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Register a new userInsights into ultrafast Ge-Te bond dynamics in a phase-change superlattice
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Marco Malvestuto Marco Malvestuto
Publication date
2016
fields
Physics
and research's language is
English
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A long-standing question for avant-grade data storage technology concerns the nature of the ultrafast photoinduced phase transformations in the wide class of chalcogenide phase-change materials (PCMs). Overall, a comprehensive understanding of the microstructural evolution and the relevant kinetics mechanisms accompanying the out-of-equilibrium phases is still missing. Here, after overheating a phase-change chalcogenide superlattice by an ultrafast laser pulse, we indirectly track the lattice relaxation by time resolved X-ray absorption spectroscopy (tr-XAS) with a sub-ns time resolution. The novel approach to the tr-XAS experimental results reported in this work provides an atomistic insight of the mechanism that takes place during the cooling process, meanwhile a first-principles model mimicking the microscopic distortions accounts for a straightforward representation of the observed dynamics. Finally, we envisage that our approach can be applied in future studies addressing the role of dynamical structural strain in phase-change materials.
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Ge2Sb2Te5 and related phase change materials are highly unusual in that they can be readily transformed between amorphous and crystalline states using very fast melt, quench, anneal cycles, although the resulting states are extremely long lived at ambient temperature. These states have remarkably different physical properties including very different optical constants in the visible in strong contrast to common glass formers such as silicates or phosphates. This behavior has been described in terms of resonant bonding, but puzzles remain, particularly regarding different physical properties of crystalline and amorphous phases. Here we show that there is a strong competition between ionic and covalent bonding in cubic phase providing a link between the chemical basis of phase change memory property and origins of giant responses of piezoelectric materials (PbTiO3, BiFeO3). This has important consequences for dynamical behavior in particular leading to a simultaneous hardening of acoustic modes and softening of high frequency optic modes in crystalline phase relative to amorphous. This different bonding in amorphous and crystalline phases provides a direct explanation for different physical properties and understanding of the combination of long time stability and rapid switching and may be useful in finding new phase change compositions with superior properties.
We examine the ultrafast optical response of the crystalline and amorphous phases of the phase change material Ge$_2$Sb$_2$Te$_5$ below the phase transformation threshold. Simultaneous measurement of the transmissivity and reflectivity of thin film samples yields the time-dependent evolution of the dielectric function for both phases. We then identify how lattice motion and electronic excitation manifest in the dielectric response. The dielectric response of both phases is large but markedly different. At 800 nm, the changes in amorphous GST are well described by the Drude response of the generated photo-carriers, whereas the crystalline phase is better described by the depopulation of resonant bonds. We find that the generated coherent phonons have a greater influence in the amorphous phase than the crystalline phase. Furthermore, coherent phonons do not influence resonant bonding. For fluences up to 50% of the transformation threshold, the structure does not exhibit bond softening in either phase, enabling large changes of the optical properties without structural modification.
High-speed electrical switching of Ge2Sb2Te5 (GST) remains a challenging task due to the large impedance mismatch between the low-conductivity amorphous state and the high-conductivity crystalline state. In this letter, we demonstrate an effective doping scheme using nickel to reduce the resistivity contrast between the amorphous and crystalline states by nearly three orders of magnitude. Most importantly, our results show that doping produces the desired electrical performance without adversely affecting the films optical properties. The nickel doping level is approximately 2% and the lattice structure remains nearly unchanged when compared with undoped-GST. The refractive indices at amorphous and crystalline states were obtained using ellipsometry which echoes the results from XRD. The materials thermal transport properties are measured using time-domain thermoreflectance (TDTR), showing no change upon doping. The advantages of this doping system will open up new opportunities for designing electrically reconfigurable high speed optical elements in the near-infrared spectrum.
We report the investigation of the generation and detection of GHz coherent acoustic phonons in plasmonic gold nanoparticles superlattices (NPS). The experiments have been performed from an optical femtosecond pump-probe scheme across the optical plasmon resonance of the superlattice. Our experiments allow to estimate the collective elastic response (sound velocity) of the NPS as well as an estimate of the nano-contact elastic stiffness. It appears that the light-induced coherent acoustic phonon pulse has a typical in-depth spatial extension of about 45 nm which is roughly 4 times the optical skin depth in gold. The modeling of the transient optical reflectivity indicates that the mechanism of phonon generation is achieved through ultrafast heating of the NPS assisted by light excitation of the volume plasmon. These results demonstrate how it is possible to map the photon-electron-phonon interaction in subwavelength nanostructures.
Phase change superlattice is one of the emerging material technologies for ultralow-power phase change memories. However, the resistance switching mechanism of phase change superlattice is still hotly debated. Early electrical measurements and recent materials characterizations have suggested that the Kooi phase is very likely to be the as-fabricated low-resistance state. Due to the difficulty in in-situ characterization at atomic resolution, the structure of the electrically switched superlattice in its high-resistance state is still unknown and mainly investigated by theoretical modellings. So far, there has been no simple model that can unify experimental results obtained from device-level electrical measurements and atomic-level materials characterizations. In this work, we carry out atomistic transport modellings of the phase change superlattice device and propose a simple mechanism accounting for its high resistance. The modeled high-resistance state is based on the interfacial phase changed superlattice that has previously been mistaken for the low-resistance state. This work advances the understanding of phase change superlattice for emerging memory applications.
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