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61.
X Fang KW Ledingham P Graham DJ Smith T McCanny RP Singhal AJ Langley PF Taday 《Rapid communications in mass spectrometry : RCM》1999,13(14):1390-1397
The potential of femtosecond laser time-of-flight mass spectrometry (FLMS) for uniform quantitative analysis of molecules has been investigated. Various samples of molecular gases and vapours have been studied, using ultra-fast ( approximately 50 fs) laser pulses with very high intensity (up to 1.6 x 10(16) Wcm(-2)) for non-resonant multiphoton ionisation/tunnel ionisation. Some of these molecules have high ionisation potentials, requiring up to ten photons for non-resonant ionisation. The relative sensitivity factors (RSF) have been determined as a function of the laser intensity and it has been demonstrated that for molecules with very different masses and ionisation potentials, uniform ionisation has been achieved at the highest laser intensities. Quantitative laser mass spectrometry of molecules is therefore a distinct possibility. Copyright 1999 John Wiley & Sons, Ltd. 相似文献
62.
Wm. G. Hoover Harald A. Posch Christina Forster Christoph Dellago Mary Zhou 《Journal of statistical physics》2002,109(3-4):765-776
The dynamical instability of many-body systems can best be characterized through the local Lyapunov spectrum {}, its associated eigenvectors {}, and the time-averaged spectrum {}. Each local Lyapunov exponent describes the degree of instability associated with a well-defined direction—given by the associated unit vector —in the full many-body phase space. For a variety of hard-particle systems it is by now well-established that several of the vectors, all with relatively-small values of the time-averaged exponent , correspond to quite well-defined long-wavelength modes. We investigate soft particles from the same viewpoint here, and find no convincing evidence for corresponding modes. The situation is similar—no firm evidence for modes—in a simple two-dimensional lattice-rotor model. We believe that these differences are related to the form of the time-averaged Lyapunov spectrum near =0. 相似文献
63.
The effects of particle composition on heterogeneous catalysis were studied using dendrimer-encapsulated nanoparticles (DENs) as precursors to supported Pt-Cu catalysts. Bimetallic Pt-Cu DENs with varying Pt/Cu ratios were prepared in an anaerobic aqueous solution and deposited onto a high-purity commercial alumina support. The dendrimer template was then thermally removed to yield supported nanoparticle catalysts, which were studied with toluene hydrogenation and CO oxidation catalysis as well as infrared spectroscopy of adsorbed CO. Incorporating Cu into Pt nanoparticles had opposite effects on the two test reactions. Cu acted as a mild promoter for CO oxidation catalysis, and the promoting effect was independent of the amount of Cu present. Conversely, Cu acted as a strong poison for toluene hydrogenation catalysis, and the normalized rate tracked inversely with Cu content. Infrared spectroscopy of the supported nanoparticles indicated that electronic effects (electron donation from Cu to Pt) were minimal for these materials. Consequently, the catalysis results are interpreted in terms of potential structural differences as a function of Cu incorporation and reaction conditions. 相似文献
64.
R.Y. Vun K. Hoover J. Janowiak M. Bhardwaj 《Applied Physics A: Materials Science & Processing》2008,90(1):191-196
Numerous handheld moisture meters are available for measuring moisture levels of wood and building materials for a vast range
of quality control and moisture diagnosis applications. However, many methods currently available require physical contact
of a probe with the test material to operate. The contact requirement of such devices has limited applications for these purposes.
There is a tremendous demand for dynamic online quality assessment of in-process materials for moisture content (MC) measurements.
In this paper, a non-destructive non-contact ultrasound technology was used to evaluate the effects of increasing temperature
in two MC levels and of increasing MC in lumber. The results show that the ultrasonic absolute transmittance and velocity
parameters are directly correlated very well (R2≥0.87) with temperature for the two moisture levels in wood. At constant temperature, however, the velocity is inversely correlated
with MC. It was also found that the distribution of MC along the length is marginally insignificant to both ultrasonic measurements.
The transmittance measurement along the orthogonal thickness direction is insignificant above the fiber saturation MC; similarly,
the velocity measurement is marginally insignificant. The study concludes a positive correlation and a good fit for this technology
to advance into the development of an automated device for determining wood moisture levels, which will in turn be used to
control the dynamics of wood drying/sterilization processes. Further calibration research is recommended to ascertain the
constraints and limitations of the technology to specific wood species and dimension.
PACS 43.35.Zc; 43.60.Vx; 43.35.Yb; 43.35.Mr; 81.05.Rm; 81.70.Cv; 83.80.Mc; 87.50.yg 相似文献
65.
Michele M. Schantz Gauthier Eppe Jean-François Focant Coreen Hamilton N. Alan Heckert Rebecca M. Heltsley Dale Hoover Jennifer M. Keller Stefan D. Leigh Donald G. Patterson Jr Adam L. Pintar Katherine E. Sharpless Andreas Sjödin Wayman E. Turner Stacy S. Vander Pol Stephen A. Wise 《Analytical and bioanalytical chemistry》2013,405(4):1203-1211
Four new Standard Reference Materials (SRMs) have been developed to assist in the quality assurance of chemical contaminant measurements required for human biomonitoring studies, SRM 1953 Organic Contaminants in Non-Fortified Human Milk, SRM 1954 Organic Contaminants in Fortified Human Milk, SRM 1957 Organic Contaminants in Non-Fortified Human Serum, and SRM 1958 Organic Contaminants in Fortified Human Serum. These materials were developed as part of a collaboration between the National Institute of Standards and Technology (NIST) and the Centers for Disease Control and Prevention (CDC) with both agencies contributing data used in the certification of mass fraction values for a wide range of organic contaminants including polychlorinated biphenyl (PCB) congeners, chlorinated pesticides, polybrominated diphenyl ether (PBDE) congeners, and polychlorinated dibenzo-p-dioxin (PCDD) and dibenzofuran (PCDF) congeners. The certified mass fractions of the organic contaminants in unfortified samples, SRM 1953 and SRM 1957, ranged from 12 ng/kg to 2200 ng/kg with the exception of 4,4′-DDE in SRM 1953 at 7400 ng/kg with expanded uncertainties generally <14 %. This agreement suggests that there were no significant biases existing among the multiple methods used for analysis. Figure
Comparison of Concentrations of Selected Compounds in Human Serum and Human Milk Standard Reference Materials (SRMs) 相似文献
66.
Dr. Haifeng Yang Dr. Peter G. Dormer Nelo R. Rivera Dr. Andrew J. Hoover 《Angewandte Chemie (International ed. in English)》2018,57(7):1883-1887
Tritium‐labeled molecules are critical tools for elucidating the binding and metabolic properties of bioactive compounds, particularly during pharmaceutical discovery. Direct tritiation of inert C?H bonds with T2 gas is an ideal approach for tritium labeling, but significant gaps remain for direct tritiation of structurally complex molecules with diverse functional groups. Here we report the first application of palladium(II) C?H activation chemistry for tritiation with T2 gas. This practical transformation exhibits novel substrate scope and greater functional group tolerance compared to previous state of the art tritiation methods, and has been applied to directly tritiate 9 complex pharmaceuticals and an unprotected dipeptide. The isolated tritium‐labeled products exhibit >15 Ci mmol?1 specific activity, exceeding the typical requirements for application in studies of molecular interaction and metabolism. 相似文献
67.
Jacob J. Piane Steven Huss Lucas T. Alameda Stephen J. Koehler Lauren E. Chamberlain Matthew J. Schubach Ashley C. Hoover Elizabeth Elacqua 《Journal of polymer science. Part A, Polymer chemistry》2021,59(22):2867-2877
Single-chain polymer nanoparticles (SCNPs) are emerging as versatile catalytic platforms that provide excellent control over solubility. The confined nature of SCNPs can improve the rate of catalysis. While significant headway has been made in thermally-induced transition-metal catalysis with SCNPs, light-activated SCNP catalysts have received little attention. We are developing triarylpyrylium tetrafluoroborate (TPT)-functionalized SCNPs as oxidative photocatalysts. Herein, we comprehensively study the impact of light source on both SCNP compaction and TPT absorbance through gel-permeation chromatography and UV/Vis spectroscopy. We observe that compaction is expedited using light sources that excite the photocatalyst (e.g., blue LEDs), which is attributed to the ability of TPT to dimerize sytrenics under similar photoredox conditions. The resultant metal-free SCNP photocatalysts enable the oxidation of benzyl alcohols in good yields. The SCNP is further investigated for the amidation of 4-bromobenzaldehyde, wherein it affords higher yields of the benzamide product compared to both small-molecule and unfolded polymer controls. We attribute the combined results to the colocalization of the TPT photoredox catalyst and pyrene electron relay within the SCNP, which likely aids in single-electron transfer processes. The scope of amidation reactions was also extended to other aryl aldehydes, wherein deactivated substrates afforded the highest yield of the desired amide. 相似文献
68.
The first total synthesis of 5-desoxyleukotriene D () is reported. The route of synthesis utilizes a novel method for five-carbon chain extension. The availability of allowed experimental demonstration that the 5-hydroxyl function is important for biological activity of the slow reacting substances. 相似文献
69.
Gorga MP Neely ST Dierking DM Dorn PA Hoover BM Fitzpatrick DF 《The Journal of the Acoustical Society of America》2003,114(1):263-278
Distortion product otoacoustic emission (DPOAE) suppression measurements were made in 20 subjects with normal hearing and 21 subjects with mild-to-moderate hearing loss. The probe consisted of two primary tones (f2, f1), with f2 held constant at 4 kHz and f2/f1 = 1.22. Primary levels (L1, L2) were set according to the equation L1 = 0.4 L2 + 39 dB [Kummer et al., J. Acoust. Soc. Am. 103, 3431-3444 (1998)], with L2 ranging from 20 to 70 dB SPL (normal-hearing subjects) and 50-70 dB SPL (subjects with hearing loss). Responses elicited by the probe were suppressed by a third tone (f3), varying in frequency from 1 octave below to 1/2 octave above f2. Suppressor level (L3) varied from 5 to 85 dB SPL. Responses in the presence of the suppressor were subtracted from the unsuppressed condition in order to convert the data into decrements (amount of suppression). The slopes of the decrement versus L3 functions were less steep for lower frequency suppressors and more steep for higher frequency suppressors in impaired ears. Suppression tuning curves, constructed by selecting the L3 that resulted in 3 dB of suppression as a function of f3, resulted in tuning curves that were similar in appearance for normal and impaired ears. Although variable, Q10 and Q(ERB) were slightly larger in impaired ears regardless of whether the comparisons were made at equivalent SPL or equivalent sensation levels (SL). Larger tip-to-tail differences were observed in ears with normal hearing when compared at either the same SPL or the same SL, with a much larger effect at similar SL. These results are consistent with the view that subjects with normal hearing and mild-to-moderate hearing loss have similar tuning around a frequency for which the hearing loss exists, but reduced cochlear-amplifier gain. 相似文献
70.
Wm. G. Hoover H. A. Posch V. M. Castillo C. G. Hoover 《Journal of statistical physics》2000,100(1-2):313-326
We simulate the far-from-equilibrium irreversible expansion of a compressed ideal gas in two space dimensions. For this problem the particle trajectories from conventional smooth particle applied mechanics are isomorphic to those from a corresponding molecular dynamics simulation. The smooth-particle weight function used to describe the expanding gas is identical to the pair potential governing the molecular dynamics simulation. These many-body particle simulations are compared with those using a modified smooth-particle algorithm invented by Monaghan, as well as with those based on conventional grid-based Eulerian and Lagrangian methods. 相似文献