Refine
Year of publication
Document Type
- Article (80)
- Postprint (13)
- Other (2)
- Monograph/Edited Volume (1)
Is part of the Bibliography
- yes (96)
Keywords
- Phonons (6)
- nanoparticles (6)
- Lasers (5)
- Bragg peak (4)
- Crystal lattices (4)
- Heterostructures (4)
- Magnetism (4)
- Thermal effects (4)
- Ultrafast X-ray diffraction (4)
- wavelength (4)
- SERS (3)
- gold (3)
- magnetostriction (3)
- ultrafast (3)
- 4-nitrobenzenethiol (2)
- AU (2)
- Femtosecond lasers (2)
- Gold (2)
- HRTEM (2)
- Lattice dynamics (2)
- Magnetooptical effects (2)
- Metal oxides (2)
- Perovskites (2)
- Photoexcitations (2)
- Strain measurement (2)
- Thermodynamic properties (2)
- Thin films (2)
- Transition metals (2)
- Ultrafast X-rays (2)
- aminothiophenol (2)
- catalysis (2)
- charge-transfer (2)
- core-shell nanostructure (2)
- enhanced raman-scattering (2)
- gold nanotriangles (2)
- metal (2)
- monolayer formation (2)
- nanoflowers (2)
- nanoscale heat transfer (2)
- nanotriangles (2)
- negative thermal expansion (2)
- optical-properties (2)
- photocatalysis (2)
- picosecond ultrasonics (2)
- sers (2)
- size (2)
- surface-enhanced Raman scattering (2)
- ultrafast X-ray diffraction (2)
- ultrafast photoacoustics (2)
- ultrafast x-ray diffraction (2)
- Catalytic reaction (1)
- Coherent phonons (1)
- Dynamical X-ray theory (1)
- Gold nanoparticles (1)
- Heat diffusion (1)
- Heterogeneous catalysis (1)
- Incoherent phonons (1)
- Irradiation (1)
- LSPR (1)
- Molecular orientation (1)
- Monomolecular reaction (1)
- N-temperature model (1)
- Nanoparticles (1)
- Nanoscale heat transfer (1)
- Negative (1)
- Picosecond ultrasonics (1)
- Raman spectroscopy (1)
- Reaction mechanism (1)
- SEM (1)
- Silicon (1)
- Surface enhanced Raman scattering (SERS) (1)
- Surface-enhanced Raman scattering (1)
- Thermoelasticity (1)
- Ultrafast dynamics (1)
- Ultrafast photoacoustics (1)
- Ultrafast x-ray (1)
- Ultrafast x-ray diffraction (1)
- X-ray diffraction (1)
- X-ray switching (1)
- absorption measurements (1)
- acoustic waves (1)
- bimetallic nanoparticles (1)
- catanionic surfactant bilayer (1)
- catanionic vesicles (1)
- coherent phonons (1)
- crystal growth (1)
- dimerization (1)
- dynamics (1)
- electron (1)
- epitaxial layers (1)
- exciton plasmon coupling (1)
- gelatin (1)
- gold cluster (1)
- gold nanoflowers (1)
- gold nanostructures (1)
- heat diffusion (1)
- heat measurement (1)
- heat-capacity (1)
- heterogeneous catalysis (1)
- heterostructures (1)
- hyaluronic acid (1)
- hybrid material (1)
- hybrid nanoparticles (1)
- layer-by-layer deposition (1)
- nanoscale energy transports (1)
- nanostructures (1)
- non-equilibrium (1)
- nonequilibrium (1)
- optical pump (1)
- optical pump X-ray probe (1)
- optical-excitation (1)
- phonon (1)
- phonon dispersion relations (1)
- pulse shortening (1)
- rare earth (1)
- scattering (1)
- spin (1)
- strong coupling (1)
- surface deformation (1)
- terahertz waves (1)
- thermal (1)
- thermal expansion (1)
- thin film (1)
- thin film devices (1)
- thin magnetic layers (1)
- time-resolved (1)
- transports (1)
- ultrafast phenomena (1)
- undulated nanoplatelets (1)
- x-ray diffraction (1)
Owing to their ability of concentrating electromagnetic fields to subwavelength mode volumes, plasmonic nanoparticles foster extremely high light-matter coupling strengths reaching far into the strong-coupling regime of light matter interaction. In this article, we present an experimental investigation on the dependence of coupling strength on the geometrical size of the nanoparticle. The coupling strength for differently sized hybrid plasmon-core exciton-shell nanorods was extracted from the typical resonance anticrossing of these systems, obtained by controlled modification of the environment permittivity using layer-by-layer deposition of polyelectrolytes. The observed size dependence of the coupling strength can be explained by a simple model approximating the electromagnetic mode volume by the geometrical volume of the particle. On the basis of this model, the coupling strength for particles of arbitrary size can be predicted, including the particle size necessary to support single-emitter strong coupling.
In the strong coupling regime, exciton and plasmon excitations are hybridized into combined system excitations. The correct identification of the coupling regime in these systems is currently debated, from both experimental and theoretical perspectives. In this article we show that the extinction spectra may show a large peak splitting, although the energy loss encoded in the absorption spectra clearly rules out the strong coupling regime. We investigate the coupling of J-aggregate excitons to the localized surface plasmon polaritons on gold nanospheres and nanorods by fine-tuning the plasmon resonance via layer-by-layer deposition of polyelectrolytes. While both structures show a characteristic anticrossing in extinction and scattering experiments, the careful assessment of the systems’ light absorption reveals that strong coupling of the plasmon to the exciton is not present in the nanosphere system. In a phenomenological model of two classical coupled oscillators, a Fano-like regime causes only the resonance of the light-driven oscillator to split up, while the other one still dissipates energy at its original frequency. Only in the strong-coupling limit do both oscillators split up the frequencies at which they dissipate energy, qualitatively explaining our experimental finding.
The electromagnetic coupling of molecular excitations to plasmonic nanoparticles offers a promising method to manipulate the light-matter interaction at the nanoscale. Plasmonic nanoparticles foster exceptionally high coupling strengths, due to their capacity to strongly concentrate the light-field to sub-wavelength mode volumes. A particularly interesting coupling regime occurs, if the coupling increases to a level such that the coupling strength surpasses all damping rates in the system. In this so-called strong-coupling regime hybrid light-matter states emerge, which can no more be divided into separate light and matter components. These hybrids unite the features of the original components and possess new resonances whose positions are separated by the Rabi splitting energy h Omega. Detuning the resonance of one of the components leads to an anticrossing of the two arising branches of the new resonances omega(+) and omega(-) with a minimal separation of Omega = omega(+) - omega(-).
We report on synchrotron-based high-repetition rate ultrafast x-ray diffraction (UXRD) experiments monitoring the transport of heat from an epitaxial La(0.7)Sr(0.3)MnO(3)/SrTiO(3) superlattice (SL) into the substrate on timescales from 100 ps to 4 mu s. Transient thermal lattice expansion was determined with an accuracy of 10(-7), corresponding to a sensitivity to temperature changes down to 0.01 K. We follow the heat flow within the SL and into the substrate after the impulsive laser heating leads to a small temperature rise of Delta T = 6 K. The transient lattice temperature can be simulated very well using the bulk heat conductivities. This contradicts the interpretation of previous UXRD measurements, which predicted a long-lasting expansion of SrRuO(3) for more than 200 ps. The disagreement could be resolved by assuming that the heat conductivity changes in the first hundred picoseconds.
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.
We report generation of ultra-broadband longitudinal acoustic coherent phonon wavepackets in SrTiO3 (STO) with frequency components extending throughout the first Brillouin zone. The wavepackets are efficiently generated in STO using femtosecond infrared laser excitation of an atomically flat 1.6 nm-thick epitaxial SrRuO3 film. We use femtosecond x-ray diffraction at the European X-Ray Free Electron Laser Facility to study the dispersion and damping of phonon wavepackets. The experimentally determined damping constants for multi-THz frequency phonons compare favorably to the extrapolation of a simple ultrasound damping model over several orders of magnitude.
A diffractometer setup is presented, based on a laser-driven plasma X-ray source for reciprocal-space mapping with femtosecond temporal resolution. In order to map out the reciprocal space, an X-ray optic with a convergent beam is used with an X-ray area detector to detect symmetrically and asymmetrically diffracted X-ray photons simultaneously. The setup is particularly suited for measuring thin films or imperfect bulk samples with broad rocking curves. For quasi-perfect crystalline samples with insignificant in-plane Bragg peak broadening, the measured reciprocal-space maps can be corrected for the known resolution function of the diffractometer in order to achieve high-resolution rocking curves with improved data quality. In this case, the resolution of the diffractometer is not limited by the convergence of the incoming X-ray beam but is solely determined by its energy bandwidth.
Localized excited charge carriers generate ultrafast inhomogeneous strain in the multiferroic BiFeO3
(2014)
We apply ultrafast x-ray diffraction with femtosecond temporal resolution to monitor the lattice dynamics in a thin film of multiferroic BiFeO3 after above-band-gap photoexcitation. The sound-velocity limited evolution of the observed lattice strains indicates a quasi-instantaneous photoinduced stress which decays on a nanosecond time scale. This stress exhibits an inhomogeneous spatial profile evidenced by the broadening of the Bragg peak. These new data require substantial modification of existing models of photogenerated stresses in BiFeO3: the relevant excited charge carriers must remain localized to be consistent with the data.
Using ultrafast X-ray diffraction, we study the coherent picosecond lattice dynamics of photoexcited thin films in the two limiting cases, where the photoinduced stress profile decays on a length scale larger and smaller than the film thickness. We solve a unifying analytical model of the strain propagation for acoustic impedance-matched opaque films on a semi-infinite transparent substrate, showing that the lattice dynamics essentially depend on two parameters: One for the spatial profile and one for the amplitude of the strain. We illustrate the results by comparison with high-quality ultrafast X-ray diffraction data of SrRuO3 films on SrTiO3 substrates. (C) 2014 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License.
Normalization schemes for ultrafast x-ray diffraction using a table-top laser-driven plasma source
(2012)
We present an experimental setup of a laser-driven x-ray plasma source for femtosecond x-ray diffraction. Different normalization schemes accounting for x-ray source intensity fluctuations are discussed in detail. We apply these schemes to measure the temporal evolution of Bragg peak intensities of perovskite superlattices after ultrafast laser excitation.
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.
We investigate coherent phonon propagation in a thin film of ferroelectric PbZr0.2Ti0.8O3 (PZT) by ultrafast x-ray diffraction experiments, which are analyzed as time-resolved reciprocal space mapping 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 time scale, which is not observed for out-of-plane compression.
The importance of plasmonic heating for the plasmondriven photodimerization of 4-nitrothiophenol
(2018)
Metal nanoparticles form potent nanoreactors, driven by the optical generation of energetic electrons and nanoscale heat. The relative influence of these two factors on nanoscale chemistry is strongly debated. This article discusses the temperature dependence of the dimerization of 4-nitrothiophenol (4-NTP) into 4,4′-dimercaptoazobenzene (DMAB) adsorbed on gold nanoflowers by Surface-Enhanced Raman Scattering (SERS). Raman thermometry shows a significant optical heating of the particles. The ratio of the Stokes and the anti-Stokes Raman signal moreover demonstrates that the molecular temperature during the reaction rises beyond the average crystal lattice temperature of the plasmonic particles. The product bands have an even higher temperature than reactant bands, which suggests that the reaction proceeds preferentially at thermal hot spots. In addition, kinetic measurements of the reaction during external heating of the reaction environment yield a considerable rise of the reaction rate with temperature. Despite this significant heating effects, a comparison of SERS spectra recorded after heating the sample by an external heater to spectra recorded after prolonged illumination shows that the reaction is strictly photo-driven. While in both cases the temperature increase is comparable, the dimerization occurs only in the presence of light. Intensity dependent measurements at fixed temperatures confirm this finding.
The importance of plasmonic heating for the plasmondriven photodimerization of 4-nitrothiophenol
(2019)
Metal nanoparticles form potent nanoreactors, driven by the optical generation of energetic electrons and nanoscale heat. The relative influence of these two factors on nanoscale chemistry is strongly debated. This article discusses the temperature dependence of the dimerization of 4-nitrothiophenol (4-NTP) into 4,4′-dimercaptoazobenzene (DMAB) adsorbed on gold nanoflowers by Surface-Enhanced Raman Scattering (SERS). Raman thermometry shows a significant optical heating of the particles. The ratio of the Stokes and the anti-Stokes Raman signal moreover demonstrates that the molecular temperature during the reaction rises beyond the average crystal lattice temperature of the plasmonic particles. The product bands have an even higher temperature than reactant bands, which suggests that the reaction proceeds preferentially at thermal hot spots. In addition, kinetic measurements of the reaction during external heating of the reaction environment yield a considerable rise of the reaction rate with temperature. Despite this significant heating effects, a comparison of SERS spectra recorded after heating the sample by an external heater to spectra recorded after prolonged illumination shows that the reaction is strictly photo-driven. While in both cases the temperature increase is comparable, the dimerization occurs only in the presence of light. Intensity dependent measurements at fixed temperatures confirm this finding.
Nanoscale heating by optical excitation of plasmonic nanoparticles offers a new perspective of controlling chemical reactions, where heat is not spatially uniform as in conventional macroscopic heating but strong temperature gradients exist around microscopic hot spots. In nanoplasmonics, metal particles act as a nanosource of light, heat, and energetic electrons driven by resonant excitation of their localized surface plasmon resonance. As an example of the coupling reaction of 4-nitrothiophenol into 4,4′-dimercaptoazobenzene, we show that besides the nanoscopic heat distribution at hot spots, the microscopic distribution of heat dictated by the spot size of the light focus also plays a crucial role in the design of plasmonic nanoreactors. Small sizes of laser spots enable high intensities to drive plasmon-assisted catalysis. This facilitates the observation of such reactions by surface-enhanced Raman scattering, but it challenges attempts to scale nanoplasmonic chemistry up to large areas, where the excess heat must be dissipated by one-dimensional heat transport.
We present time-resolved x-ray reflectivity measurements on laser excited coherent and incoherent surface deformations of thin metallic films. Based on a kinematical diffraction model, we derive the surface amplitude from the diffracted x-ray intensity and resolve transient surface excursions with sub-angstrom spatial precision and 70 ps temporal resolution. The analysis allows for decomposition of the surface amplitude into multiple coherent acoustic modes and a substantial contribution from incoherent phonons which constitute the sample heating. Published by AIP Publishing.
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. Published by AIP Publishing.
X-ray reflectivity measurements of femtosecond laser-induced transient gratings (TG) are applied to demonstrate the spatiotemporal coherent control of thermally induced surface deformations on ultrafast time scales. Using grazing incidence x-ray diffraction we unambiguously measure the amplitude of transient surface deformations with sub-angstrom 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. can be canceled by a second, time-delayed TG excitation shifted by Lambda/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.
We employ ultrafast X-ray diffraction to compare the lattice dynamics of laser-excited continuous and granular FePt films on MgO (100) substrates. Contrary to recent results on free-standing granular films, we observe in both cases a pronounced and long-lasting out-of-plane expansion. We attribute this discrepancy to the in-plane expansion, which is suppressed by symmetry in continuous films. Granular films on substrates are less constrained and already show a reduced out-of-plane contraction. Via the Poisson effect, out-of-plane contractions drive in-plane expansion and vice versa. Consistently, the granular film exhibits a short-lived out-of-plane contraction driven by ultrafast demagnetization which is followed by a reduced and delayed expansion. From the acoustic reflections of the observed strain waves at the film-substrate interface, we extract a 13% reduction of the elastic constants in thin 10 nm FePt films compared to bulk-like samples. (C) 2018 Author(s).
Watching the Vibration and Cooling of Ultrathin Gold Nanotriangles by Ultrafast X-ray Diffraction
(2016)
We study the vibrations of ultrathin gold nanotriangles upon optical excitation of the electron gas by ultrafast X-ray diffraction. We quantitatively measure the strain evolution in these highly asymmetric nano-objects, providing a direct estimation of the amplitude and phase of the excited vibrational motion. The maximal strain value is well reproduced by calculations addressing pump absorption by the nanotriangles and their resulting thermal expansion. The amplitude and phase of the out-of-plane vibration mode with 3.6 ps period dominating the observed oscillations are related to two distinct excitation mechanisms. Electronic and phonon pressures impose stresses with different time dependences. The nanosecond relaxation of the expansion yields a direct temperature sensing of the nano-object. The presence of a thin organic molecular layer at the nanotriangle/substrate interfaces drastically reduces the thermal conductance to the substrate.