R. V. Benjaminsen, Maria A Mattebjerg, J. Henriksen
et al.
Polycations such as polyethylenimine (PEI) are used in many novel nonviral vector designs and there are continuous efforts to increase our mechanistic understanding of their interactions with cells. Even so, the mechanism of polyplex escape from the endosomal/lysosomal pathway after internalization is still elusive. The "proton sponge " hypothesis remains the most generally accepted mechanism, although it is heavily debated. This hypothesis is associated with the large buffering capacity of PEI and other polycations, which has been interpreted to cause an increase in lysosomal pH even though no conclusive proof has been provided. In the present study, we have used a nanoparticle pH sensor that was developed for pH measurements in the endosomal/lysosomal pathway. We have carried out quantitative measurements of lysosomal pH as a function of PEI content and correlate the results to the "proton sponge " hypothesis. Our measurements show that PEI does not induce change in lysosomal pH as previously suggested and quantification of PEI concentrations in lysosomes makes it uncertain that the "proton sponge " effect is the dominant mechanism of polyplex escape.
Abstract. Particle water and pH are predicted using meteorological observations (relative humidity (RH), temperature (T)), gas/particle composition, and thermodynamic modeling (ISORROPIA-II). A comprehensive uncertainty analysis is included, and the model is validated. We investigate mass concentrations of particle water and related particle pH for ambient fine-mode aerosols sampled in a relatively remote Alabama forest during the Southern Oxidant and Aerosol Study (SOAS) in summer and at various sites in the southeastern US during different seasons, as part of the Southeastern Center for Air Pollution and Epidemiology (SCAPE) study. Particle water and pH are closely linked; pH is a measure of the particle H+ aqueous concentration and depends on both the presence of ions and amount of particle liquid water. Levels of particle water, in turn, are determined through water uptake by both the ionic species and organic compounds. Thermodynamic calculations based on measured ion concentrations can predict both pH and liquid water but may be biased since contributions of organic species to liquid water are not considered. In this study, contributions of both the inorganic and organic fractions to aerosol liquid water were considered, and predictions were in good agreement with measured liquid water based on differences in ambient and dry light scattering coefficients (prediction vs. measurement: slope = 0.91, intercept = 0.5 μg m−3, R2 = 0.75). ISORROPIA-II predictions were confirmed by good agreement between predicted and measured ammonia concentrations (slope = 1.07, intercept = −0.12 μg m−3, R2 = 0.76). Based on this study, organic species on average contributed 35% to the total water, with a substantially higher contribution (50%) at night. However, not including contributions of organic water had a minor effect on pH (changes pH by 0.15 to 0.23 units), suggesting that predicted pH without consideration of organic water could be sufficient for the purposes of aqueous secondary organic aerosol (SOA) chemistry. The mean pH predicted in the Alabama forest (SOAS) was 0.94 ± 0.59 (median 0.93). pH diurnal trends followed liquid water and were driven mainly by variability in RH; during SOAS nighttime pH was near 1.5, while daytime pH was near 0.5. pH ranged from 0.5 to 2 in summer and 1 to 3 in the winter at other sites. The systematically low pH levels in the southeast may have important ramifications, such as significantly influencing acid-catalyzed reactions, gas–aerosol partitioning, and mobilization of redox metals and minerals. Particle ion balances or molar ratios, often used to infer pH, do not consider the dissociation state of individual ions or particle liquid water levels and do not correlate with particle pH.
If the quantum mechanical recoil of the electron due to its scattering from the undulator and laser fields dominates the dynamics, a regime of the free-electron laser emerges where quantum effects lead to a drastic change in the radiation properties. However, the large interaction length required for a single-pass quantum free-electron laser impedes the experimental realization. The quantum free-electron laser oscillator, proposed in the present article, is a possible scheme to resolve this issue. Here we show that this device features a photon statistics that is closer to a coherent state in comparison to existing classical free-electron lasers. The device can be even operated in such a way that a sub-Poissonian statistics is obtained. Beside the benefit of demonstrating this pure quantum effect, the narrowing of the photon distribution implies reduced intensity fluctuations of the emitted radiation, which in turn lead to decreased noise in imaging experiments or to an enhanced sensitivity in interferometric applications.
We use numerical simulations to determine whether the saturation length of the self-modulation (SM) instability of a long proton bunch in plasma could be determined by measuring the radius of the bunch halo SM produces. Results show that defocused protons acquire their maximum transverse momentum and exit the wakefields at a distance approximately equal to the saturation length of the wakefields. This suggests that measuring the radius of the halo as a function of plasma length in the AWAKE experiment would yield a very good estimate for the saturation length of SM.
We present a Hamiltonian-based, 3D theory in paraxial approximation for X-ray amplified spontaneous emission (or superfluorescence) pumped by X-ray free-electron laser. The seed field is included. The ensemble-averaged Heisenberg equations become Maxwell-Bloch equations if factorization of operator products is assumed and are adequate when the stimulated emission is dominant. The spontaneous emission is accounted for by adding a random noise term to the atomic coherence, the magnitude of which is uniquely determined from the fact that the expectation value of the normally-ordered product electric field operators associated with an atom does not factorize. The modified Maxwell-Bloch equation we developed reproduces the results of the previous 1D theory based on correlation functions.