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Light scattering from plasmonic nanojunctions is routinely used to assess their optical properties. However, the microscopic mechanism remains imperfectly understood, and an accurate description requires the experiment in a well-defined environment with a highly precise control of the nanojunction. Here we report on inelastic light scattering (ILS) from plasmonic scanning tunneling microscope (STM) junctions under ultrahigh vacuum and cryogenic conditions. We particularly focus on anti-Stokes continuum generation in the ILS spectra with a narrowband continuous-wave laser excitation, which appears when an electrical bias is applied between the tip and the surface. This anti-Stokes continuum is commonly observed for various STM junctions at ∼10 K, corroborating that it is a universal phenomenon in electrically biased plasmonic nanojunctions. We propose that the microscopic mechanism underlying the anti-Stokes continuum generation is explained by ILS accompanied by electron transfer across the STM junction, whereby the excess energy is provided by the applied bias voltage. This process occurs through either photoluminescence (PL) or electronic Raman scattering (ERS). By recording the ILS spectra in parallel with STM-induced luminescence, we show that ERS becomes dominant when the excitation wavelength matches the plasmonic resonance of the STM junction, whereas PL mainly contributes to the off-resonance excitation. Our results provide an in-depth understanding of ILS by plasmonic nanojunctions and demonstrate that the anti-Stokes continuum can arise from a nonthermal mechanism.

Two-dimensional quantum spin Hall (QSH) insulators are a promising material class for spintronic applications based on topologically-protected spin currents in their edges. Yet, they have not lived up to their technological potential, as experimental realizations are scarce and limited to cryogenic temperatures. These constraints have also severely restricted characterization of their dynamical properties. Here, we report on the electron dynamics of the novel room-temperature QSH candidate bismuthene after photoexcitation using time- and angle-resolved photoemission spectroscopy. We map the transiently occupied conduction band and track the full relaxation pathway of hot photocarriers. Intriguingly, we observe photocarrier lifetimes much shorter than in \red{conventional} semiconductors. This is ascribed to the presence of topological in-gap states already established by local probes. Indeed, we find spectral signatures consistent with these earlier findings. Demonstration of the large band gap and the view into photoelectron dynamics mark a critical step toward optical control of QSH functionalities., Comment: 13 pages, 11 figures

Abnormal cerebral accumulation of amyloid-beta peptide (Aβ) is a major hallmark of Alzheimer’s disease. Non-invasive monitoring of Aβ deposits enables assessing the disease burden in patients and animal models mimicking aspects of the human disease as well as evaluating the efficacy of Aβ-modulating therapies. Previous in vivo assessments of plaque load have been predominantly based on macroscopic fluorescence reflectance imaging (FRI) and confocal or two-photon microscopy using Aβ-specific imaging agents. However, the former method lacks depth resolution, whereas the latter is restricted by the limited field of view preventing a full coverage of the large brain region. Here, we utilized a fluorescence molecular tomography (FMT)-magnetic resonance imaging (MRI) pipeline with the curcumin derivative fluorescent probe CRANAD-2 to achieve full 3D brain coverage for detecting Aβ accumulation in the arcAβ mouse model of cerebral amyloidosis. A homebuilt FMT system was used for data acquisition, whereas a customized software platform enabled the integration of MRI-derived anatomical information as prior information for FMT image reconstruction. The results obtained from the FMT-MRI study were compared to those from conventional planar FRI recorded under similar physiological conditions, yielding comparable time courses of the fluorescence intensity following intravenous injection of CRANAD-2 in a region-of-interest comprising the brain. In conclusion, we have demonstrated the feasibility of visualizing Aβ deposition in 3D using a multimodal FMT-MRI strategy. This hybrid imaging method provides complementary anatomical, physiological and molecular information, thereby enabling the detailed characterization of the disease status in arcAβ mouse models, which can also facilitate monitoring the efficacy of putative treatments targeting Aβ.

The visual evoked potential (VEP) has been shown to reflect the size of the neural population activated by a processing mechanism selective to the temporal - and spatial luminance contrast property of a stimulus. We set out to better understand how the factors determining the neural response associated with these mechanisms. To do so we recorded the VEP from 14 healthy volunteers viewing two series of pattern reversing stimuli with identical temporal-and spatial luminance contrast properties. In one series the size of the elements increased towards the edge of the image, in the other it decreased. In the former element size was congruent with receptive field size across eccentricity, in the later it was incongruent. P100 amplitude to the incongruent series exceeded that obtained to the congruent series. Using electric dipoles due the excitatory neural response we accounted for this using dipole cancellation of electric dipoles of opposite polarity originating in supra- and infragranular layers of V1. The phasic neural response in granular lamina of V1 exhibited magnocellular characteristics, the neural response outside of the granular lamina exhibited parvocellular characteristics and was modulated by re-entrant projections. Using electric current density, we identified areas of the dorsal followed by areas of the ventral stream as the source of the re-entrant signal modulating infragranular activity. Our work demonstrates that the VEP does not signal reflect the overall level of a neural response but is the result of an interaction between electric dipoles originating from neural responses in different lamina of V1.

Characterization of the electronic band structure of solid state materials is routinely performed using photoemission spectroscopy. Recent advancements in short-wavelength light sources and electron detectors give rise to multidimensional photoemission spectroscopy, allowing parallel measurements of the electron spectral function simultaneously in energy, two momentum components and additional physical parameters with single-event detection capability. Efficient processing of the photoelectron event streams at a rate of up to tens of megabytes per second will enable rapid band mapping for materials characterization. We describe an open-source workflow that allows user interaction with billion-count single-electron events in photoemission band mapping experiments, compatible with beamlines at 3rd and 4rd generation light sources and table-top laser-based setups. The workflow offers an end-to-end recipe from distributed operations on single-event data to structured formats for downstream scientific tasks and storage to materials science database integration. Both the workflow and processed data can be archived for reuse, providing the infrastructure for documenting the provenance and lineage of photoemission data for future high-throughput experiments. Deutsche Forschungsgemeinschaft (German Research Foundation) https://doi.org/10.13039/501100001659 Villum Fonden (Villum Foundation) https://doi.org/10.13039/100008398 EC | EU Framework Programme for Research and Innovation H2020 | H2020 Priority Excellent Science | H2020 European Research Council (H2020 Excellent Science - European Research Council) https://doi.org/10.13039/100010663 Max-Planck-Gesellschaft (Max Planck Society) https://doi.org/10.13039/501100004189

A pecuniary externality in economies with downward nominal wage rigidity leads firms to hire too many workers in expansions, which leads to too much unemployment in recessions. When firms hire more workers, firms fail to internalize that competition for workers between firms pushes up the aggregate wage, which imposes a negative externality over other firms. The externality can be resolved by a macroprudential tax on labor in expansions. In the calibrated model, the tax reduces the welfare cost of downward nominal wage rigidity by up to 90%, as it makes the economy significantly less exposed to unemployment crises.

We report on the nanoscale heating mechanism of an ultrathin ZnO film using low-temperature tip-enhanced Raman spectroscopy. Under the resonance condition, intense Stokes and anti-Stokes Raman scattering can be observed for the phonon modes of a two-monolayer (ML) ZnO on an Ag(111) surface, enabling us to monitor local heating at the nanoscale. It is revealed that the local heating originates mainly from inelastic electron tunneling through the electronic resonance when the bias voltage exceeds the conduction band edge of the 2-ML ZnO. When the bias voltage is lower than the conduction band edge, the local heating arises from two different contributions, namely direct optical excitation between the interface state and the conduction band of 2-ML ZnO or injection of photoexcited electrons from an Ag tip into the conduction band. These optical heating processes are promoted by localized surface plasmon excitation. Simultaneous mapping of tip-enhanced Raman spectroscopy and scanning tunneling spectroscopy for 2-ML ZnO including an atomic-scale defect demonstrates visualizing a correlation between the heating efficiency and the local density of states, which further allows us to analyze the local electron-phonon coupling strength with ∼2 nm spatial resolution.

The realtime follow-up of neutrino events is a promising approach to search for astrophysical neutrino sources. It has so far provided compelling evidence for a neutrino point source: the flaring gamma-ray blazar TXS 0506+056 observed in coincidence with the high-energy neutrino IceCube-170922A detected by IceCube. The detection of very-high-energy gamma rays (VHE, $\mathrm{E} > 100\,\mathrm{GeV}$) from this source helped establish the coincidence and constrained the modeling of the blazar emission at the time of the IceCube event. The four major imaging atmospheric Cherenkov telescope arrays (IACTs) - FACT, H.E.S.S., MAGIC, and VERITAS - operate an active follow-up program of target-of-opportunity observations of neutrino alerts sent by IceCube. This program has two main components. One are the observations of known gamma-ray sources around which a cluster of candidate neutrino events has been identified by IceCube (Gamma-ray Follow-Up, GFU). Second one is the follow-up of single high-energy neutrino candidate events of potential astrophysical origin such as IceCube-170922A. GFU has been recently upgraded by IceCube in collaboration with the IACT groups. We present here recent results from the IACT follow-up programs of IceCube neutrino alerts and a description of the upgraded IceCube GFU system., Presented at the 37th International Cosmic Ray Conference (ICRC 2021). See arXiv:2107.06966 for all IceCube contributions. See arXiv:2108.05257 for all H.E.S.S. contributions

Few data exist on health-related quality of life (QoL) in patients with metastatic pancreatic cancer (mPC) receiving first-line chemotherapy (Awad L ZE, Mesbah M Boston, MA. Applying survival data methodology to analyze quality of life data, in Mesbah M, Cole BF, Ting Lee M-L (eds): Statistical Methods for Quality of Life Studies: Design, Measurements and Analysis. Kluwer Academic Publishers 2002). The QOLIXANE study is a prospective, noninterventional, multicenter substudy of the Platform for Outcome, Quality of Life and Translational Research on Pancreatic Cancer (PARAGON) registry, which evaluated QoL in patients with mPC receiving first-line gemcitabine and nab-paclitaxel chemotherapy in real-life setting. QoL was prospectively measured via EORTC QLQ-C30 questionnaires at baseline and every month thereafter. Therapy and efficacy parameters were prospectively collected. Main objectives were the rate of patients without deterioration of Global Health Status/QoL (GHS/QoL) at 3 and 6 months. Six hundred patients were enrolled in 95 German study sites. Median progression-free survival was 5.9 months (95% confidence interval [CI], 5.2-6.3). Median overall survival (OS) was 8.9 months (95% CI, 7.9-10.2), while median time to deterioration of GHS/QoL was 4.7 months (95% CI, 4.0-5.6). With a baseline GHS/QoL score of 46 (SD, 22.8), baseline QoL of the patients was severely impaired, in most cases due to loss in role functioning and fatigue. In the Kaplan-Meier analysis, 61% and 41% of patients had maintained GHS/QoL after 3 and 6 months, respectively. However, in the QoL response analysis, 35% and 19% of patients had maintained (improved or stable) GHS/QoL after 3 and 6 months, respectively, while 14% and 9% had deteriorated GHS/QoL with the remaining patients being nonevaluable. In the Cox regression analysis, GHS/QoL scores strongly predicted survival with a hazard ratio of 0.86 (P < .0001). Patients with mPC have poor QoL at baseline that deteriorates within a median of 4.7 months. Treatment with gemcitabine and nab-paclitaxel is associated with maintained QoL in relevant proportions of patients. However, overall, results remain poor, reflecting the aggressive nature of the disease.

We resolve the real-time coherent rotational motion of isolated water molecules encapsulated in fullerene-C60 cages by time-domain terahertz (THz) spectroscopy. We employ single-cycle THz pulses to excite the low-frequency rotational motion of water and measure the subsequent coherent emission of electromagnetic waves by water molecules. At temperatures below ~ 100 K, C60 lattice vibrational damping is mitigated and the quantum dynamics of confined water are resolved with a markedly long rotational coherence, extended beyond 10 ps. The observed rotational transitions agree well with low-frequency rotational dynamics of single water molecules in the gas phase. However, some additional spectral features with their major contribution at ~2.26 THz are also observed which may indicate interaction between water rotation and the C60 lattice phonons. We also resolve the real-time change of the emission pattern of water after a sudden cooling to 4 K, signifying the conversion of ortho-water to para-water over the course of 10s hours. The observed long coherent rotational dynamics of isolated water molecules confined in C60 makes this system an attractive candidate for future quantum technology., Deutsche Forschungsgemeinschaft, EPSRC-UK, Projekt DEAL

Direct-deposition Additive Manufacturing technologies like Fused Deposition Modeling suffer from several drawbacks such as anisotropic mechanical properties which impair part quality. Multi-Axis Additive Manufacturing (MAAM) promises to significantly reduce these drawbacks. However, path-planning for the complex kinematics still poses a problem which has only been solved partly and for very specific applications. This paper proposes a software architecture for a general purpose path-planning tool for MAAM technologies enabling the simultaneous implementation of different strategies. The architecture is designed to be extensible, largely machine independent and enables granular multi-scale optimizations. First implementation results and illustrating examples demonstrate the modularity and extensibility.

International audience; The large tolerance of hybrid perovksites to the trapping of electrons by defects is a key asset in photovoltaic applications. Here, the ionic surface terminations of CH3NH3PbI3 are employed as a testbed to study the effect of electrostatic fields on the dynamics of excited carriers. We characterize the transition across the tetragonal to orthorhombic phase. The observed type II band offset and drift of the excited electrons highlight the important role that organic cations have on the screening of local electrostatic fields. When the orientation of organic cations is frozen in the orthorhombic phase, the positively charged termination induces a massive accumulation of excited electrons at the surface of the sample. Conversely, no electron accumulation is observed in the tetragonal phase. We conclude that the local fields cannot penetrate in the sample when the polarizability of freely moving cations boosts the dielectric constant up to ϵ = 120.

Magnetic Weyl semimetals are an emerging material class that combines magnetic order and a topologically non-trivial band structure. Here, we study ultrafast optically driven spin injection from thin films of the magnetic Weyl semimetals Co2MnGa and Co2MnAl into an adjacent Pt layer by means of terahertz emission spectroscopy. We find that (i) Co2MnGa and Co2MnAl are efficient terahertz spin-current generators reaching efficiencies of typical 3d-transition-metal ferromagnets such as Fe. (ii) The relaxation of the spin current provides an estimate of the electron-spin relaxation time of Co2MnGa (170 fs) and Co2MnAl (100 fs), which is comparable to Fe (90 fs). Both observations are consistent with a simple analytical model and highlight the large potential of magnetic Weyl semimetals as spin-current sources in terahertz spintronic devices. Finally, our results provide a strategy to identify magnetic materials that offer maximum spin-current amplitudes for a given deposited optical energy density.

Spin transport is crucial for future spintronic devices operating at bandwidths up to the terahertz range. In F|N thin-film stacks made of a ferromagnetic/ferrimagnetic layer F and a normal-metal layer N, spin transport is mediated by (1) spin-polarized conduction electrons and/or (2) torque between electron spins. To identify a crossover from (1) to (2), we study laser-driven spin currents in F|Pt stacks where F consists of model materials with different degrees of electrical conductivity. For the magnetic insulators yttrium iron garnet, gadolinium iron garnet (GIG) and γ−Fe2O3, identical dynamics is observed. It arises from the terahertz interfacial spin Seebeck effect (SSE), is fully determined by the relaxation of the electrons in the metal layer, and provides a rough estimate of the spin-mixing conductance of the GIG/Pt and γ−Fe2O3/Pt interfaces. Remarkably, in the half-metallic ferrimagnet Fe3O4 (magnetite), our measurements reveal two spin-current components with opposite direction. The slower, positive component exhibits SSE dynamics and is assigned to torque-type magnon excitation of the A- and B-spin sublattices of Fe3O4. The faster, negative component arises from the pyrospintronic effect and can consistently be assigned to ultrafast demagnetization of minority-spin hopping electrons. This observation supports the magneto-electronic model of Fe3O4. In general, our results provide a route to the contact-free separation of torque- and conduction-electron-mediated spin currents., The authors acknowledge funding by the German Research Foundation through the collaborative research centers SFB TRR 227 “Ultrafast spin dynamics” (Project ID 328545488, projects A05, B02, and B03), SFB TRR 173 “Spin + X” (Project No. 358671374, projects A01 and B02), the European Union H2020 program through the project CoG TERAMAG(GrantNo.681917), the Spanish Ministry of Science and Innovation (Project No. PID2020-112914RB-I00), the National Natural Science Foundation of China (Grants No. 61988102 and No. 61975110), and the Czech Science Foundation through Project GA CR/Grant No. 21-28876J. P.J.-C. acknowledges the Spanish MECD for support through the FPU program (References No. FPU014/02546 and No. EST17/00382.)

We present a model that reproduces two salient facts characterizing the international monetary system: Fast growing emerging countries i) run current account surpluses, ii) accumulate international reserves and receive net private inflows. We study a two-sector, tradable and non-tradable, small open economy. There is a growth externality in the tradable sector and agents have imperfect access to international financial markets. By accumulating foreign reserves, the government induces a real exchange rate depreciation and a reallocation of production towards the tradable sector that boosts growth. Financial frictions generate imperfect substitutability between private and public debt flows so that private agents do not perfectly offset the government policy. The possibility of using reserves to provide liquidity during crises amplifies the positive impact of reserve accumulation on growth. The optimal reserve management entails a fast rate of reserve accumulation, as well as higher growth and larger current account surpluses compared to the economy with no policy intervention. Financial support from the ESRC Grant on the Macroeconomics of Capital Account Liberalization is acknowledged. Luca Fornaro acknowledges financial support from the European Research Council under the European Union's Horizon 2020 research and innovation program, Starting Grant (851896-KEYNESGROWTH) and the Spanish Ministry of Economy and Competitiveness, through the Severo Ochoa Programme for Centres of Excellence in R&D (SEV2015-0563 and CEX2019-000915-S), and from the Generalitat de Catalunya, through CERCA and SGR Programme (2017-SGR-1393).

The solvation of ions changes the physical, chemical and thermodynamic properties of water, and the microscopic origin of this behaviour is believed to be ion-induced perturbation of water’s hydrogen-bonding network. Here we provide microscopic insights into this process by monitoring the dissipation of energy in salt solutions using time-resolved terahertz–Raman spectroscopy. We resonantly drive the low-frequency rotational dynamics of water molecules using intense terahertz pulses and probe the Raman response of their intermolecular translational motions. We find that the intermolecular rotational-to-translational energy transfer is enhanced by highly charged cations and is drastically reduced by highly charged anions, scaling with the ion surface charge density and ion concentration. Our molecular dynamics simulations reveal that the water–water hydrogen-bond strength between the first and second solvation shells of cations increases, while it decreases around anions. The opposite effects of cations and anions on the intermolecular interactions of water resemble the effects of ions on the stabilization and denaturation of proteins.

This report is the second part of a comprehensive two-part series aimed at reviewing an extensive and diverse toolkit of novel methods to explore brain health and function. While the first report focused on neurophotonic tools mostly applicable to animal studies, here, we highlight optical spectroscopy and imaging methods relevant to noninvasive human brain studies. We outline current state-of-the-art technologies and software advances, explore the most recent impact of these technologies on neuroscience and clinical applications, identify the areas where innovation is needed, and provide an outlook for the future directions.

SIGNIFICANCE: Multi-laboratory initiatives are essential in performance assessment and standardization-crucial for bringing biophotonics to mature clinical use-to establish protocols and develop reference tissue phantoms that all will allow universal instrument comparison. AIM: The largest multi-laboratory comparison of performance assessment in near-infrared diffuse optics is presented, involving 28 instruments and 12 institutions on a total of eight experiments based on three consolidated protocols (BIP, MEDPHOT, and NEUROPT) as implemented on three kits of tissue phantoms. A total of 20 synthetic indicators were extracted from the dataset, some of them defined here anew. APPROACH: The exercise stems from the Innovative Training Network BitMap funded by the European Commission and expanded to include other European laboratories. A large variety of diffuse optics instruments were considered, based on different approaches (time domain/frequency domain/continuous wave), at various stages of maturity and designed for different applications (e.g., oximetry, spectroscopy, and imaging). RESULTS: This study highlights a substantial difference in hardware performances (e.g., nine decades in responsivity, four decades in dark count rate, and one decade in temporal resolution). Agreement in the estimates of homogeneous optical properties was within 12% of the median value for half of the systems, with a temporal stability of

Polaritons can provide strong optical field enhancement allowing to boostlight-matter interaction. Here, we experimentally observe enhancement ofmid-infrared second-harmonic generation (SHG) using grating-coupled surfacephonon polaritons of the 6H-SiC surface. In our experiment, we measure the SHGalong the polariton dispersion by changing the incidence angle of theexcitation beam. We observe hybridization between the propagating surfacephonon polaritons and localized plasmon resonances in the gold grating,evidenced by the modification of the polariton dispersion as we change the arearatio of grating and substrate. Design options for engineering theplasmon-phonon polariton hybridization are discussed. Overall, we find a ratherlow yield of polariton-enhanced SHG in this geometry compared to prism-couplingand nanostructures, and discuss possible origins.

We correct an error in equation (60) of the original publication.

Recent years have seen a huge progress in the development of phase-sensitive second-order laser spectroscopy which has proven to be a very powerful tool for the investigation of interfaces. In these techniques, the nonlinear interaction between two short laser pulses and the sample yields a signal pulse which subsequently interferes with a third pulse, the so-called local oscillator. To obtain accurate phase information, the relative phases between the signal and local oscillator pulses must be stabilized and their timings precisely controlled. Despite much progress made, fulfilling both requirements remains a formidable experimental challenge. The two common approaches employ different beam geometries which each yields its particular advantages and deficiencies. While noncollinear spectrometers allow for a relatively simple timing control they typically yield poor phase stability and require a challenging alignment. Collinear approaches in contrast come with a simplified alignment and improved phase stability but typically suffer from a highly limited timing control. In this contribution we present a general experimental solution which allows for combining the advantages of both approaches while being compatible with most of the common spectrometer types. On the basis of a collinear geometry, we exploit different selected polarization states of the light pulses in well-defined places in the spectrometer to achieve a precise timing control. The combination of this technique with a balanced detection scheme allows for the acquisition of highly accurate phase-resolved nonlinear spectra without any loss in experimental flexibility. In fact, we show that the implementation of this technique allows us to employ advanced pulse timing schemes inside the spectrometer, which can be used to suppress nonlinear background signals and extend the capabilities of our spectrometer to measure phase-resolved sum frequency spectra of interfaces in a liquid cell.

In a study by Law and colleagues recently published in Neuroimage, the authors reported that wearing a surgical mask during an fMRI scan leads to a statistically significant subject-specific change (30%) in the baseline BOLD level in gray matter, although the response to a sensory-motor task was unaffected. An average increase in end-tidal CO2 of 7.4% was found when wearing a mask, despite little support in the literature for major effects of mask wearing on blood gas levels. We comment on these findings, point out a several relevant limitations of the study design and provide alternative interpretations of these data.