Conical emission by femtosecond pulses with different spectral bandwidths

Conical emission (CE) has been investigated experimentally by laser pulses with different pulse durations and spectral bandwidths. The results show that the overall CE curve will shift as the varying of spectral bandwidth of pump laser pulse. But for pump laser pulses which have same spectral bandwidth but different pulse duration, the CE angles will be same at the spectral region close to the pump wavelength while will be different at the spectral region far away from the pump wavelength. We have also fitted the measured CE angles with X-wave model. The calculated curves and the measured CE curves match reasonably well. The best fits indicate that the group velocity of the filament pulse may be greatly controlled by controlling the spectral bandwidth of pump laser pulse.     

Dye laser multipass amplifier system

A system is described for producing high power, narrow bandwidth pulses by injecting electro-optically a dye laser pulse to a multipass flashlamp pumped amplifier cavity. Pulses of 280 MHz bandwidth have been generated with peak powers of 100 kW at 5 Hz repetition rate. A simple modification allows 300 ns long pulse trains to be obtained with pulse separations determined by the round trip time of the cavity.     

Practical Aspects of Copper Ion-Based Double Electron Electron Resonance Distance Measurements

We present experimental conditions that lead to high-quality Cu²⁺-based double electron electron resonance (DEER) data. Such experiments are feasible at temperature of about 20 K, and sample concentrations in the range of 0.15–1.5 mM. By systematically investigating the effects of pulse lengths, we find that observer π pulse lengths of 20–48 ns provide reasonable modulation depths as well as signals. The length of the pump pulse needs to be minimized (16 ns in our case). For a Cu²⁺–Cu²⁺ DEER measurement, the optimal frequency offset is about 100 MHz. For a Cu²⁺–nitroxide DEER measurement, the frequency offset is often varied in the range of 100–500 MHz, to probe orientational selectivity. For both cases, the frequency of the pump pulse should be smaller than the observer pulse in order to obtain a larger modulation depth.     

Broadband attosecond pulse shaping

We use semiconductor (Si) and metallic (Al, Zr) transmission filters to shape, in amplitude and phase, high-order harmonics generated from the interaction of an intense titanium sapphire laser field with a pulsed neon gas target. Depending on the properties of the filter, the emitted attosecond pulses can be optimized in bandwidth and/or pulse length. We demonstrate the generation of attosecond pulses centered at energies from 50 to 80 eV, with bandwidths as large as 45 eV and with pulse durations compressed to 130 as.     

Broadband pulses for excitation and inversion in I = 1 systems

New composite pulses for exciting and inverting three-level systems are presented. The π/2 pulse is designed for use in quadrupole echo spectroscopy and has a bandwidth comparable to existing sequences and is slightly shorter. Two new broadband π pulses are presented which have bandwidths larger than other existing I = 1 inverting pulses without being significantly longer. Numerical calculations and experimental examples demonstrate the usefulness of the new sequences.     

Distance measurements in the borderline region of applicability of CW EPR and DEER: a model study on a homologous series of spin-labelled peptides

Inter-spin distances between 1 nm and 4.5 nm are measured by continuous wave (CW) and pulsed electron paramagnetic resonance (EPR) methods for a series of nitroxide-spin-labelled peptides. The upper distance limit for measuring dipolar coupling by the broadening of the CW spectrum and the lower distance limit for the present optimally-adjusted double electron electron resonance (DEER) set-up are determined and found to be both around 1.6-1.9 nm. The methods for determining distances and corresponding distributions from CW spectral line broadening are reviewed and further developed. Also, the work shows that a correction factor is required for the analysis of inter-spin distances below approximately 2 nm for DEER measurements and this is calculated using the density matrix formalism.     

kJ级宽带低相干激光驱动装置

激光等离子体相互作用的不稳定性将有望通过降低高功率激光装置输出光束的相干性得到大幅缓解。利用低相干光源作为种子源,采用钕玻璃放大介质,研制成功国际首台kJ级大带宽低相干激光装置,实现了带宽13 nm、能量960 J、脉宽3～10 ns可调,相干时间仅为300 fs的大能量光脉冲输出。输出脉冲光谱匀滑无纵模结构,且谱相位随机分布,可实现脉冲波形和光谱分布的无关联精密调控。该装置不仅成功演示验证了低相干激光驱动器的单元技术及系统集成技术,同时也为激光等离子体相互作用及高能量密度物理研究提供了全新的实验研究平台。     

Visualization of distance distribution from pulsed double electron-electron resonance data

Double electron-electron resonance (DEER), also known as pulsed electron-electron double resonance (PELDOR), is a time-domain electron paramagnetic resonance method that can measure the weak dipole-dipole interactions between unpaired electrons. DEER has been applied to discrete pairs of free radicals in biological macromolecules and to clusters containing small numbers of free radicals in polymers and irradiated materials. The goal of such work is to determine the distance or distribution of distances between radicals, which is an underdetermined problem. That is, the spectrum of dipolar interactions can be readily calculated for any distribution of free radicals, but there are many, quite different distributions of radicals that could produce the same experimental dipolar spectrum. This paper describes two methods that are useful for approximating the distance distributions for the large subset of cases in which the mutual orientations of the free radicals are uncorrelated and the width of the distribution is more than a few percent of its mean. The first method relies on a coordinate transformation and is parameter-free, while the second is based on iterative least-squares with Tikhonov regularization. Both methods are useful in DEER studies of spin-labeled biomolecules containing more than two labels.     

Spin pair geometry revealed by high-field DEER in the presence of conformational distributions

Orientation selection on two nitroxide-labelled shape-persistent molecules is demonstrated by high-field pulsed electron-electron double resonance experiments at a frequency of 95 GHz with a commercial spectrometer. The experiments are performed with fixed observer and pump frequencies by variation of the magnetic field, so that the variation of both the dipolar frequencies and the modulation depths can be analyzed. By applying the deadtime-free four-pulse double electron-electron resonance (DEER) sequence, the lineshapes of the dipolar spectra are obtained. In the investigated linear biradical and equilateral triradical the nitroxide labels undergo restricted dynamics, so that their relative orientations are not fixed, but are correlated to some extent. In this situation, the general dependence of the dipolar spectra on the observer field can be satisfyingly modelled by simple geometrical models that involve only one rotational degree of freedom for the biradical and two rotational degrees of freedom for the triradical. A somewhat better agreement of the dipolar lineshapes for the biradical is obtained by simulations based on a molecular dynamics trajectory. For the triradical, small but significant deviations of the lineshape are observed with both models, indicating that the technique can reveal deficiencies in modelling of the conformational ensemble of a macromolecule.     

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.     

Band-selective recoupling of homonuclear double-quantum dipolar interaction with a generalized composite 0 degrees pulse: application to 13C aliphatic region-selective magnetization transfer in solids

Recoupling of homonuclear double quantum (DQ)-dipolar interactions is a useful technique for the structural analysis of molecules in solids. We have designed a series of elemental 0 degrees pulses for the recoupling sequences with the rf phase rotation about the z-axis, known as CN. The proposed 0 degrees pulses whose total flip angle >/=360 degrees provide spin rotation vectors in the xy-plane. Thus, the residual spin rotation can be canceled by rf phase rotation about the z-axis. An analysis by the coherent averaging theory showed that effective bandwidths of the recoupling sequences are limited not by the reduction in the dipolar scaling factor but by the increase in the residual spin rotation due to offset. A CN sequence with these elemental pulses provides an effective bandwidth of DQ-dipolar recoupling from ca. 0.5nu(R) to 4nu(R) for numerical simulations. Here, nu(R) is the sample spinning frequency. The 0 degrees pulses were applied to band-selective recoupling for the magnetization transfer in uniformly 13C-labeled molecules. Narrow-band recoupling enhances the magnetization transfer between spins within the effective range by decoupling the dipolar interactions between spins one of which is outside the range. The narrow band operation reduces rf field strength, which improves the CH decoupling. Increases in signal intensities by the use of the proposed 0 degrees pulses are experimentally shown for 13C-labeled amino acids.     

Two-Dimensional Distance Correlation Maps from Pulsed Triple Electron Resonance (TRIER) on Proteins with Three Paramagnetic Centers

Recently, we introduced the pulsed triple electron resonance (TRIER) experiment, which correlates dipolar frequencies of molecules with three electron spins. These correlation patterns contain valuable information: in combination with double electron–electron resonance (DEER) they allow to interpret distance distributions of biological systems that exist in more than one conformation. Together with an improved sequence and new data processing, we were now for the first time able to obtain two-dimensional distance correlation maps of the previously investigated model compounds as well as of spin-labeled proteins. For this we applied two-dimensional approximate Pake transformation to TRIER data. This enabled us to get distance correlation plots from two triple-labeled protein samples that were in good agreement with DEER data and simulations. With such information it should then be possible to assign peaks in DEER distance distributions for macromolecules that can exist in more than one conformation.     

Influences of finite gain bandwidth on pulse propagation in parabolic fiber amplifiers with distributed gain profiles

The evolutions of the pulses propagating in decreasing and increasing gain distributed fiber amplifiers with finite gain bandwidths are investigated by simulations with the nonlinear Schr¨odinger equation. The results show that the parabolic pulse propagations in both the decreasing and the increasing gain amplifiers are restricted by the finite gain bandwidth. For a given input pulse, by choosing a small initial gain coefficient and gain variation rate, the whole gain for the pulse amplification limited by the gain bandwidth may be higher, which is helpful for the enhancement of the output linearly chirped pulse energy. Compared to the decreasing gain distributed fiber amplifier, the increasing gain distributed amplifier may be more conducive to suppress the pulse spectral broadening and increase the critical amplifier length for achieving a larger output linearly chirped pulse energy.     

Generation of long bursts of high-repetition-rate arbitrarily shaped optical pulses using time lens

A technique for the generation of long ultrahigh-speed bursts of optical pulses with arbitrary shapes is proposed. A laser pulse is temporally chirped by a time lens and then passes through a filter with a reconfigurable periodic spectral response, which produces time-delayed replicas of the chirped pulse and recombines them. As a result of the temporal interference between the replicas, the chirped pulse is broken up into short pulses with the shape determined by the chosen filter response. It is demonstrated that the filter acts on a long chirped optical pulse as a temporal modulator with a periodic modulation function. The modulation frequency and bandwidth of the modulator can be much higher than for commercially available high-frequency modulators. The additional advantage of this modulator is the arbitrary shape of the modulation function. A 2.4 ns burst of nearly flat-top pulses with a repetition rate of about 400 GHz is obtained in numerical simulations. In addition, the technique proposed can act as a pulse repetition rate multiplier and a pulse compressor. A repetition rate of 1.589 THz and an individual pulse width of 212 fs are achieved in simulations for a 9.7 ns sinusoidally phase modulated pulse burst.     

Influences of finite gain bandwidth on pulse propagating in parabolic fiber amplifiers with distributed gain profiles

The evolutions of the pulses propagating in decreasing and increasing gain distributed fiber amplifiers with finite gain bandwidths are investigated by simulating with the nonlinear Schrödinger equation. The results show that the parabolic pulse propagations in both the decreasing and the increasing gain amplifiers are restricted by the finite gain bandwidth. For a given input pulse, by choosing small initial gain coefficient and gain variation rate, the whole gain for the pulse amplification limited by the gain bandwidth may be higher, which is helpful to the enhancement of the output linearly chirped pulse energy. Compared to the decreasing gain distributed fiber amplifier, the increasing gain distributed amplifier may be more conducive to suppress the pulse spectral broadening and increase the critical amplifier length for achieving a larger output linearly chirped pulse energy.     

基于耗散孤子种子的啁啾脉冲光纤放大系统输出特性

以不同滤波器带宽下获得的全正色散光纤激光器耗散孤子作为啁啾脉冲放大(CPA)系统的种子脉冲, 研究了光栅对和光纤展宽器CPA系统输出脉冲的可压缩性. 结果表明, 对于大能量耗散孤子种子脉冲, 当CPA系统采用正色散光纤展宽器时, 光纤群速色散与自相位调制之间的相互作用不仅可抑制耗散孤子脉冲光谱调制的影响, 还可使脉冲在光纤展宽器中自相似演化, 从而可提高CPA输出脉冲的可压缩性. 通过优化光纤展宽器长度, 对于耗散孤子种子源, 采用光纤展宽器的CPA系统输出脉冲可压缩性与主脉冲所占脉冲总能量之比均优于采用光栅对展宽器时的情况.     

Time-resolved 2PPE: Probing adsorbate motion on femtosecond time-scales – what is the role of the laser bandwidth?

Recently it has been shown that time-resolved two photon photoemission spectroscopy (TR 2PPE) is capable of probing the atomic motion of an adsorbate after excitation by a femtosecond laser-pulse. In this paper we address the question in how far the bandwidth of the used laser pulse is of importance with respect to the sensitivity of TR 2PPE to the actual nuclear dynamics. In particular, we find that the use of laser pulses of different spectral bandwidth may simplify the interpretation of the measured TR 2PPE autocorrelation traces and help to distinguish between purely electron related contributions and the nuclear dynamics. Our experimental results indicate that for pulses of small bandwidth only the lifetime of the electronic adsorbate excitation at the ground state equilibrium distance is probed. This information can be used as input for the interpretation of autocorrelation traces obtained with large bandwidth pulses, which in addition contain information about the nuclear dynamics of the adsorbate.     

Compensating for pulse imperfections in REDOR

Rotational-echo double resonance (REDOR) is a magic-angle spinning technique for measuring heteronuclear dipolar couplings. Rotor-synchronized pi pulses recouple the dipolar interaction. The accuracy of a REDOR determination of distance or orientation depends totally on the quality of the dephased (recoupled) and full-echo spectra. We present a scheme for measuring and compensating for the effects of pulse imperfections in REDOR experiments. No assumptions are made about the quality of the pi pulses, and no pulses are added or taken away in implementing the compensation for incomplete REDOR dephasing by imperfect pi pulses.     

Selective excitation in pulsed EPR of a spin-correlated triplet-radical pair

Experiments are described in which a low-amplitude microwave pulse excites only one out of three allowed transitions of the quinone radical (Q(A)(-)) in a spin-correlated triplet-radical pair 3PQ(A)(-) of the bacterial photosynthetic reaction center. A second high-amplitude pulse produces a FID whose temporal shape is strongly modulated with frequencies determined by electron-electron dipolar interaction in the pair. The FID is detected in both the in-phase and the out-of-phase channels. The out-of-phase FID is a result of switching off the magnetic dipolar interaction between 3P and Q(A)(-) due to decay of 3P during the time interval between the two pulses. Refocusing of FID by an additional non-selective pulse allows a dead-time free measurement of this modulation. The influence of the dead-time problem on the distance determination is discussed.     

Improved Broadband Inversion Performance for NMR in Liquids

New NMR broadband inversion pulses that compensate both for resonance offset and radiofrequency (RF) inhomogeneity are described. The approach described is a straightforward computer optimization of an initial digitized waveform generated from either a constant-amplitude frequency sweep or from an existing composite inversion pulse. Problems with convergence to local minima are alleviated by the way the optimization is carried out. For a given duration and maximum allowable RF field strength B₁ (but not necessarily given RMS power deposition), the resultant broadband inversion pulse (BIP) shows superior inversion compared to inversion pulses obtained from previous methods, including adiabatic inversion pulses. Any existing BIP can be systematically elaborated to build up longer inversion pulses that perform over larger and larger bandwidths. The resulting pulse need not be adiabatic throughout its duration or across the entire operational bandwidth.