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1.
Nano Lett ; 21(16): 6983-6989, 2021 08 25.
Artigo em Inglês | MEDLINE | ID: mdl-34346219

RESUMO

Semiconductive metal-organic frameworks (MOFs) obtained by specific host-guest interactions have attracted a large interest in the last two decades, promising development of next-generation electronic devices. Herein, we designed and presented flexible X-ray detectors using Ni-DABDT (DABDT = 2,5-diamino-1,4-benzenedithiol dihydrochloride) MOFs as the absorbing layer. The π-d coupling interactions of Ni-DABDT throughout the framework implement a conspicuous carrier transportation pathway. The detector that converts X-ray photons directly into carriers manifests an attractive achievement with high detection sensitivity of 98.6 µC Gyair-1 cm-2, with a low detection limit of 7.2 µGyair s-1 for the radiation robustness. This work provides insights for next-generation green and high-performance flexible sensor detectors by utilizing MOF materials with the benefits of a designable structure and tunable property, demonstrating a proof-of-concept in wearable X-ray detectors for radiation monitoring and imaging.


Assuntos
Estruturas Metalorgânicas , Fótons , Raios X
2.
Chem Commun (Camb) ; 2021 Aug 09.
Artigo em Inglês | MEDLINE | ID: mdl-34369527

RESUMO

Here, we constructed Pb-free Cu-DABDT-MOFs-based (DABDT = 2,5-diamino-1,4-benzenedithiol) X-ray detectors. Combined with the advantage of high activation energy, the Cu-DABDT-MOFs-based detector can effectively generate and capture electrons under X-ray exposure and presents a high mobility-lifetime (µτ) product of 6.49 × 10-4 cm2 V-1 and promising detection sensitivity of 78.7 µC Gyair-1 cm-2. As groundbreaking work, these discoveries have provided information for exploring MOF materials toward green and high-performance high-energy radiation detectors by exploiting the designable structure and tunable properties of the MOF family.

3.
Adv Mater ; 33(39): e2103000, 2021 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-34397123

RESUMO

The competing and non-equilibrium phase transitions, involving dynamic tunability of cooperative electronic and magnetic states in strongly correlated materials, show great promise in quantum sensing and information technology. To date, the stabilization of transient states is still in the preliminary stage, particularly with respect to molecular electronic solids. Here, a dynamic and cooperative phase in potassium-7,7,8,8-tetracyanoquinodimethane (K-TCNQ) with the control of pulsed electromagnetic excitation is demonstrated. Simultaneous dynamic and coherent lattice perturbation with 8 ns pulsed laser (532 nm, 15 MW cm-2 , 10 Hz) in such a molecular electronic crystal initiates a stable long-lived (over 400 days) conducting paramagnetic state (≈42 Ωcm), showing the charge-spin bistability over a broad temperature range from 2 to 360 K. Comprehensive noise spectroscopy, in situ high-pressure measurements, electron spin resonance (ESR), theoretical model, and scanning tunneling microscopy/spectroscopy (STM/STS) studies provide further evidence that such a transition is cooperative, requiring a dedicated charge-spin-lattice decoupling to activate and subsequently stabilize nonequilibrium phase. The cooperativity triggered by ultrahigh-strain-rate (above 106 s- 1 ) pulsed excitation offers a collective control toward the generation and stabilization of strongly correlated electronic and magnetic orders in molecular electronic solids and offers unique electro-magnetic phases with technological promises.

4.
Artigo em Inglês | MEDLINE | ID: mdl-34101425

RESUMO

Two-dimensional (2D) metal-molecule hybrid frameworks have attracted great attention due to their π-d interactions for the charge-spin-lattice coupling, promising for next-generation molecular electronics. However, a high electrical conductivity is indispensable to realize such potential. Herein, we design and assemble a conductive 2D conjugated coordination thin film through an interfacial reaction between the aqueous and organic phases. Its electronic conducting properties are derived from the π-d coupling interactions to achieve an electrical conductivity of 1.05 S/cm, while the stimulus-dependent π-d interactions induce multifunctional sensory capabilities. The Co-DABDT (DABDT = 2,5-diamino-1,4-benzenedithiol dihydrochloride) thin films demonstrate an excellent performance for sensing light, strain, temperature, and humidity, as well as robust mechanical stability. The 2D frameworks with multisensing properties for real-time static and dynamic monitoring are promising for smart wearable electronic systems.

5.
ACS Nano ; 2021 Apr 09.
Artigo em Inglês | MEDLINE | ID: mdl-33834763

RESUMO

Printed copper materials have been attracting significant attention prominently due to their electric, mechanical, and thermal properties. The emerging copper-based flexible electronics and energy-critical applications rely on the control of electric conductivity, current-carrying capacity, and reliability of copper nanostructures and their printable ink materials. In this review, we describe the growth of copper nanostructures as the building blocks for printable ink materials on which a variety of conductive features can be additively manufactured to achieve high electric conductivity and stability. Accordingly, the copper-based flexible hybrid electronics and energy-critical devices printed by different printing techniques are reviewed for emerging applications.

6.
Nano Lett ; 2021 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-33886320

RESUMO

Magnetoelectrics are witnessing an ever-growing success toward the voltage-controlled magnetism derived from inorganic materials. However, these inorganic materials have predominantly focused on the ferroelectromagnetism at solid-to-solid interfaces and suffered several drawbacks, including the interface-sensitive coupling mediators, high-power electric field, and limited chemical tunability. Here, we report a promising design strategy to shift the paradigm of next-generation molecular magnetoelectrics, which relies on the integration between molecular magnetism and electric conductivity though an in situ cross-linking strategy. Following this approach, we demonstrate a versatile and efficient synthesis of flexible molecular-based magnetoelectronics by cross-linking of magnetic coordination networks that incorporate conducting chain building blocks. The as-grown compounds feature an improved critical temperature up to 337 K and a room-temperature magnetism control of low-power electric field. It is envisaged that the cross-linking of molecular interfaces is a feasible method to couple and modulate magnetism and electron conducting systems.

7.
ACS Appl Mater Interfaces ; 12(44): 50024-50032, 2020 Nov 04.
Artigo em Inglês | MEDLINE | ID: mdl-33086781

RESUMO

Nature has inspired the design of next-generation lightweight architectured structural materials, for example, nacre-bearing extreme impact and paw-pad absorbing energy. Here, a bioinspired functional gradient structure, consisting of an impact-resistant hard layer and an energy-absorbing ductile layer, is applied to additively manufacture ultrahigh-molecular-weight polyethylene (UHMWPE). Its crystalline graded and directionally solidified structure enables superior impact resistance. In addition, we demonstrate nonequilibrium processing, ultrahigh strain rate pulsed laser shock wave peening, which could trigger surface hardening for enhanced crystallinity and polymer phase transformation. Moreover, we demonstrate the paw-pad-inspired soft- and hard-fiber-reinforced composite structure to absorb the impact energy. The bioinspired design and nonequilibrium processing of graded UHMWPE shed light on lightweight engineering polymer materials for impact-resistant and threat-protection applications.

8.
Proc Natl Acad Sci U S A ; 117(44): 27204-27210, 2020 Nov 03.
Artigo em Inglês | MEDLINE | ID: mdl-33077582

RESUMO

Molecular ferroelectrics combine electromechanical coupling and electric polarizabilities, offering immense promise in stimuli-dependent metamaterials. Despite such promise, current physical realizations of mechanical metamaterials remain hindered by the lack of rapid-prototyping ferroelectric metamaterial structures. Here, we present a continuous rapid printing strategy for the volumetric deposition of water-soluble molecular ferroelectric metamaterials with precise spatial control in virtually any three-dimensional (3D) geometry by means of an electric-field-assisted additive manufacturing. We demonstrate a scaffold-supported ferroelectric crystalline lattice that enables self-healing and a reprogrammable stiffness for dynamic tuning of mechanical metamaterials with a long lifetime and sustainability. A molecular ferroelectric architecture with resonant inclusions then exhibits adaptive mitigation of incident vibroacoustic dynamic loads via an electrically tunable subwavelength-frequency band gap. The findings shown here pave the way for the versatile additive manufacturing of molecular ferroelectric metamaterials.

9.
Nano Lett ; 20(11): 7852-7859, 2020 Nov 11.
Artigo em Inglês | MEDLINE | ID: mdl-33054240

RESUMO

Vertical van der Waals (vdWs) heterostructures based on layered materials are attracting interest as a new class of quantum materials, where interfacial charge-transfer coupling can give rise to fascinating strongly correlated phenomena. Transition metal chalcogenides are a particularly exciting material family, including ferromagnetic semiconductors, multiferroics, and superconductors. Here, we report the growth of an organic-inorganic heterostructure by intercalating molecular electron donating bis(ethylenedithio)tetrathiafulvalene into (Li,Fe)OHFeSe, a layered material in which the superconducting ground state results from the intercalation of hydroxide layer. Molecular intercalation in this heterostructure induces a transformation from a paramagnetic to spin-glass-like state that is sensitive to the stoichiometry of molecular donor and an applied magnetic field. Besides, electron-donating molecules reduce the electrical resistivity in the heterostructure and modify its response to laser illumination. This hybrid heterostructure provides a promising platform to study emerging magnetic and electronic behaviors in strongly correlated layered materials.

10.
Nanotechnology ; 31(46): 465606, 2020 Nov 13.
Artigo em Inglês | MEDLINE | ID: mdl-32877374

RESUMO

Magnetic ferrite materials have been extensively studied for a range of technological applications, such as magnetic motors, recording media, and millimetre-wave devices. In this context, the nanosized epsilon phase of Fe2O3 (ϵ-Fe2O3) attracts significant attention due to its high coercive field at room temperature. Here, we report the in-situ aerogel nanoreactor growth of magnetic ϵ-Fe2O3 nanoparticles, exhibiting a coercive field (Hc) of 4000 Oe. We show that the control of nanoreactor plays an important role in the growth of ϵ-Fe2O3 nanoparticles. The findings provide a versatile reaction pathway for the growth of magnetically hard ferrite nanoparticles.

11.
J Phys Chem Lett ; 11(19): 8352-8357, 2020 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-32914983

RESUMO

Using scanning tunneling microscopy/spectroscopy (STM/STS), we investigate the evolution of electronic structures across the boundaries of 7,7,8,8-tetracyanoquinodimethane (TCNQ) and K-TCNQ assemblies on a weakly interacting substrate. Despite the semiconducting/insulating nature of TCNQ (TCNQ0) and K-TCNQ (TCNQ-1), a continuum metallic-like density of states extending deep (∼1.5 nm) into the TCNQ assembly is observed near the domain boundary. We attribute the formation of these states to the abrupt change of molecular valence, which perturbs the electrostatics of the junction and creates local electric fields as evidenced by the band bending near the domain boundary. To the best of our knowledge, this study provides the first microscopic understanding of the crucial physics occurring near domain boundaries of mixed valence in K-TCNQ, or broadly speaking charge-transfer complexes, which highlights these boundaries as potential "weak" points to initiate the electric field-induced insulator-to-metal transition.

12.
Chem Commun (Camb) ; 56(48): 6555-6558, 2020 Jun 16.
Artigo em Inglês | MEDLINE | ID: mdl-32396159

RESUMO

Magnetically hard nanoparticles have been widely explored in colloidal solution synthesis, while a high temperature-induced phase transformation is indispensable to achieve its high magnetocrystalline anisotropy. However, a long-standing challenge of magnetic nanoparticles is the inaccessibility of size-controlled growth without sintering-induced agglomeration. Here, we report a universal one-pot eutectic reaction scheme of magnetically hard FePd nanoparticles, in which the crystallization conditions are critical for its magnetic performance. We demonstrate that the stoichiometry between transition metal and eutectic salt and sintering temperature can play an important role in the magnetic coercivity of FePd nanoparticles. In addition, gallium liquid metal is employed as the conductivity filler for the formation of a magnetorheological fluid after mixing with metallic FePd nanoparticles. The liquid composite shows a high metallic and thermal conductivity as an unconventional cooling metallic ferrofluid conductor, and we further demonstrate its potential application in sensors, conductors and thermal interfaces.

13.
Nano Lett ; 20(5): 3828-3835, 2020 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-32267711

RESUMO

To exploit the high-temperature superinsulation potential of anisotropic thermal management materials, the incorporation of ceramic aerogel into the aligned structural networks is indispensable. However, the long-standing obstacle to exploring ultralight superinsulation ceramic aerogels is the inaccessibility of its mechanical elasticity, stability, and anisotropic thermal insulation. In this study, we report a recoverable, flexible ceramic fiber-aerogel composite with anisotropic lamellar structure, where the interfacial cross-linking between ceramic fiber and aerogel is important in its superinsulation performance. The resulting ultralight aerogel composite exhibits a density of 0.05 g/cm3, large strain recovery (over 50%), and low thermal conductivity (0.0224 W m-1 K-1), while its hydrophobicity is achieved by in situ trichlorosilane coating with the water contact angle of 135°. The hygroscopic tests of such aerogel composites demonstrate a reversible thermal insulation. The mechanical elasticity and stability of the anisotropic composites, with its soundproof performance, shed light on the low-cost superelastic aerogel manufacturing with scalability for energy saving building applications.

14.
Chem Commun (Camb) ; 56(15): 2332-2335, 2020 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-31990279

RESUMO

Lightweight and printable polymer dielectrics are ubiquitous in flexible hybrid electronics, exhibiting high breakdown strength and mechanical reliability. However, their advanced electronic applications are limited due to their relatively low permittivity, compared to their ceramic counterparts. Here, we report flexible all organic percolative nanocomposites that contain in situ grown conductive polymer networks and dielectric polymer matrix, in which their dielectric properties can be designed and guided from the percolation theory. High dielectric constant of all organic percolative nanocomposites is shown over a broad frequency range under intensive bending cycles, while their thermal stability is attributed to thermally conductive 2D montmorillonite nanosheets. The printable polymer composites with high dielectric performance and thermal stability will find broader interest in flexible hybrid electronics and radio frequency devices.

15.
Nano Lett ; 20(2): 1110-1116, 2020 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-31891269

RESUMO

Light-weight ceramic aerogels hold promise for superinsulation. However, its mechanical instability and complex manufacturing hampered its technical applications. In this study, we demonstrate lightweight pore-gradient ceramic aerogel-like foam monoliths (PGAFoams) through one-pot and in situ bubble supported pore gradient formation. The mechanically strong PGAFoams exhibit a low thermal conductivity of 0.036 W m-1 K-1 and a compressive strength of 89.85 MPa. The pore gradient and integral ceramic monolith nature provides such hydrophobic PGAFoams with thermal management, robust soundproof, and fire-resistance performance. Highly machinable PGAFoams can be adapted into a variety of shapes and dimensions to accommodate complex geometry applications. The scalable manufacturing of lightweight PGAFoams opens up building insulation with remarkable thermal management, high mechanical strength, low mass density, superior soundproofing, and fire-retardant performances.

16.
Nanotechnology ; 31(10): 105703, 2020 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-31751954

RESUMO

Alumina (Al2O3) is one of the most widely used ceramic materials for innumerable applications, due to its unique combination of attractive physical and mechanical properties. These intrinsic properties are dictated by the numerous phases that Al2O3 forms and its related phase transformations. Transition metal (TM) cation dopants (iron (Fe), cobalt (Co), nickel (Ni) and manganese (Mn)), even in sparse amounts, have been shown to significantly affect the phase transformation and microstructural evolution of Al2O3. Small concentrations of TM cation dopants have successfully been incorporated to synthesize magnetically active Al2O3, while reducing the θ to α phase transformation temperature by 150 °C, and maintaining the outstanding mechanical properties. In addition, first-principle calculations based on density-functional theory with hybrid functional (HSE06) and the PBE+U methods have provided a mechanistic understanding of the formation energy and magnetism of the TM-doped α and θ phases of Al2O3. The results reveal a potential route for phase transition regulation and external magnetic field-induced texturing of Al2O3 ceramics.

17.
Adv Sci (Weinh) ; 6(24): 1802230, 2019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31871856

RESUMO

Since their debut in 2012, triboelectric nanogenerators (TENGs) have attained high performance in terms of both energy density and instantaneous conversion, reaching up to 500 W m-2 and 85%, respectively, synchronous with multiple energy sources and hybridized designs. Here, a comprehensive review of the design guidelines of TENGs, their performance, and their designs in the context of Internet of Things (IoT) applications is presented. The development stages of TENGs in large-scale self-powered systems and technological applications enabled by harvesting energy from water waves or wind energy sources are also reviewed. This self-powered capability is essential considering that IoT applications should be capable of operation anywhere and anytime, supported by a network of energy harvesting systems in arbitrary environments. In addition, this review paper investigates the development of self-charging power units (SCPUs), which can be realized by pairing TENGs with energy storage devices, such as batteries and capacitors. Consequently, different designs of power management circuits, supercapacitors, and batteries that can be integrated with TENG devices are also reviewed. Finally, the significant factors that need to be addressed when designing and optimizing TENG-based systems for energy harvesting and self-powered sensing applications are discussed.

18.
Nanoscale ; 11(46): 22585-22589, 2019 Nov 28.
Artigo em Inglês | MEDLINE | ID: mdl-31746911

RESUMO

We report the controlled interfacial interaction in crystallized organic charge transfer thin films, consisting of bis(ethylenedithio)tetrathiafulvalene and C60. The induced broad-band absorption from the UV to near-infrared region leads to a wavelength dependent ambipolar (negative/positive) photoresponse, while multi-stimuli responsive behavior is achieved through charge-transfer interactions. In addition, by coupling with the tetrathiafulvalene-(7,7,8,8-tetracyanoquinodimethane) charge transfer complex, a significantly increased conductivity is achieved. The controlled interfacial charge transfer interaction provides an efficient approach to obtain multifunctional molecular crystallized thin films with a superior external stimuli response.

19.
Adv Mater ; 31(48): e1904857, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-31588656

RESUMO

Circularly polarized light emission promotes the development of smart photonic materials for advanced applications in chiral sensing and information storage. The orbital angular momentum is a unique property for organic chiral helical materials. In this work, a type of organic chiral polymeric nanowires is designed with strong chirality induced orbital angular momentum. Under the stimulus of an external magnetic field of 600 mT, circularly polarized emission from the chiral polymeric nanowire becomes more pronounced, where the g factor increases from 0.21 to 0.3. The observed phenomena mainly originate from the chirality-dependent orbital angular momentum. Moreover, the orbital angular momentum in helical chiral nanowire structures can be suppressed by inhibiting electron transport in a helical way to diminish circularly polarized light emission at room temperature.

20.
Chem Commun (Camb) ; 55(84): 12643-12646, 2019 Oct 17.
Artigo em Inglês | MEDLINE | ID: mdl-31580340

RESUMO

The charge transfer and spin coupling effects are explored at the interface of two-dimensional (2D) superconducting FeSe nanosheets and molecular photochromic potassium-7,7,8,8-tetracyanoquinodimethane (KTCNQ). Light-induced conductivity in 2D FeSe nanosheets is enhanced by the electron doping from KTCNQ by the destabilized spin-Peierls phase through their interface. Furthermore, the spin coupling at the interface of FeSe and KTCNQ shifts the dimerization transition temperature of KTCNQ. Our results suggest 2D exfoliated FeSe nanosheets as a versatile strongly correlated platform for the study of interfacial electron doping and spin coupling.

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