Spectral characterization and intracellular detection of Surface‐Enhanced Raman Scattering (SERS)‐encoded plasmonic gold nanostars

Plasmonic gold nanostars offer a new platform for surface‐enhanced Raman scattering (SERS). However, due to the presence of organic surfactant on the nanoparticles, SERS characterization and application of nanostar ensembles in solution have been challenging. Here, we applied our newly developed surfactant‐free nanostars for SERS characterization and application. The SERS enhancement factors (EF) of silver spheres, gold spheres and nanostars of similar sizes and concentration were compared. Under 785 nm excitation, nanostars and silver spheres have similar EF, and both are much stronger than gold spheres. Having plasmon matching the incident energy and multiple ‘hot spots’ on the branches bring forth strong SERS response without the need to aggregate. Intracellular detection of silica‐coated SERS‐encoded nanostars was also demonstrated in breast cancer cells. The non‐aggregated field enhancement makes the gold nanostar ensemble a promising agent for SERS bioapplications. Copyright © 2012 John Wiley & Sons, Ltd.     

Cancellation of light shifts in an N-resonance clock

We demonstrate that first-order light shifts can be canceled for an all-optical, three-photon-absorption resonance (N-resonance) on the D1 transition of 87Rb. This light-shift cancellation facilitates improved frequency stability for an N-resonance clock. For example, by using a tabletop apparatus designed for N-resonance spectroscopy, we measured a short-term fractional frequency stability (Allan deviation) of approximately/= 1.5 x 10(-11) tao1/2 for observation times of 1 s < or = tao < or = 50 s. Further improvements in frequency stability should be possible with an apparatus designed as a dedicated N-resonance clock.     

Capillary discharge tabletop soft X-ray lasers reach new wavelengths and applications

For many years, researchers have envisioned the development of compact high repetition rate tabletop soft X-ray lasers that could be routinely used in application in numerous disciplines. With demonstrated average powers of several mW and mJ-level pulse energy at 46.9 nm, capillary discharge-pumped lasers are the first compact lasers to reach this goal. In this paper we summarize the development status of high repetition rate tabletop soft X-ray lasers based on capillary discharge excitation, and give examples of their successful use in several applications. Results of the use of a capillary discharge pumped 46.9 nm laser in dense plasma interferometry, soft X-ray reflectometry for the determination of optical constants, and laser ablation are described. The observation of lasing at 53 nm line in Ne-like Cl with output pulse energy up to 10 μJ is also reported.     

Positrons and electrons in primary cosmic rays as measured in the PAMELA experiment

The PAMELA experiment is being carried out on board the Russian satellite Resurs DK1 placed in the near-earth near-polar orbit on June 15, 2006. The apparatus comprising a silicon-strip magnetic spectrometer and an electromagnetic calorimeter allows measurement of electron and positron fluxes in cosmic rays in a wide energy interval from ～100 MeV to hundreds of GeV. The high-energy electron and positron separation technique is discussed and the data on positron-to-electron ratio in primary cosmic rays up to E ≈ 10 GeV from the 2006–2007 measurements are reported in this work.     

光辐照精确调控金纳米星枝杈长度及其光热性能探究

金纳米星是一种具有尖状结构的多分枝纳米颗粒.为了使金纳米星枝杈长度可控,利用HEPES作为体系的还原剂、稳定剂及形状诱导剂,在制备过程中进行光辐照,得到的金纳米星枝杈长度比无光辐照时的金纳米星枝杈长度短,而且不同波长光辐照得到的金纳米星枝杈长度有显著不同.在此基础上,分析了金纳米星枝杈长度变化的物理过程,提出光诱导金纳米星生长过程中枝杈长度变化的理论模型.测量了不同枝杈长度的金纳米星在光辐照下一定时间内的温度变化,计算了金纳米星的光热转换效率.实验结果表明,光辐照制备金纳米星能够精确控制金纳米星枝杈长度范围,从而调控金纳米星的光热转换效率.     

The HERO project for the study of high-energy primary cosmic radiation

Proposals for the High-Energy Ray Observatory (HERO) comprising scientific equipment with increased power availability are presented. Under the long exposure (>7 years), it is proposed to investigate the spectrum and charge composition of cosmic-ray nuclei up to E ₀ ～ 10¹⁶ eV and to determine the behavior of the energy spectrum in the energy regions >100 GeV for cosmic-ray electrons and >50 GeV for γ radiation. The geometrical factor of the apparatus is 6.0–9.0 m² sr depending on the type of particles.     

Optically (solar) pumped oxygen-iodine lasers

We present the results of theoretical and experimental studies demonstrating the possibility of developing an oxygen-iodine laser (OIL) with direct optical pumping of molecular oxygen involving inter-molecular interaction with charge transfer from donor molecule (buffer gas) to acceptor molecule (oxygen). This interaction lifts degeneracy of the lower energy states of molecular oxygen and increases its absorption cross section in the visible spectral region and the UV Herzberg band, where high quantum yield of singlet oxygen is achieved (QY ～ 1 and QY ～ 2, respectively) at the same time. A pulse-periodic optical pump sources with pulse energy of ～50 kJ, pulse duration of ～25 μs, and repetition rate of ～10 Hz, which are synchronized with the mechanism of singlet oxygen generation, are developed. This allows implementation of a pulse-periodic oxygen-iodine laser with an efficiency of ～25%, optical efficiency of ～40%, and parameter L/T ～ 1/1.5, where T is the thermal energy released in the laser active medium upon generation of energy L. It is demonstrated that, under direct solar pumping of molecular oxygen, the efficiency parameter of the OIL can reach L/T ～ 1/0.8 in a wide range of scaling factors.     

DNA template-driven synthesis of HgTe nanoparticles

Nanoparticle (mercury telluride (HgTe))–single-stranded (ss) DNA complex has been synthesized using an electrodeposition technique. As demonstrated by transmission electron microscopic measurements, the morphology of these particles is found to depend upon the ssDNA sequence. The surface feature of HgTe–ssDNA deposit gives an appearance of nanostars with an average size as 1.4 nm and exhibits the single crystalline cubic phase, contrary to the polydispersity and polycrystallinity observed with HgTe nanoparticles alone. The change in infrared absorption band of ssDNA as a consequence of its association with HgTe nanoparticles have been confirmed from Fourier transform infrared spectroscopic measurements. Photoluminescence (PL) at 300 K of these nanostars have yielded a unique single PL of line width 8 nm at wavelength 548.4 nm     

金纳米星诊疗剂的光热特性及其在光热治疗和光学相干层析成像中的应用研究

为了开发一种优异的用于光热治疗和光学相干层析成像的金纳米星诊疗剂,对金纳米星的制备、光热特性以及光热治疗和光学相干层析成像中的应用进行研究.利用尖端结构增强金纳米材料的局域表面等离子体共振特性,通过种子介导法制备了多枝化的金纳米星,多尖端的结构使其具有明显的光热效果,并探究了其作为光热治疗的诊疗剂和光学相干层析成像造影...     

Modulated photoemission spectroscopy: Application to Au

We describe modulated photoemission spectroscopy, in which an internal (sample) parameter such as temperature, or an external (apparatus) parameter such as wavelength is varied. A general formalism is developed for modulated photoemission spectroscopy and then illustrated using temperature modulated photoemission spectra and yields for Au obtained in the ～ 6 to 11.6 eV photon energy range. Modulated s-p band photoemission data are described in terms of photoemission critical points in order to explain the nature of the modulated structures in the s-p band region and relate experiment to energy band thresholds obtained from a recent band calculation for Au. Application of the formalism to modulated d-band emission leads to a method for extracting d-band deformation potentials. For example, we find that the upper d band edge moves upward with respect to E_F at a rate of 2 to 6 × 10^?4 eV/K. Modulation of the quantum yield is described and our measurements are compared with modulated optical data.     

Surface‐enhanced Raman scattering spectroscopy via gold nanostars

Anisotropic metallic nanoparticles (NPs) have unique optical properties, which lend them to applications such as surface‐enhanced Raman scattering (SERS) spectroscopy. Star‐shaped gold (Au) NPs were prepared in aqueous solutions by the seed‐mediated growth method and tested for Raman enhancement using 2‐mercaptopyridine (2‐MPy) and crystal violet (CV) probing molecules. For both molecules, the SERS activity of the nanostars was notably stronger than that of the spherical Au NPs of similar size. The Raman enhancement factors (EFs) for 2‐MPy on Au nanostars and nanorods are comparable and estimated as greater than 5 orders of magnitude. However, the enhancement for CV on nanostars was significantly higher than for nanorods, in particular at CV concentrations of 100 nM or lower. This article is a US Government work and is in the public domain in the USA. Published in 2008 by John Wiley & Sons, Ltd.     

Fe3O4@Au纳米星颗粒作为循环SERS基底用于农药残留物的检测

本文首先采用共沉淀的方法制备了Fe3O4纳米颗粒,随后经柠檬酸钠和对苯二酚还原氯金酸的方法在Fe3O4纳米颗粒的表面生成刺状Au纳米结构,进而获得Fe3O4@Au纳米星颗粒。该Fe3O4@Au纳米星颗粒作为SERS基底,用作农药残留物福美双和敌瘟磷的检测。由于高密度的Au纳米结构的尖端效应,该基底显示出高敏感的SERS活性。最后利用Fe3O4纳米颗粒的磁性,将其用于循环SERS测试,研究了其循环使用特性。     

Synthesis of gold nanostars with fractal structure: application in surface-enhanced Raman scattering

Multi-branched gold nanostars with fractal feature were synthesized using the Triton X-100 participant seed-growth method. By increasing the amount of ascorbic acid, the branch length of gold nanostars could be greatly increased. It has been interesting to find that the secondary growth of new branches takes place from the elementary structure when the aspect ratio of the branches is greater than 8.0 and the corresponding plasmon absorption wavelength is greater than 900 nm. Raman activity of the gold nanostar films has been investigated by using the 4-mercaptobenzoic acid (4-MBA) as Raman active probe. Experimental results show that the surface-enhanced Raman scattering (SERS) ability of the gold nanostars could be efficiently improved when the fractal structure appears. The physical mechanism has been attributed to the intense increased secondary branch number and the increased “hot spots”. These unique multi-branched gold nanostars with fractal feature and great SERS activity should have great potential in sensing applications.     

Thermonuclear gain of a two-cascade laser-fusion target

One-dimensional numerical calculations are used to explore the possibility of thermonuclear fuel “ignition” (achieving an energy gainG ～ 1) in two-cascade laser-fusion targets with a relatively small aspect ratio for the inner shell. It is demonstrated that the parameters of the laser-produced thermonuclear plasma for a laser pulse energy of 200 kJ, various wavelengths of the laser radiation, and a simple pulse shape closely correspond to the “ignition” state for a target with an inner shell having an aspect ratio of ～ 3–10. This is indicative of the high energy efficiency of two-cascade targets that appear to be characterized by high reliability with respect to evolution of hydrodynamic instabilities.     

Generation of millijoule-level soft-x-ray laser pulses at a 4-Hz repetition rate in a highly saturated tabletop capillary discharge amplifier

Laser pulses with energies of as much as 1 mJ were generated at a wavelength of 46.9 nm by single-pass amplification in a 34.5 cm-long Ne-like Ar capillary discharge plasma. The large gain-length product of this plasma column allows for soft-x-ray amplification in a highly saturated regime, resulting in efficient energy extraction. Average laser output pulse energy of 0.88 mJ and peak power of 0.6 MW were obtained at a repetition rate of 4 Hz. With an estimated peak spectral brightness of approximately 1x10(23)photons /(s mm(2)mrad> (2)0.01% bandwidth) this tabletop laser is one of the brightest soft-x-ray sources to date.     

Simulation of sputtering and desorption of gold nanoclusters under bombardment with 180-eV/atom Au400 nanoclusters using the classical molecular dynamics method

Computer simulation of the interaction of an Au₄₀₀ nanocluster (the total energy E = 72 keV) with free spherical Au _N nanoclusters (6 and 12 nm in diameter) and Au₆₀₅₁ clusters deposited on the (111) surface of an Al substrate is performed by means of the classical molecular dynamics method. The distributions of the absorbed energy (ε) converted to one atom of the bombarded nanocluster and the sputtering yield are analyzed. It has been ascertained that the most probable values are either the small (ε ? ε_max = E/N) or the maximum possible (ε ～ ε_max) values of absorbed energy. The total sputtering yield and the absorbed energy decrease with increasing impact parameter. It has been demonstrated that, with a probability of ～10%, a direct impact can lead to ejection of the entire bombarded nanocluster from the substrate. This event occurs in the case where an incident cluster initiates the secondary emission of target-cluster atoms mainly in the direction of the substrate. As a result, the nonsputtered part of the target cluster acquires the momentum in the opposite direction. This recoil effect can be regarded as one of the possible mechanisms by which nanoclusters deposited on substrate surfaces desorb under ion and cluster bombardment.     

Author index to volume 148B

We show that the modification of the photon propagator in the presence of the conducting walls of an apparatus leads to a new contribution Δg_e to the magnetic moment g_e of the electron. This change is of order Δg_e ～ αlog(2Λa)/ma, where a is the characteristic size of the apparatus, and Λ is the frequency above which the apparatus becomes transparent to photons. Numerically Δg_e is comparable to other contributions which arise in order (α/π)⁴, which is the current level of sensitivity of theory and experiment.     

Initiation of ecton processes by interaction of a plasma with a microprotrusion on a metal surface

Evolution of rapid (～10 ns) Ohmic overheating of a microprotrusion on a surface in contact with a plasma by emission current is studied taking into account the energy carried by plasma ions and electrons, as well as Ohmic heating, emissive source of energy release (Nottingham effect), and heat removal due to heat conduction. Plasma parameters were considered in the range of n = 10¹⁴?10²⁰ cm^?3 and T _e = 0.1 eV?10 keV. The threshold value of energy transferred to the surface from the plasma is found to be 200 MW/cm²; above this value, heating becomes explosive (namely, an increase in the temperature growth rate (δ² T/δt ² > 0) and in passing current (δJ/δt > 0) is observed in the final stage at T ～ 10⁴ K and j ～ 10⁸ A/cm²). In spite of the fact that Ohmic heating does not play any significant role for plasmas with a density lower than 10 18 cm^?3 because the current is limited by the space charge of electrons, rapid overheating of top of microprotrusion is observed much sooner (over a time period of ～1 ns) when the threshold is exceeded. In this case, intense ionization of vapor of the wall material leads to an increase in the plasma density at the surface, and the heating becomes of the Ohmic explosion type. Such conditions for the formation of a micr?xplosion on the surface and of an ecton accompanying it can be created during the interaction of a plasma with the cathode, anode, or an insulated wall and may lead to the formation of cathode and anode spots, as well as unipolar arcs.     

Nanostars on a fiber facet with near field enhancement for surface-enhanced Raman scattering detection

A 4-pointed gold nanostar is proposed to form the array on a fiber facet to achieve a greatly enhanced near field intensity for Surface-Enhanced Raman Scattering (SERS) detection. The proposed gold nanostar array has a Surface Plasmon Resonance (SPR) peaked at a wavelength of ～650 nm with up to 45 times electric field intensity enhancement compared with the state-of-the-art nanorod design. It has a wideband SPR field enhancement spanned from 600 to 720 nm, which covers the wavelengths for both the excitation light (632.8 nm) and the Raman signal of the analytes (675–706 nm); With symmetrical structure it forms four hot spots in every unit cell and can detect best for light polarized horizontal or perpendicular to the waist of the nanostars. It also could be altered to tune the SPR and allows the fiber sensor to resonate at different wavelengths, as demonstrated by an example at 533 nm. All the above features make the gold nanostar-based compact and portable fiber sensor an attractive solution for SERS detection.     

Long term performance evaluation of the TACTIC imaging telescope using ∼400 h Crab Nebula observation during 2003–2010

The TeV atmospheric Cherenkov telescope with imaging camera (TACTIC) γ-ray telescope has been in operation at Mt. Abu, India since 2001 to study TeV γ-ray emission from celestial sources. During the last 10 years, apart from consistently detecting a steady signal from the Crab Nebula above ～1.2 TeV energy, at a sensitivity level of ～5.0 σ in ～25 h, the telescope has also detected flaring activity from Mrk 421 and Mrk 501 on several occasions. Although we used Crab Nebula data partially, in some of the reported results, primarily for testing the validity of the full data analysis chain, the main aim of this work is to study the long term performance of the TACTIC telescope by using consolidated data collected between 2003 and 2010. The total on-source data, comprising ～402 h, yields an excess of ～(3742±192) γ-ray events with a statistical significance of ～19.9 σ. The off-source data, comprising ～107 h of observation, is found to be consistent with a no-emission hypothesis, as expected. The resulting γ-ray rate for the on-source data is determined to be ～(9.31±0.48) h ^?1. A power law fit (dΦ/dE=f ₀ E ^?Γ ) with f ₀ ～ (2.66±0.29) × 10^?11 cm^?2 s^?1 TeV^?1 and Γ ～ 2.56±0.10 is found to provide reasonable fit to the inferred differential spectrum within statistical uncertainties. The spectrum matches reasonably well with that obtained by other groups. A brief summary of the improvements in the various subsystems of the telescope carried out recently, which has resulted in a substantial improvement in its detection sensitivity (viz., ～5 σ in an observation period of ～13 h as compared to ～25 h earlier) are also presented in this paper. Encouraged by the detection of strong γ-ray signals from Mrk 501 and Mrk 421 on several occasions, there is considerable scope for the TACTIC telescope to monitor similar TeV γ-ray emission activity from other active galactic nuclei on a long-term basis.