Photon Correlation Research Articles

Salt induced slowdown of kinetics and dynamics during thermal gelation of egg-yolk.

We investigated the effect of the NaCl concentration (0.3-2M) on the structure and dynamics of hen egg yolk at room temperature and during thermal gelation at temperatures in the range of 66-90 °C utilizing low-dose x-ray photon correlation spectroscopy in ultra-small angle x-ray scattering geometry. With an increase in the salt concentration, we observe progressive structural and dynamic changes at room temperature, indicating the disruption of yolk components such as yolk-granules and yolk-plasma proteins. Temperature- and salt-dependent structural and dynamic investigations suggest a delay in the gel formation and aggregation of yolk low-density lipoproteins with increasing ionic strength. However, the time-temperature superposition relationship observed in all samples suggests an identical mechanism underlying protein aggregation-gelation with a temperature-dependent reaction rate. The sol-gel transition time extracted from kinetic and dynamic information follows Arrhenius's behavior, and the activation energy (460kJ/mol) is found to be independent of the salt concentration.

Colossal Core/Shell CdSe/CdS Quantum Dot Emitters.

Single-photon sources are essential for advancing quantum technologies with scalable integration being a crucial requirement. To date, deterministic positioning of single-photon sources in large-scale photonic structures remains a challenge. In this context, colloidal quantum dots (QDs), particularly core/shell configurations, are attractive due to their solution processability. However, traditional QDs are typically small, about 3 to 6 nm, which restricts their deterministic placement and utility in large-scale photonic devices, particularly within optical cavities. The largest existing core/shell QDs are a family of giant CdSe/CdS QDs, with total diameters ranging from about 20 to 50 nm. Pushing beyond this size limit, we introduce a synthesis strategy for colossal CdSe/CdS QDs, with sizes ranging from 30 to 100 nm, using a stepwise high-temperature continuous injection method. Electron microscopy reveals a consistent hexagonal diamond morphology composed of 12 semipolar {101̅1} facets and one polar (0001) facet. We also identify conditions where shell growth is disrupted, leading to defects, islands, and mechanical instability, which suggest synthetic requirements for growing crystalline particles beyond 100 nm. The stepwise growth of thick CdS shells on CdSe cores enables the synthesis of emissive QDs with long photoluminescence lifetimes of a few microseconds and suppressed blinking at room temperature. Notably, QDs with 80 and 100 CdS monolayers exhibit high single-photon emission purity with second-order photon correlation g(2)(0) values below 0.2.

Transport coefficient approach for characterizing nonequilibrium dynamics in soft matter

Nonequilibrium states in soft condensed matter require a systematic approach to characterize and model materials, enhancing predictability and applications. Among the tools, X-ray photon correlation spectroscopy (XPCS) provides exceptional temporal and spatial resolution to extract dynamic insight into the properties of the material. However, existing models might overlook intricate details. We introduce an approach for extracting the transport coefficient, denoted as [Formula: see text], from the XPCS studies. This coefficient is a fundamental parameter in nonequilibrium statistical mechanics and is crucial for characterizing transport processes within a system. Our method unifies the Green-Kubo formulas associated with various transport coefficients, including gradient flows, particle-particle interactions, friction matrices, and continuous noise. We achieve this by integrating the collective influence of random and systematic forces acting on the particles within the framework of a Markov chain. We initially validated this method using molecular dynamics simulations of a system subjected to changes in temperatures over time. Subsequently, we conducted further verification using experimental systems reported in the literature and known for their complex nonequilibrium characteristics. The results, including the derived [Formula: see text] and other relevant physical parameters, align with the previous observations and reveal detailed dynamical information in nonequilibrium states. This approach represents an advancement in XPCS analysis, addressing the growing demand to extract intricate nonequilibrium dynamics. Further, the methods presented are agnostic to the nature of the material system and can be potentially expanded to hard condensed matter systems.

Dynamic particle size study of immunogenic complexes of PF4/heparin based on photon correlation spectroscopy

In this work, the process of forming PF4/heparin complex was described based on their sizes measured with PCS. PF4/heparin complexes formed when a small amount of heparin was added to PF4, and they grew to bigger particles when more heparin was added, but they started to decompose after a certain amount of heparin was added. The larger the molecular weight of heparin has, the less amount of heparin is required to form the complex with PF4. This process was verified by the results of the complex surface charge. This method was used to compare the immunogenicity among the different batches of nadroparin after its specificity and stability were validated.

Time-bin entanglement in the deterministic generation of linear photonic cluster states

We theoretically investigate strategies for the deterministic creation of trains of time-bin entangled photons using an individual quantum emitter described by a Λ-type electronic system. We explicitly demonstrate the theoretical generation of linear cluster states with substantial numbers of entangled photonic qubits in full microscopic numerical simulations. The underlying scheme is based on the manipulation of ground state coherences through precise optical driving. One important finding is that the most easily accessible quality metrics, the achievable rotation fidelities, fall short in assessing the actual quantum correlations of the emitted photons in the face of losses. To address this, we explicitly calculate stabilizer generator expectation values as a superior gauge for the quantum properties of the generated many-photon state. With widespread applicability in other emitter and excitation–emission schemes also, our work lays the conceptual foundations for an in-depth practical analysis of time-bin entanglement based on full numerical simulations with predictive capabilities for realistic systems and setups, including losses and imperfections. The specific results shown in the present work illustrate that with controlled minimization of losses and realistic system parameters for quantum-dot type systems, useful linear cluster states of significant lengths can be generated in the calculations, discussing the possibility of scalability for quantum information processing endeavors.

AI-NERD: Elucidation of relaxation dynamics beyond equilibrium through AI-informed X-ray photon correlation spectroscopy

Understanding and interpreting dynamics of functional materials in situ is a grand challenge in physics and materials science due to the difficulty of experimentally probing materials at varied length and time scales. X-ray photon correlation spectroscopy (XPCS) is uniquely well-suited for characterizing materials dynamics over wide-ranging time scales. However, spatial and temporal heterogeneity in material behavior can make interpretation of experimental XPCS data difficult. In this work, we have developed an unsupervised deep learning (DL) framework for automated classification of relaxation dynamics from experimental data without requiring any prior physical knowledge of the system. We demonstrate how this method can be used to accelerate exploration of large datasets to identify samples of interest, and we apply this approach to directly correlate microscopic dynamics with macroscopic properties of a model system. Importantly, this DL framework is material and process agnostic, marking a concrete step towards autonomous materials discovery.

On the analysis of two-time correlation functions: equilibrium versus non-equilibrium systems.

X-ray photon correlation spectroscopy (XPCS) is a powerful tool for the investigation of dynamics covering a broad range of timescales and length scales. The two-time correlation function (TTC) is commonly used to track non-equilibrium dynamical evolution in XPCS measurements, with subsequent extraction of one-time correlations. While the theoretical foundation for the quantitative analysis of TTCs is primarily established for equilibrium systems, where key parameters such as the diffusion coefficient remain constant, non-equilibrium systems pose a unique challenge. In such systems, different projections ('cuts') of the TTC may lead to divergent results if the underlying fundamental parameters themselves are subject to temporal variations. This article explores widely used approaches for TTC calculations and common methods for extracting relevant information from correlation functions, particularly in the light of comparing dynamics in equilibrium and non-equilibrium systems.

Temporal coherences of atomic chaotic light sources: The Siegert relation and its generalisation to higher-order correlation functions

Light is characterized by its electric field, yet quantum optics has revealed the importance of monitoring photon-photon correlations at all orders. We here present a comparative study of two experimental setups, composed of cold and warm rubidium atoms, respectively, which allow us to probe and compare photon correlations. The former operates in the quantum regime where spontaneous emission dominates, whereas the latter exhibits a temperature-limited coherence time. We demonstrate our capability to measure photon correlations up to the fourth order which could be useful to better characterize light scattered by cold atoms beyond the chaotic statistics.

Antioxidant, antiglycation, and antibacterial of copper oxide nanoparticles synthesized using Caesalpinia Sappan extract.

Synthesis of metal nanoparticles using plant extracts is environmentally friendly and of increasing interest. However, not all plant extracts can meet successfully on the synthesis. Therefore, searching for the high potential extracts that can reduce the metal salt precursor in the synthesis reaction is essential. The present study explores the synthesis of copper oxide nanoparticles (CuONPs) using Caesalpinia sappan heartwood extract. Phytochemical analysis and determination of the total phenolic content of the extract were performed before use as a reducing agent. Under the suitable synthesized condition, a color change in the color of the solutions to brown confirmed the formation of CuONPs. The obtained CuONPs were confirmed using ultraviolet-visible spectroscopy, photon correlation spectroscopy, X-ray diffraction, scanning electron microscope, energy dispersive X-ray, and Fourier transform infrared analysis. The synthesized CuONPs investigated for antioxidant, antiglycation, and antibacterial activities. CuONPs possessed antioxidant activities by quenching free radicals with an IC50 value of 63.35 µg/mL and reducing activity with an EC range of 3.19-10.27 mM/mg. CuONPs also inhibited the formation of advanced glycation end products in the bovine serum albumin/ribose model with an IC50 value of 17.05 µg/mL. In addition, CuONPs showed inhibition of human pathogens, including Gram-positive Staphylococcus aureus and Gram-negative Escherichia coli, and prevention of biofilm formation and biofilm eradication, with maximum inhibition of approx. 75%. Our findings suggest that C. sappan extract can be used to obtain highly bioactive CuONPs for the development of certain medical devices and therapeutic agents.

Tracking Prenucleation Molecular Clustering of Salicylamide in Organic Solvents.

Crystal nucleation shapes the structure and product size distribution of solid-state pharmaceuticals and is seeded by early-stage molecular self-assemblies formed in host solution. Here, molecular clustering of salicylamide in ethyl acetate, methanol, and acetonitrile was investigated using photon correlation spectroscopy. Cluster size steadily increased over 3 days and with concentration across the range from undersaturated to supersaturated solutions. Solute concentration normalized by solubility provided more sensitive characterization of molecular-level conditions than concentration alone. In saturated solution, cluster size is independent of solvent, while at equal supersaturation, solvent-dependent cluster size increases as methanol < acetonitrile < ethyl acetate, commensurate with increasing nucleation propensity. In ethyl acetate, with largest prenucleation clusters, the driving force required for nucleation is lowest, compared to methanol with smallest clusters and highest driving force. To understand solvent-solute effects, we performed IR spectroscopy supported by molecular simulations. We observe solute-solvent interaction weakening in the same order: methanol < acetonitrile < ethyl acetate, quantifying the weaker solvent-solute interactions that permit the formation of larger prenucleation clusters. Our results support the hypothesis that nucleation is easier in weaker solvents because weak solute-solvent interactions favor growth of large clusters, as opposed to relying solely on ease of desolvation.

Non‐Hermitian Control of Multimode Duan‐PPT Criteria and Steering in Energy‐Level Cascaded Four‐Wave Mixing Processes

AbstractThe non‐Hermitian singularity control of multimode entanglement in the energy‐level cascaded four‐wave mixing system within a single atomic vapor is of great significance and importance. In this study, a non‐Hermiticity system by means of quasi‐quantization of energy‐band based on non‐Hermiticity systems is constructed. By employing atomic coherence in the non‐Hermiticity system, high‐dimensional quantized photon correlations underdressed field‐induced parity‐time (PT) symmetry and symmetry breaking through the quantization of energy levels are studied. Such a phenomenon happens at microscopic (nanoscale) when the eigenvalues of dressed energy‐level and multimode entanglement are considered for both real and imaginary parts symmetry breaking. Double dressing effect is observed with more coherent channels and larger information capacity than single dressing in the energy‐level cascaded four‐wave mixing system. The study found that the splitting of the real part is larger than an imaginary part in a second‐order system, and the imaginary part splitting is also greater than the real part splitting in a third‐order system. The real part (in phase) is constructive dressing quantization, and the imaginary (out of phase) is destructive dressing quantization. Exceptional points (EP points) can be used to enhance sensitivity detection of entanglement quantum state.

Towards quantum technologies with gamma photons

In the context of the second quantum revolution, the ability to manipulate quantum systems is already used for various techniques and a growing number of technology demonstrators, mostly with low energy photons. In this frame, our intention is to extend quantum technologies to gamma photons. Our aim is to take advantage of resources brought by entanglement with higher energy particles, particularly electron-positron annihilation quanta. Tools for low frequency quantum experiments are not suitable for penetrant radiation, consequently we need to use effects typical to the keV-MeV energy range instead. High energy photon protocols would include fundamental properties testing, industrial imaging, quantum random number generators, quantum simulators, military applications and improvement of already existing medical procedures. In this paper we review some important steps in the study of annihilation photon correlations, we point out the experimental differences and necessities with respect to the energy increase in quantum photonic experiments and we describe the design of a quantum gamma device we propose for experiments meant to prove feasibility of gamma ray based protocols. The perspective behind our project is to evidence the possibility to communicate via entangled quanta through media which are not transparent for low energy photons.

Phase retrieval in incoherent diffractive imaging using higher-order photon correlation functions

To obtain spatial information about an arbitrary atomic distribution in x-ray structure analysis, e.g. in molecules or proteins, the standard method is to measure the intensity in the far field, i.e. the first-order photon correlation function of the coherently scattered x-ray photons (coherent diffractive imaging). Recently, it was suggested to record alternatively the incoherently scattered photons and measure the second-order photon correlation function to reconstruct the geometry of the unknown atomic distribution (incoherent diffractive imaging). Yet, besides various advantages of the latter method, both techniques suffer from the so-called phase retrieval problem. Lately, an ab-initio phase retrieval algorithm to reconstruct the phase of the so-called structure factor of the scattering objects based on the third-order photon correlation function was reported. The algorithm makes use of the closure phase, which contains important, yet incomplete phase information, well-known from triple correlations and their bispectrum in speckle masking and astronomy applications. Here, we provide a detailed analysis of the underlying scheme and quantities in the context of x-ray structure analysis. In particular, we explicitly calculate for the first time the third-order photon correlation function for single photon emitters in a full quantum mechanical treatment and discuss the uniqueness of the closure phase equations constructed from. In this context, we recapitulate the sign problem of the closure phase and how it can be lifted using redundant information. We further show how the algorithm can be improved using even higher-order photon correlation functions produced by single photon emitters, e.g. the fourth-order correlation function, delivering new phase relations appearing in the four-point correlations.

Strong Raman enhancement in structured colloids: localization of light

Raman spectroscopy is a powerful technique for studying the interaction between light and matter. Here we show a significant enhancement of Raman emission over a broad range of pumping wavelengths from strongly scattering media comprising spatially correlated photonic structures of core–shell TiO2@Silica scatterers mixed with silica nanoparticles and suspended in ethanol. Long-range Coulomb interactions between nanoparticles inside these photonic colloidal structures induce a correlation in the scatterers’ positions (TiO2@Silica), affecting local and global photonic properties. The anomalous enhancement in Raman signal increases as the scattering strength is increased (through either scatterer concentration or pumping wavelength); however, the signal strength continues to behave linearly with excitation power, ruling out classical nonlinear and interferential phenomena. These observations may indicate strong photon correlation in strongly localized electromagnetic modes, inducing successive photon interactions with the atoms or molecules. Aside from the fundamental relevance to understanding measurable properties in this regime of strongly localized electromagnetic modes, our demonstration of strongly enhanced Raman emission over a broad range of pumping wavelengths provides new opportunities for the development of advanced photonic materials and devices.

Time-gated imaging through dense fog via physics-driven Swin transformer

Imaging through the fog is valuable for many areas, such as autonomous driving and cosmic exploration. However, due to the influence of strong backscattering and diffuse reflection generated by the dense fog on the temporal-spatial correlations of photons returning from the target object, the reconstruction quality of most existing methods is significantly reduced under dense fog conditions. In this study, we describe the optical scatter imaging process and propose a physics-driven Swin Transformer method utilizing Time-of-Flight (ToF) and Deep Learning principles to mitigate scattering effects and reconstruct targets in conditions of heterogeneous dense fog. The results suggest that, despite the exponential decrease in the number of ballistic photons as the optical thickness of fog increases, the Physics-Driven Swin Transformer method demonstrates satisfactory performance in imaging targets obscured by dense fog. Importantly, this article highlights that even in dense fog imaging experiments with optical thickness reaching up to 3.0, which exceeds previous studies, commonly utilized quantitative evaluation metrics like PSNR and SSIM indicate that our method is cutting-edge in imaging through dense fog.

Tailoring micellar nanocarriers for pemetrexed in breast cancer: design, fabrication and in vitro evaluation.

Aim: To investigate the pemetrexed encapsulated polymeric mixed micelles (PMMs) against breast cancer treatment.Methods: We meticulously optimized the formulation and conducted extensive characterizations, including photon correlation spectroscopy for micellization, advanced analytical techniques and in vitro cell line assessments.Results: The PMM exhibited favorable characteristics, with a spherical morphology, hydrodynamic particle size of 19.58±0.89nm, polydispersity index of 0.245±0.1, and a surface charge of -9.70±0.61mV. Encapsulation efficiency and drug payload reached 96.16±0.37% and 4.5±0.32%, respectively. Cytotoxicity analysis indicated superior efficacy of the PMM over the drug solution.Conclusion: The PMM formulation exhibited controlled release of the drug, and demonstrated enhanced cytotoxicity against breast cancer cells, highlighting its therapeutic promise.

In situ coherent x-ray scattering reveals polycrystalline structure and discrete annealing events in strongly coupled nanocrystal superlattices

Solution-phase bottom up self-assembly of nanocrystals into superstructures such as ordered superlattices is an attractive strategy to generate functional materials of increasing complexity, including very recent advances that incorporate strong interparticle electronic coupling. While the self-assembly kinetics in these systems have been elucidated and related to the product characteristics, the weak interparticle bonding interactions suggest the superstructures formed could continue to order within the solution long after the primary nucleation and growth have occurred, even though the mechanism of annealing remains to be elucidated. Here, we use a combination of Bragg coherent diffractive imaging and x-ray photon correlation spectroscopy to create real-space maps of supercrystalline order along with a real-time view of the strain fluctuations in aging strongly coupled nanocrystal superlattices while they remain suspended and immobilized in solution. By combining the results, we deduce that the self-assembled superstructures are polycrystalline, initially comprising multiple nucleation sites, and that shear avalanches at grain boundaries continue to increase crystallinity long after growth has substantially slowed. This multimodal approach should be generalizable to characterize a breadth of materials in their native chemical environments, thus extending the reach of high-resolution coherent x-ray characterization to the benefit of a much wider range of physical systems. Published by the American Physical Society 2024

New pathways to control the evolution of the atomic motion in metallic glasses

Metallic glass formers are a relatively new entry in glass physics, which has attracted large interest in both physics and materials science communities due to the unique mechanical and structural properties of these materials. Physical aging is however one of the main obstacle to their widespread use as it affects their properties at all length scales. The knowledge of the microscopic mechanisms inducing aging and relaxation is therefore extremely important for both fundamental and applied sciences. In this article we present a review of the recent advances made with the X-ray photon correlation spectroscopy technique on the study of the collective particle motion and physical aging in metallic glasses at the atomic level. We show that a careful tuning of the sample preparation or the application of specific thermal protocols have the potential to drive the glass into more aged or rejuvenated microscopic configurations with different stabilities.

A new experimental setup for combined fast differential scanning calorimetry and X-ray photon correlation spectroscopy.

Synchrotron-radiation-based techniques are a powerful tool for the investigation of materials. In particular, the availability of highly brilliant sources has opened the possibility to develop techniques sensitive to dynamics at the atomic scale such as X-ray photon correlation spectroscopy (XPCS). XPCS is particularly relevant in the study of glasses, which have been often investigated at the macroscopic scale by, for example, differential scanning calorimetry. Here, we show how to adapt a Flash calorimeter to combine XPCS and calorimetric scans. This setup paves the way to novel experiments requiring dynamical and thermodynamic information, ranging from the study of the crystallization kinetics to the study of the glass transition in systems that can be vitrified thanks to the high cooling rates reachable with an ultrafast calorimeter.

Real-time swelling-collapse kinetics of nanogels driven by XFEL pulses.

Stimuli-responsive polymers are an important class of materials with many applications in nanotechnology and drug delivery. The most prominent one is poly-N-isopropylacrylamide (PNIPAm). The characterization of the kinetics of its change after a temperature jump is still a lively research topic, especially at nanometer-length scales where it is not possible to rely on conventional microscopic techniques. Here, we measured in real time the collapse of a PNIPAm shell on silica nanoparticles with megahertz x-ray photon correlation spectroscopy at the European XFEL. We characterize the changes of the particles diffusion constant as a function of time and consequently local temperature on sub-microsecond timescales. We developed a phenomenological model to describe the observed data and extract the characteristic times associated to the swelling and collapse processes. Different from previous studies tracking the turbidity of PNIPAm dispersions and using laser heating, we find collapse times below microsecond timescales and two to three orders of magnitude slower swelling times.