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Register a new userPhotocurrent Imaging of Multi-Memristive Charge Density Wave Switching in Two-Dimensional 1T-TaS2
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Transport studies of atomically thin 1T-TaS2 have demonstrated the presence of intermediate resistance states across the nearly commensurate (NC) to commensurate (C) charge density wave (CDW) transition, which can be further switched electrically. While this presents exciting opportunities for the material in memristor applications, the switching mechanism has remained elusive and could be potentially attributed to the formation of inhomogeneous C and NC domains across the 1T-TaS2 flake. Here, we present simultaneous electrical driving and scanning photocurrent imaging of CDWs in ultrathin 1T-TaS2 using a vertical heterostructure geometry. While micron-sized CDW domains form upon changing temperature, electrically driven transitions result in largely uniform changes, indicating that states of intermediate resistance for the latter likely correspond to true metastable CDW states in between the NC and C phases, which we then explain by a free energy analysis. Additionally, we are able to perform repeatable and bidirectional switching across the multiple CDW states without changing sample temperature, demonstrating that atomically thin 1T-TaS2 can be further used as a robust and reversible multi-memristor material.
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The layered transition metal dichalcogenides host a rich collection of charge density wave (CDW) phases in which both the conduction electrons and the atomic structure display translational symmetry breaking. Manipulating these complex states by purely electronic methods has been a long-sought scientific and technological goal. Here, we show how this can be achieved in 1T-TaS2 in the two-dimensional (2D) limit. We first demonstrate that the intrinsic properties of atomically-thin flakes are preserved by encapsulation with hexagonal boron nitride in inert atmosphere. We use this facile assembly method together with TEM and transport measurements to probe the nature of the 2D state and show that its conductance is dominated by discommensurations. The discommensuration structure can be precisely tuned in few-layer samples by an in-plane electric current, allowing continuous electrical control over the discommensuration-melting transition in 2D.
We investigate the Ti-doping effect on the charge density wave (CDW) of 1T-TaS2 by combining scanning tunneling microscopy (STM) measurements and first-principle calculations. Although the Ti-doping induced phase evolution seems regular with increasing of the doping concentration (x), an unexpected chiral CDW phase is observed in the sample with x = 0.08, in which Ti atoms almost fully occupy the central Ta atoms in the CDW clusters. The emergence of the chiral CDW is proposed to be from the doping-enhanced orbital order. Only when x = 0.08, the possible long-range orbital order can trigger the chiral CDW phase. Compared with other 3d-elements doped 1T-TaS2, the Ti-doping retains the electronic flat band and the corresponding CDW phase, which is a prerequisite for the emergence of chirality. We expect that introducing elements with a strong orbital character may induce a chiral charge order in a broad class of CDW systems. The present results open up another avenue for further exploring the chiral CDW materials.
We report the interplay between charge-density-wave (CDW) and superconductivity of 1$T$-Fe$_{x}$Ta$_{1-x}$S$_{2}$ ($0leq x leq 0.05$) single crystals. The CDW order is gradually suppressed by Fe-doping, accompanied by the disappearance of pseudogap/Mott-gap as shown by the density functional theory (DFT) calculations. The superconducting state develops at low temperatures within the CDW state for the samples with the moderate doping levels. The superconductivity strongly depends on $x$ within a narrow range, and the maximum superconducting transition temperature is 2.8 K as $x=0.02$. We propose that the induced superconductivity and CDW phases are separated in real space. For high doping level ($x>0.04$), the Anderson localization (AL) state appears, resulting in a large increase of resistivity. We present a complete electronic phase diagram of 1$T$-Fe$_{x}$Ta$_{1-x}$S$_{2}$ system that shows a dome-like $T_{c}(x)$.
Memristive devices whose resistance can be hysteretically switched by electric field or current are intensely pursued both for fundamental interest as well as potential applications in neuromorphic computing and phase-change memory. When the underlying material exhibits additional charge or spin order, the resistive states can be directly coupled, further allowing for electrical control of the collective phases. Here, we report the observation of abrupt, memristive switching of tunneling current in nanoscale junctions of ultrathin CrI$_3$, a natural layer antiferromagnet. The coupling to spin order enables both tuning of the resistance hysteresis by magnetic field, and electric-field switching of magnetization even in multilayer samples.
The transition metal dichalcogenide 1T-TaS2 attract growing attention because of the formation of rich density-wave (DW) and superconducting transitions. However, the origin of the incommensurate DW state at the highest temperature (~ 550 K), which is the parent state of the rich physical phenomena, is still uncovered. Here, we present a natural explanation for the triple-q incommensurate DW in 1T-TaS2 based on the first-principles Hubbard model with on-site U. We apply the paramagnon interference mechanism that gives the nematic order in Fe-based superconductors. The derived order parameter has very unique characters: (i) the orbital-selective nature, and (ii) the unconventional sign-reversal in both momentum and energy spaces. The present study will be useful for understanding rich physics in 1T-TaS2, 1T-VSe2, and other transition metal dichalcogenides.
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