Resonant Three-Photon Ionization of Atomic Hydrogen in a Finite-Bandwidth Laser Field and a Static Electric Field

We derive a set of density matrix equations describing laser photo-excitation and ionization of atomic hydrogen in the presence of an external electric field. The equations are relevant as a description of multiphoton ionization of hydrogen (or deuterium) atoms in laser-produced transient plasmas. The laser wavelength is 243 nm, so that the photoionization is resonant with the 2 s 1/2 level. The electric field causes Stark mixing of the 2 s 1/2 level with the 2 p 1/2 and 2 p 3/2 levels. Because the electric field is taken in the same direction as the linear polarization of the laser, only states with equal m j are coupled, and the atom can be described with a four-level density matrix. The laser bandwidth is taken into account by using the stochastic model of a chaotic laser field introduced by Zoller [1]. We present a few calculations of the probabilities for ionization and excitation of a single hydrogen atom as a function of laser intensity and wavelength

Wavelength dependent collective effects in the multiphoton ionization of atomic deuterium

This paper presents the results of an experimental investigation into collective effects in the transient plasma formed by multiphoton ionization of atomic deuterium with a pulsed laser. The laser wavelength is varied in a narrow range around 243 nm, so that the photoionization is resonant with the metastable 2S1/2 state. The ion yield, the ion time-of-flight spectra, and the yield of Lyman-a photons have been measured as a function of laser intensity ~from 1 to 340 MW/cm2! and laser detuning around the 1S1/2-2S1/2 two-photon resonance. During and shortly after the laser pulse, collective effects resulting from the mutual interaction of the photoelectrons and the ions affect the spatial and temporal distribution of the ions. Because of the near-degeneracy of the 2S1/2, 2P1/2 , and 2P3/2 states, the resonant multiphoton ionization is affected by the Stark mixing of these states in the collective field. As a result, the time-dependent yields of ions and of Lyman-a photons are modulated by the interplay of the multiphoton ionization of the atoms and the collective effects in the plasma. From the measurements it is deduced that collective effects are important above a critical charge density of 33108 ions/cm3. An asymmetry is observed in the line profile of the total ion yield as a function of laser detuning. This asymmetry is interpreted to be due to the effect of the collective field upon the intermediate resonant 2S1/2 state of the photoionization process

Wavelength dependent collective effects in the multiphoton ionization of atomic deuterium

This paper presents the results of an experimental investigation into collective effects in the transient plasma formed by multiphoton ionization of atomic deuterium with a pulsed laser. The laser wavelength is varied in a narrow range around 243 nm, so that the photoionization is resonant with the metastable 2S1/2 state. The ion yield, the ion time-of-flight spectra, and the yield of Lyman-a photons have been measured as a function of laser intensity ~from 1 to 340 MW/cm2! and laser detuning around the 1S1/2-2S1/2 two-photon resonance. During and shortly after the laser pulse, collective effects resulting from the mutual interaction of the photoelectrons and the ions affect the spatial and temporal distribution of the ions. Because of the near-degeneracy of the 2S1/2, 2P1/2 , and 2P3/2 states, the resonant multiphoton ionization is affected by the Stark mixing of these states in the collective field. As a result, the time-dependent yields of ions and of Lyman-a photons are modulated by the interplay of the multiphoton ionization of the atoms and the collective effects in the plasma. From the measurements it is deduced that collective effects are important above a critical charge density of 33108 ions/cm3. An asymmetry is observed in the line profile of the total ion yield as a function of laser detuning. This asymmetry is interpreted to be due to the effect of the collective field upon the intermediate resonant 2S1/2 state of the photoionization process

Structural Characterization of Biofunctionalized Gold Nanoparticles by Ultrahigh-Resolution Mass Spectrometry

Bio-organic Synthesi

Analysis of Synthetic Monodisperse Polysaccharides by Wide Mass Range Ultrahigh-Resolution MALDI Mass Spectrometry

Carbohydrates, such as oligo- and polysaccharides, are highly abundant biopolymers that are involved in numerous processes. The study of their structure and functions is commonly based on a material that is isolated from complex natural sources. However, a more precise analysis requires pure compounds with well-defined structures that can be obtained from chemical or enzymatic syntheses. Novel synthetic strategies have increased the accessibility of larger monodisperse polysaccharides, posing a challenge to the analytical methods used for their molecular characterization. Here, we present wide mass range ultrahigh-resolution matrix-assisted laser desorption/ionization (MALDI) Fourier transform ion cyclotron resonance (FT-ICR) mass spectrometry (MS) as a powerful platform for the analysis of synthetic oligo- and polysaccharides. Synthetic carbohydrates 16-, 64-, 100-, and 151-mers were mass analyzed and characterized by MALDI in-source decay FT-ICR MS. Detection of fragment ions generated from glycosidic bond cleavage (or cross-ring cleavage) provided information of the monosaccharide content and the linkage type, allowing for the corroboration of the carbohydrate compositions and structures

Fragmentation processes of ionized 5-fluorouracil in the gas phase and within clusters

We have measured mass spectra for positive ions produced from neutral 5-fluorouracil by electron impact at energies from 0 to 100 eV. Fragment ion appearance energies of this (radio-)chemotherapy agent have been determined for the first time and we have identified several new fragment ions of low abundance. The main fragmentations are similar to uracil, involving HNCO loss and subsequent HCN loss, CO loss, or FCCO loss. The features adjacent to these prominent peaks in the mass spectra are attributed to tautomerization preceding the fragmentation and/or the loss of one or two additional hydrogen atoms. A few fragmentions are distinct for 5-fluorouracil compared to uracil, most notably the production of the reactive moiety CF+. Finally, multiphoton ionization mass spectra are compared for 5-fluorouracil from a laser thermal desorption source and from a supersonic expansion source. The detection of a new fragment ion at 114 u in the supersonic expansion experiments provides the first evidence for a clustering effect on the radiation response of 5-fluorouracil. By analogy with previous experiments and calculations on protonated uracil, this is assigned to NH3 loss from protonated 5-fluorouracil

Tackling bovine TB

On 18 December Defra revealed that during 2018, 32,601 badgers were killed, bringing the total number slaughtered under licence since 2013 to almost 67,000.1 ‘Effectiveness’ claims relate not to the impact on cattle TB, but rather to the ability of the contracted shooters to kill sufficient badgers to satisfy their licence requirements, which they can hardly fail to reach given that target numbers are ‘adjusted’ by Natural England part-way through the culls according to the contractors’ progress. Sixty per cent of the badgers have been killed by ‘controlled shooting’, a method rejected by both the government’s Independent Expert Panel2 and the BVA3 because of animal welfare concerns. During 2018 Natural England directly monitored just 89 (0.43 per cent) of controlled shooting events. It is deplorable that the chief veterinary officer (CVO) continues to support the roll-out of a policy that permits controlled shooting, when veterinary organisations have condemned the method on animal welfare grounds. It is particularly concerning that the CVO appears to have deflected responsibility for humaneness to Natural England’s chief scientist who, as far as we are aware, has no background in animal welfare science. It is also unacceptable for government to attribute reductions in herd bovine TB (bTB) incidents over the first four years of culling in the original ‘pilot’ cull zones to its badger culling policy.4 Independent analysis of this and more recent data from the Gloucestershire pilot cull zone5 indicate that new herd incidence is rising sharply, with 22 herd breakdowns in the 12 months to September 2017 (an increase of 29.4 per cent when compared to the 17 breakdowns reported by APHA for the previous 12 months). Analysis of the 2018 figures indicates that both incidence and prevalence are now rising even faster, with a further 24 herd breakdowns occurring between 1 January and 5 December 2018. To date, the government and its officials cite data that are two years out of date, but have declined to comment on this emerging evidence that, far from resulting in a substantial disease control benefit, badger culls may be leading to a sharp increase in bTB in cattle. Natural England’s chief scientist and the UK’s CVO continue to endorse a failing and inhumane policy, bringing their offices into serious disrepute. We urge them, and the BVA, to reconsider their support for further badger culling, and instead focus on the actual cause of bTB’s epidemic spread – a cattle skin test with a sensitivity of only 50 per cent,6,7 and the ongoing problems associated with cattle movements and on-farm biosecurity

Animal welfare impacts of badger culling operations

We are writing to express our extreme concern following recent media coverage1, 2 relating to the methodology being used by contractors to kill badgers under licence, as part of the government’s policy to control bovine TB in cattle. The coverage relates to the shooting of badgers that have been captured in live traps. Covert video footage (https://bit.ly/2Eud1iR ) from Cumbria shows a trapped badger being shot with a firearm at close range, following which it appears to take close to a minute to stop moving. The contractor clearly observes the animal during this time but makes no attempt to expedite the death of the badger and prevent further suffering, as required by the current Natural England best practice guide which states: ‘Immediately after shooting, the animal should be checked to ensure it is dead, and if there is any doubt, a second shot must be taken as soon as possible.’3 The conversation between the contractor and his companion also suggests they were considering moving the badger to another site before finally bagging the carcase, again breaching the best practice guide. While the footage only relates to the experience of a single badger, and while the degree to which the badger was conscious in the period immediately following the shot is unclear, we can by no means be certain that the badger did not suffer. It also raises serious questions about the training, competence and behaviour of contractors, in relation to both badger welfare, and biosecurity. This adds to existing concerns relating to the humaneness of ‘controlled shooting’ (targeting free-roaming badgers with rifles), which continues to be a permitted method under culling licences, in spite of the reservations expressed by both the government-commissioned Independent Expert Panel in its 2014 report,4 and the BVA, which concluded in 2015 that it ‘can no longer support the continued use of controlled shooting as part of the badger control policy’.5 (However, it has since continued to support the issuing of licences which permit the method). The BVA has consistently indicated its support for what it calls the ‘tried and tested’ method of trapping and shooting, but has thus far failed to provide comprehensive and robust evidence for the humaneness of this method. Figure1 Download figure Open in new tab Download powerpoint Natural England reported that its monitors observed 74 (just over 0.6 per cent) of controlled shooting events for accuracy and humaneness During 2017, almost 20,000 badgers were killed under licence across 19 cull zones, around 60 per cent of which were killed by controlled shooting, the remainder being trapped and shot.6 Natural England reported that its monitors observed 74 (just over 0.6 per cent) of controlled shooting events for accuracy and humaneness. No information has been provided on the extent to which trapping and shooting activities were monitored. This raises serious concerns about the extent of suffering that might be experienced by very large numbers of animals, for which contractors are not being held to account. If contractors reach their maximum culling targets set by Natural England for 2018, as many as 41,000 additional badgers could be killed.7 The extent to which these animals will suffer is once again being left in the hands of contractors, with woefully inadequate oversight, and in the face of anecdotal evidence of breaches of best practice guidance. This situation is clearly unacceptable from an animal welfare perspective and it is our view that by endorsing the policy, the BVA is contradicting the principles contained within its own animal welfare strategy.8 We therefore urge the BVA to withdraw its support for any further licensed badger culling, and the RCVS to make it clear that any veterinarian who provides support for culling activities that result in unnecessary and avoidable animal suffering could face disciplinary proceedings. The veterinary profession has no business supporting this licensed mass killing with all its inherent negative welfare and biosecurity implications, and for which the disease control benefits are, at best, extremely uncertain. We believe the continued support for the culls by veterinary bodies in the face of poor evidence for its efficacy damages the credibility of the profession, and that same support in the face of potential animal suffering on a large scale undermines its reputation. We stand ready to discuss these issues in more detail

Analysis of synthetic monodisperse polysaccharides by wide mass range ultrahigh-resolution MALDI mass spectrometry

Carbohydrates, such as oligo- and polysaccharides, are highly abundant biopolymers that are involved in numerous processes. The study of their structure and functions is commonly based on a material that is isolated from complex natural sources. However, a more precise analysis requires pure compounds with well-defined structures that can be obtained from chemical or enzymatic syntheses. Novel synthetic strategies have increased the accessibility of larger monodisperse polysaccharides, posing a challenge to the analytical methods used for their molecular characterization. Here, we present wide mass range ultrahigh-resolution matrix-assisted laser desorption/ionization (MALDI) Fourier transform ion cyclotron resonance (FT-ICR) mass spectrometry (MS) as a powerful platform for the analysis of synthetic oligo- and polysaccharides. Synthetic carbohydrates 16-, 64-, 100-, and 151-mers were mass analyzed and characterized by MALDI in-source decay FT-ICR MS. Detection of fragment ions generated from glycosidic bond cleavage (or cross-ring cleavage) provided information of the monosaccharide content and the linkage type, allowing for the corroboration of the carbohydrate compositions and structures.Proteomic

Magnetotransport in a pseudomorphic GaAs/GaInAs/GaAlAs heterostructure with a Si delta-doping layer

Magnetotransport properties of a pseudomorphic GaAs/Ga0.8In0.2As/Ga0.75Al0.25As heterostructure are investigated in pulsed magnetic fields up to 50 T and at temperatures of T=1.4 K and 4.2 K. The structure studied consists of a Si delta-layer parallel to a Ga0.8In0.2As quantum well (QW). The dark electron density of the structure is n_e=1.67x 10^16 m^-2. By illumination the density can be increased up to a factor of 4; this way the second subband in the Ga0.8In0.2As QW can become populated as well as the Si delta-layer. The presence of electrons in the delta-layer results in drastic changes in the transport data, especially at magnetic fields beyond 30 T. The phenomena observed are interpreted as: 1) magnetic freeze-out of carriers in the delta-layer when a low density of electrons is present in the delta-layer, and 2) quantization of the electron motion in the two dimensional electron gases in both the Ga0.8In0.2As QW and the Si delta-layer in the case of high densities. These conclusions are corroborated by the numerical results of our theoretical model. We obtain a satisfactory agreement between model and experiment.Comment: 23 pages, RevTex, 11 Postscript figures (accepted for Phys. Rev. B