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1.
ACS Nano ; 2020 Jan 03.
Artigo em Inglês | MEDLINE | ID: mdl-31887010

RESUMO

Neuromorphic visual sensory and memory systems, which can perceive, process, and memorize optical information, represent core technology for artificial intelligence and robotics with autonomous navigation. An optoelectronic synapse with an elegant integration of biometric optical sensing and synaptic learning functions can be a fundamental element for the hardware-implementation of such systems. Here, we report a class of ferroelectric field-effect memristive transistors made of a two-dimensional WS2 semiconductor atop a ferroelectric PbZr0.2Ti0.8O3 (PZT) thin film for optoelectronic synaptic devices. The WS2 channel exhibits voltage- and light-controllable memristive switching, dependent on the optically and electrically tunable ferroelectric domain patterns in the underlying PZT layer. These devices consequently show the emulation of optically driven synaptic functionalities including both short- and long-term plasticity as well as the implementation of brainlike learning rules. Integration of these rich synaptic functionalities into one single artificial optoelectronic device could allow the development of future neuromorphic electronics capable of optical information sensing and learning.

2.
Adv Mater ; 31(48): e1902890, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-31588637

RESUMO

Domain wall nanoelectronics is a rapidly evolving field, which explores the diverse electronic properties of the ferroelectric domain walls for application in low-dimensional electronic systems. One of the most prominent features of the ferroelectric domain walls is their electrical conductivity. Here, using a combination of scanning probe and scanning transmission electron microscopy, the mechanism of the tunable conducting behavior of the domain walls in the sub-micrometer thick films of the technologically important ferroelectric LiNbO3 is explored. It is found that the electric bias generates stable domains with strongly inclined domain boundaries with the inclination angle reaching 20° with respect to the polar axis. The head-to-head domain boundaries exhibit high conductance, which can be modulated by application of the sub-coercive voltage. Electron microscopy visualization of the electrically written domains and piezoresponse force microscopy imaging of the very same domains reveals that the gradual and reversible transition between the conducting and insulating states of the domain walls results from the electrically induced wall bending near the sample surface. The observed modulation of the wall conductance is corroborated by the phase-field modeling. The results open a possibility for exploiting the conducting domain walls as the electrically controllable functional elements in the multilevel logic nanoelectronics devices.

3.
ACS Appl Mater Interfaces ; 11(38): 35115-35121, 2019 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-31460741

RESUMO

Ferroelectric (FE) HfO2-based thin films, which are considered as one of the most promising material systems for memory device applications, exhibit an adverse tendency for strong imprint. Manifestation of imprint is a shift of the polarization-voltage (P-V) loops along the voltage axis due to the development of an internal electric bias, which can lead to the failure of the writing and retention functions. Here, to gain insight into the mechanism of the imprint effect in La-doped HfO2 (La:HfO2) capacitors, we combine the pulse switching technique with high-resolution domain imaging by means of piezoresponse force microscopy. This approach allows us to establish a correlation between the macroscopic switching characteristics and domain time-voltage-dependent behavior. It has been shown that the La:HfO2 capacitors exhibit a much more pronounced imprint compared to Pb(Zr,Ti)O3-based FE capacitors. Also, in addition to conventional imprint, which evolves with time in the poled capacitors, an easily changeable imprint, termed as "fluid imprint", with a strong dependence on the switching prehistory and measurement conditions, has been observed. Visualization of the domain structure reveals a specific signature of fluid imprint-continuous switching of polarization in the same direction as the previously applied field that continues a long time after the field was turned off. This effect, termed as "inertial switching", is attributed to charge injection and subsequent trapping at defect sites at the film-electrode interface.

4.
Adv Mater ; 31(36): e1902099, 2019 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-31353633

RESUMO

Ferroelectric domain walls exhibit a number of new functionalities that are not present in their host material. One of these functional characteristics is electrical conductivity that may lead to future device applications. Although progress has been made, the intrinsic conductivity of BiFeO3 domain walls is still elusive. Here, the intrinsic conductivity of 71° and 109° domain walls is reported by probing the local conductance over a cross section of the BiFeO3 /TbScO3 (001) heterostructure. Through a combination of conductive atomic force microscopy, high-resolution electron energy loss spectroscopy, and phase-field simulations, it is found that the 71° domain wall has an inherently charged nature, while the 109° domain wall is close to neutral. Hence, the intrinsic conductivity of the 71° domain walls is an order of magnitude larger than that of the 109° domain walls associated with bound-charge-induced bandgap lowering. Furthermore, the interaction of adjacent 71° domain walls and domain wall curvature leads to a variation of the charge distribution inside the walls, and causes a discontinuity of potential in the [110]p direction, which results in an alternative conductivity of the neighboring 71° domain walls, and a low conductivity of the 71° domain walls when measurement is taken from the film top surface.

5.
Nano Lett ; 19(5): 3194-3198, 2019 05 08.
Artigo em Inglês | MEDLINE | ID: mdl-30943040

RESUMO

We introduce a concept of programmable ferroelectric devices composed of two-dimensional (2D) and ferroelectric (FE) materials. It enables precise modulation of the in-plane conductivity of a 2D channel material through nanoengineering FE domains with out-of-plane polarization. The functionality of these new devices has been demonstrated using field-effect transistors (FETs) fabricated with monolayer molybdenum disulfide (MoS2) channels on the Pb(Zr,Ti)O3 substrates. Using piezoresponse force microscopy (PFM), we show that local switching of FE polarization by a conductive probe can be used to tune the conductivity of the MoS2 channel. Specifically, patterning of the nanoscale domains with downward polarization creates conductive paths in a resistive MoS2 channel so that the conductivity of an FET is determined by the number and length of the paths connecting source and drain electrodes. In addition to the device programmability, we demonstrate the device ON/OFF cyclic endurance by successive writing and erasing of conductive paths in a MoS2 channel. These findings may inspire the development of advanced energy-efficient programmable synaptic devices based on a combination of 2D and FE materials.

6.
Nat Commun ; 10(1): 1661, 2019 04 10.
Artigo em Inglês | MEDLINE | ID: mdl-30971688

RESUMO

Since its inception more than 25 years ago, Piezoresponse Force Microscopy (PFM) has become one of the mainstream techniques in the field of nanoferroic materials. This review describes the evolution of PFM from an imaging technique to a set of advanced methods, which have played a critical role in launching new areas of ferroic research, such as multiferroic devices and domain wall nanoelectronics. The paper reviews the impact of advanced PFM modes concerning the discovery and scientific understanding of novel nanoferroic phenomena and discusses challenges associated with the correct interpretation of PFM data. In conclusion, it offers an outlook for future trends and developments in PFM.

7.
ACS Nano ; 12(12): 12713-12720, 2018 Dec 26.
Artigo em Inglês | MEDLINE | ID: mdl-30499656

RESUMO

Quasi-one-dimensional (quasi-1D) materials enjoy growing interest due to their unusual physical properties and promise for miniature electronic devices. However, the mechanical exfoliation of quasi-1D materials into thin flakes and nanoribbons received considerably less attention from researchers than the exfoliation of conventional layered crystals. In this study, we investigated the micromechanical exfoliation of representative quasi-1D crystals, TiS3 whiskers, and demonstrate that they typically split into narrow nanoribbons with very smooth, straight edges and clear signatures of 1D TiS3 chains. Theoretical calculations show that the energies required for breaking weak interactions between the two-dimensional (2D) layers and between 1D chains within the layers are comparable and, in turn, are considerably lower than those required for breaking the covalent bonds within the chains. We also emulated macroscopic exfoliation experiments on the nanoscale by applying a local shear force to TiS3 crystals in different crystallographic directions using a tip of an atomic force microscopy (AFM) probe. In the AFM experiments, it was possible to slide the 2D TiS3 layers relative to each other as well as to remove selected 1D chains from the layers. We systematically studied the exfoliated TiS3 crystals by Raman spectroscopy and identified the Raman peaks whose spectral positions were most dependent on the crystals' thickness. These results could be used to distinguish between TiS3 crystals with thickness ranging from one to about seven monolayers. The conclusions established in this study for the exfoliated TiS3 crystals can be extended to a variety of transition metal trichalcogenide materials as well as other quasi-1D crystals. The possibility of exfoliation of TiS3 into narrow (few-nm wide) crystals with smooth edges could be important for the future realization of miniature device channels with reduced edge scattering of charge carriers.

8.
Adv Mater ; 30(51): e1803249, 2018 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-30334281

RESUMO

Collective ferroic orders in van der Waals (vdW) crystals are receiving increasing attention in 2D materials research. The interplay between spatial quantum confinement and long-range cooperative phenomena not only broadens the horizon of fundamental physics, but also enables new device paradigms and functionalities built upon vdW heterostructures. Here, the in-plane ferroelectric properties in thin flakes of vdW hybrid perovskite bis(benzylammonium) lead tetrachloride are studied. The ordering of electric dipoles along the layer plane circumvents the depolarization field and preserves the ferroelectricity down to one unit-cell thickness or two vdW layers at room temperature. The superior performance of the electromechanical energy conversion is demonstrated by exploiting its in-plane piezoelectricity. The successful isolation of ferroelectric order in atomically thin vdW hybrid perovskite paves the way for nonvolatile flexible electronic devices with the cross-coupling between strain, charge polarization, and valley degrees of freedom.

9.
Nat Nanotechnol ; 13(12): 1191, 2018 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-30291315

RESUMO

In the version of this Letter originally published, the right-hand arrow in Fig. 3b was incorrectly labelled; see correction note for details. Also, ref. 29 was incorrectly included in the reference list; it has now been removed.

10.
Nat Mater ; 17(12): 1164, 2018 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-30315212

RESUMO

In the version of this Article originally published, the y axis of Fig. 1c was incorrectly labelled 'S (%)'; it should have been '-S (%)'. Also, the link for the Supplementary Video was missing from the online version of the Article. These errors have now been corrected.

11.
Nat Mater ; 17(11): 1020-1026, 2018 11.
Artigo em Inglês | MEDLINE | ID: mdl-30250177

RESUMO

Lead halide perovskites have demonstrated outstanding performance in photovoltaics, photodetectors, radiation detectors and light-emitting diodes. However, the electromechanical properties, which are the main application of inorganic perovskites, have rarely been explored for lead halide perovskites. Here, we report the discovery of a large electrostrictive response in methylammonium lead triiodide (MAPbI3) single crystals. Under an electric field of 3.7 V µm-1, MAPbI3 shows a large compressive strain of 1%, corresponding to a mechanical energy density of 0.74 J cm-3, comparable to that of human muscles. The influences of piezoelectricity, thermal expansion, intrinsic electrostrictive effect, Maxwell stress, ferroelectricity, local polar fluctuation and methylammonium cation ordering on this electromechanical response are excluded. We speculate, using density functional theory, that electrostriction of MAPbI3 probably originates from lattice deformation due to formation of additional defects under applied bias. The discovery of large electrostriction in lead iodide perovskites may lead to new potential applications in actuators, sonar and micro-electromechanical systems and aid the understanding of other field-dependent material properties.

12.
Nat Nanotechnol ; 13(12): 1132-1136, 2018 12.
Artigo em Inglês | MEDLINE | ID: mdl-30250247

RESUMO

Coupling between different degrees of freedom, that is, charge, spin, orbital and lattice, is responsible for emergent phenomena in complex oxide heterostrutures1,2. One example is the formation of a two-dimensional electron gas (2DEG) at the polar/non-polar LaAlO3/SrTiO3 (LAO/STO)3-7 interface. This is caused by the polar discontinuity and counteracts the electrostatic potential build-up across the LAO film3. The ferroelectric polarization at a ferroelectric/insulator interface can also give rise to a polar discontinuity8-10. Depending on the polarization orientation, either electrons or holes are transferred to the interface, to form either a 2DEG or two-dimensional hole gas (2DHG)11-13. While recent first-principles modelling predicts the formation of 2DEGs at the ferroelectric/insulator interfaces9,10,12-14, experimental evidence of a ferroelectrically induced interfacial 2DEG remains elusive. Here, we report the emergence of strongly anisotropic polarization-induced conductivity at a ferroelectric/insulator interface, which shows a strong dependence on the polarization orientation. By probing the local conductance and ferroelectric polarization over a cross-section of a BiFeO3-TbScO3 (BFO/TSO) (001) heterostructure, we demonstrate that this interface is conducting along the 109° domain stripes in BFO, whereas it is insulating in the direction perpendicular to these domain stripes. Electron energy-loss spectroscopy and theoretical modelling suggest that the anisotropy of the interfacial conduction is caused by an alternating polarization associated with the ferroelectric domains, producing either electron or hole doping of the BFO/TSO interface.

13.
Nat Commun ; 9(1): 3344, 2018 08 21.
Artigo em Inglês | MEDLINE | ID: mdl-30131577

RESUMO

In the ferroelectric devices, polarization control is usually accomplished by application of an electric field. In this paper, we demonstrate optically induced polarization switching in BaTiO3-based ferroelectric heterostructures utilizing a two-dimensional narrow-gap semiconductor MoS2 as a top electrode. This effect is attributed to the redistribution of the photo-generated carriers and screening charges at the MoS2/BaTiO3 interface. Specifically, a two-step process, which involves formation of intra-layer excitons during light absorption followed by their decay into inter-layer excitons, results in the positive charge accumulation at the interface forcing the polarization reversal from the upward to the downward direction. Theoretical modeling of the MoS2 optical absorption spectra with and without the applied electric field provides quantitative support for the proposed mechanism. It is suggested that the discovered effect is of general nature and should be observable in any heterostructure comprising a ferroelectric and a narrow gap semiconductor.

14.
Sci Adv ; 4(6): eaat0491, 2018 06.
Artigo em Inglês | MEDLINE | ID: mdl-29922719

RESUMO

Two-dimensional (2D) transition metal carbides and nitrides, known as MXenes, are a large class of materials that are finding numerous applications ranging from energy storage and electromagnetic interference shielding to water purification and antibacterial coatings. Yet, despite the fact that more than 20 different MXenes have been synthesized, the mechanical properties of a MXene monolayer have not been experimentally studied. We measured the elastic properties of monolayers and bilayers of the most important MXene material to date, Ti3C2T x (T x stands for surface termination). We developed a method for preparing well-strained membranes of Ti3C2T x monolayers and bilayers, and performed their nanoindentation with the tip of an atomic force microscope to record the force-displacement curves. The effective Young's modulus of a single layer of Ti3C2T x was found to be 0.33 ± 0.03 TPa, which is the highest among the mean values reported in nanoindentation experiments for other solution-processed 2D materials, including graphene oxide. This work opens a pathway for investigating the mechanical properties of monolayers and bilayers of other MXenes and extends the already broad range of MXenes' applications to structural composites, protective coatings, nanoresonators, and membranes that require materials with exceptional mechanical properties.

15.
Nat Commun ; 9(1): 1625, 2018 04 24.
Artigo em Inglês | MEDLINE | ID: mdl-29691390

RESUMO

The efficiencies of perovskite solar cells (PSCs) are now reaching such consistently high levels that scalable manufacturing at low cost is becoming critical. However, this remains challenging due to the expensive hole-transporting materials usually employed, and difficulties associated with the scalable deposition of other functional layers. By simplifying the device architecture, hole-transport-layer-free PSCs with improved photovoltaic performance are fabricated via a scalable doctor-blading process. Molecular doping of halide perovskite films improved the conductivity of the films and their electronic contact with the conductive substrate, resulting in a reduced series resistance. It facilitates the extraction of photoexcited holes from perovskite directly to the conductive substrate. The bladed hole-transport-layer-free PSCs showed a stabilized power conversion efficiency above 20.0%. This work represents a significant step towards the scalable, cost-effective manufacturing of PSCs with both high performance and simple fabrication processes.

16.
ACS Appl Mater Interfaces ; 10(15): 12862-12869, 2018 Apr 18.
Artigo em Inglês | MEDLINE | ID: mdl-29617112

RESUMO

Brain-inspired computing is an emerging field, which intends to extend the capabilities of information technology beyond digital logic. The progress of the field relies on artificial synaptic devices as the building block for brainlike computing systems. Here, we report an electronic synapse based on a ferroelectric tunnel memristor, where its synaptic plasticity learning property can be controlled by nanoscale interface engineering. The effect of the interface engineering on the device performance was studied. Different memristor interfaces lead to an opposite virgin resistance state of the devices. More importantly, nanoscale interface engineering could tune the intrinsic band alignment of the ferroelectric/metal-semiconductor heterostructure over a large range of 1.28 eV, which eventually results in different memristive and spike-timing-dependent plasticity (STDP) properties of the devices. Bidirectional and unidirectional gradual resistance modulation of the devices could therefore be controlled by tuning the band alignment. This study gives useful insights on tuning device functionalities through nanoscale interface engineering. The diverse STDP forms of the memristors with different interfaces may play different specific roles in various spike neural networks.


Assuntos
Plasticidade Neuronal , Encéfalo , Semicondutores , Sinapses
17.
ACS Appl Mater Interfaces ; 10(10): 8818-8826, 2018 Mar 14.
Artigo em Inglês | MEDLINE | ID: mdl-29464951

RESUMO

Because of their full compatibility with the modern Si-based technology, the HfO2-based ferroelectric films have recently emerged as viable candidates for application in nonvolatile memory devices. However, despite significant efforts, the mechanism of the polarization switching in this material is still under debate. In this work, we elucidate the microscopic nature of the polarization switching process in functional Hf0.5Zr0.5O2-based ferroelectric capacitors during its operation. In particular, the static domain structure and its switching dynamics following the application of the external electric field have been monitored with the advanced piezoresponse force microscopy (PFM) technique providing a nm resolution. Separate domains with strong built-in electric field have been found. Piezoresponse mapping of pristine Hf0.5Zr0.5O2 films revealed the mixture of polar phase grains and regions with low piezoresponse as well as the continuum of polarization orientations in the grains of polar orthorhombic phase. PFM data combined with the structural analysis of pristine versus trained film by plan-view transmission electron microscopy both speak in support of a monoclinic-to-orthorhombic phase transition in ferroelectric Hf0.5Zr0.5O2 layer during the wake-up process under an electrical stress.

18.
Nano Lett ; 18(1): 491-497, 2018 01 10.
Artigo em Inglês | MEDLINE | ID: mdl-29236501

RESUMO

Strontium titanate (SrTiO3) is the "silicon" in the emerging field of oxide electronics. While bulk properties of this material have been studied for decades, new unexpected phenomena have recently been discovered at the nanoscale, when SrTiO3 forms an ultrathin film or an atomically sharp interface with other materials. One of the striking discoveries is room-temperature ferroelectricity in strain-free ultrathin films of SrTiO3 driven by the TiSr antisite defects, which generate a local dipole moment polarizing the surrounding nanoregion. Here, we demonstrate that these polar defects are not only responsible for ferroelectricity, but also propel the appearance of highly conductive channels, "hot spots", in the ultrathin SrTiO3 films. Using a combination of scanning probe microscopy experimental studies and theoretical modeling, we show that the hot spots emerge due to resonant tunneling through localized electronic states created by the polar defects and that the tunneling conductance of the hot spots is controlled by ferroelectric polarization. Our finding of the polarization-controlled defect-assisted tunneling reveals a new mechanism of resistive switching in oxide heterostructures and may have technological implications for ferroelectric tunnel junctions. It is also shown that the conductivity of the hot spots can be modulated by mechanical stress, opening a possibility for development of conceptually new electronic devices with mechanically tunable resistive states.

19.
Adv Mater ; 29(46)2017 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-29064154

RESUMO

Observation of a new type of nanoscale ferroelectric domains, termed as "bubble domains"-laterally confined spheroids of sub-10 nm size with local dipoles self-aligned in a direction opposite to the macroscopic polarization of a surrounding ferroelectric matrix-is reported. The bubble domains appear in ultrathin epitaxial PbZr0.2 Ti0.8 O3 /SrTiO3 /PbZr0.2 Ti0.8 O3 ferroelectric sandwich structures due to the interplay between charge and lattice degrees of freedom. The existence of the bubble domains is revealed by high-resolution piezoresponse force microscopy (PFM), and is corroborated by aberration-corrected atomic-resolution scanning transmission electron microscopy mapping of the polarization displacements. An incommensurate phase and symmetry breaking is found within these domains resulting in local polarization rotation and hence impart a mixed Néel-Bloch-like character to the bubble domain walls. PFM hysteresis loops for the bubble domains reveal that they undergo an irreversible phase transition to cylindrical domains under the electric field, accompanied by a transient rise in the electromechanical response. The observations are in agreement with ab-initio-based calculations, which reveal a very narrow window of electrical and elastic parameters that allow the existence of bubble domains. The findings highlight the richness of polar topologies possible in ultrathin ferroelectric structures and bring forward the prospect of emergent functionalities due to topological transitions.

20.
J Phys Condens Matter ; 29(28): 284001, 2017 Jul 19.
Artigo em Inglês | MEDLINE | ID: mdl-28593933

RESUMO

The instability of ferroelectric ordering in ultra-thin films is one of the most important fundamental issues pertaining realization of a number of electronic devices with enhanced functionality, such as ferroelectric and multiferroic tunnel junctions or ferroelectric field effect transistors. In this paper, we investigate the polarization state of archetypal ultrathin (several nanometres) ferroelectric heterostructures: epitaxial single-crystalline BaTiO3 films sandwiched between the most habitual perovskite electrodes, SrRuO3, on top of the most used perovskite substrate, SrTiO3. We use a combination of piezoresponse force microscopy, dielectric measurements and structural characterization to provide conclusive evidence for the ferroelectric nature of the relaxed polarization state in ultrathin BaTiO3 capacitors. We show that even the high screening efficiency of SrRuO3 electrodes is still insufficient to stabilize polarization in SrRuO3/BaTiO3/SrRuO3 heterostructures at room temperature. We identify the key role of domain wall motion in determining the macroscopic electrical properties of ultrathin capacitors and discuss their dielectric response in the light of the recent interest in negative capacitance behaviour.

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