Atomic Correlation Research Articles

Stochastic electrodynamics simulations for collective atom response in optical cavities

We study the collective optical response of an atomic ensemble confined within a single-mode optical cavity by stochastic electrodynamics simulations that include the effects of atomic position correlations, internal level structure, and spatial variations in cavity coupling strength and atom density. In the limit of low light intensity the simulations exactly reproduce the full quantum field-theoretical description for cold stationary atoms and at higher light intensities we introduce semiclassical approximations to atomic saturation that we compare with the exact solution in the case of two atoms. We find that collective subradiant modes of the atoms, with very narrow linewidths, can be coupled to the cavity field by spatial variation of the atomic transition frequency and resolved at low intensities, and show that they can be specifically driven by tailored transverse pumping beams. We show that the cavity optical response, in particular both the subradiant mode profile and the resonance shift of the cavity mode, can be used as a diagnostic tool for the position correlations of the atoms and hence the atomic quantum many-body phase. The quantum effects are found to be most prominent close to the narrow subradiant mode resonances at high light intensities. Although an optical cavity can generally strongly enhance quantum fluctuations via light confinement, we show that the semiclassical approximation to the stochastic electrodynamics model provides at least a qualitative agreement with the exact optical response outside the subradiant mode resonances even in the presence of significant saturation of the atoms.

First principles computational study on hydrolysis of hazardous chemicals phosphorus trichloride and oxychloride (PCl3 and POCl3) catalyzed by molecular water clusters

Using first principles calculations we unveil fundamental mechanism of hydrolysis reactions of two hazardous chemicals PCl3 and POCl3 with explicit molecular water clusters nearby. It is found that the water molecules play a key role as a catalyst significantly lowing activation barrier of the hydrolysis via transferring its protons to reaction intermediates. Interestingly, torsional angle of the molecular complex at transition state is identified as a vital descriptor on the reaction rate. Analysis of charge distribution over the complex further reinforces the finding with atomic level correlation between the torsional angle and variation of the orbital hybridization state of phosphorus (P) in the complex. Electronic charge separation (or polarization) enhances thermodynamic stability of the activated complex and reduces the activation energy through hydrogen bonding network with water molecules nearby. Calculated potential energy surfaces (PES) for the hydrolysis of PCl3 and POCl3 depict their two contrastingly different profiles of double- and triple-depth wells, respectively. It is ascribed to the unique double-bonding O=P in the POCl3. Our results on the activation free energy show well agreements with previous experimental data within 7kcalmol−1 deviation.

Signature of microscale kinetics in mesoscale description of epitaxial growth.

We describe the effect of kinetic interactions of adsorbed atoms in a mesoscale model of epitaxial growth without elasticity. Our goal is to understand how atomic correlations due to kinetics leave their signature in mechanisms governing the motion of crystal line defects (steps) at the nanoscale. We focus on the key atomistic processes related to external material deposition, desorption, and asymmetric energy barriers on a stepped surface. By starting with a kinetic, restricted solid-on-solid model in 1+1 dimensions, we derive laws that govern the motion of a single step when deposition is nearly balanced out by desorption. These mesoscale laws reveal how kinetic processes, e.g., bond breaking at the step edge, influence step motion via the correlated motion of atoms.

Coopetition and manipulation of quantum correlations in Rydberg atoms

We study the steady-state quantum correlations arising from the atom–field and interatomic interplays in two-level Rydberg atoms coherently driven by an external laser field. Three kinds of quantum correlations, i.e., atom–atom correlation, atom–field entanglement and photon–photon correlation, are simultaneously examined by considering dipole–dipole interactions (DDI) for pairwise Rydberg atoms. They are shown to be closely linked with single and double Rydberg excitations, which can be modulated to work in the blockade or antiblockade regime depending on the driving field frequency, the DDI strength and the Rydberg decay rate. As a result, we obtain strongly correlated atoms and highly antibunching photons (indispensable resources in applications of quantum information processing) intermediated with robust atom–field entanglement.

Observation of dynamic atom-atom correlation in liquid helium in real space

Liquid 4He becomes superfluid and flows without resistance below temperature 2.17 K. Superfluidity has been a subject of intense studies and notable advances were made in elucidating the phenomenon by experiment and theory. Nevertheless, details of the microscopic state, including dynamic atom–atom correlations in the superfluid state, are not fully understood. Here using a technique of neutron dynamic pair-density function (DPDF) analysis we show that 4He atoms in the Bose–Einstein condensate have environment significantly different from uncondensed atoms, with the interatomic distance larger than the average by about 10%, whereas the average structure changes little through the superfluid transition. DPDF peak not seen in the snap-shot pair-density function is found at 2.3 Å, and is interpreted in terms of atomic tunnelling. The real space picture of dynamic atom–atom correlations presented here reveal characteristics of atomic dynamics not recognized so far, compelling yet another look at the phenomenon.

The kinetic fragility of Pt-P- and Ni-P-based bulk glass-forming liquids and its thermodynamic and structural signature

The thermodynamic and kinetic properties of Pt-P- and Ni-P-based bulk glass-forming liquids are investigated using differential scanning calorimetry and three-point beam bending. The kinetic fragility of the alloys is determined by measuring relaxation times and equilibrium viscosities. In the Pt-P-based alloy family a Pt-rich alloy is one of the most fragile bulk glass-forming liquids in the vicinity of the glass transition reported so far. The fragility parameter D∗ increases significantly with decreasing Pt-content, which is due to a more pronounced loss of excess entropy upon undercooling for the fragile liquids. Relying on previous observations made for Pd-P-based alloys, it is argued that a bifurcation of the P environment into Pt-Ni-P and Pt-Cu-P structural units stabilizes the deeply undercooled liquid due to formation of medium range order (MRO). This is supported by synchrotron X-ray scattering experiments, which reveal the formation of a pre-peak in the total structure factor with increasing fragility. Adapting a previously reported empirical correlation, we show that the more fragile liquid alloys are characterized by a more pronounced dilatation of atomic pair correlations on the length scale of 1 nm, corroborating the idea that the observed fragility behavior of Pt-P-based bulk glass-forming liquids is inherently related to structural changes on the length scale of MRO.

Role of the local structure in superconductivity of LaO0.5F0.5BiS2−xSex system

We have studied the local structure of LaO0.5F0.5BiS2−xSex by Bi L1-edge extended x-ray absorption fine structure (EXAFS). We find a significant effect of Se substitution on the local atomic correlations with a gradual elongation of average in-plane Bi-S bondlength. The associated mean square relative displacement, measuring average local distortions in the BiS2 plane, hardly shows any change for small Se substitution, but decreases significantly for . The Se substitution appears to suppress the local distortions within the BiS2 plane that may optimize in-plane orbital hybridization and hence the superconductivity. The results suggest that the local structure of the BiS2-layer is one of the key ingredients to control the physical properties of the BiS2-based dichalcogenides.

Structural evolution on medium-range-order during the fragile-strong transition in Ge15Te85

Using synchrotron X-ray scattering, we investigate liquid Ge15Te85 spanning a wide temperature range from near Tg to the melt, and demonstrate that the density anomaly and fragile-strong transition are not only related to short-range-order (SRO) structural change (e.g. Peierls-like distortion), but also accompanied by a remarkable development of medium-range-order (MRO). The latter manifests as an emerging pre-peak in total structure factor S(Q) and atomic pair correlations on the length scale of ∼8 Å in the real space G(r) function. The results highlight the role of medium-range structural ordering in the evolution of the configurational entropy which, according to the Adam-Gibbs theory, can be linked to the fragile-strong transition (FS-transition). Based on the relation between structure and liquid dynamics, the FS-transitions at high pressures are examined in terms of experimental data and the Ehrenfest relation. This work identifies the length scale for the atomic correlations in MRO structural evolutions and presents a structural approach to exploring liquid dynamics, which may be useful for investigating relevant phase-change alloys.

Development of Glass Matrix for Radioactive Waste Conditioning

Understanding of the incorporation of actinides in borosilicate matrix used for nuclear waste storage is of a great importance for radioactive waste immobilization. This study carried out on matrix glasses doped respectively with 30wt% UO3 and CeO2, Nd2O3 used for chemical modelling of the actinides. Neutron and X-ray diffraction measurements and Reverse Monte Carlo (RMC) simulations were performed. For several glasses, it was found that the basic network structure consists of tetrahedral SiO4 units and of mixed trigonal BO3 and tetrahedral BO4. The BO3 and BO4 units are linked to SiO4, forming mixed [4]Si-O-[3]B and [4]Si-O-[4]B bond-linkages. From significant second neighbour atomic pair correlations have been revealed that U, Ce, Nd accommodates in both silicate and borate site.

B2-disorder phase boundary calculations in Fe rich region of Fe-Si binary system with tetrahedron approximation of CVM

The phase boundary between B2 ordered and disordered phases in the Fe-rich region of the Fe-Si binary system is calculated by Cluster Variation Method (CVM). The configurational entropy is formulated within the tetrahedron approximation of CVM, and the internal energy is derived by Cluster Expansion Method (CEM) operated on a set of total energies calculated by DFT. The Debye Gruneisen model is employed to introduce the vibrational effect. The second order transition for the B2 order-disorder transition is confirmed, which is in agreement with the published phase diagram data and the results of previous CALPHAD calculations. The calculated transition temperature in the present study is higher around the stoichiometric composition and lower in the Fe-rich region compared to the experimental transition temperature. One reason for this overestimation and underestimation of the transition temperature may stem from the facts that the local atomic displacement and wide range atomic correlations are not considered in the present study. The transition temperature is also determined using Thermo-Calc software with the SSOL4 database. The transition temperature obtained by Thermo-Calc calculations accurately reproduces the experimental results. Hence, it is considered that the interaction parameters and the ordering parameters of CALPHAD free energy implicitly include the contributions of short range ordering and local atomic displacement.

Weak correlation dictionary construction method for sparse coding

For sparse coding, the weaker the correlation of dictionary atoms is, the better the representation capacity of dictionary will be. A weak correlation dictionary construction method for sparse coding has been proposed in this paper. Firstly, a new dictionary atom initialization is proposed in which data samples with weak correlation are selected as the initial dictionary atoms in order to effectively reduce the correlation among them. Then, in the process of dictionary learning, the correlation between atoms has been measured by correlation coefficient, and strong correlation atoms have been eliminated and replaced by weak correlation atoms in order to improve the representation capacity of the dictionary. An image classification scheme has been achieved by applying the weak correlation dictionary construction method proposed in this paper. Experimental results show that, the proposed method averagely improves image classification accuracy by more than 2%, compared to sparse coding spatial pyramid matching (ScSPM) and other existing methods for image classification on the datasets of Caltech-101, Scene-15, etc.

Linear entropy and squeezing of the interaction between two quantum system described by su (1, 1) and su(2) Lie group in presence of two external terms

A Hamiltonian, that describes the interaction between a two-level atom (su(2) algebra) and a system governed by su(1,1) Lie algebra besides two external interaction, is considered. Two canonical transformations are used, which results into removing the external terms and changing the frequencies of the interacting systems. The solution of the equations of motion of the operators is obtained and used to discuss the atomic inversion, entanglement, squeezing and correlation functions of the present system. Initially the atom is considered to be in the excited state while the other systems is in the Perelomov coherent state. Effects of the variations in the coupling parameters to the external systems are considered. They are found to be sensitive to changing entanglement, variance and entropy squeezing.

Network structure of Mo-oxide glasses

The structure of molybdate glasses have been investigated by neutron and high-energy X-ray diffraction coupled with Reverse Monte Carlo (RMC) simulation technique. From the modelling the partial atomic correlation functions gij(r), the coordination number distributions CNij and bond angle distributions have been revealed. For binary 90MoO3-10Nd2O3 glass composition the fraction of MoO4/MoO6 was 0.55/0.25. Three type of ternary system have been studied, where the most important structural units was authenticated. For MoO3-Nd2O3-B2O3 sample mixed MoO4-BO4 and MoO4-BO3 linkages form pronounced intermediate-range order. In case of MoO3-ZnO-B2O3 series the BO3 and BO4 units are linked to MoO4 and/or ZnO4, forming mixed MoO4-BO4(BO3), MoO4-ZnO4 and ZnO4-BO4(BO3) bond-linkages.

Concurrent magnetic and structural reconstructions at the interface of (111)-oriented La0.7Sr0.3MnO3/LaFeO3

We observe an induced switchable magnetic moment of $1.6\ifmmode\pm\else\textpm\fi{}0.40\phantom{\rule{0.16em}{0ex}}{\ensuremath{\mu}}_{\mathrm{B}}/\mathrm{Fe}$ for the nominally antiferromagnetic $\mathrm{LaFe}{\mathrm{O}}_{3}$ extending two to four interface layers into the non--charge transfer system $\mathrm{L}{\mathrm{a}}_{0.7}\mathrm{S}{\mathrm{r}}_{0.3}\mathrm{Mn}{\mathrm{O}}_{3}\text{/}\mathrm{LaFe}{\mathrm{O}}_{3}\text{/}\mathrm{SrTi}{\mathrm{O}}_{3}(111)$. Simultaneously a mismatch of oxygen octahedra rotations at the interface implies an atomic reconstruction of reduced symmetry at the interface, reaching two to five layers into $\mathrm{LaFe}{\mathrm{O}}_{3}$. Density functional theory of a structure with atomic reconstruction and different correlation strength shows a ferrimagnetic state with a net Fe moment at the interface. Together these results suggest that engineered oxygen octahedra rotations, affecting the local symmetry, affect electron correlations and can be used to promote magnetic properties.

Two-dimensional interaction of spin chains in the Si(553)-Au nanowire system

Adsorption of Au on Si(553) results in the self-assembly of highly ordered step arrays of one-dimensional (1D) Au atomic wires along the step direction. Charge transfer from the terrace to the step edge causes every third Si atom at the step edge to exhibit a partially filled dangling bond hosting a single fully spin-polarized electron which forms in an ordered 1D spin chain along the step. The interstep correlation of this threefold periodicity in neighboring Si step edges and the geometry of the unit cell has been determined by means of high-resolution spot profile analysis low-energy electron diffraction, scanning tunneling microscopy, and density functional theory. While the twofold periodicity of the Au wires exhibits a weak interwire interaction, leading to streaks in the diffraction pattern, the correlation of the Si step edge atoms is by far a stronger interaction, resulting in clear spots. The corresponding unit cell spanned by threefold ordered step edge atoms can be described as a centered structure which is magnetically frustrated and may stabilize a (two-dimensional) quantum spin liquid.

Modeling Pair Distribution Functions of Rare-Earth Phosphate Glasses Using Principal Component Analysis.

The use of principal component analysis (PCA) to statistically infer features of local structure from experimental pair distribution function (PDF) data is assessed on a case study of rare-earth phosphate glasses (REPGs). Such glasses, codoped with two rare-earth ions (R and R') of different sizes and optical properties, are of interest to the laser industry. The determination of structure-property relationships in these materials is an important aspect of their technological development. Yet, realizing the local structure of codoped REPGs presents significant challenges relative to their singly doped counterparts; specifically, R and R' are difficult to distinguish in terms of establishing relative material compositions, identifying atomic pairwise correlation profiles in a PDF that are associated with each ion, and resolving peak overlap of such profiles in PDFs. This study demonstrates that PCA can be employed to help overcome these structural complications, by statistically inferring trends in PDFs that exist for a restricted set of experimental data on REPGs, and using these as training data to predict material compositions and PDF profiles in unknown codoped REPGs. The application of these PCA methods to resolve individual atomic pairwise correlations in t(r) signatures is also presented. The training methods developed for these structural predictions are prevalidated by testing their ability to reproduce known physical phenomena, such as the lanthanide contraction, on PDF signatures of the structurally simpler singly doped REPGs. The intrinsic limitations of applying PCA to analyze PDFs relative to the quality control of source data, data processing, and sample definition, are also considered. While this case study is limited to lanthanide-doped REPGs, this type of statistical inference may easily be extended to other inorganic solid-state materials and be exploited in large-scale data-mining efforts that probe many t(r) functions.

Correlation Between Local Structure and Boson Peak in Metallic Glasses

We made a systematic study of the boson peak for six different Zr-based metallic glasses and found a universal correlation between average local atomic structure and boson peak. It is found that the boson peak can be decomposed into six characteristic vibratory modes, i.e., Debye’s vibratory mode and five Einstein’s vibratory modes. By using the Ioffe–Regel condition over all studied Zr-based metallic glasses, we reveal that atomic pair correlation function exactly maps on the low-temperature dynamics and the origin of the boson peak, which is the sum of vibrations of local density fluctuation domains in the glasses. In addition, it is found that the Debye’s type oscillators are the major contributors to the low-temperature specific heat capacities. This study opens a new way of understanding the relationship of the physical properties with the atomic arrangements in glasses.

Biophysical approaches promote advances in the understanding of von Willebrand factor processing and function.

The large multimeric plasma glycoprotein von Willebrand factor (VWF) is essential for primary hemostasis by recruiting platelets to sites of vascular injury. VWF multimers respond to elevated hydrodynamic forces by elongation, thereby increasing their adhesiveness to platelets. Thus, the activation of VWF is force-induced, as is its inactivation. Due to these attributes, VWF is a highly interesting system from a biophysical point of view, and is well suited for investigation using biophysical approaches. Here, we give an overview on recent studies that predominantly employed biophysical methods to gain novel insights into multiple aspects of VWF: Electron microscopy was used to shed light on the domain structure of VWF and the mechanism of VWF secretion. High-resolution stochastic optical reconstruction microscopy, atomic force microscopy (AFM), microscale thermophoresis and fluorescence correlation spectroscopy allowed identification of protein disulfide isomerase isoform A1 as the VWF dimerizing enzyme and, together with molecular dynamics simulations, postulation of the dimerization mechanism. Advanced mass spectrometry led to detailed identification of the glycan structures carried by VWF. Microfluidics was used to illustrate the interplay of force and VWF function. Results from optical tweezers measurements explained mechanisms of the force-dependent functions of VWF's domains A1 and A2 and, together with thermodynamic approaches, increased our understanding of mutation-induced dysfunctions of platelet-binding. AFM-based force measurements and AFM imaging enabled exploration of intermonomer interactions and their dependence on pH and divalent cations. These advances would not have been possible by the use of biochemical methods alone and show the benefit of interdisciplinary research approaches.

Relaxation time for monitoring the quantumness of an intense cavity field

Recently it was shown that the quantum behavior of an intense cavity field can be revealed by measuring the steady atomic correlations between two ideal atoms, which interact with the same leaking cavity mode. Considering a weak atom-field coupling regime and large average number of photons in the cavity mode ($\bar{n}$), one expects that a semiclassical theory could explain the whole dynamics of the system. However, this system presents the generation of correlations between the atoms, which is a signature of the quantumness of the cavity field even in the limit of $\bar{n} \gg 1$ [Phys. Rev. Lett. \textbf{107}, 153601 (2011)]. Here, we extend this result by investigating the relaxation time for such a system. We have shown that the relaxation time of the system varies proportionally to $\bar{n}$ for a coherent driving, but it is inversely proportional to $\bar{n}$ for an incoherent pumping. Thus, the time required to observe the manifestation of the quantum aspects of a cavity field on the atomic correlations diverges as $\bar{n}$ tends to macroscopic values due to a coherent driving, while it goes to zero for incoherent pumping. For a coherent driving, we can also see that this system presents metastability, i.e., firstly the atomic system reaches a quasi-stationary state which last for a long time interval, but eventually it reaches the real steady state. We have also discussed the effects of small atomic decay. In this case, the steady correlations between the atoms disappear for long times, but the intense cavity field is still able to generate atomic correlations at intermediate times. Then, considering a real scenario, we would be able to monitor the quantumness of a cavity field in a certain time interval.

Network structure of molybdate glasses by neutron and X-ray diffraction and reverse Monte Carlo modelling

Rare-earth molybdate glasses have been prepared by rapid quench technique, the network structure was investigated by neutron and high-energy X-ray diffraction. For data evaluation the reverse Monte Carlo simulation technique was applied to obtain a possible 3dimensional network configuration, which is consistent with the experimental data. From the modelling the partial atomic correlation functions giJ(r) and the coordination number distributions CNij have been revealed. Formation of MoO4 (55%) and MoO6 (25%) units was established for the binary 90MoO3-10Nd2O3 glass. The B-O first neighbour distribution show a relatively broad first neighbour distance at 1.40A, the average coordination numbers show the presents of trigonal BO3 and tetrahedral BO4 groups. For 50MoO3-25Nd2O3-25B2O3 sample mixed MoO4-BO4 and MoO4-BO3 linkages form pronounced intermediate-range order.