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At least 595 records · Page 33

Colloidal quantum dot lasers

We report semiconductor nanocrystals represent a promising class of solution-processable optical-gain media that can be manipulated via inexpensive, easily scalable colloidal techniques. Due to their extremely small sizes (typically <10 nm), their properties can be directly controlled via effects of quantum confinement; therefore, they are often termed colloidal quantum dots (CQDs). In addition to size-tunable emission wavelengths, CQDs offer other benefits for lasing applications, including low optical-gain thresholds and high temperature stability of lasing characteristics. Recent progress in understanding and practical control of processes impeding light amplification in CQDs has resulted in several breakthroughs, including the demonstration of optically pumped continuous-wave lasing, the realization of optical gain with direct current electrical injection and the development of dual-function electroluminescent devices that also operate as optically pumped lasers. The purpose of this Review is to assess the status of the field of CQD lasing and discuss the existing challenges and opportunities. A particular focus is on approaches for suppressing nonradiative Auger recombination, novel optical-gain concepts enabled by strong exciton-exciton interactions and controlled CQD charging, effects of nanocrystal form factors on light amplification and practical architectures for realizing electrically pumped CQD lasers. This overview suggests that the accumulated knowledge, along with the approaches developed for manipulating the optical-gain properties of colloidal nanostructures, perfectly position the CQD field for successfully addressing a long-standing challenge: the realization of CQD-based laser diodes. Colloidal quantum dots are promising materials for realizing versatile, wavelength-tunable, solution-processed lasers. This Review surveys recent advances in colloidal quantum dot lasing, provides an in-depth analysis of outstanding challenges and discusses a path forward to implementing technologically viable lasing devices.

36 MATERIALS SCIENCE↗

MoO3 as combined hole injection layer and tapered spacer in combinatorial multicolor microcavity organic light emitting diodes

Multicolor microcavity ({mu}C) organic light-emitting diode (OLED) arrays were fabricated simply by controlling the hole injection and spacer MoO{sub 3} layer thickness. The normal emission was tunable from {approx}490 to 640 nm and can be further expanded. A compact, integrated spectrometer with two-dimensional combinatorial arrays of {mu}C OLEDs was realized. The MoO{sub 3} yields more efficient and stable devices, revealing a new breakdown mechanism. The pixel current density reaches {approx}4 A/cm{sup 2} and a maximal normal brightness {approx}140 000 Cd/m{sup 2}, which improves photoluminescence-based sensing and absorption measurements.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Efficient Trainability of Linear Optical Modules in Quantum Optical Neural Networks

The existence of “barren plateau landscapes” for generic discrete-variable quantum neural networks, which obstructs efficient gradient-based optimization of cost functions defined by global measurements, would be surprising in the case of generic linear optical modules in quantum optical neural networks due to the tunability of the intensity of continuous variable states and the relevant unitary group having exponentially smaller dimension. We demonstrate that coherent light in m modes can be generically compiled efficiently if the total intensity scales sublinearly with m, and extend this result to cost functions based on homodyne, heterodyne, or photon detection measurement statistics, and to noisy cost functions in the presence of attenuation. Here, we further demonstrate efficient trainability of m mode linear optical quantum circuits for variational mean field energy estimation of positive quadratic Hamiltonians for input states that do not have energy exponentially vanishing with m.

47 OTHER INSTRUMENTATION↗

A historical overview of the activation and porosity of metal–organic frameworks

Since the first reports of metal–organic frameworks (MOFs), this unique class of crystalline, porous materials has garnered increasing attention in a wide variety of applications such as gas storage and separation, catalysis, enzyme immobilization, drug delivery, water capture, and sensing. A fundamental feature of MOFs is their porosity which provides space on the micro- and meso-scale for confining and exposing their functionalities. Therefore, designing MOFs with high porosity and developing suitable activation methods for preserving and accessing their pore space have been a common theme in MOF research. Reticular chemistry allows for the facile design of MOFs from highly tunable metal nodes and organic linkers in order to realize different pore structures, topologies, and functionalities. With the hope of shedding light on future research endeavors in MOF porosity, it is worthwhile to examine the development of MOFs, with an emphasis on their porosity and how to properly access their pore space. In this review, we will provide an overview of the historic evolution of porosity and activation of MOFs, followed by a synopsis of the strategies to design and preserve permanent porosity in MOFs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Thermal tuning of infrared resonant absorbers based on hybrid gold-VO{sub 2} nanostructures

Resonant absorbers based on plasmonic materials, metamaterials, and thin films enable spectrally selective absorption filters, where absorption is maximized at the resonance wavelength. By controlling the geometrical parameters of nano/microstructures and materials' refractive indices, resonant absorbers are designed to operate at wide range of wavelengths for applications including absorption filters, thermal emitters, thermophotovoltaic devices, and sensors. However, once resonant absorbers are fabricated, it is rather challenging to control and tune the spectral absorption response. Here, we propose and demonstrate thermally tunable infrared resonant absorbers using hybrid gold-vanadium dioxide (VO{sub 2}) nanostructure arrays. Absorption intensity is tuned from 90% to 20% and 96% to 32% using hybrid gold-VO{sub 2} nanowire and nanodisc arrays, respectively, by heating up the absorbers above the phase transition temperature of VO{sub 2} (68 °C). Phase change materials such as VO{sub 2} deliver useful means of altering optical properties as a function of temperature. Absorbers with tunable spectral response can find applications in sensor and detector applications, in which external stimulus such as heat, electrical signal, or light results in a change in the absorption spectrum and intensity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Mode coupling in hybrid square-rectangular lasers for single mode operation

Mode coupling between a square microcavity and a Fabry-Pérot (FP) cavity is proposed and demonstrated for realizing single mode lasers. The modulations of the mode Q factor as simulation results are observed and single mode operation is obtained with a side mode suppression ratio of 46 dB and a single mode fiber coupling loss of 3.2 dB for an AlGaInAs/InP hybrid laser as a 300-μm-length and 1.5-μm-wide FP cavity connected to a vertex of a 10-μm-side square microcavity. Furthermore, tunable single mode operation is demonstrated with a continuous wavelength tuning range over 10 nm. The simple hybrid structure may shed light on practical applications of whispering-gallery mode microcavities in large-scale photonic integrated circuits and optical communication and interconnection.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Coupling between gap plasmon polariton and magnetic polariton in a metallic-dielectric multilayer structure

The excitation of plasmons in a metallic nanostructure represents a feasible and practical approach for manipulating the propagation and absorption of light at the subwavelength scale. Of particular interest is the coupling between plasmons, which can be used to facilitate the spectral tunability and tailor the optical response of the structure. In this paper, we study the coupling between two highly localized plasmonic modes: gap plasmon polariton mode and magnetic polariton mode, supported by a metallic-dielectric multilayer structure. The strong coupling gives rise to the formation of hybrid plasmon modes and large mode splitting. These hybrid modes result in unique spectral-directional absorption characteristics in the structure. The findings hold promise in applications such as photonic and energy conversion systems as well as the design of plasmonic nanodevices.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Validating Laser-Induced Birefringence Theory with Plasma Interferometry

Intense laser beams crossing paths in plasma is theorized to induce birefringence in the medium, resulting from density and refractive index modulations that affect the polarization of incoming light. The goal of the associated experiment, conducted on Janus at Lawrence Livermore’s Jupiter Laser Facility, was to create a tunable laser-plasma waveplate to verify the relationship between dephasing angle and beam intensity, plasma density, plasma temperature, and interaction length. Interferometry analysis of the plasma channel was performed to obtain a density map and to constrain temperature measured from Thomson scattering. Various analysis techniques, including Fast Fourier transform (FFT) and two variations of fringe-counting, were tried because interferograms captured in this experiment contained unusual features such as fringe discontinuity at channel edges, saddle points, and islands. The chosen method is flexible, semi-automated, and uses a fringe tracking algorithm on a reduced image of pre-traced synthetic fringes. Ultimately, a maximum dephasing angle of 49.6° was achieved using a 1200 μm interaction length, and the experimental results appear to agree with predictions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Evaluating Polymer Properties with Different Additives for Carbon Capture and Other Applications

Anthropogenic climate change is one of this generation’s most pressing concerns, with the potential to completely alter the delicate balance we’ve struck with nature. Already, global temperatures have risen 1.29°C, leading to disrupted weather systems, extinctions, increased risks of wildfires, and sea level rise, to name a few effects. Carbon dioxide emission from the combustion of fossil fuels and other industrial activity is a large driver of this phenomenon, as it absorbs heat before it can be radiated away from Earth, trapping it. Carbon dioxide has reached unprecedented levels in our atmosphere, showing a 50% increase from preindustrial averages to a whopping 430 ppm. Thus, reducing the amount of carbon dioxide via carbon capture technology is an important endeavor that serves to benefit everyone. The Microencapsulated CO 2 Sorbent (MECS) team at Lawrence Livermore National Laboratory (LLNL) has turned to microencapsulation to approach this endeavor. Microcapsules provide an attractive approach to carbon capture, combining large surface areas for more efficient mass transfer, regenerative abilities, reduced solvent loss, and improved handling. Additionally, while existing carbon capture technology relies on industrial plants, capsules could present a modular approach to carbon capture, reducing the need for extensive physical infrastructure. The MECS team’s design consists of a polymer membrane that contains a liquid carbon sequestering sorbent, aqueous sodium carbonate. The carbon capturing reaction occurs in three distinct steps, the first of which is the dissolution of carbon dioxide into the sorbent solution and its conversion into carbonic acid (H 2 CO 3 ), shown in equations 1 and 2 respectively. Because this step hinges upon the ability of carbon dioxide to reach the solution inside the capsule, it is necessary that the microcapsule shell is permeable to carbon dioxide gas. The MECS team produces these microcapsules using the in-air droplet encapsulation apparatus (IDEA) shown in figure 1, which can produce uniform micron-scale droplets at speeds much faster than traditional single-dispersal microfluidic-based techniques. The IDEA Is 100 times faster than these current techniques and can reach up to 1000 times their speed when incorporating a multi-nozzle design. Additionally, because droplets are produced in-air via vibration, IDEA can decrease post-processing times and material waste by 99% and can fabricate microgels that are 10 to 100 times more viscous than can be produced via traditional microfluidics. While this design represents a breakthrough in the throughput, efficiency, and tunability of microcapsule production, it imposes a major constraint on the microcapsule curing process. Because microcapsule shells are crosslinked with UV light while falling 30 cm through the air, this gives them a reaction window of approximately 0.2 seconds. Thus, the system and shell formulations must be optimized such that the shells can be fully crosslinked within this very narrow window, prompting investigations into curing behavior.

36 MATERIALS SCIENCE↗

Broadband optical absorption by tunable Mie resonances in silicon nanocone arrays

Nanostructure arrays such as nanowire, nanopillar, and nanocone arrays have been proposed to be promising antireflection structures for photovoltaic applications due to their great light trapping ability. In this paper, the optical properties of Si nanopillar and nanocone arrays in visible and infrared region were studied by both theoretical calculations and experiments. The results show that the Mie resonance can be continuously tuned across a wide range of wavelength by varying the diameter of the nanopillars. However, Si nanopillar array with uniform diameter exhibits only discrete resonance mode, thus can't achieve a high broadband absorption. On the other hand, the Mie resonance wavelength in a Si nanocone array can vary continuously as the diameters of the cross sections increase from the apex to the base. Therefore Si nanocone arrays can strongly interact with the incident light in the broadband spectrum and the absorbance by Si nanocone arrays is higher than 95% over the wavelength from 300 to 2000 nm. In addition to the Mie resonance, the broadband optical absorption of Si nanocone arrays is also affected by Wood-Rayleigh anomaly effect and metal impurities introduced in the fabrication process.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Tunable Dual Semiconductor Laser

Parallel lasers interact in shared space to alter output wavelength. New device consists of two stripe lasers in aluminum gallium arsenide chip. Parallel stripes close enough so light from lower laser coupled into upper laser and vice versa. Lasers operated by low-duty-cycle current pulses. Lasing threshold of each about 100 mA. Currents controlled independently. Useful in optical communications systems employing wavelength-division multiplexing.

Mukai, Seiji↗

Tunable plasmonic color device and method of making the same

A plasmonic system is disclosed. The system includes at least one polarizer that is configured to provide at least one linearly polarized broadband light beam, an anisotropic plasmonic metasurface (APM) assembly having a plurality of nanoantennae each having a predetermined orientation with respect to a global axis representing encoded digital data, the APM assembly configured to receive the at least one linearly polarized broadband light beam and by applying localized surface plasmon resonance reflect light with selectable wavelengths associated with the predetermined orientations of the nanoantennae, and at least one analyzer that is configured to receive the reflected light with selectable wavelength, wherein the relative angles between each of the at least one analyzers and each of the at least one polarizers are selectable with respect to the global axis, thereby allowing decoding of the digital data.

Kildishev, Alexander V.↗

Ultralow-power all-optical tunable dual Fano resonances in nonlinear metamaterials

Dual Fano resonances are realized in a nonlinear photonic metamaterial consisting of periodic arrays of asymmetrical meta-molecules etched in a gold film coated with azobenzene polymer layer made of poly[(methyl methacrylate)-co-(disperse red 13 acrylate)]. Enormously enhanced photoisomerization associated with resonant excitation brings about a large refractive index variation in the azobenzene polymer. Under excitation of a weak pump light as low as 0.61 kW/cm{sup 2}, a large shift of 50 nm in the Fano resonance wavelength is obtained. Compared with previous reports, the threshold pump intensity is reduced by seven orders of magnitude while a large tunability is maintained simultaneously.

36 MATERIALS SCIENCE↗

Influence of Metal Identity on Light-Induced Switchable Adsorption in Azobenzene-Based Metal–Organic Frameworks

Energy-efficient capture and release of small gas molecules, particularly carbon dioxide (CO 2 ) and methane (CH 4 ), are of significant interest in academia and industry. Porous materials such as metal–organic frameworks (MOFs) have been extensively studied, as their ultrahigh porosities and tunability enable significant amounts of gas to be adsorbed while also allowing specific applications to be targeted. However, because of the microporous nature of MOFs, the gas adsorption performance is dominated by high uptake capacity at low pressures, limiting their application. Hence, methods involving stimuli-responsive materials, particularly light-induced switchable adsorption (LISA), offer a unique alternative to thermal methods. Here, we report the mechanism of a well-known LISA system, the azobenzene-based material PCN-250, for CO 2 and CH 4 adsorption. There is a noticeable difference in the LISA effect dependent on the metal cluster involved, with the most significant being PCN-250-Al, where the adsorption can change by 83.1% CH 4 and 56.1% CO 2 at 298 K and 1 bar and inducing volumetric storage changes of 36.2 and 33.9 cm 3 /cm 3 at 298 K between 5 and 85 bar (CH 4 ) and 2 and 9 bar (CO 2 ), respectively. Using UV light in both single-crystal X-ray diffraction and gas adsorption testing, we show that upon photoirradiation, the framework undergoes a “localized heating” phenomenon comparable to an increase of 130 K for PCN-250-Fe and improves the working capacity. Furthermore, this process functions because of the constrained nature of the ligand, preventing the typical trans-to-cis isomerization observed in free azobenzene. In addition, we observed that the degree of localized heating is highly dependent on the metal cluster involved, with the series of isostructural PCN-250 systems showing variable performance based upon the degree of interaction between the ligand and the metal center.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Doping-tunable thermal emission from plasmon polaritons in semiconductor epsilon-near-zero thin films

We utilize the unique dispersion properties of leaky plasmon polaritons in epsilon-near-zero (ENZ) thin films to demonstrate thermal radiation control. Owing to its highly flat dispersion above the light line, a thermally excited leaky wave at the ENZ frequency out-couples into free space without any scattering structures, resulting in a narrowband, wide-angle, p-polarized thermal emission spectrum. We demonstrate this idea by measuring angle- and polarization-resolved thermal emission spectra from a single layer of unpatterned, doped semiconductors with deep-subwavelength film thickness (d/λ{sub 0} ∼ 6×10{sup −3}, where d is the film thickness and λ{sub 0} is the free space wavelength). We show that this semiconductor ENZ film effectively works as a leaky wave thermal radiation antenna, which generates far-field radiation from a thermally excited mode. The use of semiconductors makes the radiation frequency highly tunable by controlling doping densities and also facilitates device integration with other components. Therefore, this leaky plasmon polariton emission from semiconductor ENZ films provides an avenue for on-chip control of thermal radiation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Tunable VO2/Au hyperbolic metamaterial

Vanadium dioxide (VO2) is known to have a semiconductor-to-metal phase transition at ∼68 °C. Therefore, it can be used as a tunable component of an active metamaterial. The lamellar metamaterial studied in this work is composed of subwavelength VO2 and Au layers and is designed to undergo a temperature controlled transition from the optical hyperbolic phase to the metallic phase. VO2 films and VO2/Au lamellar metamaterial stacks have been fabricated and studied in electrical conductivity and optical (transmission and reflection) experiments. The observed temperature-dependent changes in the reflection and transmission spectra of the metamaterials and VO2 thin films are in a good qualitative agreement with theoretical predictions. The demonstrated optical hyperbolic-to-metallic phase transition is a unique physical phenomenon with the potential to enable advanced control of light-matter interactions.

Prayakarao, S. (ORCID:000000018108360X)↗

A series of four-coordinate heteroleptic copper(I) complexes with diimine and β-diketiminate ligands

In this paper, a series of heteroleptic bis-chelate copper(I) complexes of the general formula Cu(N^N)(NacNac R ), where N^N is the diimine ligand and NacNac R is the β-diketiminate ligand are introduced. The complexes are easily prepared by reacting NacNac ligands with CuO t Bu in the presence of diimine ligands. The molecular structures of all complexes are characterized by NMR spectroscopy and X-ray crystallography. The studies of cyclic voltammetry and UV–vis absorption spectra show that the HOMO and the LUMO energy level can be tailored by changing the substitution pattern of each ligand. The oxidation potential is dependent on the NacNac ligand, and the reduction potential shows the dependence on the diimine ligand. In conclusion, tunable redox potentials and a wide range of visible absorption can make these copper(I) complexes promising candidates for applications in solar light harvesting.

14 SOLAR ENERGY↗

A Visual Understanding of Circular Dichroism Spectroscopy

Mapping chemical and structural properties to electronic and magnetic responses is critical to many applications such as quantum information science, where the precise storage and transmission of unique information is paramount. Specifically, constructing molecules and materials that provide strong polarized responses at tunable frequencies and with large anisotropies is key to optical processing of quantum information. Chiral molecules provide chiroptical response to circularly polarized light, making them attractive for quantum information science and other applications related to sensing, polarized photodetectors, and spintronics. Predicting a molecular design, a priori, with large anisotropies to circularly polarized light is challenging due to the complex interplay between electric and magnetic components of the optical response. In this work, we explore a visual representation of the electronic chiroptical response by decomposing the rotary strength into its constituent components. Here, we make use of the intuitive electronic oscillator framework to develop classical intuition regarding the rotary strength and its constituents. We explore three model chemical systems that exhibit local and global chirality. Our analysis reveals that local chirality necessarily exhibits competition between the local chiral center and chirality induced in other fragments of the molecule, resulting in both unexpected nonmonotonic trends and sign flips in chemically adjacent geometries. Furthermore, we can visually distinguish between local and global chirality via examination of the transition chiral tensor. Interestingly, we make strong connections to ferromagnetic and antiferromagnetic spin systems in that chiroptically inactive transitions exhibit antiferromagnetic-like alternating orbital patterns while active transitions show domain formation in an ferromagnetic-like alignment that produces a net chiroptical response.

36 MATERIALS SCIENCE↗