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"Pica, Massimo"
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Long-wavelength fluctuations and anomalous dynamics in 2-dimensional liquids
In 2-dimensional systems at finite temperature, long-wavelength Mermin–Wagner fluctuations prevent the existence of translational long-range order. Their dynamical signature which is the divergence of the vibrational amplitude with the system size also affects disordered solids and it washes out the transient solid-like response generally exhibited by liquids cooled below their melting temperatures. Through a combined numerical and experimental investigation, here we show that long-wavelength fluctuations are also relevant at high temperature, where the liquid dynamics do not reveal a transient solid-like response. In this regime these fluctuations induce an unusual but ubiquitous decoupling between long-time diffusion coefficient D and structural relaxation time τ, where D ∝ τ–κ, with κ > 1. Long-wavelength fluctuations have a negligible influence on the relaxation dynamics only at extremely high temperatures in molecular liquids or at extremely low densities in colloidal systems.
Journal Article
How one might miss early warning signals of critical transitions in time series data: A systematic study of two major currency pairs
There is growing interest in the use of critical slowing down and critical fluctuations as early warning signals for critical transitions in different complex systems. However, while some studies found them effective, others found the opposite. In this paper, we investigated why this might be so, by testing three commonly used indicators: lag-1 autocorrelation, variance, and low-frequency power spectrum at anticipating critical transitions in the very-high-frequency time series data of the Australian Dollar-Japanese Yen and Swiss Franc-Japanese Yen exchange rates. Besides testing rising trends in these indicators at a strict level of confidence using the Kendall-tau test, we also required statistically significant early warning signals to be concurrent in the three indicators, which must rise to appreciable values. We then found for our data set the optimum parameters for discovering critical transitions, and showed that the set of critical transitions found is generally insensitive to variations in the parameters. Suspecting that negative results in the literature are the results of low data frequencies, we created time series with time intervals over three orders of magnitude from the raw data, and tested them for early warning signals. Early warning signals can be reliably found only if the time interval of the data is shorter than the time scale of critical transitions in our complex system of interest. Finally, we compared the set of time windows with statistically significant early warning signals with the set of time windows followed by large movements, to conclude that the early warning signals indeed provide reliable information on impending critical transitions. This reliability becomes more compelling statistically the more events we test.
Journal Article
Dynamic phase coexistence in glass–forming liquids
One of the most controversial hypotheses for explaining the heterogeneous dynamics of glasses postulates the temporary coexistence of two phases characterized by a high and by a low diffusivity. In this scenario, two phases with different diffusivities coexist for a time of the order of the relaxation time and mix afterwards. Unfortunately, it is difficult to measure the single-particle diffusivities to test this hypothesis. Indeed, although the non-Gaussian shape of the van-Hove distribution suggests the transient existence of a diffusivity distribution, it is not possible to infer from this quantity whether two or more dynamical phases coexist. Here we provide the first direct observation of the dynamical coexistence of two phases with different diffusivities, by showing that in the deeply supercooled regime the distribution of the single-particle diffusivities acquires a transient bimodal shape. We relate this distribution to the heterogeneity of the dynamics and to the breakdown of the Stokes-Einstein relation and we show that the coexistence of two dynamical phases occurs up to a timescale growing faster than the relaxation time on cooling, for some of the considered models. Our work offers a basis for rationalizing the dynamics of supercooled liquids and for relating their structural and dynamical properties.
Journal Article
Entropy-controlled cross-linking in linker-mediated vitrimers
Recently developed linker-mediated vitrimers based on metathesis of dioxaborolanes with various commercially available polymers have shown both good processability and outstanding performance, such as mechanical, thermal, and chemical resistance, suggesting new ways of processing cross-linked polymers in industry, of which the design principle remains unknown [M. Rottger et al., Science 356, 62–65 (2017)]. Here we formulate a theoretical framework to elucidate the phase behavior of the linker-mediated vitrimers, in which entropy plays a governing role. We find that, with increasing the linker concentration, vitrimers undergo a reentrant gel–sol transition, which explains a recent experiment [S. Wu, H. Yang, S. Huang, Q. Chen, Macromolecules 53, 1180–1190 (2020)]. More intriguingly, at the low temperature limit, the linker concentration still determines the cross-linking degree of the vitrimers, which originates from the competition between the conformational entropy of polymers and the translational entropy of linkers. Our theoretical predictions agree quantitatively with computer simulations, and offer guidelines in understanding and controlling the properties of this newly developed vitrimer system.
Journal Article
Effective antibodies immobilization and functionalized nanoparticles in a quartz-crystal microbalance-based immunosensor for the detection of parathion
Biosensor-based detection provides a rapid and low-cost alternative to conventional analytical methods for revealing the presence of the contaminants in water as well as solid matrices. Although important to be detected, small analytes (few hundreds of Daltons) are an issue in biosensing since the signal they induce in the transducer, and specifically in a Quartz-Crystal Microbalance, is undetectable. A pesticide like parathion (M = 292 Da) is a typical example of contaminant for which a signal amplification procedure is desirable.
The ballasting of the analyte by gold nanoparticles has been already applied to heavy target as proteins or bacteria to improve the limit of detection. In this paper, we extend the application of such a method to small analytes by showing that once the working surface of a Quartz-Crystal Microbalance (QCM) has been properly functionalized, a limit of detection lower than 1 ppb is reached for parathion. The effective surface functionalization is achieved by immobilizing antibodies upright oriented on the QCM gold surface by a simple photochemical technique (Photonic Immobilization Technique, PIT) based on the UV irradiation of the antibodies, whereas a simple protocol provided by the manufacturer is applied to functionalize the gold nanoparticles. Thus, in a non-competitive approach, the small analyte is made detectable by weighing it down through a \"sandwich protocol\" with a second antibody tethered to heavy gold nanoparticles. The immunosensor has been proved to be effective against the parathion while showing no cross reaction when a mixture of compounds very similar to parathion is analyzed.
The immunosensor described in this paper can be easily applied to any small molecule for which polyclonal antibodies are available since both the functionalization procedure of the QCM probe surface and gold nanoparticle can be applied to any IgG, thereby making our device of general application in terms of target analyte.
Journal Article
Hidden-state modeling of a cross-section of geoelectric time series data can provide reliable intermediate-term probabilistic earthquake forecasting in Taiwan
Geoelectric time series (TS) have long been studied for their potential for probabilistic earthquake forecasting, and a recent model (GEMSTIP) directly used the skewness and kurtosis of geoelectric TS to provide times of increased probability (TIPs) for earthquakes for several months in the future. We followed up on this work by applying the hidden Markov model (HMM) to the correlation, variance, skewness, and kurtosis TSs to identify two hidden states (HSs) with different distributions of these statistical indexes. More importantly, we tested whether these HSs could separate time periods into times of higher/lower earthquake probabilities. Using 0.5 Hz geoelectric TS data from 20 stations across Taiwan over 7 years, we first computed the statistical index TSs and then applied the Baum–Welch algorithm with multiple random initializations to obtain a well-converged HMM and its HS TS for each station. We then divided the map of Taiwan into a 16-by-16 grid map and quantified the forecasting skill, i.e., how well the HS TS could separate times of higher/lower earthquake probabilities in each cell in terms of a discrimination power measure that we defined. Next, we compare the discrimination power of empirical HS TSs against those of 400 simulated HS TSs and then organized the statistical significance values from this cellular-level hypothesis testing of the forecasting skill obtained into grid maps of discrimination reliability. Having found such significance values to be high for many grid cells for all stations, we proceeded with a statistical hypothesis test of the forecasting skill at the global level to find high statistical significance across large parts of the hyperparameter spaces of most stations. We therefore concluded that geoelectric TSs indeed contain earthquake-related information and the HMM approach is capable of extracting this information for earthquake forecasting.
Journal Article
Escape rate and diffusion of a Stochastically Driven particle
The dynamical properties of a tracer repeatedly colliding with heat bath particles can be described within a Langevin framework provided that the tracer is more massive than the bath particles, and that the collisions are frequent. Here we consider the escape of a particle from a potential well, and the diffusion coefficient in a periodic potential, without making these assumptions. We have thus investigated the dynamical properties of a Stochastically Driven particle that moves under the influence of the confining potential in between successive collisions with the heat bath. In the overdamped limit, both the escape rate and the diffusion coefficient coincide with those of a Langevin particle. Conversely, in the underdamped limit the two dynamics have a different temperature dependence. In particular, at low temperature the Stochastically Driven particle has a smaller escape rate, but a larger diffusion coefficient.
Journal Article
Relaxation functions and dynamical heterogeneities in a model of chemical gel interfering with glass transition
We investigate the heterogeneous dynamics in a model, where chemical gelation and glass transition interplay, focusing on the dynamical susceptibility. Two independent mechanisms give raise to the correlations, which are manifested in the dynamical susceptibility: one is related to the presence of permanent clusters, while the other is due to the increase of particle crowding as the glass transition is approached. The superposition of these two mechanisms originates a variety of different behaviours. We show that these two mechanisms can be unentangled considering the wave vector dependence of the dynamical susceptibility.
Journal Article
Nonaffinity in amorphous solids close to the jamming transition
Nonaffinity is known to be an integral part of the response of amorphous solids. Its role is particularly relevant in particulate systems close to their jamming transition, where it dominates the elastic response. Thus, to determine the elastic properties of amorphous solids it is essential to rationalize the features of their nonaffine response. Via numerical simulations we investigate the relation between the non affine response and the vibrational properties of model amorphous materials. We show that, contrary to previous speculations, modes below the Boson peak are those mostly responsible for the nonaffine response.
Journal Article