Nonlinear Response Properties Research Articles

An Antiferromagnetic Neuromorphic Memory Based on Perpendicularly Magnetized CoO.

Antiferromagnets (AFMs) are ideal materials to boost neuromorphic computing toward the ultrahigh speed and ultracompact integration regime. However, developing a suitable AFM neuromorphic memory remains an aspirational but challenging goal. In this work, we construct such a memory based on the CoO/Pt heterostructure, in which the collinear insulating AFM CoO shows a strong perpendicular anisotropy facilitating its electrical readout and writing. Utilizing the unique nonlinear response and bipolar fading memory properties of the device, we demonstrate a multidimensional reservoir computing beyond the traditional binary paradigm. These results are expected to pave the way toward next-generation fast and massive neuromorphic computing.

Rational design and investigation of nonlinear optical response properties of pyrrolopyrrole aza-BODIPY-based novel push-pull chromophores.

Intramolecular charge transfer (ICT)-based chromophores are highly sought after for designing near-infrared (NIR) absorbing and emitting dyes as well as for designing materials for nonlinear optical (NLO) applications. The properties of these 'push-pull' molecules can easily be modified by varying the electronic donor (D) and acceptor (A) groups as well as the π-conjugation linker. This study presents a methodical approach and employs quantum chemical analysis to explore the relationship between the structural features, electro-optical properties, and the NLO characteristics of molecules with D-π-A framework. The one- and two-photon absorption (2PA), linear polarizability (α), and first hyperpolarizability (β) of some novel chromophores, consisting of a dimeric aza-Boron Dipyrromethene (aza-BODIPY) analogue, called, pyrrolopyrrole aza-BODIPY (PPAB), serving as the acceptor, have been investigated. The electronic donors used in this study are triphenylamine (TPA) and diphenylamine (DPA), and they are conjugated to the acceptor via thienyl or phenylene π-linkers. Additionally, the Hyper-Rayleigh Scattering (βHRS), which enables direct estimation of the second-order NLO properties, is calculated for the studied chromophores with 1064 nm excitation in acetonitrile. The β value shows a significant increase with increasing solvent polarity, indicating that the ICT plays a crucial role in shaping the NLO response of the studied molecules. The enhancement of the 2PA cross-section of the investigated molecules can also be achieved by modulating the combinations of donors and linkers. The results of our study indicate that the novel D-π-A molecules designed in this work demonstrate considerably higher hyperpolarizability values than the standard p-nitroaniline, making them promising candidates for future NLO applications.

Tailoring the donor moieties in TPA‐based organic dyes for efficient photovoltaic, optical and nonlinear optical response properties

AbstractThe current study reports tailoring the electronic donor structures of organic dyes to modify their optical and nonlinear optical (NLO) response properties. Five (5) tri‐phenyl amine (TPA) based Donor‐π‐Acceptor (D‐π‐A) organic dyes with the codes ICAA1, ICAA2, ICAA3, ICAA4, and ICAA5 were designed and investigated for their optical and NLO properties using quantum chemical methods. Optical and NLO properties of these dyes were studied by CAM‐B3LYP method and 6‐311G* basis set. The focus has been on the impact of adding secondary donors and shifting their substitutions at ortho (o), meta (m) and para (p) positions. Among all designed compounds, ICAA4 showed the highest amplitude of average third‐order NLO polarizability <γ>, which is calculated to be 1316 × 10−36 esu. Time‐dependent Density Functional Theory (TD‐DFT) method was used to determine how a change in the position of the donor affected the excitation energy (Eg) and NLO response properties. The findings showed that changing the position of the secondary donor results in a red shift among absorption spectra as well as the increase in their NLO responses. Complete process of intramolecular charge transfer (ICT) has been investigated in terms of different optical parameters such as frontier molecular orbitals (FMOs), molecular electrostatic potentials (MEPs), transition density matrix (TDMs), density of states (DOS), electron density difference (EDD), and natural bond orbital (NBO) analysis. Our calculations for study of ICT process indicate that p‐position of methoxy group performs better among all other positions and even it has better NLO response properties than the compound with three collective methoxy groups. The calculated Voc values of all designed molecules range from 1.09 to 1.30, all of them are positive while their ΔGinject is found to be in the range of −0.87 to −1.79 eV indicating their decent potential for photovoltaic applications. The studied optical, NLO and photovoltaic parameters illustrated that ICAA1 to ICAA5 are appropriate molecules not only for NLO applications but also for efficient photovoltaic purposes.

Mechanical Characterization of the Male Lower Urinary Tract: Comparison among Soft Tissues from the Same Human Case Study

Background: Nowadays, a challenging task concerns the biomechanical study of the human lower urinary tract (LUT) due to the variety of its tissues and the low availability of samples. Methods: This work attempted to further extend the knowledge through a comprehensive mechanical characterization of the male LUT by considering numerous tissues harvested from the same cadaver, including some never studied before. Samples of the bladder, urethra, prostate, Buck’s fascia and tunica albuginea related to corpora cavernosa were considered and distinguished according to testing direction, specimen conformation and anatomical region. Uniaxial tensile and indentation tests were performed and ad hoc protocols were developed. Results: The tissues showed a non-linear and viscoelastic response but different mechanical properties due to their specific functionality and microstructural configuration. Tunica albuginea longitudinally displayed the highest stiffness (12.77 MPa), while the prostate transversally had the lowest one (0.66 MPa). The minimum stress relaxation degree (65.74%) was reached by the tunica albuginea and the maximum (88.55%) by the bladder. The prostate elastic modulus was shown to vary according to the presence of pathological changes at the microstructure. Conclusions: This is the first experimental work that considers the mechanical evaluation of the LUT tissues in relation to the same subject, setting the basis for future developments by expanding the sample population and for the development of effective in silico models to improve the solutions for most LUT pathologies.

Molecular level interaction, electrons excitation properties, solvent effect using IEFPCM investigation, topological surface, and docking analysis of 4-pyrrolidin-2-yl-pyridine

Abstract Optimisation of molecular geometry of the headline compound, 4-pyrrolidin-2-yl-pyridine (4P2YLP) was achieved theoretically exercising Density Functional Theory using B3LYP standard approach utilising basis set, 6-311++G(d,p). Using Gaussian 09, HOMO–LUMO analysis was achieved to comprehend the chemical activity and electronic properties of the heading compound. The least HOMO–LUMO gap was obtained for gas phase (5.6486). Bonding interlinkage of the fragments is accomplished by Natural Bonding Orbitals (NBO), as steadiness and chemical reactivity depend on the border molecular orbitals. The nucleophilic & electrophilic spots along with 3D charge transmission areas are determined using the Molecular Electrostatic Potential (MEP). Multiwfn 3.8 software with Pauli Repulsion (PR) & electron localization has been used to conduct ELF and LOL research. While LOL simply displays the most closely spaced orbitals overlapping, ELF displays the electron pair density. Non-linear response properties are analysed in a variety of solvents. The dipole moment (1.9039), polarizability (3.23017E-23 esu) & first order hyperpolarizability (1.51981E-30 esu) of water are the highest values among the selected solvents. Different solvents endured UV–Vis analysis employing TD-DFT technique and the absorption of maximum wavelength is accomplished. Fructose 5-dehydrogenase inhibitor activity by docking is investigated using molecular modelling procedures.

Enzymatic cleaving of entangled DNA rings drives scale-dependent rheological trajectories.

DNA, which naturally occurs in linear, ring, and supercoiled topologies, frequently undergoes enzyme-driven topological conversion and fragmentation in vivo, enabling it to perform a variety of functions within the cell. In vitro, highly concentrated DNA polymers form entanglements that yield viscoelastic properties dependent on the topologies and lengths of the DNA. Enzyme-driven alterations of DNA size and shape therefore offer a means of designing active materials with programmable viscoelastic properties. Here, we incorporate multi-site restriction endonucleases into dense DNA solutions to linearize and fragment circular DNA molecules. We pair optical tweezers microrheology with differential dynamic microscopy and single-molecule tracking to measure the linear and nonlinear viscoelastic response and transport properties of entangled DNA solutions over a wide range of spatiotemporal scales throughout the course of enzymatic digestion. We show that, at short timescales, relative to the relaxation timescales of the polymers, digestion of these 'topologically-active' fluids initially causes an increase in elasticity and relaxation times followed by a gradual decrease. Conversely, for long timescales, linear viscoelastic moduli exhibit signatures of increasing elasticity. DNA diffusion, likewise, becomes increasingly slowed, in direct opposition to the short-time behavior. We hypothesize that this scale-dependent rheology arises from the population of small DNA fragments, which increases as digestion proceeds, driving self-association of larger fragments via depletion interactions, giving rise to slow relaxation modes of clusters of entangled chains, interspersed among shorter unentangled fragments. While these slow modes likely dominate at long times, they are presumably frozen out in the short-time limit, which instead probes the faster relaxation modes of the unentangled population.

Quantum covariant derivative: a tool for deriving adiabatic perturbation theory to all orders

The covariant derivative suitable for differentiating and parallel transporting tangent vectors and other geometric objects induced by a parameter-dependent adiabatic quantum eigenstate is introduced. It is proved to be covariant under gauge and coordinate transformations and compatible with the quantum geometric tensor. For a quantum system driven by a Hamiltonian depending on slowly-varying parameters , , the quantum covariant derivative is used to derive a recurrence relation that determines an asymptotic series for the wave function to all orders in . This adiabatic perturbation theory provides an efficient tool for calculating nonlinear response properties.

Density Functional Theory Study of the Secondorder Nonlinear Optical Properties of Novel Fluorenone Derivatives

Based on the molecular structure of novel fluorenone derivative named FO52, a series of new molecules have been designed by extending its π-conjugated bridge and introducing electron donor or acceptor substituents. The electronic transition and second-order non-linear optical response properties of these fluorenone derivatives were theoretically studied in detail by using the density functional theory computational methods. The results showed that the non-linear optical response of the molecule FO52 can be improved by introducing five-membered heterocycles into its skeleton structure. In addition, the introduction of strong substituents results in significant enhancement of the first hyperpolarizability of molecular nonlinear optical properties. These fluorenone derivatives could be treated as excellent candidates for nonlinear optical materials due to the narrow energy gap of its frontier molecular orbitals, distinct intramolecular charge transfer character and large first hyperpolarizabilities

Nonlinear analysis of vibration attenuation of ring-spring-resonator based meta-isolation system

Ring-spring-resonator (RSR) based nonlinear meta-isolation system (RSR-M) was proposed and its vibration attenuation characteristic was investigated experimentally and theoretically. The force–displacement hysteresis loops of the selected wire rope isolators (WRIs) exhibit softening under compression and hardening under extension, and are identified by a modified mathematical model combined with the normalized Bouc-Wen model. Frequency response curves of conventional isolation system and RSR-M−2 were calculated based on the single-degree-of-freedom (SDOF) and two-degree-of-freedom (TDOF) models, along with the fourth-order Runge-Kutta method. Shaking table experiments were carried out to evaluate the nonlinear dynamic response and vibration attenuation property of the RSR-M, which proves to be in good agreement with the numerical results of acceptable validity. Dynamic hysteresis loops and phase portraits were plotted to study the dynamic responses and stability of the RSR-M. The experimental results show that, no matter vertical or horizontal direction, the RSR-M possesses better vibration attenuation performance compared to conventional isolation system. In general, the meta-isolation vibration system provides a new reference and idea for the practice designing of the isolation system in some sense.

Two-photon absorption in imidazo[1,2-a]pyridine derivatives: Study of nonlinear optical response and dipolar properties

Imidazo[1,2-a]pyridine derivatives are versatile molecules with excellent emissive properties, making them interesting for various applications, from fluorescent probes to organic light-emitting diodes (OLEDs). Furthermore, such molecules enable the incorporation of different peripheral groups during the synthesis, which can improve the desired optical properties. However, there is a lack of studies that report this compounds class linear and nonlinear optical characteristics. Here, spectroscopic measurements were performed on seven imidazo[1,2-a]pyridine derivatives with different peripheral groups, to understand their influence on the two-photon absorption (2PA) cross-section. Results showed that the effective increase molecular conjugation, provided by the naphthalene substituent, leads to an increase of approximately seven times in the 2PA cross-section. Furthermore, it was shown that the same result is obtained when groups with a strong electron withdrawing or donating character are linked to the imidazo[1,2-a]pyridine core. Such results indicate a possible route to obtaining considerable nonlinear optical responses in this organic compounds class.

The prefrontal cortex of the Mexican free-tailed bat is more selective to communication calls than primary auditory cortex.

In this study, we examined the auditory responses of a prefrontal area, the frontal auditory field (FAF), of an echolocating bat (Tadarida brasiliensis) and presented a comparative analysis of the neuronal response properties between the FAF and the primary auditory cortex (A1). We compared single-unit responses from the A1 and the FAF elicited by pure tones, downward frequency-modulated sweeps (dFMs), and species-specific vocalizations. Unlike the A1, FAFs were not frequency tuned. However, progressive increases in dFM sweep rate elicited a systematic increase of response precision, a phenomenon that does not take place in the A1. Call selectivity was higher in the FAF versus A1. We calculated the neuronal spectrotemporal receptive fields (STRFs) and spike-triggered averages (STAs) to predict responses to the communication calls and provide an explanation for the differences in call selectivity between the FAF and A1. In the A1, we found a high correlation between predicted and evoked responses. However, we did not generate reasonable STRFs in the FAF, and the prediction based on the STAs showed lower correlation coefficient than that of the A1. This suggests nonlinear response properties in the FAF that are stronger than the linear response properties in the A1. Stimulating with a call sequence increased call selectivity in the A1, but it remained unchanged in the FAF. These data are consistent with a role for the FAF in assessing distinctive acoustic features downstream of A1, similar to the role proposed for primate ventrolateral prefrontal cortex.NEW & NOTEWORTHY In this study, we examined the neuronal responses of a frontal cortical area in an echolocating bat to behaviorally relevant acoustic stimuli and compared them with those in the primary auditory cortex (A1). In contrast to the A1, neurons in the bat frontal auditory field are not frequency tuned but showed a higher selectivity for social signals such as communication calls. The results presented here indicate that the frontal auditory field may represent an additional processing center for behaviorally relevant sounds.

Extended Anderson Criticality in Heavy-Tailed Neural Networks.

We investigate the emergence of complex dynamics in networks with heavy-tailed connectivity by developing a non-Hermitian random matrix theory. We uncover the existence of an extended critical regime of spatially multifractal fluctuations between the quiescent and active phases. This multifractal critical phase combines features of localization and delocalization and differs from the edge of chaos in classical networks by the appearance of universal hallmarks of Anderson criticality over an extended region in phase space. We show that the rich nonlinear response properties of the extended critical regime can account for a variety of neural dynamics such as the diversity of timescales, providing a computational advantage for persistent classification in a reservoir setting.

Semiconductor characteristics of tellurium and its implementations

Abstract Tellurium (Te) gained worldwide attention because of its excellent properties, distinctive chained structures, and potential usages. Bulk Te is a p-type elemental helical semiconductor at room temperature and it also having a very limited band gap. Te presents fascinating characteristics such as nonlinear optical response, photoconductivity, good thermoelectric and piezoelectric properties. These charming characteristics induce Te a possible nominee for applications in field-effect transistors, IR acousto-optic deflectors, solar cells, self-developing holographic recording devices, photoconductors, gas sensors, radiative cooling devices, and topological insulators. The developments in these areas are incorporated in great detail. This study opens up the possibility of designing novel devices and considering modern applications of Tellurium.

Nonlinear dynamic thermometry: Temperature measurement using immobilized magnetic nanoparticles

We present a new method for measuring the temperature of magnetic nanoparticles that can also be adapted to immobilized particles. The Néel relaxation mechanism, which dominates the dynamic magnetization process of immobilized magnetic nanoparticles, can be used as an intermediate parameter in a sensing model to obtain temperature information. In this paper, we use the nonlinear response properties of magnetic nanoparticles to derive an analytical expression for the relationship between the phase of cubic susceptibility and temperature. We also consider dipole–dipole interactions and the dependence on field amplitude. Under experimental conditions at selected frequencies and field amplitudes, we compare temperature measurements of magnetic nanoparticles obtained with the proposed thermometry model with those obtained from existing nonlinear dielectric relaxation models. The results show that the temperature measurements obtained from the proposed model are closer to the reference temperatures in the temperature range of 308–353 K, with a standard deviation of less than 0.1 K in the temperature measurement. This new method successfully applies the nonlinear properties of magnetic nanoparticles to high-precision dynamic temperature measurements. It extends the applicability range of temperature measurement methods to conditions with strong interactions or large ac field amplitudes. This new method is expected to be applicable in anti-magnetic environments, for example, in biochemical temperature measurements of magnetically labeled cells in vivo.

A fermion phenomenology of low-temperature strongly-noncrystalline solids

Insisting on the relevance of spin-statistics theorem, I propose that anomalous low-energy excitations (LEEs) of strongly-noncrystalline solids (SNSs), observed at low temperatures T<1K, are fermions, which are localized and weakly interacting. This phenomenological theory rationalizes all low-energy quantum many-body states of SNSs as Goldstone bosons-phonons and half-integer-spin fermions. Fermi glass of LEEs, rather than statistical ensemble of isolated two-level systems, appears to be a consistent theory of various thermal and nonlinear response properties of SNSs. A robust consequence of the theory is nearly constant-in-energy density of fermion states near Fermi energy, which in turn implies linear-in-temperature specific heat and dimensionless frequency-independent sound absorption. Consistent parameters of Fermi glass are estimated from theoretical scaling arguments as well as directly from experimental data.

Exploring the quinoidal oligothiophenes to their robust limit for efficient linear and nonlinear optical response properties

Exploring the quinoidal oligothiophenes to their robust limit for efficient linear and nonlinear optical response properties

Insighting the functionally modified C60 fullerenes as an efficient nonlinear optical materials: A quantum chemical study

It is well-known that π-conjugation plays an important role to tune the nonlinear optical (NLO) response of donor-π-conjugated-acceptor compounds. Fullerenes (C60) are one of a few compounds who are abounded with π-conjugation and perhaps are the largest π-conjugation compounds. In the present study, we systematically designed C60 derivatives (2 (fulleropyrrolidine) and 2a-2c (fulleropyrrolidine tetrathiafulvalene derivatives where 2a, 2b and 2c are with n = 0, n = 1 and n = 2) through the use of pyrrolidine and tetrathiafulvalene moieties. We applied density functional theory (DFT) methods to calculate their respective geometrical structures, electronic properties, linear and nonlinear optical response properties along with their respective UV–Visible spectra using CAM-B3LYP functional and 6-31G* basis set. The isotropic polarizability (αiso) and anisotropic polarizability (αaniso) of 2c was found to be 131.52 × 10-24 and 47.01 × 10-24 esu, respectively. Amongst our designed compounds, the maximum second-order nonlinear optical polarizability amplitude (β//) of 2c was found to be 15.69 × 10-30 esu. Interestingly, 2c shows the highest third-order nonlinear polarizability amplitude <γ> of 284.29 × 10-36 esu that is about three times higher than parent compound 1. Additionally, frontier molecular orbitals (FMOs), molecular electrostatic potential maps (MEPs), transition density matrix (TDM) analysis indicate more effective charge redistribution from donor moiety to acceptor fragments. The density of states (DOS) diagrams reveal distinct electronic contributions of various fragments in the formation of HOMO and LUMO orbitals resulting in efficient intramolecular charge transfer (ICT) and robust third-order NLO response properties of functionalized fullerene derivatives. The current study may arouse the attention of the scientific society to utilize the extensive π-conjugation of functionalized fullerenes for designing efficient NLO materials.

Ultrafast Broadband Nonlinear Optical Response in Co-Doped Sb2Se3 Nanofilms at Near-Infrared

Transition metal-doped Sb2Se3 has become a heated topic caused by the strong nonlinear optical response and the ultrafast response time at high laser excitation. In this paper, the Co-doped Sb2Se3 with different doping amount (0.5, 1.0, and 1.5 W) nanofilms were prepared by magnetron sputtering technology, and the nonlinear behavior of Co-doped Sb2Se3 nanofilms at near infrared were systematically studied. The results of the femtosecond Z-Scan experiment indicate that the Co-doped Sb2Se3 nanofilms exhibit broadband nonlinear response properties owing to the free carrier absorption, the Kerr refraction, the two-photon absorption, and the free carrier refraction. The nonlinear absorption coefficients of Co-doped Sb2Se3 nanofilms are from 3.0 × 10−9 to 2.03 × 10−8 m/ W under excitation at 800, 980, and 1,030 nm, and the nonlinear refractive index of the Co-doped Sb2Se3 nanofilms is from 4.0 × 10−16 to -3.89 × 10−15 m2/ W at 800, 980, and 1,030 nm. More importantly, Co-doped Sb2Se3 (1.5 W) nanofilm exhibits ultrafast carrier absorption (&amp;lt;1 ps) and a stronger transient absorption intensity of ΔOD &amp;gt; 6.3. The Co-doping content can controllably tune the crystalline degree, the ultrafast carrier absorption, the intensity of the reverse saturation absorption, the broadband nonlinear optical response, and the carrier relaxation time of Co-doped Sb2Se3 nanofilms. These results are sufficient to support their applications in broadband nonlinear photonic devices.

Learning divisive normalization in primary visual cortex.

Divisive normalization (DN) is a prominent computational building block in the brain that has been proposed as a canonical cortical operation. Numerous experimental studies have verified its importance for capturing nonlinear neural response properties to simple, artificial stimuli, and computational studies suggest that DN is also an important component for processing natural stimuli. However, we lack quantitative models of DN that are directly informed by measurements of spiking responses in the brain and applicable to arbitrary stimuli. Here, we propose a DN model that is applicable to arbitrary input images. We test its ability to predict how neurons in macaque primary visual cortex (V1) respond to natural images, with a focus on nonlinear response properties within the classical receptive field. Our model consists of one layer of subunits followed by learned orientation-specific DN. It outperforms linear-nonlinear and wavelet-based feature representations and makes a significant step towards the performance of state-of-the-art convolutional neural network (CNN) models. Unlike deep CNNs, our compact DN model offers a direct interpretation of the nature of normalization. By inspecting the learned normalization pool of our model, we gained insights into a long-standing question about the tuning properties of DN that update the current textbook description: we found that within the receptive field oriented features were normalized preferentially by features with similar orientation rather than non-specifically as currently assumed.

Symmetry properties of nonlinear hydrodynamic interactions between responsive particles.

Two identical particles driven by the same steady force through a viscous fluid may move relative to one another due to hydrodynamic interactions. The presence or absence of this relative translation has a profound effect on the dynamics of a driven suspension consisting of many particles. We consider a pair of particles which, to linear order in the force, do not interact hydrodynamically. If the system possesses an intrinsic property (such as the shape of the particles, their position with respect to a boundary, or the shape of the boundary) which is affected by the external forcing, hydrodynamic interactions that depend nonlinearly on the force may emerge. We study the general properties of such nonlinear response. Analysis of the symmetries under particle exchange and under force reversal leads to general conclusions concerning the appearance of relative translation and the motion's time reversibility. We demonstrate the applicability of the conclusions in three specific examples: (a) two spheres driven parallel to a wall; (b) two deformable objects driven parallel to their connecting line; and (c) two spheres driven along a curved path. The breaking of time reversibility suggests a possible use of nonlinear hydrodynamic interactions to disperse or assemble particles by an alternating force.