Multiphoton Transitions in a Spin System Driven by Strong Bichromatic Field

EPR transient nutation spectroscopy is used to measure the effective field (Rabi frequency) for multiphoton transitions in a two-level spin system bichromatically driven by a transverse microwave (MW) field and a longitudinal radio-frequency (RF) field. The behavior of the effective field amplitude is examined in the case of a relatively strong MW field, when the derivation of the effective Hamiltonian cannot be reduced to first-order perturbation theory in w_{1} / w_{rf} (w_{1} is the microwave Rabi frequency, w_{rf} is the RF frequency). Experimental results are consistently interpreted by taking into account the contributions of second and third order in w_{1} / w_{rf} evaluated by Krylov-Bogolyubov-Mitropolsky averaging. In the case of inhomogeneously broadened EPR line, the third-order correction modifies the nutation frequency, while the second-order correction gives rise to a change in the nutation amplitude due to a Bloch-Siegert shift.Comment: 7 pages, 6 figure

Boom‐bust dynamics in biological invasions: towards an improved application of the concept

Boom‐bust dynamics – the rise of a population to outbreak levels, followed by a dramatic decline – have been associated with biological invasions and offered as a reason not to manage troublesome invaders. However, boom‐bust dynamics rarely have been critically defined, analyzed, or interpreted. Here, we define boom‐bust dynamics and provide specific suggestions for improving the application of the boom‐bust concept. Boom‐bust dynamics can arise from many causes, some closely associated with invasions, but others occurring across a wide range of ecological settings, especially when environmental conditions are changing rapidly. As a result, it is difficult to infer cause or predict future trajectories merely by observing the dynamic. We use tests with simulated data to show that a common metric for detecting and describing boom‐bust dynamics, decline from an observed peak to a subsequent trough, tends to severely overestimate the frequency and severity of busts, and should be used cautiously if at all. We review and test other metrics that are better suited to describe boom‐bust dynamics. Understanding the frequency and importance of boom‐bust dynamics requires empirical studies of large, representative, long‐term data sets that use clear definitions of boom‐bust, appropriate analytical methods, and careful interpretations

Band structure of semimagnetic Hg1-yMnyTe quantum wells

The band structure of semimagnetic Hg_1-yMn_yTe/Hg_1-xCd_xTe type-III quantum wells has been calculated using eight-band kp model in an envelope function approach. Details of the band structure calculations are given for the Mn free case (y=0). A mean field approach is used to take the influence of the sp-d exchange interaction on the band structure of QW's with low Mn concentrations into account. The calculated Landau level fan diagram and the density of states of a Hg_0.98Mn_0.02Te/Hg_0.3Cd_0.7Te QW are in good agreement with recent experimental transport observations. The model can be used to interpret the mutual influence of the two-dimensional confinement and the sp-d exchange interaction on the transport properties of Hg_1-yMn_yTe/Hg_1-xCd_xTe QW's.Comment: 12 pages, 4 figure

Do alien species affect native freshwater megafauna?

1. Freshwater megafauna species (i.e., animals that can reach a body mass ≥30 kg, including fish, reptiles, mammals, and amphibians) play important roles in freshwater systems (e.g., by influencing habitat structure, trophic dynamics, or the dispersal of smaller species). As they tend to be large and charismatic, they may also function as flagship umbrella species in future freshwater conservation initiatives. Despite this, as a group they are highly threatened, and our knowledge of the nature of these threats is limited. In this study, we aim to improve our understanding of the impacts of alien species on native freshwater megafauna. 2. We undertook the first global assessment of the impacts of alien species on native freshwater megafauna using the Environmental Impact Classification for Alien Taxa (EICAT) framework. We conducted a literature review to identify published and grey literature on impacts, which we quantified and categorised by their severity and type, following the EICAT guidelines. 3. Negative impacts on native freshwater megafauna were caused by 61 alien species from a diverse range of taxonomic groups, including both freshwater and terrestrial alien species, and both vertebrates and invertebrates. They adversely affected 44 of 216 native freshwater megafauna species, including amphibians, fish, mammals, and reptiles. The Great Lakes Basin had the highest number of affected megafauna species (six of the 14 freshwater megafauna species it supports, mainly fish). Impacts occurred through a broad range of mechanisms (10 of the 12 identified mechanisms under EICAT); predation and competition were the most frequently reported mechanisms. Some impacts were relatively minor, adversely affecting the performance of individuals of native freshwater megafauna species. However, some reported impacts did cause declining populations of native freshwater megafauna species, and one impact contributed to the local extinction of the ship sturgeon (Acipenser nudiventris) in the Aral Sea. The vulnerability of native freshwater megafauna species to different types of impact varies during different life-cycle stages (egg, juvenile, and adult). 4. Our understanding of impacts posed by alien species on native freshwater megafauna is limited because data are unavailable for many regions, particularly the Global South, including hotspots for freshwater megafauna diversity such as the Amazon, Congo, Mekong, and Ganges-Brahmaputra basins. Freshwater megafauna species are often subject to multiple threats, which makes it difficult to determine the significance of alien species impacts relative to other threats such as habitat degradation and overexploitation. In addition, short-term studies are likely to be masking the severity of the impacts identified. We call for more long-term studies that attempt to identify population-level impacts, and for studies that identify impacts in data-deficient regions. 5. The EICAT assessments undertaken for this study will be reviewed by the EICAT Authority and subsequently incorporated into the IUCN EICAT database. They may be used to guide future research and conservation actions

Q-band EPR cryoprobe

Following the success of cryogenic EPR signal preamplification at X-band, we present a Q-band EPR cryoprobe compatible with a standard EPR resonator. The probehead is equipped with a cryogenic ultra low-noise microwave amplifier and its protection circuit that are placed close to the sample in the same cryostat. Our cryoprobe maintains the same sample access and tuning which is typical in Q-band EPR, as well as supports high-power pulsed experiments on typical samples. The performance of our setup is benchmarked against that of existing commercial and home-built Q-band spectrometers, using CW EPR and pulsed EPR/ENDOR experiments to reveal a significant sensitivity improvement which reduces the measurement time by a factor of about 40× at 6 K temperature at reduced power levels

Theory for the Ultrafast Structural Response of optically excited small clusters: Time-dependence of the Ionization Potential

Combining an electronic theory with molecular dynamics simulations we present results for the ultrafast structural changes in small clusters. We determine the time scale for the change from the linear to a triangular structure after the photodetachment process Ag$_3^- \rightarrow {\rm Ag}_3$. We show that the time-dependent change of the ionization potential reflects in detail the internal degrees of freedom, in particular coherent and incoherent motion, and that it is sensitive to the initial temperature. We compare with experiment and point out the general significance of our results.Comment: 10 pages, Revtex, 3 postscript figure

Dark Photocatalysis: Storage of Solar Energy in Carbon Nitride for Time-Delayed Hydrogen Generation

While natural photosynthesis serves as the model system for efficient charge separation and decoupling of redox reactions, bio-inspired artificial systems typically lack applicability owing to synthetic challenges and structural complexity. We present herein a simple and inexpensive system that, under solar irradiation, forms highly reductive radicals in the presence of an electron donor, with lifetimes exceeding the diurnal cycle. This radical species is formed within a cyanamide-functionalized polymeric network of heptazine units and can give off its trapped electrons in the dark to yield H$_{2}$ , triggered by a co-catalyst, thus enabling the temporal decoupling of the light and dark reactions of photocatalytic hydrogen production through the radical's longevity. The system introduced here thus demonstrates a new approach for storing sunlight as long-lived radicals, and provides the structural basis for designing photocatalysts with long-lived photo-induced states.This work was supported by the Deutsche Forschungsgemeinschaft (project LO1801/1-1) and an ERC Starting Grant (B.V.L., grant number 639233), the Max Planck Society, the cluster of excellence Nanosystems Initiative Munich (NIM), and the Center for Nanoscience (CeNS). We acknowledge support by the Christian Doppler Research Association (Austrian Federal Ministry of Science, Research and Economy, National Foundation for Research, Technology and Development) and the OMV Group (H.K., E.R.). V.W.-h.L. gratefully acknowledges a postdoctoral scholarship from the Max Planck Society

Cu2+-induced self-assembly and amyloid formation of a cyclic d,l-α-peptide: Structure and function

In a wide spectrum of neurodegenerative diseases, self-assembly of pathogenic proteins to cytotoxic intermediates is accelerated by the presence of metal ions such as Cu2+. Only low concentrations of these early transient oligomeric intermediates are present in a mixture of species during fibril formation, and hence information on the extent of structuring of these oligomers is still largely unknown. Here, we investigate dimers as the first intermediates in the Cu2+-driven aggregation of a cyclic D,L-alpha-peptide architecture. The unique structural and functional properties of this model system recapitulate the self-assembling properties of amyloidogenic proteins including beta-sheet conformation and cross-interaction with pathogenic amyloids. We show that a histidine-rich cyclic D,L-alpha-octapeptide binds Cu2+ with high affinity and selectivity to generate amyloid-like cross-beta-sheet structures. By taking advantage of backbone amide methylation to arrest the self-assembly at the dimeric stage, we obtain structural information and characterize the degree of local order for the dimer. We found that, while catalytic amounts of Cu2+ promote aggregation of the peptide to fibrillar structures, higher concentrations dose-dependently reduce fibrillization and lead to formation of spherical particles, showing self-assembly to different polymorphs. For the initial self-assembly step to the dimers, we found that Cu2+ is coordinated on average by two histidines, similar to self-assembled peptides, indicating that a similar binding interface is perpetuated during Cu2+-driven oligomerization. The dimer itself is found in heterogeneous conformations that undergo dynamic exchange, leading to the formation of different polymorphs at the initial stage of the aggregation process

Quantum control of hybrid nuclear-electronic qubits

Pulsed magnetic resonance is a wide-reaching technology allowing the quantum state of electronic and nuclear spins to be controlled on the timescale of nanoseconds and microseconds respectively. The time required to flip either dilute electronic or nuclear spins is orders of magnitude shorter than their decoherence times, leading to several schemes for quantum information processing with spin qubits. We investigate instead the novel regime where the eigenstates approximate 50:50 superpositions of the electronic and nuclear spin states forming "hybrid nuclear-electronic" qubits. Here we demonstrate quantum control of these states for the first time, using bismuth-doped silicon, in just 32 ns: this is orders of magnitude faster than previous experiments where pure nuclear states were used. The coherence times of our states are five orders of magnitude longer, reaching 4 ms, and are limited by the naturally-occurring 29Si nuclear spin impurities. There is quantitative agreement between our experiments and no-free-parameter analytical theory for the resonance positions, as well as their relative intensities and relative Rabi oscillation frequencies. In experiments where the slow manipulation of some of the qubits is the rate limiting step, quantum computations would benefit from faster operation in the hybrid regime.Comment: 20 pages, 8 figures, new data and simulation