Active phase control and frequency chirp effects on supercontinuum generation in high birefringence photonic crystal fiber

An acoustic-optics programmable dispersive filter (AOPDF) was first employed to actively control the linearly polarized femtosecond pump pulse frequency chirp for supercontinuum (SC) generation in a high birefringence photonic crystal fiber (PCF). By accurately controlling the second order phase distortion and polarization direction of incident pulses, the output SC spectrum can be tuned to various spectral energy distributions and bandwidths. The pump pulse energy and bandwidth are preserved in our experiment. It is found that SC with broader bandwidth can be generated with positive chirped pump pulses except when the chirp value is larger than the optimal value, and the same optimal value exists for the pump pulses polarized along the two principal axes. With optimal positive chirp, more than 78% of the pump energy can be transferred to below 750 nm. Otherwise, negative chirp will weaken the blue-shift broadening and the SC bandwidth. (C) 2007 Elsevier B.V. All rights reserved.

Nonlinear laser focusing using a conical guide and generation of energetic ions

Using conventional methods, a laser pulse can be focused down to around 6-8 mu m, but further reduction of the spot size has proven to be difficult. Here it is shown by particle-in-cell simulation that with a hollow cone an intense laser pulse can be reduced to a tiny, highly localized, spot of around 1 mu m radius, accompanied by much enhanced light intensity. The pulse shaping and focusing effect is due to a nonlinear laser-plasma interaction on the inner surface of the cone. When a thin foil is attached to the tip of the cone, the cone-focused light pulse compresses and accelerates the ions in its path and can punch through the thin target, creating highly localized energetic ion bunches of high density.

Multiplexed DNA-mediated electrochemistry

The aromatic core of double helical DNA possesses the unique and remarkable ability to form a conduit for electrons to travel over exceptionally long molecular distances. This core of π-stacked nucleobases creates an efficient pathway for charge transfer to proceed that is exquisitely sensitive to even subtle perturbations. Ground state electrochemistry of DNA-modified electrodes has been one of the major techniques used both to investigate and to harness the property of DNA-mediated charge transfer. DNA-modified electrodes have been an essential tool for both gaining insights into the fundamental properties of DNA and, due to the exquisite specificity of DNA-mediated charge transfer for the integrity of the π-stack, for use in next generation diagnostic sensing. Here, multiplexed DNA-modified electrodes are used to (i) gain new insights on the electrochemical coupling of metalloproteins to the DNA π-stack with relevance to the fundaments of in vivo DNA-mediated charge transfer and (ii) enhance the overall sensitivity of DNA-mediated reduction for use in the detection of low abundance diagnostic targets.

First, Methylene Blue (MB′) was covalently attached to DNA through a flexible C12 alkyl linker to yield a new redox reporter for DNA electrochemistry measurements with enhanced sensitivity. Tethered, intercalated MB′ was reduced through DNA-mediated charge transport. The redox signal intensity for MB′-dT-C12-DNA was found to be at least 3 fold larger than that of previously used Nile Blue (NB)-dT-DNA, which is coupled to the base stack via direct conjugation. The signal attenuation, due to an intervening mismatch, and therefore the degree of DNA-mediated reduction, does, however, depend on the DNA film morphology and the backfilling agent used to passivate the surface. These results highlight two possible mechanisms for the reduction of MB′ on the DNA-modified electrode that are distinguishable by their kinetics: reduction mediated by the DNA base pair stack and direct surface reduction of MB′ at the electrode. The extent of direct reduction at the surface can be minimized by overall DNA assembly conditions.

Next, a series of intercalation-based DNA-mediated electrochemical reporters were developed, using a flexible alkane linkage to validate and explore their DNA-mediated reduction. The general mechanism for the reduction of distally bound redox active species, covalently tethered to DNA through flexible alkyl linkages, was established to be an intraduplex DNA-mediated pathway. MB, NB, and anthraquinone were covalently tethered to DNA with three different covalent linkages. The extent of electronic coupling of the reporter was shown to correlate with the DNA binding affinity of the redox active species, supporting an intercalative mechanism. These electrochemical signals were shown to be exceptionally sensitive to a single intervening π-stack perturbation, an AC mismatch, in a densely packed DNA monolayer, which further supports that the reduction is DNA-mediated. Finally, this DNA-mediated reduction of MB occurs primarily via intra- rather than inter duplex intercalation, as probed through varying the proximity and integrity of the neighboring duplex DNA. Further gains to electrochemical sensitivity of our DNA-modified devices were then achieved through the application of electrocatalytic signal amplification using these solvent accessible intercalative reporters, MB-dT-C8, and hemoglobin as a novel electron sink. Electrocatalysis offers an excellent means of electrochemical signal amplification, yet in DNA based sensors, its application has been limited due to strict assembly conditions. We describe the use of hemoglobin as a robust and effective electron sink for electrocatalysis in DNA sensing on low density DNA films. Protein shielding of the heme redox center minimizes direct reduction at the electrode surface and permits assays on low density DNA films. Electrocatalysis of MB that is covalently tethered to the DNA by a flexible alkyl linkage allows for efficient interactions with both the base stack and hemoglobin. Consistent suppression of the redox signal upon incorporation of single CA mismatch in the DNA oligomer demonstrates that both the unamplified and the electrocatalytically amplified redox signals are generated through DNA-mediated charge transport. Electrocatalysis with hemoglobin is robust: it is stable to pH and temperature variations. The utility and applicability of electrocatalysis with hemoglobin is demonstrated through restriction enzyme detection, and an enhancement in sensitivity permits femtomole DNA sampling.

Finally, we expanded the application of our multiplexed DNA-modified electrodes to the electrochemical characterization of DNA-bound proteins containing [4Fe-4S] clusters. DNA-modified electrodes have become an essential tool for the characterization of the redox chemistry of DNA repair proteins that contain redox cofactors. Multiplexed analysis of EndonucleaseIII (EndoIII), a DNA repair protein containing a [4Fe-4S] cluster known to be accessible via DNA-mediated charge transport, elucidated subtle differences in the electrochemical behavior as a function of DNA morphology. DNA-bound EndoIII is seen to have two different electron transfer pathways for reduction, either through the DNA base stack or through direct surface reduction. Closely packed DNA films, where the protein has limited surface accessibility, produce electrochemical signals reflecting electron transfer that is DNA-mediated. The electrochemical comparison of EndoIII mutants, including a new family of mutations altering the electrostatics surrounding the [4Fe-4S] cluster, was able to be quantitatively performed. While little change in the midpoint potential was found for this family of mutants, significant variations in the efficiency of DNA-mediated electron transfer were apparent. Based on the stability of these proteins, examined by circular dichroism, we propose that the electron transfer pathway can be perturbed not only by the removal of aromatic residues, but also through changes in solvation near the cluster.

Spectral evolution of angularly resolved third-order harmonic generation by infrared femtosecond laser-pulse filamentation in air

We experimentally investigate the evolution of an angularly resolved spectrum of third harmonic generated by infrared femtosecond laser pulse filamentation in air. We show that at low pump intensity, phase matching between the fundamental and third-harmonic waves dominates the nonlinear optical effect and induces a ring structure of the third-harmonic beam, whereas at high pump intensity, the dispersion properties of air begin to affect the angular spectrum, leading to the formation of a nonlinear X wave at third harmonic.

Theoretical investigation of single attosecond pulse generation in an orthogonally polarized two-color laser field

We theoretically demonstrate the generation of extreme ultraviolet supercontinua in an orthogonally polarized two-color few-cycle laser field. We show that the ionized electrons can be driven back to their parent ion after traveling along curved trajectories in a plane perpendicular to the beam propagation direction, giving rise to a train of attosecond pulses at different polarization angles. A single isolated attosecond pulse can be obtained by blocking the low-order high harmonics, which contribute to the formation of the satellite pulses. (C) 2008 Optical Society of America.

Tunable high-order harmonic generation and the role of the folded quantum path

We theoretically demonstrate the selective enhancement of high-order harmonic generation (HHG) in two-color laser fields consisting of a single-cycle fundamental wave (800 nm wavelength) and a multicycle subharmonic wave (2400 nm wavelength). By performing time-frequency analyses based on a single-active-electron model, we reveal that such an enhancement is a result of the modified electron trajectories in the two-color field. Furthermore, we show that selectively enhanced HHG gives rise to a bandwidth-controllable extreme ultraviolet supercontinuum in the plateau region, facilitating the generation of intense single isolated attosecond pulses.

Single sub-100 attosecond pulse generation in a two-colour time-gating laser field

We theoretically propose a method of generating a single sub-100 attosecond (as) pulse with a two-colour time-gating laser field. The field is synthesized by an 8 fs/800 nm (three optical cycles) pulse and a 24 fs/2400 nm (three optical cycles) pulse with an optimal time delay between them. In our simulation, we obtain a supercontinuum with an extremely broad spectrum of 150 eV and generate an isolated attosecond pulse with 96 as pulse duration without any dispersion compensation.

Generation of sub-5 fs pulses through cascade of filamentation and hollow fiber compression

A pulse-compression scheme based on cascade of filamentation and hollow fiber has been demonstrated, Pulses with duration of sub-5 fs and energy of 0.2 mJ near 800 nm have been generated by compressing the similar to 40 fs pulses from a commercial laser system. This method is promising to generate near monocycle high energy pulses. [GRAPHICS] Measured autocorrelation curve of the final compressed pulses with duration of sub-5 fs (black solid) and the simulated autocorrelation curve of 4.6 fs pulse near 800 rim (red dash) (C) 2008 by Astro Ltd. Published exclusively by WILEY-VCH Verlag GmbH & Co. KGaA

Two-color two-photon excitation of indole using a femtosecond laser regenerative amplifier

The fluorescence emission from indole resulting from two-color two-photon (2C2P) excitation with 400 and 800 nm wavelengths is observed, using the second harmonic and fundamental wavelength of a 800 nm 40 fs pulsed Ti:Sapphire femtosecond (fs) regenerative amplifier operating at a repetition rate of 1 kHz. By delaying one fs laser pulse relative to the other, the cross correlation of fluorescence is observed, which indicates the generation of 2C2P fluorescence signal in the experiment. The strongest 2C2P fluorescence emission characterized by the peak of cross correlation curve suggests optimal temporal overlap of the two fs laser pulses. The 2C2P fluorescence signal is linearly dependent on the total excitation intensity. The fluorescence signals with 400 nm and 800 nm irradiation alone are also demonstrated and discussed in this paper. (C) 2008 Elsevier B.V. All rights reserved.

Phase-matched high-order harmonic generation in a gas cell with midinfrared femtosecond pulses

We experimentally investigate the generation of high-order harmonics in a 4-mm-long gas cell using midinfrared femtosecond pulses at various wavelengths of 1240 nm, 1500 nm, and 1800 nm. It is observed that the yield and cutoff energy of the generated high-order harmonics critically depend on focal position, gas pressure, and size of the input beam which can be controlled by an aperture placed in front of the focal lens. By optimizing the experimental parameters, we achieve a cutoff energy at similar to 190 eV with the 1500 nm driving pulses, which is the highest for the three wavelengths chosen in our experiment.

Generation of plasma intrinsic oscillation at the front surface of a target irradiated by a circularly polarized laser pulse

In laser-target interaction, the effects of laser intensity on plasma oscillation at the front surface of targets have been investigated by one-dimensional particle in cell simulations. The periodical oscillations of the ion density and electrostatic field at the front surface of the targets are reported for the first time, which is considered as an intrinsic property of the target excited by the laser. The oscillation period depends only on initial plasma density and is irrelevant with laser intensity. Flattop structures with curves in ion phase space are found with a more intense laser pulse due to the larger amplitude variation of the electrostatic field. A simple but valid model is proposed to interpret the curves.

Optimization of optical parametric chirped pulse amplification with different pump wavelengths

Optical parametric chirped pulse amplification with different pump wavelengths was investigated using LBO crystal, at signal central wavelength of 800 nm. According to our theoretical simulation, when pump wavelength is 492.5 nm, there is a maximal gain bandwidth of 190 nm. centered at 805 nm in optimal noncollinear angle using LBO. Presently, pump wavelength of 492.5 nm can be obtained from second harmonic generation of a Yb:Sr-5(PO4)(3)F laser. The broad gain bandwidth can completely support similar to 6 fs with a spectral centre of seed pulse at 800 nm. The deviation from optimal noncollinear angle can be compensated by accurately tuning crystal angle for phase matching. The gain spectrum with pump wavelength of 492.5 nm is much better than those with pump wavelengths of 400, 526.5 and 532 nm, at signal centre of 800 nm. (c) 2005 Elsevier B.V. All rights reserved.