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1.
Nat Phys ; 20(9): 1441-1447, 2024.
Artículo en Inglés | MEDLINE | ID: mdl-39282552

RESUMEN

Light and sound waves can move objects through the transfer of linear or angular momentum, which has led to the development of optical and acoustic tweezers, with applications ranging from biomedical engineering to quantum optics. Although impressive manipulation results have been achieved, the stringent requirement for a highly controlled, low-reverberant and static environment still hinders the applicability of these techniques in many scenarios. Here we overcome this challenge and demonstrate the manipulation of objects in disordered and dynamic media by optimally tailoring the momentum of sound waves iteratively in the far field. The method does not require information about the object's physical properties or the spatial structure of the surrounding medium but relies only on a real-time scattering matrix measurement and a positional guide-star. Our experiment demonstrates the possibility of optimally moving and rotating objects to extend the reach of wave-based object manipulation to complex and dynamic scattering media. We envision new opportunities for biomedical applications, sensing and manufacturing.

2.
Sci Technol Adv Mater ; 25(1): 2312148, 2024.
Artículo en Inglés | MEDLINE | ID: mdl-38361531

RESUMEN

Already in 2012, Blom et al. reported (Nature Materials 2012, 11, 882) in semiconducting polymers on a general electron-trap density of ≈3 × 1017 cm-3, centered at an energy of ≈3.6 eV below vacuum. It was suggested that traps have an extrinsic origin, with the water-oxygen complex [2(H2O)-O2] as a possible candidate, based on its electron affinity. However, further evidence is lacking and the origin of universal electron traps remained elusive. Here, in polymer diodes, the temperature-dependence of reversible electron traps is investigated that develop under bias stress slowly over minutes to a density of 2 × 1017 cm-3, centered at an energy of 3.6 eV below vacuum. The trap build-up dynamics follows a 3rd-order kinetics, in line with that traps form via an encounter between three diffusing precursor particles. The accordance between universal and slowly evolving traps suggests that general electron traps in semiconducting polymers form via a triple-encounter process between oxygen and water molecules that form the suggested [2(H2O)-O2] complex as the trap origin.


Formation of universal electron traps in polymer light-emitting diodes is a dynamic process that occurs via a slow triple-encounter between trap precursor species, with the water-oxygen [2(H2O)-O2] complex as a likely candidate.

3.
Adv Mater ; 36(16): e2311892, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38214416

RESUMEN

Organic light-emitting diodes (OLEDs) employing a single active layer potentially offer a number of benefits compared to multilayer devices; reduced number of materials and deposition steps, potential for solution processing, and reduced operating voltage due to the absence of heterojunctions. However, for single-layer OLEDs to achieve efficiencies approaching those of multilayer devices, balanced charge transport is a prerequisite. This requirement excludes many efficient emitters based on thermally activated delayed fluorescence (TADF) that exhibit electron trapping, such as the green-emitting bis(4-(9,9-dimethylacridin-10(9H)-yl)phenyl)methanone (DMAC-BP). By employing a recently developed trap-free large band gap material as a host for DMAC-BP, nearly balanced charge transport is achieved. The single-layer OLED reaches an external quantum efficiency (EQE) of 19.6%, which is comparable to the reported EQEs of 18.9-21% for multilayer devices, but achieves a record power efficiency for DMAC-BP OLEDs of 82 lm W-1, clearly surpassing the reported multilayer power efficiencies of 52.9-59 lm W-1. In addition, the operational stability is greatly improved compared to multilayer devices and the use of conventional host materials in combination with DMAC-BP as an emitter. Next to the obvious reduction in production costs, single-layer OLEDs therefore also offer the advantage of reduced energy consumption and enhanced stability.

4.
Adv Sci (Weinh) ; 10(3): e2205342, 2023 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-36453563

RESUMEN

Organic-inorganic perovskite solar cells (PSCs) have achieved great attention due to their expressive power conversion efficiency (PCE) up to 25.7%. To improve the photovoltaic performance of PSCs, interface engineering between the perovskite and hole transport layer (HTL) is a widely used strategy. Following this concept, benzyl trimethyl ammonium chlorides (BTACls) are used to modify the wet chemical processed perovskite film in this work. The BTACl-induced low dimensional perovskite is found to have a bilayer structure, which efficiently decreases the trap density and improves the energy level alignment at the perovskite/HTL interface. As a result, the BTACl-modified PSCs show an improved PCE compared to the control devices. From device modeling, the reduced charge carrier recombination and promoted charge carrier transfer at the perovskite/HTL interface are the cause of the open-circuit (Voc ) and fill factor (FF) improvement, respectively. This study gives a deep understanding for surface modification of perovskite films from a perspective of the morphology and the function of enhancing photovoltaic performance.

5.
Commun Phys ; 6(1): 93, 2023.
Artículo en Inglés | MEDLINE | ID: mdl-38665400

RESUMEN

Reciprocity guarantees that in most media, sound transmission is symmetric between two points of space when the location of the source and receiver are interchanged. This fundamental law can be broken in non-linear media, often at the cost of detrimental input power levels, large insertion losses, and ideally prepared single-frequency input signals. Thus, previous observations of non-reciprocal sound transmission have focused on pure tones, and cannot handle real sounds composed of various harmonics of a low-frequency fundamental note, as generated for example by musical instruments. Here, we extend the reach of non-reciprocal acoustics by achieving large, tunable, and timbre-preserved non-reciprocal transmission of sound notes composed of several harmonics, originating from musical instruments. This is achieved in a non-linear, actively reconfigurable, and non-Hermitian isolator that can handle arbitrarily low input power at any audible frequency, while providing isolation levels up to 30dB and a tunable level of non-reciprocal gain. Our findings may find applications in sound isolation, noise control, non-reciprocal and non-Hermitian metamaterials, and analog audio processing.

6.
Adv Mater ; 34(13): e2108887, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-34786784

RESUMEN

The various contributions to the external quantum efficiency (EQE) of polymer light-emitting diodes (PLEDs) are discussed. The EQE of an organic light-emitting diode is governed by a number of parameters, such as the electrical efficiency, the photoluminescence quantum yield (PLQY), the optical outcoupling efficiency and the spin statistics for singlet exciton generation. In the last decade, the electrical efficiency has been determined from a numerical PLED device model. More recently, an optical model to simulate the fraction of photons outcoupled to air for PLEDs with a broad recombination zone has been developed. Together with the directly measured PLQY, the EQE of a PLED can then be estimated. However, it has been observed that the measured EQEs of fluorescent PLEDs, including the model system super-yellow poly(p-phenylene vinylene) (SY-PPV) often exceed the expected values. To solve this discrepancy, it is demonstrate that the electrical PLED model has to be expanded by the inclusion of triplet-triplet annihilation (TTA), which is shown to be responsible for a substantial EQE enhancement. Experimentally, it is obtained that TTA contributes to a singlet-exciton generation efficiency of ≈40% in SY-PPV PLEDs, giving rise to an EQE of ≈4% instead of the expected value of 2.5%.

7.
Nano Lett ; 21(23): 10092-10098, 2021 Dec 08.
Artículo en Inglés | MEDLINE | ID: mdl-34797661

RESUMEN

A requirement for quantum information processors is the in situ tunability of the tunnel rates and the exchange interaction energy within the device. The large energy level separation for atom qubits in silicon is well suited for qubit operation but limits device tunability using in-plane gate architectures, requiring vertically separated top-gates to control tunnelling within the device. In this paper, we address control of the simplest tunnelling device in Si:P, the tunnel junction. Here we demonstrate that we can tune its conductance by using a vertically separated top-gate aligned with ±5 nm precision to the junction. We show that a monolithic 3D epitaxial top-gate increases the capacitive coupling by a factor of 3 compared to in-plane gates, resulting in a tunnel barrier height tunability of 0-186 meV. By combining multiple gated junctions in series we extend our monolithic 3D gating technology to implement nanoscale logic circuits including AND and OR gates.

8.
Environ Sci Pollut Res Int ; 28(20): 25382-25389, 2021 May.
Artículo en Inglés | MEDLINE | ID: mdl-33454826

RESUMEN

Organic-inorganic metal halide perovskite materials, i.e., ABX3 (A = methylammonium, B = Pb, X = Cl, Br, I) have been proved to be outstanding for solar energy conversion. They provide a solution to renewable energy problems with good efficiency and cost-effective technology. Here, we report the initial calculations done by solving Kohn-Sham equations by the use of density function theory. The electronic structural and band gap of CH3NH3PbI3 material are obtained by using different exchange-correlation potential (PBE, PBE-sol, GGA). Further, solar cell devices with CH3NH3PbI3 as absorption layer and CdS/TiO2/ZnTe as buffer layer have been modeled; device physics is discussed and performance of solar cell structure is analyzed in terms of short circuit current density, open circuit voltage, efficiency, fill factor, and quantum efficiency. The maximum efficiency of CH3NH3PbI3 solar cell is found to be 19.6% with TiO2 buffer layer, whereas efficiency with ZnTe buffer layer is also comparable which is 19.5%. Further the effect of layer thickness and temperature are analyzed for maximum efficiency.


Asunto(s)
Yoduros , Plomo , Compuestos de Calcio , Electrónica , Metilaminas , Óxidos , Titanio
9.
ACS Appl Mater Interfaces ; 12(43): 48845-48853, 2020 Oct 28.
Artículo en Inglés | MEDLINE | ID: mdl-33064440

RESUMEN

Perovskite light-emitting diodes have been gaining attention in recent years due to their high efficiencies. Despite of the recent progress made in device efficiency, the operation mechanisms of these devices are still not well understood, especially the effects of ion migration. In this work, the role of ion migration is investigated by measuring the transient electroluminescence and current responses, with both the current and efficiency showing a slow response in a time scale of tens of milliseconds. The results of the charge injection dynamics show that the slow response of the current is attributed to the migration and accumulation of halide ions at the anode interface, facilitating hole injection and leading to a strong charge imbalance. Further, the results of the charge recombination dynamics show that the slow response of the efficiency is attributed to enhanced charge injection facilitated by ion migration, which leads to an increased carrier density favoring bimolecular radiative recombination. Through a combined analysis of both charge injection and recombination dynamics, we finally present a comprehensive picture of the role of ion migration in device operation.

10.
Nano Lett ; 20(8): 5799-5806, 2020 Aug 12.
Artículo en Inglés | MEDLINE | ID: mdl-32634316

RESUMEN

Electron-transport-layer free perovskite solar cells (ETL-free PSCs) have attracted great attention due to their low cost and simple manufacturing process. However, an additional interface layer has to be introduced, and the currently achieved efficiency remains far from full-structure PSCs. Here, we report an in situ interface engineering strategy by the methylammonium acetate (MAAc) ionic liquid perovskite precursor. We found that a dipole layer was in situ constructed through the physical adsorption of the residual MAAc polar molecules on the indium tin oxide electrode, which is significantly different from the treatment by the interface layer in previous reports. This allows a decrease of the effective work function and enables in situ band bending in the perovskite semiconductor. The in situ band bending facilitates charge collection and hinders interfacial charge recombination, leading to ETL-free PSCs with a maximum power conversion efficiency of 21.08%, which is the highest report to date.

11.
Light Sci Appl ; 9: 120, 2020.
Artículo en Inglés | MEDLINE | ID: mdl-32695317

RESUMEN

The photothermoelectric (PTE) effect enables efficient harvesting of the energy of photogenerated hot carriers and is a promising choice for high-efficiency photoelectric energy conversion and photodetection. Recently, the PTE effect was reported in low-dimensional nanomaterials, suggesting the possibility of optimizing their energy conversion efficiency. Unfortunately, the PTE effect becomes extremely inefficient in low-dimensional nanomaterials, owing to intrinsic disadvantages, such as low optical absorption and immature fabrication methods. In this study, a giant PTE effect was observed in lightly doped p-type silicon nanoribbons caused by photogenerated hot carriers. The open-circuit photovoltage responsivity of the device was 3-4 orders of magnitude higher than those of previously reported PTE devices. The measured photovoltage responses fit very well with the proposed photothermoelectric multiphysics models. This research proposes an application of the PTE effect and a possible method for utilizing hot carriers in semiconductors to significantly improve their photoelectric conversion efficiency.

12.
Light Sci Appl ; 9: 54, 2020.
Artículo en Inglés | MEDLINE | ID: mdl-32284856

RESUMEN

Quasi-crystal distributed feedback lasers do not require any form of mirror cavity to amplify and extract radiation. Once implemented on the top surface of a semiconductor laser, a quasi-crystal pattern can be used to tune both the radiation feedback and the extraction of highly radiative and high-quality-factor optical modes that do not have a defined symmetric or anti-symmetric nature. Therefore, this methodology offers the possibility to achieve efficient emission, combined with tailored spectra and controlled beam divergence. Here, we apply this concept to a one-dimensional quantum cascade wire laser. By lithographically patterning a series of air slits with different widths, following the Octonacci sequence, on the top metal layer of a double-metal quantum cascade laser operating at THz frequencies, we can vary the emission from single-frequency-mode to multimode over a 530-GHz bandwidth, achieving a maximum peak optical power of 240 mW (190 mW) in multimode (single-frequency-mode) lasers, with record slope efficiencies for multimode surface-emitting disordered THz lasers up to ≈570 mW/A at 78 K and ≈720 mW/A at 20 K and wall-plug efficiencies of η ≈ 1%.

13.
Light Sci Appl ; 9: 59, 2020.
Artículo en Inglés | MEDLINE | ID: mdl-32337023

RESUMEN

Optical logic operations lie at the heart of optical computing, and they enable many applications such as ultrahigh-speed information processing. However, the reported optical logic gates rely heavily on the precise control of input light signals, including their phase difference, polarization, and intensity and the size of the incident beams. Due to the complexity and difficulty in these precise controls, the two output optical logic states may suffer from an inherent instability and a low contrast ratio of intensity. Moreover, the miniaturization of optical logic gates becomes difficult if the extra bulky apparatus for these controls is considered. As such, it is desirable to get rid of these complicated controls and to achieve full logic functionality in a compact photonic system. Such a goal remains challenging. Here, we introduce a simple yet universal design strategy, capable of using plane waves as the incident signal, to perform optical logic operations via a diffractive neural network. Physically, the incident plane wave is first spatially encoded by a specific logic operation at the input layer and further decoded through the hidden layers, namely, a compound Huygens' metasurface. That is, the judiciously designed metasurface scatters the encoded light into one of two small designated areas at the output layer, which provides the information of output logic states. Importantly, after training of the diffractive neural network, all seven basic types of optical logic operations can be realized by the same metasurface. As a conceptual illustration, three logic operations (NOT, OR, and AND) are experimentally demonstrated at microwave frequencies.

14.
Light Sci Appl ; 9: 39, 2020.
Artículo en Inglés | MEDLINE | ID: mdl-32194953

RESUMEN

Semiconductors that can provide optical gain at extremely low carrier density levels are critically important for applications such as energy efficient nanolasers. However, all current semiconductor lasers are based on traditional semiconductor materials that require extremely high density levels above the so-called Mott transition to realize optical gain. The new emerging 2D materials provide unprecedented opportunities for studying new excitonic physics and exploring new optical gain mechanisms at much lower density levels due to the strong Coulomb interaction and co-existence and mutual conversion of excitonic complexes. Here, we report a new gain mechanism involving charged excitons or trions in electrically gated 2D molybdenum ditelluride well below the Mott density. Our combined experimental and modelling study not only reveals the complex interplay of excitonic complexes well below the Mott transition but also establishes 2D materials as a new class of gain materials at densities 4-5 orders of magnitude lower than those of conventional semiconductors and provides a foundation for lasing at ultralow injection levels for future energy efficient photonic devices. Additionally, our study could help reconcile recent conflicting results on 2D materials: While 2D material-based lasers have been demonstrated at extremely low densities with spectral features dominated by various excitonic complexes, optical gain was only observed in experiments at densities several orders of magnitude higher, beyond the Mott density. We believe that our results could lead to more systematic studies on the relationship between the mutual conversion of excitonic species and the existence of optical gain well below the Mott transition.

15.
Light Sci Appl ; 9: 10, 2020.
Artículo en Inglés | MEDLINE | ID: mdl-32025293

RESUMEN

The orbital angular momentum (OAM) of light has been shown to be useful in diverse fields ranging from astronomy and optical trapping to optical communications and data storage. However, one of the primary impediments preventing such applications from widespread adoption is the lack of a straightforward and dynamic method to sort incident OAM states without altering the states. Here, we report a technique that can dynamically filter individual OAM states and preserve the incident OAM states for subsequent processing. Although the working principle of this technique is based on resonance, the device operation is not limited to a particular wavelength. OAM states with different wavelengths can resonate in the resonator without any additional modulation other than changing the length of the cavity. Consequently, we are able to demonstrate a reconfigurable OAM sorter that is constructed by cascading such optical resonators. This approach does not require specially designed components and is readily amenable to integration into potential applications.

16.
Light Sci Appl ; 9: 5, 2020.
Artículo en Inglés | MEDLINE | ID: mdl-31934337

RESUMEN

Organic light-emitting diodes (OLEDs) have become a major pixel technology in the display sector, with products spanning the entire range of current panel sizes. The ability to freely scale the active area to large and random surfaces paired with flexible substrates provides additional application scenarios for OLEDs in the general lighting, automotive, and signage sectors. These applications require higher brightness and, thus, current density operation compared to the specifications needed for general displays. As extended transparent electrodes pose a significant ohmic resistance, OLEDs suffering from Joule self-heating exhibit spatial inhomogeneities in electrical potential, current density, and hence luminance. In this article, we provide experimental proof of the theoretical prediction that OLEDs will display regions of decreasing luminance with increasing driving current. With a two-dimensional OLED model, we can conclude that these regions are switched back locally in voltage as well as current due to insufficient lateral thermal coupling. Experimentally, we demonstrate this effect in lab-scale devices and derive that it becomes more severe with increasing pixel size, which implies its significance for large-area, high-brightness use cases of OLEDs. Equally, these non-linear switching effects cannot be ignored with respect to the long-term operation and stability of OLEDs; in particular, they might be important for the understanding of sudden-death scenarios.

17.
Light Sci Appl ; 8: 121, 2019.
Artículo en Inglés | MEDLINE | ID: mdl-31871673

RESUMEN

Transparent solar cells (TSCs) are emerging devices that combine the advantages of visible transparency and light-to-electricity conversion. Currently, existing TSCs are based predominantly on organics, dyes, and perovskites; however, the rigidity and color-tinted transparent nature of those devices strongly limit the utility of the resulting TSCs for real-world applications. Here, we demonstrate a flexible, color-neutral, and high-efficiency TSC based on a freestanding form of n-silicon microwires (SiMWs). Flat-tip SiMWs with controllable spacing are fabricated via deep-reactive ion etching and embedded in a freestanding transparent polymer matrix. The light transmittance can be tuned from ~10 to 55% by adjusting the spacing between the microwires. For TSCs, a heterojunction is formed with a p-type polymer in the top portion of the n-type flat-tip SiMWs. Ohmic contact with an indium-doped ZnO film occurs at the bottom, and the side surface has an Al2O3 passivation layer. Furthermore, slanted-tip SiMWs are developed by a novel solvent-assisted wet etching method to manipulate light absorption. Finite-difference time-domain simulation revealed that the reflected light from slanted-tip SiMWs helps light-matter interactions in adjacent microwires. The TSC based on the slanted-tip SiMWs demonstrates 8% efficiency at a visible transparency of 10% with flexibility. This efficiency is the highest among Si-based TSCs and comparable with that of state-of-the-art neutral-color TSCs based on organic-inorganic hybrid perovskite and organics. Moreover, unlike others, the stretchable and transparent platform in this study is promising for future TSCs.

18.
Light Sci Appl ; 8: 78, 2019.
Artículo en Inglés | MEDLINE | ID: mdl-31645924

RESUMEN

The manipulation and characterization of light polarization states are essential for many applications in quantum communication and computing, spectroscopy, bioinspired navigation, and imaging. Chiral metamaterials and metasurfaces facilitate ultracompact devices for circularly polarized light generation, manipulation, and detection. Herein, we report bioinspired chiral metasurfaces with both strong chiral optical effects and low insertion loss. We experimentally demonstrated submicron-thick circularly polarized light filters with peak extinction ratios up to 35 and maximum transmission efficiencies close to 80% at near-infrared wavelengths (the best operational wavelengths can be engineered in the range of 1.3-1.6 µm). We also monolithically integrated the microscale circular polarization filters with linear polarization filters to perform full-Stokes polarimetric measurements of light with arbitrary polarization states. With the advantages of easy on-chip integration, ultracompact footprints, scalability, and broad wavelength coverage, our designs hold great promise for facilitating chip-integrated polarimeters and polarimetric imaging systems for quantum-based optical computing and information processing, circular dichroism spectroscopy, biomedical diagnosis, and remote sensing applications.

19.
Light Sci Appl ; 8: 89, 2019.
Artículo en Inglés | MEDLINE | ID: mdl-31645933

RESUMEN

Understanding the interplay between illumination and the electron distribution in metallic nanostructures is a crucial step towards developing applications such as plasmonic photocatalysis for green fuels, nanoscale photodetection and more. Elucidating this interplay is challenging, as it requires taking into account all channels of energy flow in the electronic system. Here, we develop such a theory, which is based on a coupled Boltzmann-heat equations and requires only energy conservation and basic thermodynamics, where the electron distribution, and the electron and phonon (lattice) temperatures are determined uniquely. Applying this theory to realistic illuminated nanoparticle systems, we find that the electron and phonon temperatures are similar, thus justifying the (classical) single-temperature models. We show that while the fraction of high-energy "hot" carriers compared to thermalized carriers grows substantially with illumination intensity, it remains extremely small (on the order of 10-8). Importantly, most of the absorbed illumination power goes into heating rather than generating hot carriers, thus rendering plasmonic hot carrier generation extremely inefficient. Our formulation allows for the first time a unique quantitative comparison of theory and measurements of steady-state electron distributions in metallic nanostructures.

20.
Light Sci Appl ; 8: 97, 2019.
Artículo en Inglés | MEDLINE | ID: mdl-31645938

RESUMEN

There is an increasing need to remotely monitor people in daily life using radio-frequency probe signals. However, conventional systems can hardly be deployed in real-world settings since they typically require objects to either deliberately cooperate or carry a wireless active device or identification tag. To accomplish complicated successive tasks using a single device in real time, we propose the simultaneous use of a smart metasurface imager and recognizer, empowered by a network of artificial neural networks (ANNs) for adaptively controlling data flow. Here, three ANNs are employed in an integrated hierarchy, transforming measured microwave data into images of the whole human body, classifying specifically designated spots (hand and chest) within the whole image, and recognizing human hand signs instantly at a Wi-Fi frequency of 2.4 GHz. Instantaneous in situ full-scene imaging and adaptive recognition of hand signs and vital signs of multiple non-cooperative people were experimentally demonstrated. We also show that the proposed intelligent metasurface system works well even when it is passively excited by stray Wi-Fi signals that ubiquitously exist in our daily lives. The reported strategy could open up a new avenue for future smart cities, smart homes, human-device interaction interfaces, health monitoring, and safety screening free of visual privacy issues.

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