After decades of searching for robust nanoscale ferroelectricity that could enable integration into the next generation memory and logic devices, hafnia-based thin films have appeared as the ultimate candidate because their ferroelectric (FE) polarization becomes more robust as the size is reduced. This exposes a new kind of ferroelectricity, whose mechanism still needs to be understood. Towards this end, thin films with increased crystal quality are needed. We report the epitaxial growth of Hf0.5Zr0.5O2 (HZO) thin films on (001)-oriented La0.7Sr0.3MnO3/SrTiO3 (STO) substrates. The films, which are under epitaxial compressive strain and are predominantly (111)-oriented, display large FE polarization values up to 34 μC/cm 2 and do not need wake-up cycling. Structural characterization reveals a rhombohedral phase, different from the commonly reported polar orthorhombic phase. This unexpected finding allows us to propose a compelling model for the formation of the FE phase. In addition, these results point towards nanoparticles of simple oxides as a vastly unexplored class of nanoscale ferroelectrics.
Phase-change materials undergo rapid and reversible crystalline-to-amorphous structural transformation and are being used for nonvolatile memory devices. However, the transformation mechanism remains poorly understood. We have studied the effect of electrical pulses on the crystalline-to-amorphous phase change in a single-crystalline Ge(2)Sb(2)Te(5) (GST) nanowire memory device by in situ transmission electron microscopy. We show that electrical pulses produce dislocations in crystalline GST, which become mobile and glide in the direction of hole-carrier motion. The continuous increase in the density of dislocations moving unidirectionally in the material leads to dislocation jamming, which eventually induces the crystalline-to-amorphous phase change with a sharp interface spanning the entire nanowire cross section. The dislocation-templated amorphization explains the large on/off resistance ratio of the device.
Unconventional ferroelectricity exhibited by hafnia-based thin films, robust at nanoscale sizes, presents tremendous opportunities in nanoelectronics. However, the exact nature of polarization switching remains controversial. We investigated La0.67Sr0.33MnO3/Hf0.5Zr0.5O2 capacitor interfaced with various top electrodes while in situ electrical biasing using atomic resolution microscopy with direct oxygen imaging, as well as synchrotron nanobeam diffraction. When the top electrode is oxygen reactive, we clearly show reversible oxygen vacancy migration with electrodes being the source and sink of oxygen, and the dielectric layer acting as a fast conduit at millisecond timescales. With non-reactive top electrodes and at longer time scales (seconds), the dielectric layer also acts as an oxygen source/sink. Our results show that ferroelectricity in hafnia-based thin films is unmistakably intertwined to oxygen voltammetry.
Strong coupling of light with excitons in direct bandgap semiconductors leads to the formation of composite photonic-electronic quasi-particles (polaritons), in which energy oscillates coherently between the photonic and excitonic states with the vacuum Rabi frequency. The light-matter coherence is maintained until the oscillator dephases or the photon escapes. Exciton-polariton formation has enabled the observation of Bose-Einstein condensation in the solid-state, low-threshold polariton lasing and is also useful for terahertz and slow-light applications. However, maintaining coherence for higher carrier concentration and temperature applications still requires increased coupling strengths. Here, we report on size-tunable, exceptionally high exciton-polariton coupling strengths characterized by a vacuum Rabi splitting of up to 200 meV as well as a reduction in group velocity, in surfacepassivated, self-assembled semiconductor nanowire cavities. These experiments represent systematic investigations on light-matter coupling in one-dimensional optical nanocavities, demonstrating the ability to engineer light-matter coupling strengths at the nanoscale, even in non-quantum-confined systems, to values much higher than in bulk.cavity | waveguide | cadmium sulfide E xciton-polaritons (1, 2) are fundamental to many exciting observations due to their hybrid photonic-electronic properties, including reduced effective mass when compared with excitons, bosonic particle statistics, long coherence lengths, and large scattering cross-sections (3). While strong optical coupling in the single-quantum limit provides tremendous possibilities for quantum information processing through quantum electrodynamic effects, (4, 5) it is through the use of strong optical coupling in many particle systems that phenomena such as Bose-Einstein condensation in the solid-state (6, 7) and low-threshold polariton lasing and light emission (8, 9) have been discovered. In addition, many particle strong coupling provides tremendous possibilities for slow-light (10) and terahertz (11) applications using collective effects.The strong-coupling regime in the solid-state is generally obtained by confining excitons in semiconductor quantum dots (QD) and wells (QW) in order to enhance their oscillator transition strengths and coupling them to the low-loss optical mode of small mode volume optical cavities that enhance the electromagnetic field density (2, 12-15). The coupling strength is expressed as the Rabi frequency, g ∝ ffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi ffi n à f ∕V m p , (4, 13, 16) with n the number of oscillators, f their oscillator strength, and V m the mode volume, noting that the photon lifetime as determined by cavity quality factor (Q) should be long enough to allow for the Rabi oscillation to occur. The extremely high Q of micropillar cavities, (13) photonic slab crystals (14), and micro-toroids (15) have previously allowed QWs and QDs embedded at optical field antinodes to exhibit strong coupling, even though the oscillato...
Piezoelectric actuators transform electrical energy into mechanical energy, and because of their compactness, quick response time and accurate displacement, they are sought after in many applications. Polycrystalline piezoelectric ceramics are technologically more appealing than single crystals due to their simpler and less expensive processing, but have yet to display electrostrain values that exceed 1%. Here we report a material design strategy wherein the efficient switching of ferroelectric-ferroelastic domains by an electric field is exploited to achieve a high electrostrain value of 1.3% in a pseudo-ternary ferroelectric alloy system, BiFeO-PbTiO-LaFeO. Detailed structural investigations reveal that this electrostrain is associated with a combination of several factors: a large spontaneous lattice strain of the piezoelectric phase, domain miniaturization, a low-symmetry ferroelectric phase and a very large reverse switching of the non-180° domains. This insight for the design of a new class of polycrystalline piezoceramics with high electrostrains may be useful to develop alternatives to costly single-crystal actuators.
Phase change materials (PCMs) are highly attractive for nonvolatile electrical and all-optical memory applications because of unique features such as ultrafast and reversible phase transitions, long-term endurance, and high scalability to nanoscale dimensions. Understanding their transient characteristics upon phase transition in both the electrical and the optical domains is essential for using PCMs in future multifunctional optoelectronic circuits. Here, we use a PCM nanowire embedded into a nanophotonic circuit to study switching dynamics in mixed-mode operation. Evanescent coupling between light traveling along waveguides and a phase-change nanowire enables reversible phase transition between amorphous and crystalline states. We perform time-resolved measurements of the transient change in both the optical transmission and resistance of the nanowire and show reversible switching operations in both the optical and the electrical domains. Our results pave the way toward on-chip multifunctional optoelectronic integrated devices, waveguide integrated memories, and hybrid processing applications.
Structural defects and their dynamics play an important role in controlling the behavior of phase-change materials (PCM) used in low-power nonvolatile memory devices. However, not much is known about the influence of disorder on the electronic properties of crystalline PCM prior to a structural phase-change. Here, we show that the application of voltage pulses to single-crystalline GeTe nanowire memory devices introduces structural disorder in the form of dislocations and antiphase boundaries (APB). The dynamic evolution and pile-up of APBs increases disorder at a local region of the nanowire, which electronically transforms it from a metal to a dirty metal to an insulator, while still retaining single-crystalline long-range order. We also observe that close to this metal-insulator transition, precise control over the applied voltage is required to create an insulating state; otherwise the system ends up in a more disordered amorphous phase suggesting the role of electronic instabilities during the structural phase-change.
Crystal–amorphous transformation achieved via the melt-quench pathway in phase-change memory involves fundamentally inefficient energy conversion events; and this translates to large switching current densities, responsible for chemical segregation and device degradation. Alternatively, introducing defects in the crystalline phase can engineer carrier localization effects enhancing carrier–lattice coupling; and this can efficiently extract work required to introduce bond distortions necessary for amorphization from input electrical energy. Here, by pre-inducing extended defects and thus carrier localization effects in crystalline GeTe via high-energy ion irradiation, we show tremendous improvement in amorphization current densities (0.13–0.6 MA cm−2) compared with the melt-quench strategy (∼50 MA cm−2). We show scaling behaviour and good reversibility on these devices, and explore several intermediate resistance states that are accessible during both amorphization and recrystallization pathways. Existence of multiple resistance states, along with ultralow-power switching and scaling capabilities, makes this approach promising in context of low-power memory and neuromorphic computation.
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