Ultrafast Photovoltaic Response in Ferroelectric Nanolayers

Daranciang, Dan; Highland, Matthew J.; Wen, Haidan; Young, Steve M.; Brandt, Nathaniel C.; Hwang, Harold Y.; Vattilana, Michael; Nicoul, M.; Quirin, F.; Goodfellow, John; Qi, Tingting; Grinberg, Ilya; Fritz, David; Cammarata, Marco; Zhu, Diling; Lemke, Henrik T.; Walko, Donald A.; Đufresne, Eric M.; Li, Yuelin; Larsson, Jörgen; Reis, David A.; Sokolowski‐Tinten, K.; Nelson, Keith A.; Rappe, Andrew M.; Fuoss, P. H.; Stephenson, G. B.; Lindenberg, Aaron M.

doi:10.1103/physrevlett.108.087601

Cited by 170 publications

(140 citation statements)

References 45 publications

(35 reference statements)

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“…9,16,25 In the restrained thermal expansion, the thermal strains were measured in a laser-pump Xray-probe style [26][27][28][29] , as shown in Fig. 1 30,31 and that of the h-LuFeO 3 film (2.0 eV) 25,32 .…”

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Effects of biaxial strain on the improper multiferroicity inh−LuFeO3films studied using the restrained thermal expansion method

et al. 2017

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Elastic strain is potentially an important approach in tuning the properties of the improperly multiferroic hexagonal ferrites, the details of which have however been elusive due to the experimental difficulties. Employing the method of restrained thermal expansion, we have studied the effect of isothermal biaxial strain in the basal plane of h-LuFeO3 (001) films. The results indicate that a compressive biaxial strain significantly enhances the ferrodistortion, and the effect is larger at higher temperatures. The compressive biaxial strain and the enhanced ferrodistortion together, cause an increase in the electric polarization and a reduction in the canting of the weak ferromagnetic moments in h-LuFeO3, according to our first principle calculations. These findings are important for understanding the strain effect as well as the coupling between the lattice and the improper multiferroicity in h-LuFeO3. The experimental elucidation of the strain effect in h-LuFeO3 films also suggests that the restrained thermal expansion can be a viable method to unravel the strain effect in many other epitaxial thin film materials.

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Effects of biaxial strain on the improper multiferroicity inh−LuFeO3films studied using the restrained thermal expansion method

et al. 2017

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“…In turn, these mechanical properties and associated anisotropic response or shape changes are intrinsically linked to the functionality and stability of nanoscale optoelectronic and nanoelectromechanical devices. As such, a real-time probe sensitive to atomic length-scale rearrangements and nanoscale morphological changes is required to elucidate their dynamical and functional response in-situ [13][14][15] .…”

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Visualization of nanocrystal breathing modes at extreme strains

et al. 2015

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Nanoscale dimensions in materials lead to unique electronic and structural properties with applications ranging from site-specific drug delivery to anodes for lithium-ion batteries. These functional properties often involve large-amplitude strains and structural modifications, and thus require an understanding of the dynamics of these processes. Here we use femtosecond X-ray scattering techniques to visualize, in real time and with atomic-scale resolution, light-induced anisotropic strains in nanocrystal spheres and rods. Strains at the percent level are observed in CdS and CdSe samples, associated with a rapid expansion followed by contraction along the nanosphere or nanorod radial direction driven by a transient carrierinduced stress. These morphological changes occur simultaneously with the first steps in the melting transition on hundreds of femtosecond timescales. This work represents the first direct real-time probe of the dynamics of these large-amplitude strains and shape changes in few-nanometre-scale particles.

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“…[7,8] Ultrafast x-ray diffraction (UXRD) emerged as a powerful tool to observe lattice motion in real time [9][10][11] and has provided a deeper insight in the structure-property relations of functional oxides on ultrashort timescales. Recent femtosecond x-ray scattering experiments on ferroelectric oxides showed that electron screening induces an ultrafast piezoelectric response of the lattice [12] and that in turn the deformation leads to a change of the polarization. [13] However, these experiments were conducted on rather perfect epitaxial crystals.…”

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Following Strain-Induced Mosaicity Changes of Ferroelectric Thin Films by Ultrafast Reciprocal Space Mapping

et al. 2013

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We investigate coherent phonon propagation in a thin film of ferroelectric PbZr0.2Ti0.8O3 (PZT) by ultrafast x-ray diffraction (UXRD) experiments, which are analyzed as time-resolved reciprocal space mapping (RSM) in order to observe the in-and out-of-plane structural dynamics simultaneously. The mosaic structure of the PZT leads to a coupling of the excited out-of-plane expansion to in-plane lattice dynamics on a picosecond timescale, which is not observed for out-of-plane compression.Oxides are attractive constituents of future nanoelectronic devices, because of their broad spectrum of outstanding physical properties, such as ferroelectricity and ferromagnetism, and owing to the progress made in the fabrication of high quality epitaxial heterostructures.[1] Epitaxial strain engineering and the careful choice of mechanical and electrical boundary conditions enable a direct influence on these functionalities.[2-6] Structural defects and nanoscale inhomogeneities, such as dislocations and domains, typically affect the properties of functional oxides and have been extensively studied by experiment and theory. [7,8] Ultrafast x-ray diffraction (UXRD) emerged as a powerful tool to observe lattice motion in real time [9][10][11] and has provided a deeper insight in the structure-property relations of functional oxides on ultrashort timescales. Recent femtosecond x-ray scattering experiments on ferroelectric oxides showed that electron screening induces an ultrafast piezoelectric response of the lattice [12] and that in turn the deformation leads to a change of the polarization.[13] However, these experiments were conducted on rather perfect epitaxial crystals. The influence of nano-domains has been considered in experiments on transient phases [14], but the role of static structural defects remained unexplored on such ultrafast timescale.Here we exemplify how ultrafast reciprocal space mapping (URSM) using a laser-based plasma x-ray source yields direct additional information on the reversible inplane structure dynamics in a ferroelectric perovskite PbZr 0.2 Ti 0.8 O 3 (PZT) film which is solely induced by the existence of dislocations typical of such materials. In particular, the width of the PZT Bragg reflection reports that tensile out of plane strain leads to drastically increased damping. The energy flows into in-plane strain which is evidenced by the in-plane component of the reciprocal space map. Our results indicate that in mismatched epitaxial films of oxide materials, with their high * daniel.schick@uni-potsdam.de • a-domains are embedded in the matrix of the c-axis grown tetragonal PZT film, as proved by the AFM topography image in b) as well. Misfit dislocations (MD) and threading dislocations (TD) formed at the SRO-PZT interface and across the PZT film, accounting for the lateral inhomogeneity on a sub-100 nm length scale.susceptibility to the formation of domains and dislocations, in-plane phenomena emerge on a hundred picosecond timescale. URSM yields the relevant information on lateral lattice dynamic...

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Ultrafast Photovoltaic Response in Ferroelectric Nanolayers

Cited by 170 publications

References 45 publications

Effects of biaxial strain on the improper multiferroicity inh−LuFeO3films studied using the restrained thermal expansion method

Effects of biaxial strain on the improper multiferroicity inh−LuFeO3films studied using the restrained thermal expansion method

Visualization of nanocrystal breathing modes at extreme strains

Following Strain-Induced Mosaicity Changes of Ferroelectric Thin Films by Ultrafast Reciprocal Space Mapping

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