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Strong quantum-correlated sources are essential but delicate resources for quantum information science and engineering protocols. Decoherence and loss are the two main disruptive processes that lead to the loss of nonclassical behavior in quantum correlations. In quantum systems, scattering can contribute to both decoherence and loss. In this work, we present an experimental scheme capable of significantly mitigating the adverse impact of scattering in quantum systems. Our quantum system is composed of a two-mode squeezed light generated with the four-wave mixing process in hot rubidium vapor, and a scatterer is introduced to one of the two modes. An integrating sphere is then placed after the scatterer to recollect the scattered photons. We use mutual information between the two modes as the measure of quantum correlations, and demonstrate a 47.5% mutual information recovery from scattering, despite an enormous photon loss of greater than 85%. Our scheme is a pioneering step towards recovering quantum correlations from disruptive random processes, thus has the potential to bridge the gap between proof-of-principle demonstrations and practical real-world deployments of quantum protocols., Comment: 7 pages, 4 figures

The development and application of upconversion nanoparticles (UCNPs) have garnered significant attention due to their unique optical properties and potential uses in bioimaging, drug delivery, and solar cells. However, the hydrophobic nature of UCNPs presents challenges in their synthesis and application, particularly in aqueous environments. We provide an overview of UCNPs, their synthesis challenges, and the importance of surface modification. Furthermore, we discuss the properties of \textit{LiYF_{4}:Yb, Er, Tm} UCNPs synthesized using novel 2,2-[ethylenebis(oxy)] bisacetic acid (EBAA) method and their versatile applications. Notably, the first Dynamic Light Scattering measurement on 05/22/2022 showed a size of 11.39 nm, and after 348 days on 04/05/2023, the same batch maintained a size of 13.8 nm, indicating excellent stability and no particle agglomeration over this extended period. This remarkable stability underscores the potential of UCNPs synthesized with the EBAA method for long-term applications. Finally, we compare the EBAA method with other surface modification techniques, exploring challenges and future perspectives for the use of hydrophilic UCNPs in various applications. This review aims to emphasize the significance of the EBAA method in advancing the field of upconversion nanoparticles and broadening their potential integration into diverse applications., Comment: 21 Pages, 1 table, 13 figures

Fundamental understanding of macroscopic properties of polymer nanocomposites (PNCs) remains difficult due to the complex interplay of microscopic dynamics and structure, namely interfacial layer relaxations and three-dimensional nanoparticle arrangements. The effect of surface modification by alkyl methoxysilanes at different grafting densities has been studied in PNCs made of poly(2-vinylpyridine) and spherical 20 nm silica nanoparticles (NPs). The segmental dynamics has been probed by broadband dielectric spectroscopy, and the filler structure by small-angle X-ray scattering and reverse Monte Carlo simulations. By combining the particle configurations with the interfacial layer properties, it is shown how surface modification tunes the attractive polymer-particle interactions: bare NPs slow down the polymer interfacial layer dynamics over a thickness of ca. 5 nm, while grafting screens these interactions. Our analysis of interparticle spacing and segmental dynamics provides unprecedented insight into the effect of surface modification on the main characteristics of PNCs: particle interactions and polymer interfacial layers.

Both the dispersion state of nanoparticles (NPs) within polymer nanocomposites (PNCs) and the dynamical state of the polymer altered by the presence of the NP/polymer interfaces have a strong impact on the macroscopic properties of PNCs. In particular, mechanical properties are strongly affected by percolation of hard phases, which may be NP networks, dynamically modified polymer regions, or combinations of both. In this article, the impact on dispersion and dynamics of surface modification of the NPs by short monomethoxysilanes with eight carbons in the alkyl part (C8) is studied. As a function of grafting density and particle content, polymer dynamics is followed by broadband dielectric spectroscopy and analyzed by an interfacial layer model, whereas the particle dispersion is investigated by small-angle X-ray scattering and analyzed by reverse Monte Carlo simulations. NP dispersions are found to be destabilized only at the highest grafting. The interfacial layer formalism allows the clear identification of the volume fraction of interfacial polymer, with its characteristic time. The strongest dynamical slow-down in the polymer is found for unmodified NPs, while grafting weakens this effect progressively. The combination of all three techniques enables a unique measurement of the true thickness of the interfacial layer, which is ca. 5 nm. Finally, the comparison between longer (C18) and shorter (C8) grafts provides unprecedented insight into the efficacy and tunability of surface modification. It is shown that C8-grafting allows for a more progressive tuning, which goes beyond a pure mass effect.

Quantum frequency up-conversion is a cutting-edge technique that leverages the interaction between photons and quantum systems to shift the frequency of single photons from a lower frequency to a higher frequency. If the photon before up-conversion was one of the entangled pair, then it is important to understand how much entanglement is preserved after up-conversion. In this study, we present a theoretical analysis of the transformation of the time-dependent second-order quantum correlations in photon pairs and find the preservation of such correlations under fairly general conditions. We also analyze the two-photon Hong-Ou-Mandel interference between the frequency-converted idler photon and the signal photon. The visibility of the two-photon interference is sensitive to the magnitude of the frequency conversion, and it improves when the frequency separation between two photons goes down.

We study coherent anti-Stokes Raman spectroscopy in air-filled anti-resonance hollow-core photonic crystal fiber, otherwise known as 'revolver' fiber. We compare the vibrational coherent anti-Stokes Raman signal of N$_2$, at 2331 cm$^{-1}$, generated in ambient air (no fiber present), with the one generated in a 2.96 cm of a revolver fiber. We show a 170 times enhancement for the signal produced in the fiber, due to an increased interaction path. Remarkably, the N$_2$ signal obtained in the revolver fiber shows near-zero non-resonant background, due to near-zero overlap between the laser field and the fiber cladding. Through our study, we find that the revolver fiber properties make it an ideal candidate for the coherent Raman spectroscopy signal enhancement.

In a viral pandemic, a few important tests are required for successful containment of the virus and reduction in severity of the infection. Among those tests, a test for the neutralizing ability of an antibody is crucial for assessment of population immunity gained through vaccination, and to test therapeutic value of antibodies made to counter the infections. Here, we report a sensitive technique to detect the relative neutralizing strength of various antibodies against the SARS-CoV-2 virus. We used bright, photostable, background-free, fluorescent upconversion nanoparticles conjugated with SARS-CoV-2 receptor binding domain as a phantom virion. A glass bottom plate coated with angiotensin-converting enzyme 2 (ACE-2) protein imitates the target cells. When no neutralizing IgG antibody was present in the sample, the particles would bind to the ACE-2 with high affinity. In contrast, a neutralizing antibody can prevent particle attachment to the ACE-2-coated substrate. A prototype system consisting of a custom-made confocal microscope was used to quantify particle attachment to the substrate. The sensitivity of this assay can reach 4.0 ng/ml and the dynamic range is from 1.0 ng/ml to 3.2 {\mu}g/ml. This is to be compared to 19 ng/ml sensitivity of commercially available kits.

Spontaneous emission from individual atoms in vapor lasts nanoseconds, if not microseconds, and beatings in this emission involve only directly excited energy sublevels. In contrast, the superfluorescent emissions burst on a much-reduced timescale and their beatings involve both directly and indirectly excited energy sublevels. In this work, picosecond and femtosecond superfluorescent beatings are observed from a dense cesium atomic vapor. Cesium atoms are excited by 60-femtosecond long, 800 nm laser pulses via two-photon processes into their coherent superpositions of the ground 6S and excited 8S states. As a part of the transient four wave mixing process, the yoked superfluorescent blue light at lower transitions of 6S - 7P are recorded and studied. Delayed buildup time of this blue light is measured as a function of the input laser beam power using a high-resolution 2 ps streak camera. The power dependent buildup delay time is consistently doubled as the vapor temperature is lowered to cut the number of atoms by half. At low power and density, a beating with a period of 100 picoseconds representing the ground state splitting is observed. The autocorrelation measurements of the generated blue light exhibit a beating with a quasi-period of 230 fs corresponding to the splitting of the 7P level primarily at lower input laser power. Understanding and, eventually, controlling the intriguing nature of superfluorescent beatings may permit a rapid quantum operation free from the rather slow spontaneous emission processes from atoms and molecules., Comment: 7 pages, 5 figures

In this work, we implement a scheme to combine six coherent, spatially separated Raman sidebands generated in single-crystal diamond into a collinear beam. With appropriate phase tuning, this results in a pulse much shorter than the generating pump. We elucidate the characteristics of the synthesized pulse by using an interferometric collinear cross-correlation frequency-resolved optical gating setup (ix-FROG). The beating of the synchronized sidebands results in an additional component in the signal, which we use to optimize the relative phases of our sidebands. In this way, we synthesize and measure visible-range, near-single cycle isolated pulses of approximately 5 fs total pulse duration., Comment: 7 pages, 3 figures, one conference paper, two conference abstracts, two workshops

The Winter Colloquium on the Physics of Quantum Electronics (PQE) has been a seminal force in quantum optics and related areas since 1971. It is rather mindboggling to recognize how the concepts presented at these conferences have transformed scientific understanding and human society. In January, 2017, the participants of PQE were asked to consider the equally important prospects for the future, and to formulate a set of questions representing some of the greatest aspirations in this broad field. The result is this multi-authored paper, in which many of the world's leading experts address the following fundamental questions: (1) What is the future of gravitational wave astronomy? (2) Are there new quantum phases of matter away from equilibrium that can be found and exploited - such as the time crystal? (3) Quantum theory in uncharted territory: What can we learn? (4) What are the ultimate limits for laser photon energies? (5) What are the ultimate limits to temporal, spatial, and optical resolution? (6) What novel roles will atoms play in technology? (7) What applications lie ahead for nitrogen-vacancy centers in diamond? (8) What is the future of quantum coherence, squeezing, and entanglement for enhanced superresolution and sensing? (9) How can we solve (some of) humanity's biggest problems through new quantum technologies? (10) What new understanding of materials and biological molecules will result from their dynamical characterization with free electron lasers? (11) What new technologies and fundamental discoveries might quantum optics achieve by the end of this century? (12) What novel topological structures can be created and employed in quantum optics?, Comment: A review of the leading topics in quantum optics and related areas. Accepted for publication in J. Modern Optics (42 figures, 74 pages)

Recently, optimization techniques have had a significant impact in a variety of fields, leading to a higher signal-to-noise and more streamlined techniques. We consider the possibility for using programmable phase-only spatial optimization of the pump beam to influence the supercontinuum generation process. Preliminary results show that significant broadening and rough control of the supercontinuum spectrum are possible without loss of input energy. This serves as a proof-of-concept demonstration that spatial effects can controllably influence the supercontinuum spectrum, leading to possibilities for utilizing supercontinuum power more efficiently and achieving arbitrary spectral control.

One century ago pioneering dielectric results obtained for water and n-alcohols triggered the advent of molecular rotation diffusion theory considered by Debye to describe the primary dielectric absorption in these liquids. Comparing dielectric, viscoelastic, and light scattering results we unambiguously demonstrate that the structural relaxation appears only as a high-frequency shoulder in the dielectric spectra of water. In contrast, the main dielectric peak is related to a supramolecular structure, analogous to the Debye-like peak observed in mono-alcohols., Comment: 5 pages, 3 figures

Two-dimensional (2D) materials beyond graphene such as transition metal dichalcogenides (TMDs) have unique mechanical, optical and electronic properties with promising applications in flexible devices, catalysis and sensing. Optical imaging of TMDs using photoluminescence and Raman spectroscopy can reveal the effects of structure, strain, doping, defects, edge states, grain boundaries and surface functionalization. However, Raman signals are inherently weak and so far have been limited in spatial resolution in TMDs to a few hundred nanometres which is much larger than the intrinsic scale of these effects. Here we overcome the diffraction limit by using resonant tip-enhanced Raman scattering (TERS) of few-layer MoS2, and obtain nanoscale optical images with ~ 20 nm spatial resolution. This becomes possible due to electric field enhancement in an optimized subnanometre-gap resonant tip-substrate configuration. We investigate the limits of signal enhancement by varying the tip-sample gap with sub-Angstrom precision and observe a quantum quenching behavior, as well as a Schottky-Ohmic transition, for subnanometre gaps, which enable surface mapping based on this new contrast mechanism. This quantum regime of plasmonic gap-mode enhancement with a few nanometre thick MoS2 junction may be used for designing new quantum optoelectronic devices and sensors.

The detailed nature of spatially heterogeneous dynamics of glycerol-silica nanocomposites is unraveled by combining dielectric spectroscopy with atomistic simulation and statistical mechanical theory. Analysis of the spatial mobility gradient shows no 'glassy' layer, but the alpha relaxation time near the nanoparticle grows with cooling faster than the alpha relaxation time in the bulk, and is ~ 20 times longer at low temperatures. The interfacial layer thickness increases from ~ 1.8 nm at higher temperatures to ~ 3.5 nm upon cooling to near Tg. A real space microscopic description of the mobility gradient is constructed by synergistically combining high temperature atomistic simulation with theory. Our analysis suggests that the interfacial slowing down arises mainly due to an increase of the local cage scale barrier for activated hopping induced by enhanced packing and densification near the nanoparticle surface. The theory is employed to predict how local surface densification can be manipulated to control layer dynamics and shear rigidity over a wide temperature range., Comment: To be submitted to The Journal of Chemical Physics

Coherent anti-Stokes Raman scattering (CARS) and, in particular, femtosecond adaptive spectroscopic techniques (FAST CARS) have been successfully used for molecular spectroscopy and microscopic imaging. Recent progress in ultrafast nanooptics provides flexibility in generation and control of optical near fields, and holds promise to extend CARS techniques to the nanoscale. In this theoretical study, we demonstrate ultrafast subwavelentgh control of coherent Raman spectra of molecules in the vicinity of a plasmonic nanostructure excited by ultrashort laser pulses. The simulated nanostructure design provides localized excitation sources for CARS by focusing incident laser pulses into subwavelength hot spots via two self-similar nanolens antennas connected by a waveguide. Hot-spot-selective dual-tip-enhanced CARS (2TECARS) nanospectra of DNA nucleobases are obtained by simulating optimized pump, Stokes and probe near fields using tips, laser polarization- and pulse-shaping. This technique may be used to explore ultrafast energy and electron transfer dynamics in real space with nanometre resolution and to develop novel approaches to DNA sequencing., Comment: 11 pages, 6 figures

We study the possibility of creating spatial patterns having subwavelength size by using the so-called dark states formed by the interaction between atoms and optical fields. These optical fields have a specified spatial distribution. Our experiments in Rb vapor display spatial patterns that are smaller than the length determined by the diffraction limit of the optical system used in the experiment. This approach may have applications to interference lithography and might be used in coherent Raman spectroscopy to create patterns with subwavelength spatial resolution., Comment: 5 pages, 5 figures