presented. The first assigns each processor a fixed subset of atoms; the second assigns each a fixed subset of inter-atomic forces to compute; the third assigns each a fixed spatial region. The algorithms are suitable for molecular dynamics models which can be difficult to parallelize efficiently—those with short-range forces where the neighbors of each atom change rapidly. They can be implemented on any distributed-memory parallel machine which allows for message-passing of data between independently executing processors. The algorithms are tested on a standard Lennard-Jones benchmark problem for system sizes ranging from 500 to 100,000,000 atoms on several parallel supercomputers--the nCUBE 2, Intel iPSC/860 and Paragon, and Cray T3D. Comparing the results to the fastest reported vectorized Cray Y-MP and C90 algorithm shows that the current generation of parallel machines is competitive with conventional vector supercomputers even for small problems. For large problems, the spatial algorithm achieves parallel efficiencies of 90% and a 1840-node Intel Paragon performs up to 165 faster than a single Cray C9O processor. Trade-offs between the three algorithms and guidelines for adapting them to more complex molecular dynamics simulations are also discussed.

疟原虫var基因转换速率变化导致抗原变异[英]／Paul H, Robert P, Christodoulou Z, et al//Proc Natl Acad Sci U S A

Abstract: 抗原变异可使得多种致病微生物易于逃避宿主免疫应答。表达在感染红细胞表面的恶性疟原虫红细胞表面蛋白1（PfPMP1）与感染红细胞、内皮细胞、树突状细胞以及胎盘的单个或多个受体作用，在黏附及免疫逃避中起关键的作用。每个单倍体基因组var基因家族编码约60种成员，通过启动转录不同的var基因变异体为抗原变异提供了分子基础。

Gold nanoparticles in chemical and biological sensing.

Abstract: Detection of chemical and biological agents plays a fundamental role in biomedical, forensic and environmental sciences1–4 as well as in anti bioterrorism applications.5–7 The development of highly sensitive, cost effective, miniature sensors is therefore in high demand which requires advanced technology coupled with fundamental knowledge in chemistry, biology and material sciences.8–13 In general, sensors feature two functional components: a recognition element to provide selective/specific binding with the target analytes and a transducer component for signaling the binding event. An efficient sensor relies heavily on these two essential components for the recognition process in terms of response time, signal to noise (S/N) ratio, selectivity and limits of detection (LOD).14,15 Therefore, designing sensors with higher efficacy depends on the development of novel materials to improve both the recognition and transduction processes. Nanomaterials feature unique physicochemical properties that can be of great utility in creating new recognition and transduction processes for chemical and biological sensors15–27 as well as improving the S/N ratio by miniaturization of the sensor elements.28 Gold nanoparticles (AuNPs) possess distinct physical and chemical attributes that make them excellent scaffolds for the fabrication of novel chemical and biological sensors (Figure 1).29–36 First, AuNPs can be synthesized in a straightforward manner and can be made highly stable. Second, they possess unique optoelectronic properties. Third, they provide high surface-to-volume ratio with excellent biocompatibility using appropriate ligands.30 Fourth, these properties of AuNPs can be readily tuned varying their size, shape and the surrounding chemical environment. For example, the binding event between recognition element and the analyte can alter physicochemical properties of transducer AuNPs, such as plasmon resonance absorption, conductivity, redox behavior, etc. that in turn can generate a detectable response signal. Finally, AuNPs offer a suitable platform for multi-functionalization with a wide range of organic or biological ligands for the selective binding and detection of small molecules and biological targets.30–32,36 Each of these attributes of AuNPs has allowed researchers to develop novel sensing strategies with improved sensitivity, stability and selectivity. In the last decade of research, the advent of AuNP as a sensory element provided us a broad spectrum of innovative approaches for the detection of metal ions, small molecules, proteins, nucleic acids, malignant cells, etc. in a rapid and efficient manner.37 Figure 1 Physical properties of AuNPs and schematic illustration of an AuNP-based detection system. In this current review, we have highlighted the several synthetic routes and properties of AuNPs that make them excellent probes for different sensing strategies. Furthermore, we will discuss various sensing strategies and major advances in the last two decades of research utilizing AuNPs in the detection of variety of target analytes including metal ions, organic molecules, proteins, nucleic acids, and microorganisms.