We measured the ultrafast optical response of metal-dielectric superlattices by broadband all-optical pump-probe spectroscopy. The observed phase of the superlattice mode depends on the probe wavelength, making assignments of the excitation mechanism difficult. Ultrafast x-ray diffraction data reveal the true oscillation phase of the lattice which changes as a function of the excitation fluence. This result is confirmed by the fluence dependence of optical transients. We set up a linear chain model of the lattice dynamics and successfully simulated the broadband optical reflection by unit-cell resolved calculation of the strain-dependent dielectric functions of the constituting materials.

Wavevector-selective impulsive excitation of phonon-polaritons by a spectrally broad femtosecond transient grating produces wavepackets propagating in opposite directions. The photons in spectrally narrow probe pulses are scattered from these elementary excitations in lithium niobate (LiNbO3). Both elastically and inelastically scattered photons are simultaneously detected in a spectrometer. The Stokes- and anti-Stokes shifted probe pulses uniquely determine the propagation direction of the detected polariton wavepacket components and correspond to creation or annihilation of phonon-polaritons. Our experiments with spectrally broad pump and spectrally narrow probe pulses allows dissecting the four-wave-mixing process into two sequential stimulated Raman scattering events.

We synthesize sub-THz longitudinal quasimonochromatic acoustic phonons in a SrTiO3 single crystal using a SrRuO3/SrTiO3 superlattice as an optical-acoustic transducer. The generated acoustic phonon spectrum is determined using ultrafast x-ray diffraction. The analysis of the generated phonon spectrum in the time domain reveals a k-vector dependent phonon lifetime. It is observed that even at sub-THz frequencies the phonon lifetime agrees with the 1/omega(2) power law known from Akhiezer's model for hyper sound attenuation. The observed shift of the synthesized spectrum to the higher q is discussed in the framework of nonlinear effects appearing due to the high amplitude of the synthesized phonons.

Phonons are often regarded as delocalized quasiparticles with certain energy and momentum. The anharmonic interaction of phonons determines macroscopic properties of the solid, such as thermal expansion or thermal conductivity, and a detailed understanding becomes increasingly important for functional nanostructures. Although phonon-phonon scattering processes depicted in simple wave-vector diagrams are the basis of theories describing these macroscopic phenomena, experiments directly accessing these coupling channels are scarce. We synthesize monochromatic acoustic phonon wave packets with only a few cycles to introduce nonlinear phononics as the acoustic counterpart to nonlinear optics. Control of the wave vector, bandwidth, and consequently spatial extent of the phonon wave packets allows us to observe nonlinear phonon interaction, in particular, second harmonic generation, in real time by wave-vector-sensitive Brillouin scattering with x-rays and optical photons.

The UDKM1DSIM toolbox is a collection of MATLAB (MathWorks Inc.) classes and routines to simulate the structural dynamics and the according X-ray diffraction response in one-dimensional crystalline sample structures upon an arbitrary time-dependent external stimulus, e.g. an ultrashort laser pulse. The toolbox provides the capabilities to define arbitrary layered structures on the atomic level including a rich database of corresponding element-specific physical properties. The excitation of ultrafast dynamics is represented by an N-temperature model which is commonly applied for ultrafast optical excitations. Structural dynamics due to thermal stress are calculated by a linear-chain model of masses and springs. The resulting X-ray diffraction response is computed by dynamical X-ray theory. The UDKM1DSIM toolbox is highly modular and allows for introducing user-defined results at any step in the simulation procedure. Program summary Program title: udkm1Dsim Catalogue identifier: AERH_v1_0 Program summary URL: http://cpc.cs.qub.ac.uk/summaries/AERH_v1_0.html Licensing provisions: BSD No. of lines in distributed program, including test data, etc.: 130221 No. of bytes in distributed program, including test data, etc.: 2746036 Distribution format: tar.gz Programming language: Matlab (MathWorks Inc.). Computer: PC/Workstation. Operating system: Running Matlab installation required (tested on MS Win XP -7, Ubuntu Linux 11.04-13.04). Has the code been vectorized or parallelized?: Parallelization for dynamical XRD computations. Number of processors used: 1-12 for Matlab Parallel Computing Toolbox; 1 - infinity for Matlab Distributed Computing Toolbox External routines: Optional: Matlab Parallel Computing Toolbox, Matlab Distributed Computing Toolbox Required (included in the package): mtimesx Fast Matrix Multiply for Matlab by James Tursa, xml io tools by Jaroslaw Tuszynski, textprogressbar by Paul Proteus Nature of problem: Simulate the lattice dynamics of 1D crystalline sample structures due to an ultrafast excitation including thermal transport and compute the corresponding transient X-ray diffraction pattern. Solution method: Restrictions: The program is restricted to 1D sample structures and is further limited to longitudinal acoustic phonon modes and symmetrical X-ray diffraction geometries. Unusual features: The program is highly modular and allows the inclusion of user-defined inputs at any time of the simulation procedure. Running time: The running time is highly dependent on the number of unit cells in the sample structure and other simulation parameters such as time span or angular grid for X-ray diffraction computations. However, the example files are computed in approx. 1-5 min each on a 8 Core Processor with 16 GB RAM available.