Synthetic metals based on tetramethyltetraselenafulvalene(TMTSF): Varied anisotropy in the low temperature (125K) structures of (TMTSF)2X,X=C104-, PF6-, and AsF6-.

The low temperature (125K) X-ray crystal structures of (TMTSF)₂X, X=C10₄^-, PF₆^-, and AsF₆^- reveal decreases in the intermolecular interand intrastack Se-Se contact distances upon cooling (298K to 125K) which are highly anisotropic and different from one salt to another. The changes in the interstack distances, which are normal to the stacking direction, are approximately twice those involving intrastack Se-Se interactions. These observations establish that the anisotropic structural changes which accompany decreased temperature are common to numerous (TMTSF)₂X radical cation conducting salts.     

Ultrafast noncollinear optical parametric chirped pulse amplification in KTiOAsO4

Amplification of femtosecond pulses at 1.56 microm based on noncollinear parametric chirped pulse amplification in a potassium titanyl arsenate (KTA) crystal with pumping at 1.05 microm is reported. The 100 fs pulses of an erbium fiber laser are parametrically amplified while synchronously pumped by an amplified mode-locked Nd:YLF laser. This amplifier has a saturated gain of 65 dB with 30% conversion efficiency and has produced 160 fs pulses with peak powers of up to 0.75 GW. The system produced 380 mW before compression and can be readily scaled to the multiwatt range with bandwidths to support sub-100 fs pulses.     

Asymptotic formulae for likelihood-based tests of new physics

We describe likelihood-based statistical tests for use in high energy physics for the discovery of new phenomena and for construction of confidence intervals on model parameters. We focus on the properties of the test procedures that allow one to account for systematic uncertainties. Explicit formulae for the asymptotic distributions of test statistics are derived using results of Wilks and Wald. We motivate and justify the use of a representative data set, called the “Asimov data set”, which provides a simple method to obtain the median experimental sensitivity of a search or measurement as well as fluctuations about this expectation.     

Traveling-wave Thomson scattering and optical undulators for high-yield EUV and X-ray sources

We present a novel high-yield Thomson scattering geometry that takes advantage of compact electron bunches, as available in advanced, low-emittance linear accelerators or laser wakefield accelerators. In order to avoid the restrictions on the X-ray photon yield imposed by the Rayleigh limit, we use ultrashort, pulse-front tilted laser pulses in a side-scattering geometry. Such a traveling-wave setup allows an overlap of electron and laser beams, even after propagating over distances much longer than the Rayleigh length. Experimental designs are discussed and optimized for different scattering angles. Specifically, to minimize group delay dispersion at large scattering angles >10°, we propose the use of varied-line spacing (VLS) gratings for spatio-temporal laser pulse shaping. Compared to head-on (180°) Thomson scattering, interaction lengths are in the centimeter to meter range and photon numbers for ultrashort X-ray pulses can increase by several orders of magnitudes.     

A sequential molecular mechanics/quantum mechanics study of the electronic spectra of amides

We report gas-phase electronic spectra of formamide, N-methyformamide, acetamide, and N-methylacetamide at 300 K calculated using a combination of classical molecular dynamics and time-dependent density functional theory (TDDFT). In comparison to excitation energies computed using the global minima structures, the valence npi* and pi(nb)pi* states show a significant red-shift of 0.1-0.35 eV, while smaller shifts are found for the n3s and pi(nb)3s Rydberg states. In this work, we have identified the physical origin of these shifts arising from variations of the molecular structure. We present simple relationships between key geometrical parameters and spectral shifts. Consequently, electronic spectra can be generated directly from ground-state structures, without additional quantum chemical calculations. The electronic spectrum of formamide in aqueous solution is computed using TDDFT using an explicit solvent model. This provides a quantitative determination of the condensed-phase spectrum. In general, this study shows that temperature effects can change the predicted excitation energies significantly and demonstrates how electronic spectra at elevated temperatures can be computed in a computationally efficient way.     

Targeted catalytic inactivation of angiotensin converting enzyme by lisinopril-coupled transition-metal chelates

A series of compounds that target reactive transition-metal chelates to somatic angiotensin converting enzyme (sACE-1) have been synthesized. Half-maximal inhibitory concentrations (IC(50)) and rate constants for both inactivation and cleavage of full-length sACE-1 have been determined and evaluated in terms of metal chelate size, charge, reduction potential, coordination unsaturation, and coreactant selectivity. Ethylenediaminetetraacetic acid (EDTA), nitrilotriacetic acid (NTA), 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid (DOTA), and tripeptide GGH were linked to the lysine side chain of lisinopril by 1-ethyl-3-[3-(dimethylamino)propyl]carbodiimide hydrochloride/N-hydroxysuccinimide coupling. The resulting amide-linked chelate-lisinopril (EDTA-lisinopril, NTA-lisinopril, DOTA-lisinopril, and GGH-lisinopril) conjugates were used to form coordination complexes with iron, cobalt, nickel, and copper, such that lisinopril could mediate localization of the reactive metal chelates to sACE-1. ACE activity was assayed by monitoring cleavage of the fluorogenic substrate Mca-RPPGFSAFK(Dnp)-OH, a derivative of bradykinin, following preincubation with metal chelate-lisinopril compounds. Concentration-dependent inhibition of sACE-1 by metal chelate-lisinopril complexes revealed IC(50) values ranging from 44 to 4500 nM for Ni-NTA-lisinopril and Ni-DOTA-lisinopril, respectively, versus 1.9 nM for lisinopril. Stronger inhibition was correlated with smaller size and lower negative charge of the attached metal chelates. Time-dependent inactivation of sACE-1 by metal chelate-lisinopril complexes revealed a remarkable range of catalytic activities, with second-order rate constants as high as 150,000 M(-1) min(-1) (Cu-GGH-lisinopril), while catalyst-mediated cleavage of sACE-1 typically occurred at much lower rates, indicating that inactivation arose primarily from side chain modification. Optimal inactivation of sACE-1 was observed when the reduction potential for the metal center was poised near 1000 mV, reflecting the difficulty of protein oxidation. This class of metal chelate-lisinopril complexes possesses a range of high-affinity binding to ACE, introduces the advantage of irreversible catalytic turnover, and marks an important step toward the development of multiple-turnover drugs for selective inactivation of sACE-1.     

A compact solution for ion beam therapy with laser accelerated protons

The recent advancements in the field of laser-driven particle acceleration have made Laser-driven Ion Beam Therapy (L-IBT) an attractive alternative to the conventional particle therapy facilities. To bring this emerging technology to clinical application, we introduce the broad energy assorted depth dose deposition model which makes efficient use of the large energy spread and high dose-per-pulse of Laser Accelerated Protons (LAP) and is capable of delivering homogeneous doses to tumors. Furthermore, as a key component of L-IBT solution, we present a compact iso-centric gantry design with 360° rotation capability and an integrated shot-to-shot energy selection system for efficient transport of LAP with large energy spread to the patient. We show that gantry size could be reduced by a factor of 2–3 compared to conventional gantry systems by utilizing pulsed air-core magnets.