pH drives electron density fluctuations that enhance electric field-induced liquid flow.

Liquid flow along a charged interface is commonly described by classical continuum theory, which represents the electric double layer by uniformly distributed point charges. The electrophoretic mobility of hydrophobic nanodroplets in water doubles in magnitude when the pH is varied from neutral to mildly basic (pH 7 → 11). Classical continuum theory predicts that this increase in mobility is due to an increased surface charge. Here, by combining all-optical measurements of surface charge and molecular structure, as well as electronic structure calculations, we show that surface charge and molecular structure at the nanodroplet surface are identical at neutral and mildly basic pH. We propose that the force that propels the droplets originates from two factors: Negative charge on the droplet surface due to charge transfer from and within water, and anisotropic gradients in the fluctuating polarization induced by the electric field. Both charge density fluctuations couple with the external electric field, and lead to droplet flow. Replacing chloride by hydroxide doubles both the charge conductivity via the Grotthuss mechanism, and the droplet mobility. This general mechanism deeply impacts a plethora of processes in biology, chemistry, and nanotechnology and provides an explanation of how pH influences hydrodynamic phenomena and the limitations of classical continuum theory currently used to rationalize these effects.

Comparing individual and group-level simulated neurophysiological brain connectivity using the Jansen and Rit neural mass model.

Computational models are often used to assess how functional connectivity (FC) patterns emerge from neuronal population dynamics and anatomical brain connections. It remains unclear whether the commonly used group-averaged data can predict individual FC patterns. The Jansen and Rit neural mass model was employed, where masses were coupled using individual structural connectivity (SC). Simulated FC was correlated to individual magnetoencephalography-derived empirical FC. FC was estimated using phase-based (phase lag index (PLI), phase locking value (PLV)), and amplitude-based (amplitude envelope correlation (AEC)) metrics to analyze their goodness of fit for individual predictions. Individual FC predictions were compared against group-averaged FC predictions, and we tested whether SC of a different participant could equally well predict participants' FC patterns. The AEC provided a better match between individually simulated and empirical FC than phase-based metrics. Correlations between simulated and empirical FC were higher using individual SC compared to group-averaged SC. Using SC from other participants resulted in similar correlations between simulated and empirical FC compared to using participants' own SC. This work underlines the added value of FC simulations using individual instead of group-averaged SC for this particular computational model and could aid in a better understanding of mechanisms underlying individual functional network trajectories.

Interfacial Inversion, Interference, and IR Absorption in Vibrational Sum Frequency Scattering Experiments.

Molecular interfacial structure greatly determines the properties of nano- and microscale systems. Vibrational sum frequency scattering (SFS) spectroscopy is a unique interface-selective tool to measure the interfacial vibrational spectrum of sub-micron to micron-scale objects dispersed in liquid and solid media. The interfacial structure is extracted from the interfacial susceptibility, a physical property derived from the intensity. Here, we describe the effect of infrared absorption that occurs in a bulk medium that is spectroscopically complex and use the results to investigate the effects of interfacial inversion, interfacial interference, and interfacial interference combined with absorption. We use the same three chemicals to do so, hexadecane oil, water, and a neutral Span80 surfactant. For all cases, the effective surface susceptibility can be retrieved from the intensity. We further find that inverting the phases results in different interfacial structures, even though they are composed of the same three chemicals, and explain this in terms of the different interactions that are necessary to stabilize the drops: steric stabilization for water drops in oil vs. charge stabilization for oil drops in water. Interfacial interference can be used to estimate the surface density of different compounds.

Observation of Linear and Nonlinear Light Localization at the Edges of Moiré Arrays.

We observe linear and nonlinear light localization at the edges and in the corners of truncated moiré arrays created by the superposition of periodic mutually twisted at Pythagorean angles square sublattices. Experimentally exciting corner linear modes in the femtosecond-laser written moiré arrays we find drastic differences in their localization properties in comparison with the bulk excitations. We also address the impact of nonlinearity on the corner and bulk modes and experimentally observe the crossover from linear quasilocalized states to the surface solitons emerging at the higher input powers. Our results constitute the first experimental demonstration of localization phenomena induced by truncation of periodic moiré structures in photonic systems.

Water Structure at the Hydrophobic Nanodroplet Surface Revealed by Vibrational Sum Frequency Scattering Using Isotopic Dilution.

The water structure at the hydrophobic/water interface is key toward understanding hydrophobicity at the molecular level. Herein, we characterize the hydrogen-bonding network of interfacial water next to sub-micron-sized hydrophobic oil droplets dispersed in water using isotopic dilution vibrational sum frequency scattering (SFS) spectroscopy. The relative intensity of different modes, the frequency shift of the uncoupled O-D spectrum, and a low-frequency shoulder (2395 cm-1) reveal that water forms an overall stronger hydrogen-bonding network next to hydrophobic droplets compared to bulk water and the air/water interface. Half of the spectral width of the oil droplet SFS spectrum is determined by inter- and intramolecular coupling of water molecules. Isotopic dilution also confirms the presence of a broad distribution (ca. 2640-2745 cm-1) of non-water-hydrogen-bonded O-D modes that are red-shifted and broadened compared to similar species at the air/water interface. This band corroborates the presence of charge transfer between water and oil.

Observation of Edge Solitons in Topological Trimer Arrays.

We report the experimental observation of nonlinear light localization and edge soliton formation at the edges of fs-laser written trimer waveguide arrays, where transition from nontopological to topological phases is controlled by the spacing between neighboring trimers. We found that, in the former regime, edge solitons occur only above a considerable power threshold, whereas in the latter one they bifurcate from linear states. Edge solitons are observed in a broad power range where their propagation constant falls into one of the topological gaps of the system, while partial delocalization is observed when considerable nonlinearity drives the propagation constant into an allowed band, causing coupling with bulk modes. Our results provide direct experimental evidence of the coexistence and selective excitation in the same or in different topological gaps of two types of topological edge solitons with different internal structures, which can rarely be observed even in nontopological systems. This also constitutes the first experimental evidence of formation of topological solitons in a nonlinear system with more than one topological gap.

Waveguide-lattice-based architecture for multichannel optical transformations.

We consider waveguide lattices as the architecture to implement a wide range of multiport transformations. In this architecture, a particular transfer matrix is obtained by setting step-wise profiles of propagation constants experienced by a field evolving in a lattice. To investigate the capabilities of this architecture, we numerically study the implementation of random transfer matrices as well as several notable cases, such as the discrete Fourier transform, the Hadamard, and permutation matrices. We show that waveguide lattice schemes are more compact than their traditional lumped-parameter counterparts, thus the proposed architecture may be beneficial for photonic information processing systems of the future.

Impaired saccadic eye movements in multiple sclerosis are related to altered functional connectivity of the oculomotor brain network.

BACKGROUND: Impaired eye movements in multiple sclerosis (MS) are common and could represent a non-invasive and accurate measure of (dys)functioning of interconnected areas within the complex brain network. The aim of this study was to test whether altered saccadic eye movements are related to changes in functional connectivity (FC) in patients with MS. METHODS: Cross-sectional eye movement (pro-saccades and anti-saccades) and magnetoencephalography (MEG) data from the Amsterdam MS cohort were included from 176 MS patients and 33 healthy controls. FC was calculated between all regions of the Brainnetome atlas in six conventional frequency bands. Cognitive function and disability were evaluated by previously validated measures. The relationships between saccadic parameters and both FC and clinical scores in MS patients were analysed using multivariate linear regression models. RESULTS: In MS pro- and anti-saccades were abnormal compared to healthy controls A relationship of saccadic eye movements was found with FC of the oculomotor network, which was stronger for regional than global FC. In general, abnormal eye movements were related to higher delta and theta FC but lower beta FC. Strongest associations were found for pro-saccadic latency and FC of the precuneus (beta band ß = -0.23, p = .006), peak velocity and FC of the parietal eye field (theta band ß = -0.25, p = .005) and gain and FC of the inferior frontal eye field (theta band ß = -0.25, p = .003). Pro-saccadic latency was also strongly associated with disability scores and cognitive dysfunction. CONCLUSIONS: Impaired saccadic eye movements were related to functional connectivity of the oculomotor network and clinical performance in MS. This study also showed that, in addition to global network connectivity, studying regional changes in MEG studies could yield stronger correlations.

Non-invasively measured brain activity and radiological progression in diffuse glioma.

Non-invasively measured brain activity is related to progression-free survival in glioma patients, suggesting its potential as a marker of glioma progression. We therefore assessed the relationship between brain activity and increasing tumor volumes on routine clinical magnetic resonance imaging (MRI) in glioma patients. Postoperative magnetoencephalography (MEG) was recorded in 45 diffuse glioma patients. Brain activity was estimated using three measures (absolute broadband power, offset and slope) calculated at three spatial levels: global average, averaged across the peritumoral areas, and averaged across the homologues of these peritumoral areas in the contralateral hemisphere. Tumors were segmented on MRI. Changes in tumor volume between the two scans surrounding the MEG were calculated and correlated with brain activity. Brain activity was compared between patient groups classified into having increasing or stable tumor volume. Results show that brain activity was significantly increased in the tumor hemisphere in general, and in peritumoral regions specifically. However, none of the measures and spatial levels of brain activity correlated with changes in tumor volume, nor did they differ between patients with increasing versus stable tumor volumes. Longitudinal studies in more homogeneous subgroups of glioma patients are necessary to further explore the clinical potential of non-invasively measured brain activity.

On the stability and necessary electrophoretic mobility of bare oil nanodroplets in water.

Hydrophobic oil droplets, particles, and air bubbles can be dispersed in water as kinetically stabilized dispersions. It has been established since the 19th century that such objects harbor a negative electrostatic potential roughly twice larger than the thermal energy. The source of this charge continues to be one of the core observations in relation to hydrophobicity, and its molecular explanation is still debated. What is clear though is that the stabilizing interaction in these systems is understood in terms of electrostatic repulsion via Derjaguin, Landau, Verwey, and Overbeek theory. Recent work [A. P. Carpenter et al., Proc. Natl. Acad. Sci. U. S. A. 116, 9214 (2019)] has added another element into the discussion, reporting the creation of bare near-zero charged droplets of oil in neat water that are stable for several days. Key to the creation of the droplets is a rigorous glassware cleaning procedure. Here, we investigate these conclusions and show that the cleaning procedure of glassware has no influence on the electrophoretic mobility of the droplets and that oil droplets with near-zero charge are unstable. We provide an alternative possible explanation for the observations involving glass surface chemistry.

Optimal design of error-tolerant reprogrammable multiport interferometers.

Photonic information processing demands programmable multiport interferometers capable of implementing arbitrary transfer matrices, for which planar meshes of error-sensitive Mach-Zehnder interferometers are usually exploited. We propose an alternative design that uses a single-static beam splitter (BS) and a variable phase shift as the building blocks. The design possesses superior resilience to manufacturing errors and losses without extra elements added into the scheme. Namely, the power transmissivities of the static BSs can take arbitrary values in the range from ≈1/2 to ≈4/5. In this Letter, we show that the fraction of transfer matrices non-implementable by the interferometers of our design diminishes rapidly with its size.

Robust Architecture for Programmable Universal Unitaries.

The decomposition of large unitary matrices into smaller ones is important because it provides ways to the realization of classical and quantum information processing schemes. Today, most of the methods use planar meshes of tunable two-channel blocks; however, the schemes turn out to be sensitive to fabrication errors. We study a novel decomposition method based on multichannel blocks. We have shown that the scheme is universal even when the block's transfer matrices are chosen at random, making it virtually insensitive to errors. Moreover, the placement of the variable elements can be arbitrary, so that the scheme is not bound to specific topologies. Our method can be beneficial for large-scale implementations of unitary transformations by techniques, which are not of wide proliferation today or have yet to be developed.

Direct test of the "quantum vampire's" shadow absence with use of thermal light.

The counterintuitive nature of quantum physics leads to a number of paradoxes. One of them is a "quantum vampire" effect [Fedorov et al., Optica2, 112 (2015)OPTIC82334-253610.1364/OPTICA.2.000112], which means that the photon annihilation in a part of a large beam does not change the shape of the beam profile (i.e., does not cast a shadow), but it may change the total beam intensity. Previously, this effect was demonstrated just in a simplified double-mode regime [Fedorov et al., Optica2, 112 (2015), OPTIC82334-253610.1364/OPTICA.2.000112 Katamadze et al., Optica5, 723 (2018)OPTIC82334-253610.1364/OPTICA.5.000723]. In this Letter, a direct test of shadow absence after the photon annihilation was performed using the thermal state of light at the input.

Relativistic quantum key distribution system with one-way quantum communication.

Unambiguous state discrimination (USD) is one of the major obstacles for practical quantum key distribution (QKD). Often overlooked, it allows efficient eavesdropping in majority of practical systems, provided the overall channel loss is above a certain threshold. Thus, to remain secure all such systems must not only monitor the actual loss, but also possess a comprehensive information on the safe 'loss vs. BER' levels, which is often well beyond currently known security analyses. The more advanced the protocol the tougher it becomes to find and prove corresponding bounds. To get out of this vicious circle and solve the problem outright, we demonstrate a so called relativistic QKD system, which uses causality to become inherently immune to USD-based attacks. The system proves to be practical in metropolitan line-of-sight arrangements. At the same time it has a very basic structure that allows for a straightforward and comprehensive security analysis.

Laser-written polarizing directional coupler with reduced interaction length.

Integrated optical waveguides, manufactured with femtosecond laser writing (FSLW) technology, enable precise control and manipulation of light in complicated photonic chips. However, due to the intrinsically low anisotropy of FSLW waveguides, polarizing integrated devices have had a relatively large footprint. In this Letter, we demonstrate an approach based on stress-induced anisotropy, allowing us to decrease the size of polarizing directional couplers down to 3.7 mm, almost an order of magnitude shorter than previously reported. The measured extinction ratios at the wavelength of 808 nm are 16 dB and 20 dB for the horizontal and vertical polarizations, respectively. We provide a possible theoretical model for the observed effects.

Luminescence in germania-silica fibers in a 1-2 µm region.

We analyze the origins of the luminescence in germania-silica fibers with high germanium concentration (about 30 mol.% GeO2) in the region of 1-2 µm with a laser pump at the wavelength 532 nm. We show that such fibers demonstrate the high level of luminescence which unlikely allows the observation of photon triplets, generated in a third-order spontaneous parametric downconversion process in such fibers. The only efficient approach to the luminescence reduction is the hydrogen saturation of fiber samples; however, even in this case, the level of residual luminescence is still too high for three-photon registration.

Spatial Bell-State Generation without Transverse Mode Subspace Postselection.

Spatial states of single photons and spatially entangled photon pairs are becoming an important resource in quantum communication. This additional degree of freedom provides an almost unlimited information capacity, making the development of high-quality sources of spatial entanglement a well-motivated research direction. We report an experimental method for generation of photon pairs in a maximally entangled spatial state. In contrast to existing techniques, the method does not require postselection of a particular subspace of spatial modes and allows one to use the full photon flux from the nonlinear crystal, providing a tool for creating high-brightness sources of pure spatially entangled photons. Such sources are a prerequisite for emerging applications in free-space quantum communication.

Tomography of spatial mode detectors.

Transformation and detection of photons in higher-order spatial modes usually requires complicated holographic techniques. Detectors based on spatial holograms suffer from non-idealities and should be carefully calibrated. We report a novel method for analyzing the quality of projective measurements in spatial mode basis inspired by quantum detector tomography. It allows us to calibrate the detector response using only gaussian beams. We experimentally investigate the inherent inaccuracy of the existing methods of mode transformation and provide a full statistical reconstruction of the POVM (positive operator valued measure) elements for holographic spatial mode detectors.

Statistical estimation of the efficiency of quantum state tomography protocols.

A novel operational method for estimating the efficiency of quantum state tomography protocols is suggested. It is based on a priori estimation of the quality of an arbitrary protocol by means of universal asymptotic fidelity distribution and condition number, which takes minimal value for better protocol. We prove the adequacy of the method both with numerical modeling and through the experimental realization of several practically important protocols of quantum state tomography.

Anisotropically and high entanglement of biphoton states generated in spontaneous parametric down-conversion.

We show both theoretically and experimentally that biphoton wave packets generated via spontaneous parametric down-conversion can be strongly anisotropic and highly entangled. The conditions under which these effects exist are found and discussed.