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Vaishnavi Rajagopal Chris Stokes Alessandra Ferzoco 《Journal of the American Society for Mass Spectrometry》2018,29(2):260-269
We report a custom-geometry linear ion trap designed for fluorescence spectroscopy of gas-phase ions at ambient to cryogenic temperatures. Laser-induced fluorescence from trapped ions is collected from between the trapping rods, orthogonal to the excitation laser that runs along the axis of the linear ion trap. To increase optical access to the ion cloud, the diameter of the round trapping rods is 80% of the inscribed diameter, rather than the roughly 110% used to approximate purely quadrupolar electric fields. To encompass as much of the ion cloud as possible, the first collection optic has a 25.4 mm diameter and a numerical aperture of 0.6. The choice of geometry and collection optics yields 107 detected photons/s from trapped rhodamine 6G ions. The trap is coupled to a closed-cycle helium refrigerator, which in combination with two 50 Ohm heaters enables temperature control to below 25 K on the rod electrodes. The purpose of the instrument is to broaden the applicability of fluorescence spectroscopy of gas-phase ions to cases where photon emission is a minority relaxation pathway. Such studies are important to understand how the microenvironment of a chromophore influences excited state charge transfer processes. 相似文献
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Supramolecular Nested Microbeads as Building Blocks for Macroscopic Self‐Healing Scaffolds 下载免费PDF全文
Dr. Ziyi Yu Dr. Ji Liu Dr. Cindy Soo Yun Tan Prof. Oren A. Scherman Prof. Chris Abell 《Angewandte Chemie (International ed. in English)》2018,57(12):3079-3083
The ability to construct self‐healing scaffolds that are injectable and capable of forming a designed morphology offers the possibility to engineer sustainable materials. Herein, we introduce supramolecular nested microbeads that can be used as building blocks to construct macroscopic self‐healing scaffolds. The core–shell microbeads remain in an “inert” state owing to the isolation of a pair of complementary polymers in a form that can be stored as an aqueous suspension. An annealing process after injection effectively induces the re‐construction of the microbead units, leading to supramolecular gelation in a preconfigured shape. The resulting macroscopic scaffold is dynamically stable, displaying self‐recovery in a self‐healing electronic conductor. This strategy of using the supramolecular assembled nested microbeads as building blocks represents an alternative to injectable hydrogel systems, and shows promise in the field of structural biomaterials and flexible electronics. 相似文献
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Maram A. Q. Al-Sayaghi Jeremy Lewis Chris Buelke 《International Journal of Polymer Analysis and Characterization》2018,23(6):566-576
Aromatic polyimides are known for their remarkable thermal and chemical properties which are greatly influenced by their precursors. In this study, we report synthesis and characterization of four different aromatic polyimides. The four different dianhydrides (ODPA, BTDA, BPDA, and PMDA) were reacted with a diamine (BisAPAF) via azeotropic imidization under same conditions. FTIR analysis confirmed the formation of aromatic polyimides and all but one polyimide (HPI-BPDA) were found to be completely soluble in common solvents. The obtained molecular weights were between 16,000 and 32,000?g/mol, glass transition temperatures were between 250?°C and 275?°C, degradation temperatures were above 550?°C, and the d-spacing values were around 5?Å. These properties are promising and can be beneficial for various applications such as thin films and membranes. 相似文献
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Ewig CS Berry R Dinur U Hill JR Hwang MJ Li H Liang C Maple J Peng Z Stockfisch TP Thacher TS Yan L Ni X Hagler AT 《Journal of computational chemistry》2001,22(15):1782-1800
A class II valence force field covering a broad range of organic molecules has been derived employing ab initio quantum mechanical "observables." The procedure includes selecting representative molecules and molecular structures, and systematically sampling their energy surfaces as described by energies and energy first and second derivatives with respect to molecular deformations. In this article the procedure for fitting the force field parameters to these energies and energy derivatives is briefly reviewed. The application of the methodology to the derivation of a class II quantum mechanical force field (QMFF) for 32 organic functional groups is then described. A training set of 400 molecules spanning the 32 functional groups was used to parameterize the force field. The molecular families comprising the functional groups and, within each family, the torsional angles used to sample different conformers, are described. The number of stationary points (equilibria and transition states) for these molecules is given for each functional group. This set contains 1324 stationary structures, with 718 minimum energy structures and 606 transition states. The quality of the fit to the quantum data is gauged based on the deviations between the ab initio and force field energies and energy derivatives. The accuracy with which the QMFF reproduces the ab initio molecular bond lengths, bond angles, torsional angles, vibrational frequencies, and conformational energies is then given for each functional group. Consistently good accuracy is found for these computed properties for the various types of molecules. This demonstrates that the methodology is broadly applicable for the derivation of force field parameters across widely differing types of molecular structures. Copyright 2001 John Wiley & Sons, Inc. J Comput Chem 22: 1782-1800, 2001 相似文献
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Liu H Gaza-Bulseco G Chumsae C Radziejewski CH 《Rapid communications in mass spectrometry : RCM》2008,22(1):1-10
Nitration of a recombinant human monoclonal antibody was carried out in vitro by incubating the antibody with the nitrating reagent tetranitromethane (TNM). The susceptible sites of nitration were identified using high-performance liquid chromatography/mass spectrometry (HPLC/MS). In general, tyrosine residues in the variable domains of the antibody are more susceptible to nitration, while tyrosine residues in the constant domains are relatively resistant to nitration. However, one tyrosine residue in the CH1 domain and one tyrosine residue in the CH2 domain are highly susceptible to nitration. Interestingly, the susceptible tyrosine residue in the CH2 domain is followed by the conserved asparagine residue that is glycosylated. 相似文献
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John S. C. Kearney Miglė Graužinytė Dr. Dean Smith Daniel Sneed Christian Childs Jasmine Hinton Dr. Changyong Park Dr. Jesse S. Smith Dr. Eunja Kim Samuel D. S. Fitch Prof. Dr. Andrew L. Hector Prof. Dr. Chris J. Pickard Dr. José A. Flores‐Livas Prof. Dr. Ashkan Salamat 《Angewandte Chemie (International ed. in English)》2018,57(36):11623-11628
The application of pressure allows systematic tuning of the charge density of a material cleanly, that is, without changes to the chemical composition via dopants, and exploratory high‐pressure experiments can inform the design of bulk syntheses of materials that benefit from their properties under compression. The electronic and structural response of semiconducting tin nitride Sn3N4 under compression is now reported. A continuous opening of the optical band gap was observed from 1.3 eV to 3.0 eV over a range of 100 GPa, a 540 nm blue‐shift spanning the entire visible spectrum. The pressure‐mediated band gap opening is general to this material across numerous high‐density polymorphs, implicating the predominant ionic bonding in the material as the cause. The rate of decompression to ambient conditions permits access to recoverable metastable states with varying band gaps energies, opening the possibility of pressure‐tuneable electronic properties for future applications. 相似文献
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