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Rational design of high-quality 2D/3D perovskite heterostructure crystals for record-performance polarization-sensitive photodetection.

ABSTRACT: Polarization-sensitive photodetection is central to optics applications and has been successfully demonstrated in photodetectors of two-dimensional (2D) materials, such as layered hybrid perovskites; however, achieving high polarization sensitivity in such a photodetector remains extremely challenging. Here, for the first time, we demonstrate a high-performance polarization-sensitive photodetector using single-crystalline 2D/3D perovskite heterostructure, namely, (4-AMP)(MA)2Pb3Br10/MAPbBr3 (MA = methylammonium; 4-AMP = 4-(aminomethyl)piperidinium), which exhibits ultrahigh polarization sensitivity up to 17.6 under self-driven mode. To our knowledge, such a high polarization selectivity has surpassed all of the reported perovskite-based devices, and is comparable to, or even better than, the traditional inorganic heterostructure-based photodetectors. Further studies reveal that the built-in electric field formed at the junction can spatially separate the photogenerated electrons and holes, reducing their recombination rate and thus enhancing the performance for polarization-sensitive photodetection. This work provides a new source of polarization-sensitive materials and insights into designing novel optoelectronic devices.

SUBMITTER: Zhang X

PROVIDER: S-EPMC8566186 | biostudies-literature |

REPOSITORIES: biostudies-literature

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An Embedding 2D/3D Heterostructure Enables High-Performance FA-Alloyed Flexible Perovskite Solar Cells with Efficiency over 20.

Project description:Flexible perovskite solar cells (f-PSCs) have attracted increasing attention because of their enormous potential for use in consumer electronic devices. The key to achieve high device performance is to deposit pinhole-free, uniform and defect-less perovskite films on the rough surface of polymeric substrates. Here, a solvent engineering to tailor the crystal morphology of FA-alloyed perovskite films prepared by one-step blade coating is first deployed. It is found that the use of binary solvents DMF:NMP, rather than the conventional DMF:DMSO, enables to deposit dense and uniform FA-alloyed perovskite films on both the rigid and flexible substrates. As a decisive step, an embedding 2D/3D perovskite heterostructure is in situ formed by incorporating a small amount of 4-guanidinobutanoic acid (GBA). Accordingly, photovoltage increases up to 100 mV are realized due to the markedly suppressed nonradiative recombination, leading to high efficiencies of 21.45% and 20.16% on the rigid and flexible substrates, respectively. In parallel, improved mechanical robustness of the flexible devices is achieved due to the presence of the embedded 2D phases. The results underpin the importance of morphology control and defect passivation in delivering high-performance flexible FA-alloyed flexible perovskite devices.

| S-EPMC8596135 | biostudies-literature

Improved Photostability in Fluorinated 2D Perovskite Single Crystals.

Project description:Hybrid organic-inorganic perovskites are very promising semiconductors for many optoelectronic applications, although their extensive use is limited by their poor stability under environmental conditions. In this work, we synthesize two-dimensional perovskite single crystals and investigate their optical and structural evolution under continuous light irradiation. We found that the hydrophobic nature of the fluorinated component, together with the absence of grain boundary defects, lead to improved material stability thanks to the creation of a robust barrier that preserve the crystalline structure, hindering photo-degradation processes usually promoted by oxygen and moisture.

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Strain-controlled synthesis of ultrathin hexagonal GaTe/MoS2 heterostructure for sensitive photodetection.

Project description:Ultrathin hexagonal GaTe, with relatively high charge density, holds great potential in the field of optoelectronic devices. However, the thermodynamical stability limits it fabrications as well as applications. Here, by introducing two-dimensional MoS2 as the substrate, we successfully realized the phase-controlled synthesis of ultrathin h-GaTe, leading to high-quality h-GaTe/MoS2 heterostructures. Theoretical calculation studies reveal that GaTe with hexagonal phase is more thermodynamically stable on MoS2 templates, which can be attributed to the strain stretching and the formation energy reduction. Based on the achieved p-n heterostructures, optoelectronic devices are designed and probed, where remarkable photoresponsivity (32.5 A/W) and fast photoresponse speed (<50 μs) are obtained, indicating well-behaved photo-sensing behaviors. The study here could offer a good reference for the controlled growth of the relevant materials, and the achieved heterostructure will find promising applications in future integrated electronic and optoelectronic devices and systems.

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Rational design of Al2O3/2D perovskite heterostructure dielectric for high performance MoS2 phototransistors.

Project description:Two-dimensional (2D) Ruddlesden-Popper perovskites are currently drawing significant attention as highly-stable photoactive materials for optoelectronic applications. However, the insulating nature of organic ammonium layers in 2D perovskites results in poor charge transport and limited performance. Here, we demonstrate that Al2O3/2D perovskite heterostructure can be utilized as photoactive dielectric for high-performance MoS2 phototransistors. The type-II band alignment in 2D perovskites facilitates effective spatial separation of photo-generated carriers, thus achieving ultrahigh photoresponsivity of >108 A/W at 457 nm and >106 A/W at 1064 nm. Meanwhile, the hysteresis loops induced by ionic migration in perovskite and charge trapping in Al2O3 can neutralize with each other, leading to low-voltage phototransistors with negligible hysteresis and improved bias stress stability. More importantly, the recombination of photo-generated carriers in 2D perovskites depends on the external biasing field. With an appropriate gate bias, the devices exhibit wavelength-dependent constant photoresponsivity of 103-108 A/W regardless of incident light intensity.

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From electron crystallography of 2D crystals to MicroED of 3D crystals.

Project description:Electron crystallography is widespread in material science applications, but for biological samples its use has been restricted to a handful of examples where two-dimensional (2D) crystals or helical samples were studied either by electron diffraction and/or imaging. Electron crystallography in cryoEM, was developed in the mid-1970s and used to solve the structure of several membrane proteins and some soluble proteins. In 2013, a new method for cryoEM was unveiled and named Micro-crystal Electron Diffraction, or MicroED, which is essentially three-dimensional (3D) electron crystallography of microscopic crystals. This method uses truly 3D crystals, that are about a billion times smaller than those typically used for X-ray crystallography, for electron diffraction studies. There are several important differences and some similarities between electron crystallography of 2D crystals and MicroED. In this review, we describe the development of these techniques, their similarities and differences, and offer our opinion of future directions in both fields.

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Capturing 3D atomic defects and phonon localization at the 2D heterostructure interface.

Project description:[Figure: see text].

| S-EPMC8443181 | biostudies-literature

In Situ Analysis Reveals the Role of 2D Perovskite in Preventing Thermal-Induced Degradation in 2D/3D Perovskite Interfaces.

Project description:Engineering 2D/3D perovskite interfaces is a common route to realizing efficient and stable perovskite solar cells. Whereas 2D perovskite's main function in trap passivation has been identified and is confirmed here, little is known about its 2D/3D interface properties under thermal stress, despite being one of the main factors that induces device instability. In this work, we monitor the response of two typical 2D/3D interfaces under a thermal cycle by in situ X-ray scattering. We reveal that upon heating, the 2D crystalline structure undergoes a dynamical transformation into a mixed 2D/3D phase, keeping the 3D bulk underneath intact. The observed 3D bulk degradation into lead iodide is blocked, revealing the paramount role of 2D perovskite in engineering stable device interfaces.

| S-EPMC7901643 | biostudies-literature

Multication perovskite 2D/3D interfaces form via progressive dimensional reduction.

Project description:Many of the best-performing perovskite photovoltaic devices make use of 2D/3D interfaces, which improve efficiency and stability - but it remains unclear how the conversion of 3D-to-2D perovskite occurs and how these interfaces are assembled. Here, we use in situ Grazing-Incidence Wide-Angle X-Ray Scattering to resolve 2D/3D interface formation during spin-coating. We observe progressive dimensional reduction from 3D to n = 3 → 2 → 1 when we expose (MAPbBr3)0.05(FAPbI3)0.95 perovskites to vinylbenzylammonium ligand cations. Density functional theory simulations suggest ligands incorporate sequentially into the 3D lattice, driven by phenyl ring stacking, progressively bisecting the 3D perovskite into lower-dimensional fragments to form stable interfaces. Slowing the 2D/3D transformation with higher concentrations of antisolvent yields thinner 2D layers formed conformally onto 3D grains, improving carrier extraction and device efficiency (20% 3D-only, 22% 2D/3D). Controlling this progressive dimensional reduction has potential to further improve the performance of 2D/3D perovskite photovoltaics.

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Defect-Induced Inhomogeneous Phase Transition in 2D Perovskite Single Crystals at Low Temperatures.

Project description:The temperature-induced phase transition in two-dimensional (2D) layered perovskites was recently found to be incomplete even if the temperature dropped to tens of kelvin. However, its intrinsic cause still remains unclear, and the information on the phase transition in individual single crystals (SCs) is also limited. Herein, we study the phase transition process in individual (n-C4H9NH3)2PbI4 SCs using a home-built photoluminescence (PL)-scanned image microscope. At 83 K, the phase transition is indeed incomplete, leading to the coexistence and inhomogeneous distributions of room-temperature and low-temperature phases. We map the distribution of phase transition degree on individual SCs at 83 K, which exhibits a strong positive (negative) correlation with the distribution of local defects (PL lifetimes) at 293 K, indicating that the phase transition is enhanced by initial defects. Our findings might provide new insight into the phase transition of (n-C4H9NH3)2PbI4 crystals, which is of potential value for applications based on 2D layered perovskites.

| S-EPMC8717364 | biostudies-literature

Light-Enhanced Ion Migration in Two-Dimensional Perovskite Single Crystals Revealed in Carbon Nanotubes/Two-Dimensional Perovskite Heterostructure and Its Photomemory Application.

Project description:Two-dimensional (2D) hybrid perovskite sandwiched between two long-chain organic layers is an emerging class of low-cost semiconductor materials with unique optical properties and improved moisture stability. Unlike conventional semiconductors, ion migration in perovskite is a unique phenomenon possibly responsible for long carrier lifetime, current-voltage hysteresis, and low-frequency giant dielectric response. While there are many studies of ion migration in bulk hybrid perovskite, not much is known for its 2D counterparts, especially for ion migration induced by light excitation. Here, we construct an exfoliated 2D perovskite/carbon nanotube (CNT) heterostructure field effect transistor (FET), not only to demonstrate its potential in photomemory applications, but also to study the light induced ion migration mechanisms. We show that the FET I-V characteristic curve can be regulated by light and shows two opposite trends under different CNT oxygen doping conditions. Our temperature-dependent study indicates that the change in the I-V curve is probably caused by ion redistribution in the 2D hybrid perovskite. The first principle calculation shows the reduction of the migration barrier of I vacancy under light excitation. The device simulation shows that the increase of 2D hybrid perovskite dielectric constant (enabled by the increased ion migration) can change the I-V curve in the trends observed experimentally. Finally, the so synthesized FET shows the multilevel photomemory function. Our work shows that not only we could understand the unique ion migration behavior in 2D hybrid perovskite, it might also be used for many future memory function related applications not realizable in traditional semiconductors.

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