X-ray reflectivity (XRR) measurements of femtosecond laser-induced transient gratings (TG) are applied to demonstrate the spatio-temporal coherent control of thermally induced surface deformations on ultrafast timescales. Using grazing incidence x-ray diffraction we unambiguously measure the amplitude of transient surface deformations with sub-Å resolution. Understanding the dynamics of femtosecond TG excitations in terms of superposition of acoustic and thermal gratings makes it possible to develop new ways of coherent control in x-ray diffraction experiments. Being the dominant source of TG signal, the long-living thermal grating with spatial period Λ can be canceled by a second, time-delayed TG excitation shifted by Λ/2. The ultimate speed limits of such an ultrafast x-ray shutter are inferred from the detailed analysis of thermal and acoustic dynamics in TG experiments. [5][6][7] or plasmonic [8,9] degrees of freedom. Strain-induced phenomena may be used to discover new material properties and develop new applications, for example the modification of optical and electronic properties in semiconductor nanostructures [10]. Surface acoustic waves (SAWs) are often employed as a source of lattice strain. They can be generated [11] and controlled [12] optically via the excitation of transient gratings (TGs) [13,14]. Recently, these TG-excitations heave been used to probe heat transport in suspended thin films [15] and magneto-elastic coupling in thin nickel films [16][17][18]. Optical excitation of a solid generates not only coherent sound waves but also incoherent thermal strain. Coherent excitations can be controlled in amplitude and phase by series of light pulses in time domain, which is labeled temporal coherent control [19]. The main fraction of the deposited optical energy is stored in incoherent excitations of the lattice, i.e., heat [20,21] which can consequently not be controlled by a temporal sequence of light pulses. This thermal lattice excitation often generates a background which makes is difficult to precisely observe the coherent acoustic signal in purely optical experiments.In this letter we demonstrate, for the first time, the coherent control of incoherent, thermal transient gratings. We apply spatio-temporal coherent control showing that the spatial part of coherent control adds a new degree of freedom to control the amplitude and the phase of a thermally deformed surface. This is clearly a new approach that introduces the concept of spatial coherent control to the dynamics of incoherent excitations on ultrafast time scales, a phenomenon impossible to achieve with temporal coherent control only. We also demonstrate the control of a transient thermal grating on a timescale faster than the oscillation of the simultaneously excited coherent acoustic modes. Our new quantitative method allows for decomposing the coherent and incoherent dynamics in the sample by measuring the amplitude of the surface excursion with sub-Å precision and ≈ 70 ps temporal resolution. The modification of x-ray diffracti...
A highly regular one-dimensional domain pattern is formed in ferroelectric K 0.75 Na 0.25 NbO 3 thin films grown on (110) TbScO 3 substrates using metalorganic chemical vapour deposition (MOCVD). The domain pattern exhibits a lateral periodicity of about 50 nm and extends over several micrometres. The monoclinic symmetry of the domains is controlled by the elastic anisotropy of K 0.75 Na 0.25 NbO 3 and the anisotropic lattice strain, which is highly compressive in one in-plane direction and weakly tensile in the corresponding orthogonal direction. Using piezoresponse force microscopy and X-ray diffraction, the monoclinic M A phase is identified, which is associated with both a strong vertical and a lateral electric polarization component. The lateral component of the polarization vector is collinear with the AE[110] pc shear direction of the pseudocubic unit cell of the film and changes periodically by 180 in adjacent domains. A structural variant of a 90 rotated M A domain pattern, where the monoclinic distortion of the pseudocubic unit cells occurs along AE[110] pc , is also observed. However, this variant appears with significantly lower probability, in agreement with energy considerations based on linear elasticity theory. Thus, the incorporation of highly anisotropic lattice strain provides the opportunity to grow one-dimensional nanostructures with high ferroelectric properties.
ZrO2‐Al2O3 Bragg reflectors for future application in ZnO based resonators grown by pulsed laser deposition on c‐plane sapphire and silicon substrates show a reflectivity up to 99.8% with a layer pair number of 12.5. Layer thicknesses obtained from standard ellipsometry agree very well with thicknesses observed by transmission scanning electron microscopy. A very smooth surface roughness of Ra = 0.5 nm was observed for these Bragg reflectors. ZnO thin films grown on bulk c‐plane sapphire and on Bragg reflectors revealed comparable high photoluminescence intensity. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)
We present a nanostructured device that functions as photoacoustic hard x-ray switch. The device is triggered by femtosecond laser pulses and allows for temporal gating of hard x-rays on picosecond (ps) timescales. It may be used for pulse picking or even pulse shortening in 3rd generation synchrotron sources. Previous approaches mainly suffered from insufficient switching contrasts due to excitation-induced thermal distortions. We present a new approach where thermal distortions are spatially separated from the functional switching layers in the structure. Our measurements yield a switching contrast of 14, which is sufficient for efficient hard x-ray pulse shortening. The optimized structure also allows for utilizing the switch at high repetition rates of up to 208 kHz.
The authors report on the fabrication of high quality all-oxide Bragg reflectors (BRs) and ZnO based resonators. The resonator consists of a bulk half-wavelength ZnO microcavity embedded between two BRs, each made of 10.5 layer pairs of yttria stabilized zirconia and Al2O3. Scanning transmission electron microscopy and atomic force microscopy, yield smooth interfaces and low surface roughness for the BR as well as the resonator. For the BR with 10.5 layer pairs the authors obtain reflectivities up to 99.2% within the Bragg stop band. The exciton-polariton dispersion was determined by both, polarization- and angle-resolved photoluminescence (PL) and reflectivity (R) measurements. The detuning between the uncoupled exciton mode and photon mode was changed by shifting the exciton mode energy in the temperature range of 10–290 K. Thereby we observed that a strong exciton-photon coupling regime up to room temperature is present in our resonators with maximum values of the Rabi splitting of about 68 meV (PL, T=10 K) and 76 meV (R,T=10 K).
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