Phase change materials, which show different electrical characteristics across the phase transitions, have attracted considerable research attention for their potential electronic device applications. Materials with metal‐to‐insulator or charge density wave (CDW) transitions such as VO2and 1
The charge density wave material 1T-TaS2exhibits a pulse-induced insulator-to-metal transition, which shows promise for next-generation electronics such as memristive memory and neuromorphic hardware. However, the rational design of TaS2devices is hindered by a poor understanding of the switching mechanism, the pulse-induced phase, and the influence of material defects. Here, we operate a 2-terminal TaS2device within a scanning transmission electron microscope at cryogenic temperature, and directly visualize the changing charge density wave structure with nanoscale spatial resolution and down to 300 μs temporal resolution. We show that the pulse-induced transition is driven by Joule heating, and that the pulse-induced state corresponds to the nearly commensurate and incommensurate charge density wave phases, depending on the applied voltage amplitude. With our in operando cryogenic electron microscopy experiments, we directly correlate the charge density wave structure with the device resistance, and show that dislocations significantly impact device performance. This work resolves fundamental questions of resistive switching in TaS2devices, critical for engineering reliable and scalable TaS2electronics.
more » « less- Award ID(s):
- 2039380
- NSF-PAR ID:
- 10479031
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 14
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
Abstract T ‐TaS2have demonstrated voltage oscillations due to their robust bi‐state resistive switching behavior with some basic neuronal characteristics. BaTiS3is a small bandgap ternary chalcogenide that has recently reported the emergence of CDW order below 245 K. Here, the discovery of DC voltage / current‐induced reversible threshold switching in BaTiS3devices between a CDW phase and a room temperature semiconducting phase is reported. The resistive switching behavior is consistent with a Joule heating scheme and sustained voltage oscillations with a frequency of up to 1 kHz are demonstrated by leveraging the CDW phase transition and the associated negative differential resistance. Strategies of reducing channel sizes and improving thermal management may further improve the device's performance. The findings establish BaTiS3as a promising CDW material for future electronic device applications, especially for energy‐efficient neuromorphic computing. -
Abstract High-density phase change memory (PCM) storage is proposed for materials with multiple intermediate resistance states, which have been observed in 1
T -TaS2due to charge density wave (CDW) phase transitions. However, the metastability responsible for this behavior makes the presence of multistate switching unpredictable in TaS2devices. Here, we demonstrate the fabrication of nanothick verti-lateralH -TaS2/1T -TaS2heterostructures in which the number of endotaxial metallicH -TaS2monolayers dictates the number of resistance transitions in 1T -TaS2lamellae near room temperature. Further, we also observe optically active heterochirality in the CDW superlattice structure, which is modulated in concert with the resistivity steps, and we show how strain engineering can be used to nucleate these polytype conversions. This work positions the principle of endotaxial heterostructures as a promising conceptual framework for reliable, non-volatile, and multi-level switching of structure, chirality, and resistance. -
Abstract A charge density wave (CDW) represents an exotic state in which electrons are arranged in a long‐range ordered pattern in low‐dimensional materials. Although the understanding of the fundamental character of CDW is enriched after extensive studies, its practical application remains limited. Here, an unprecedented demonstration of a tunable charge‐spin interconversion (CSI) in graphene/1T‐TaS2van der Waals heterostructures is shown by manipulating the distinct CDW phases in 1T‐TaS2. Whereas CSI from spins polarized in all three directions is observed in the heterostructure when the CDW phase does not show commensurability, the output of one of the components disappears, and the other two are enhanced when the CDW phase becomes commensurate. The experimental observation is supported by first‐principles calculations, which evidence that chiral CDW multidomains in the heterostructure are at the origin of the switching of CSI. The results uncover a new approach for on‐demand CSI in low‐dimensional systems, paving the way for advanced spin‐orbitronic devices.
-
Abstract Charge density waves are emergent quantum states that spontaneously reduce crystal symmetry, drive metal-insulator transitions, and precede superconductivity. In low-dimensions, distinct quantum states arise, however, thermal fluctuations and external disorder destroy long-range order. Here we stabilize ordered two-dimensional (2D) charge density waves through endotaxial synthesis of confined monolayers of 1T-TaS2. Specifically, an ordered incommensurate charge density wave (oIC-CDW) is realized in 2D with dramatically enhanced amplitude and resistivity. By enhancing CDW order, the hexatic nature of charge density waves becomes observable. Upon heating via in-situ TEM, the CDW continuously melts in a reversible hexatic process wherein topological defects form in the charge density wave. From these results, new regimes of the CDW phase diagram for 1T-TaS2are derived and consistent with the predicted emergence of vestigial quantum order.
-
Ultrashort light pulses can selectively excite charges, spins, and phonons in materials, providing a powerful approach for manipulating their properties. Here we use femtosecond laser pulses to coherently manipulate the electron and phonon distributions, and their couplings, in the charge-density wave (CDW) material 1
T -TaSe2. After exciting the material with a femtosecond pulse, fast spatial smearing of the laser-excited electrons launches a coherent lattice breathing mode, which in turn modulates the electron temperature. This finding is in contrast to all previous observations in multiple materials to date, where the electron temperature decreases monotonically via electron–phonon scattering. By tuning the laser fluence, the magnitude of the electron temperature modulation changes from ∼200 K in the case of weak excitation, to ∼1,000 K for strong laser excitation. We also observe a phase change of π in the electron temperature modulation at a critical fluence of 0.7 mJ/cm2, which suggests a switching of the dominant coupling mechanism between the coherent phonon and electrons. Our approach opens up routes for coherently manipulating the interactions and properties of two-dimensional and other quantum materials using light.