Uncertainty in Composite Membranes: From Defect Engineering to Film Processing.

Composite membranes featuring metal-organic framework (MOF)-dispersed polymers have attracted tremendous attention in recent years. However, evaluating commercial viability is oftentimes obscured by the irreproducibility in both MOF synthesis and film manufacturing protocols. Variability in MOF property sets are typically ascribed to crystal defects resulting from subtle variations in synthesis, but quantitative studies investigating the role of defects on transport properties are exceedingly rare. Likewise, controlled film formation protocols are rarely reported in the open literature, making it difficult to provide substantial and informative structure-property correlations. This study aims to address these uncertainties. To this end, two samples of a prototypical MOF, UiO-66-NH2, were synthesized to feature similar particle size, morphology, and colloidal stability. However, defect engineering protocols coupled with careful screening experiments were developed to synthesize the two MOFs with maximally different porosities. Composite membranes were prepared for each MOF and a high-performance polymer, 6FDA-Durene, and then tested for light gas permeation measurements, revealing a small and unexpected enhancement in CO2/CH4 performance for samples containing low-porosity UiO-66-NH2. Mechanistic studies on sorption revealed a surprising 50% decrease in sorption capacity for high-porosity UiO-66-NH2, completely offsetting enhancements from increased gas diffusion. By using multiple replicate experiments, the sample-to-sample variation was large enough to obscure any differences in permeability and selectivity between the two types of MOF composites at low volume fractions. Application of the Maxwell model to extrapolate pure-MOF performance led to significant variations in predicted values, demonstrating the importance of collecting and reporting replicate experiments for membrane preparation and testing.

Towards Perfect Ultra-Broadband Absorbers, Ultra-Narrow Waveguides, and Ultra-Small Cavities at Optical Frequencies.

In this study, we design ultra-broadband optical absorbers, ultra-narrow optical waveguides, and ultra-small optical cavities comprising two-dimensional metallic photonic crystals that tolerate fabrication imperfections such as position and radius disorderings. The absorbers containing gold rods show an absorption amplitude of more than 90% under 54% position disordering at 200<λ<530 nm. The absorbers containing silver rods show an absorptance of more than 90% under 54% position disordering at 200<λ<400 nm. B-type straight waveguides that contain four rows of silver rods exposed to air reveal normalized transmittances of 75% and 76% under 32% position and 60% radius disorderings, respectively. B-type L-shaped waveguides containing four rows of silver rods show 76% and 90% normalized transmittances under 32% position and 40% radius disorderings, respectively. B-type cavities containing two rings of silver rods reveal 70% and 80% normalized quality factors under 32% position and 60% radius disorderings, respectively.

Super strong wide TM Mie bandgaps tolerating disorders.

This study demonstrates the appearance of super intense and wide Mie bandgaps in metamaterials composed of tellurium, germanium, and silicon rods in air that tolerate some disordering of rod position and rod radius under transverse magnetic (TM) polarized light waves. Tellurium metamaterials reveal [Formula: see text], [Formula: see text], [Formula: see text], [Formula: see text], [Formula: see text] Mie bandgap modes in which [Formula: see text], [Formula: see text], and [Formula: see text] tolerate high rod-position disordering of [Formula: see text] and rod-radius disordering of 34 and [Formula: see text], respectively. Results for germanium metamaterials show Mie bandgap modes [Formula: see text], [Formula: see text], and [Formula: see text], in which [Formula: see text] and [Formula: see text] tolerate rod-position disordering of [Formula: see text], and rod-radius disordering of 34 and [Formula: see text], respectively. Using these characteristics of [Formula: see text] in germanium metamaterials under position and radius disordering, ultra-narrow straight, L-shaped, and crossing waveguides that contain 14, four, and two rows of germanium rods in air are designed. Also, it is shown that [Formula: see text] Mie bandgap appears in metamaterials containing a high refractive index, and disappears in metamaterials with a lower refractive index such as silicon; in contrast, a new phenomenon of intense and broadband [Formula: see text], [Formula: see text], and [Formula: see text] in metamaterials with a lower refractive index such as silicon appear. In silicon-based metamaterials, [Formula: see text] tolerates high rod-position and rod-radius disordering of [Formula: see text] and [Formula: see text], respectively, and [Formula: see text] shows robustness to rod-position and rod-radius disordering of [Formula: see text]. This strong tolerance of disordering of TM modes in tellurium, germanium, and silicon metamaterials opens a new way to design small, high-efficient, and feasible fabrication optical devices for optical integrated circuits.

Locking Multi-Laser Frequencies to a Precision Wavelength Meter: Application to Cold Atoms.

We herein report a simultaneous frequency stabilization of two 780-nm external cavity diode lasers using a precision wavelength meter (WLM). The laser lock performance is characterized by the Allan deviation measurement in which we find σy=10-12 at an averaging time of 1000 s. We also obtain spectral profiles through a heterodyne spectroscopy, identifying the contribution of white and flicker noises to the laser linewidth. The frequency drift of the WLM is measured to be about 2.0(4) MHz over 36 h. Utilizing the two lasers as a cooling and repumping field, we demonstrate a magneto-optical trap of 87Rb atoms near a high-finesse optical cavity. Our laser stabilization technique operates at broad wavelength range without a radio frequency element.

Ion-Based Quantum Sensor for Optical Cavity Photon Numbers.

We dispersively couple a single trapped ion to an optical cavity to extract information about the cavity photon-number distribution in a nondestructive way. The photon-number-dependent ac Stark shift experienced by the ion is measured via Ramsey spectroscopy. We use these measurements first to obtain the ion-cavity interaction strength. Next, we reconstruct the cavity photon-number distribution for coherent states and for a state with mixed thermal-coherent statistics, finding overlaps above 99% with the calibrated states.

Three-dimensional imaging of cavity vacuum with single atoms localized by a nanohole array.

Zero-point electromagnetic fields were first introduced to explain the origin of atomic spontaneous emission. Vacuum fluctuations associated with the zero-point energy in cavities are now utilized in quantum devices such as single-photon sources, quantum memories, switches and network nodes. Here we present three-dimensional (3D) imaging of vacuum fluctuations in a high-Q cavity based on the measurement of position-dependent emission of single atoms. Atomic position localization is achieved by using a nanoscale atomic beam aperture scannable in front of the cavity mode. The 3D structure of the cavity vacuum is reconstructed from the cavity output. The root mean squared amplitude of the vacuum field at the antinode is also measured to be 0.92±0.07 V cm(-1). The present work utilizing a single atom as a probe for sub-wavelength imaging demonstrates the utility of nanometre-scale technology in cavity quantum electrodynamics.

One-pot template-free synthesis of monodisperse hollow hydrogel microspheres and their resulting properties.

Monodisperse poly(methacrylic acid/ethyleneglycoldimethacrylate) (MAA/EGDMA) hollow microcapsules, which exhibit pH-responsive behavior, are prepared by diffusion of cationic surfactants and hydrophobic interaction. During the association of the negatively charged hydrogel microspheres and an oppositely charged surfactant (cetyltrimethylammonium bromide, CTA(+)B), the hydrophobic polymer-surfactant complexes that form are separated from the internal water; consequently, a hollow structure can be formed. Confocal laser scanning microscopy, UV spectro-scopy and zeta potential are employed to study the formation of the hollow structure during the diffusion of the cationic surfactant. The controlled release behavior of methylene blue as a model drug from the as-prepared poly(MAA/EGDMA) microcapsules with a hollow structure is investigated under different pH conditions. The hollow structure can be retained, even during repetitive pH changes.

Atomic Solc filter: multi-resonant photoemission via periodic poling of atom-cavity coupling constant.

This paper describes a novel atom-cavity interaction induced by periodically poled atom-cavity coupling constant which leads to multiple narrow photoemission bands for an initially inverted two-level atom under the strong coupling condition. The emission bandpass narrowing has a close analogy with the folded Solc filter in the context of quasi-phase matching by periodic poling. We present a closed form solution of the emission probability at the end of interaction and deduce the multiple phase matching condition for this system which is programmable by the interaction time. The Bloch sphere analysis provides a clear understanding of the underlying atomic dynamics associated with the multiple resonances in the semiclassical limit. Furthermore, we show that this interaction can be applied to generation of nonclassical fields with sub-Poisson photon statistics.

Spectral line-shape measurement of an extremely weak amplitude-fluctuating light source by photon-counting-based second-order correlation spectroscopy.

We demonstrate line-shape measurement of an extremely weak amplitude-fluctuating light source by using photon-counting-based second-order correlation spectroscopy combined with the heterodyne technique. The amplitude fluctuation of a finite bandwidth introduces a low-lying spectral structure in the line shape, and thus its effect can be isolated from that of the phase fluctuation. Our technique provides extreme sensitivity suited for single-atom-level applications.