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Colossal switchable photocurrents in topological Janus transition metal dichalcogenides
Nonlinear optical properties, such as bulk photovoltaic effects, possess great potential in energy harvesting, photodetection, rectification, etc. To enable efficient light–current conversion, materials with strong photo-responsivity are highly desirable. In this work, we predict that monolayer Janus transition metal dichalcogenides (JTMDs) in the 1T' phase possess colossal nonlinear photoconductivity owing to their topological band mixing, strong inversion symmetry breaking, and small electronic bandgap. 1T'JTMDs have inverted bandgaps on the order of 10 meV and are exceptionally responsive to light in the terahertz (THz) range. By first-principles calculations, we reveal that 1T' JTMDs possess shift current (SC) conductivity as large as 2300 nm μA V -2 , equivalent to a photo-responsivity of 2800 mA/W. The circular current (CC) conductivity of 1T' JTMDs is as large as ~10 4 nm μA V -2 . These remarkable photo-responsivities indicate that the 1T' JTMDs can serve as efficient photodetectors in the THz range. We also find that external stimuli such as the in-plane strain and out-of-plane electric field can induce topological phase transitions in 1T' JTMDs and that the SC can abruptly flip their directions. The abrupt change of the nonlinear photocurrent can be used to characterize the topological transition and has potential applications in 2D optomechanics and nonlinear optoelectronics.
Energy performance analysis of smart wall system with switchable insulation and thermal storage capacity
The ever-increasing global energy demand and the issues caused by population growth and unsustainable energy resource usages have several environmental and economic impacts. The on-demand capability of dynamic wall systems with switchable insulation systems can contribute toward energy efficiency and reduced electric cost using "building-as-a-battery." In this paper, the performance of an exterior envelope system that employs a switchable insulation system is investigated. A COMSOL simulation was used to study the envelope performance under three switchable insulation locations in the wall system. The on and off switching cycle included insulating or conducting the exterior, interior, or both sides of the mass wall system. To validate the simulation work, an experimental test was conducted in climate chamber on a 4 × 8 in. wall system with identical wall components used in the COMSOL simulation. Results show a good agreement between the experiment and simulation results. The wall system with switchable insulation placed on the exterior side provided the highest interior inward heat flux when compared with the interior or split insulation. Also, an exterior switchable insulation system in addition to a thermal mass maintained a positive heat flow for more hours when the outdoor temperature was lower than the interior temperature.
Spin switchable optical phenomena in Rashba band structures through intersystem crossing in momentum space in solution-processing 2D-superlattice perovskite film
Spin-switchable phenomena are a critical element for the development of spintronic and chiroptic devices. Herein we combine a 2D-superlattice perovskite (4,4-DFPD2PbI4) film with a ferromagnetic cobalt (Co) layer to form a multiferroic perovskite/Co interface, and demonstrate spin-switchable circularly polarized luminescence (CPL) between right-handed σ+ and left-handed σ− polarizations. When the ferromagnetic spins of Co at the Co/perovskite interface are altered between positive and negative magnetic field directions, the CPL from the 2D-superlattice perovskite switches from σ+ to σ− polarization. The magnetic field effects present a unique method to confirm that CPL is generated by the circular-orbital momentum of light-emitting excitons within Rashba band structures, eliminating artifacts involving structural birefringence. Our polarized neutron reflectometry measurements confirm a super long-range spin-orbit interaction occurring in the 2D-superlattice perovskite films. The temperature dependence of spin-switchable phenomenon indicates an extraordinarily long orbital polarization lifetime, reaching microseconds at room temperature and milliseconds at 5 K.
A chiral switchable photovoltaic ferroelectric 1D perovskite
Spin and valley degrees of freedom in materials without inversion symmetry promise previously unknown device functionalities, such as spin-valleytronics. Control of material symmetry with electric fields (ferroelectricity), while breaking additional symmetries, including mirror symmetry, could yield phenomena where chirality, spin, valley, and crystal potential are strongly coupled. Here we report the synthesis of a halide perovskite semiconductor that is simultaneously photoferroelectricity switchable and chiral. Spectroscopic and structural analysis, and first-principles calculations, determine the material to be a previously unknown low-dimensional hybrid perovskite (R)-(-)-1-cyclohexylethylammonium/(S)-(+)-1 cyclohexylethylammonium) PbI 3 . Optical and electrical measurements characterize its semiconducting, ferroelectric, switchable pyroelectricity and switchable photoferroelectric properties. Temperature dependent structural, dielectric and transport measurements reveal a ferroelectric-paraelectric phase transition. Circular dichroism spectroscopy confirms its chirality. The development of a material with such a combination of these properties will facilitate the exploration of phenomena such as electric field and chiral enantiomer–dependent Rashba-Dresselhaus splitting and circular photogalvanic effects
Electrically switchable metallic polymer metasurface device with gel polymer electrolyte
Abstract We present an electrically switchable, compact metasurface device based on the metallic polymer PEDOT:PSS in combination with a gel polymer electrolyte. Applying square-wave voltages, we can reversibly switch the PEDOT:PSS from dielectric to metallic. Using this concept, we demonstrate a compact, standalone, and CMOS compatible metadevice. It allows for electrically controlled ON and OFF switching of plasmonic resonances in the 2–3 µm wavelength range, as well as electrically controlled beam switching at angles up to 10°. Furthermore, switching frequencies of up to 10 Hz, with oxidation times as fast as 42 ms and reduction times of 57 ms, are demonstrated. Our work provides the basis towards solid state switchable metasurfaces, ultimately leading to submicrometer-pixel spatial light modulators and hence switchable holographic devices.
Methods and systems for the electrochemical reduction of carbon dioxide using switchable polarity materials
A method of electrochemically reducing CO2 comprises introducing a first feed stream comprising H2O to a positive electrode of an electrolysis cell comprising the positive electrode, a negative electrode, and a proton conducting membrane. A second feed stream comprising a solvent and a non polar form of a switchable polarity material is directed into a CO2 capture apparatus. A third feed stream comprising CO2 is directed into the CO2 capture apparatus to interact with the second feed stream and form a first product stream comprising the solvent and a polar form of the switchable polarity material. The first product stream is introduced to the negative electrode. A potential difference is applied between the positive electrode and the negative electrode to convert the polar form of the switchable polarity material into CO2 and the non-polar form and to form products from the CO2 and the solvent. A CO2 treatment system is also described.
Techno-Economic Analysis of Dynamic Building Envelopes Comprising Phase Change Materials and Switchable Insulations: Preprint
Integrating phase change materials (PCMs) in building envelopes is a recognized technique to reduce the space heating/cooling loads and provide load shedding and shifting capacity. However, PCM benefits have been found to reduce dramatically with increase in the insulation requirements. Dynamic building envelopes that can alter their thermal resistance based on the indoor and outdoor conditions can effectively harness free ambient heating/cooling, thereby greatly enhancing the benefits of the PCM-integrated envelope in managing thermal loads. In this study, we examine various combinations of PCMs and switchable insulations and compare their combined impact on heat flow through the building envelope. Using numerical analysis, we investigate the PCM- and switchable insulation-integrated building walls, calculate the potential energy saving benefits compared to the conventional static walls, and finally perform technoeconomic analysis to estimate the acceptable cost of the technology under various payback period scenarios.
Techno-Economic Analysis of Dynamic Building Envelopes Comprising Phase Change Materials and Switchable Insulations
Integrating phase change materials (PCMs) in building envelopes is a recognized technique to reduce the space heating/cooling loads and provide load shedding and shifting capacity. However, PCM benefits have been found to reduce dramatically with increase in the insulation requirements. Dynamic building envelopes that can alter their thermal resistance based on the indoor and outdoor conditions can effectively harness free ambient heating/cooling, thereby greatly enhancing the benefits of the PCM-integrated envelope in managing thermal loads. In this study, we examine various combinations of PCMs and switchable insulations and compare their combined impact on heat flow through the building envelope. Using numerical analysis, we investigate the PCM- and switchable insulation-integrated building walls, calculate the potential energy saving benefits compared to the conventional static walls, and finally perform techno-economic analysis to estimate the acceptable cost of the technology under various payback period scenarios.
Magnetic‐Field‐Switchable Laser via Optical Pumping of Rubrene
Abstract Volumetric optical imaging of magnetic fields is challenging with existing magneto‐optical materials, motivating the search for dyes with strong magnetic field interactions, distinct emission spectra, and an ability to withstand high photon flux and incorporation within samples. Here, the magnetic field effect on singlet‐exciton fission is exploited to demonstrate spatial imaging of magnetic fields in a thin film of rubrene. Doping rubrene with the high‐quantum yield dye dibenzotetraphenylperiflanthene (DBP) is shown to enable optically pumped, slab waveguide lasing. This laser is magnetic‐field‐switchable: when operated just below the lasing threshold, application of a 0.4 T magnetic field switches the device between nonlasing and lasing modes, accompanied by an intensity modulation of +360%. This is thought to be the first demonstration of a magnetically switchable laser, as well as the largest magnetically induced change in emission brightness in a singlet‐fission material to date. These results demonstrate that singlet‐fission materials are promising materials for magnetic sensing applications and could inspire a new class of magneto‐optical modulators.
Polarization-Insensitive Medium-Switchable Holographic Metasurfaces
The adoption of metasurfaces has led to revolutionary advances in holography due to improved compactness, integrability, and performance. Switchable meta-holograms projecting different replay field images in a controllable manner are highly desirable. Still, existing technologies generally rely on the use of polarized light and additional optics to facilitate switching. Consequently, the potential benefits afforded through the use of metasurfaces are limited both by the system complexity and a fixed relationship between the optical input and output. In this manuscript, we demonstrate polarization-insensitive metasurfaces encoding arbitrary and independent holograms, which can be switched between by changing the refractive index of the infiltration medium while maintaining identical illumination conditions. Finally, by sidestepping the requirements for high-performance light sources, switching optics, or delicate alignment, this approach points toward ultracompact and cost-effective switchable meta-holograms for various practical applications, such as holographic image projection, eye-perceptible sensors, optical information storage, processing, and security.
Photocatalytic Methanol Dehydrogenation with Switchable Selectivity
Switchable selectivity achieved by altering reaction conditions within the same photocatalytic system offers great advantages for sustainable chemical transformations and renewable energy conversion. In this study, we investigate an efficient photocatalytic methanol dehydrogenation with controlled selectivity by varying the concentration of nickel cocatalyst, using zinc indium sulfide nanocrystals as a semiconductor photocatalyst, which enables the production of either formaldehyde or ethylene glycol with high selectivity. Control experiments revealed that formaldehyde is initially generated and can either serve as a terminal product or intermediate in producing ethylene glycol, depending on the nickel concentration in the solution. Mechanistic studies suggest a unique role of ionic nickel as an additional photoelectron competitor that can significantly influence selectivity, alongside its well-established function as a hydrogen evolution reaction cocatalyst under photocatalytic conditions. The demonstrated switchable selectivity provides a new tool for producing diverse products from methanol, while advancing the understanding of cocatalyst behavior for versatile catalytic performance.
A Novel Design for Switchable Grid-Following and Grid-Forming Control
This paper presents the design of a novel grid- forming (GFM) control structure adapted from a typical grid- following (GFL) control structure with minimal edits, thereby enabling a switchable control structure for voltage sourced converters (VSCs) to operate in either GFL or GFM mode by simply switching a flag manually. The VSC is shown to be able to operate in the GFL control mode synchronizing to the main grid through a phase-locked-loop (PLL) and operate as a GFM controller with power-based synchronization for both grid-connected and islanded conditions. To guarantee smooth operation, the control schemes and the mode switching logic have been carefully designed and examined via a series of experiments. Here, the experiment results show that the switchable control structure can fulfill the desired control and operation functions and enable smooth transition between control modes.
Enhanced Laplace Pressures for Functional Surfaces: Wicking, Switchability, and Selectivity
Abstract Wetting functionalities of rough surfaces are largely determined by the Laplace pressure generated across liquid–gas interfaces formed within surface structures. Typically, rough wetting surfaces create negative Laplace pressures, enabling capillary wicking, while rough non‐wetting surfaces create positive Laplace pressures, exhibiting fluid repellency. Here, with microfabricated reentrant structures, it is shown that the same surface can exhibit either a negative or positive Laplace pressure, regardless of its intrinsic wettability. This material‐independent Laplace pressure duality enables or enhances a range of wetting functionalities including wicking, switchability, and selectivity. On the same surface, capillary rise, capillary dip, and the combination of the two which leads to further enhancement of the total sustainable capillary height and Laplace pressure, the driving force for wicking is demonstrated. Further, active switching of wetting states between the hemiwicking and the repellent Cassie state on reentrant structures is shown. Moreover, with a water‐hexane mixture system, selective wetting of reentrant structures are demonstrated, that is, water can be selectively wicked or repelled in the presence of hexane, and vice versa. These functionalities are achieved, which would typically require complex chemical coatings, solely using surface structures, thus largely expanding the design space for a wide range of thermofluidic applications.
A structural underpinning of the lower critical solution temperature (LCST) behavior behind temperature-switchable liquids
In this work, we use state-of-the-art X-ray scattering and molecular dynamics to analyze amine-water mixtures that show the unusual lower critical solution temperature (LCST) behavior. The goal is to provide direct experimental evidence for the entropy-lowering molecular cluster formation hypothesized as necessary for LCST behavior. Differential wide-angle X-ray scattering and pair distribution analysis and small-angle X-ray scattering measurements were combined with molecular modeling and liquid-liquid equilibrium measurements, revealing direct experimental evidence for the hypothesis. However, the response of the amine phase to accommodating water is even more subtle than the simple hypothesis suggests, with the formation of robust nanoscale reverse micelles. The techniques developed in this paper can be expected to yield insights in the use of temperature-switchable liquids in solvent extraction and other separations, and the stabilization of organelles in living cells that do not have physical membranes but do require compositional gradients to operate.
Light-induced switchable adsorption in azobenzene- and stilbene-based porous materials
Despite the long history of porous materials as adsorbates, fundamental limitations remain regarding the efficient capture and release of the gas molecules, with the working capacity of the material often overlooked. In microporous materials, the uptake is dominated by low-pressure adsorption, with much of this being at pressures below the minimum working threshold for many gas utilization processes. Thus, research has focused on several advances in porous materials, including photoresponsive organic units for light-induced switchable adsorption. This process utilizes light to trigger structural or electronic changes, alter the gas uptake, and change the working capacity. Additionally, while a relatively recent development, there is a significant body of research regarding the use of light to control gas storage performance.
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.
High-Endurance Magneto-Electronic Switchable Molecular Electronic Crystal
Electrically switchable magnetic and electronic properties are promising for quantum sensing and information technology. Here, we report an electrically driven magnetic and electronic phase transition in molecular electronic crystal, potassium-7,7,8,8-tetracyanoquinodimethan, with the magneto-electric switching over 105 cycles at room temperature. Electron spin resonance study reveals the cooperative transition between spin and charge degrees of freedom. In addition, the mechanistic spectroscopy studies suggest the charges in an inhomogeneous conductor–insulator mixed state. Furthermore, the findings shown here suggest electrically controlled ordering in strongly correlated molecular crystal leads to dynamic magneto-electric switching, paving the way for developing molecular-based memory and switching devices.