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A novel fluorinated copolymer (F-PCPDTBT) is introduced and shown to exhibit significantly higher power conversion efficiency in bulk heterojunction solar cells with PC70BM compared to the well-known low-band-gap polymer PCPDTBT. Fluorination lowers the polymer HOMO level, resulting in high open-circuit voltages well exceeding 0.7 V. Optical spectroscopy and morphological studies with energy-resolved transmission electron microscopy reveal that the fluorinated polymer aggregates more strongly in pristine and blended layers, with a smaller amount of additives needed to achieve optimum device performance. Time-delayed collection field and charge extraction by linearly increasing voltage are used to gain insight into the effect of fluorination on the field dependence of free charge-carrier generation and recombination. F-PCPDTBT is shown to exhibit a significantly weaker field dependence of free charge-carrier generation combined with an overall larger amount of free charges, meaning that geminate recombination is greatly reduced. Additionally, a 3-fold reduction in non-geminate recombination is measured compared to optimized PCPDTBT blends. As a consequence of reduced non-geminate recombination, the performance of optimized blends of fluorinated PCPDTBT with PC70BM is largely determined by the field dependence of free-carrier generation, and this field dependence is considerably weaker compared to that of blends comprising the non-fluorinated polymer. For these optimized blends, a short-circuit current of 14 mA/cm(2), an open-circuit voltage of 0.74 V, and a fill factor of 58% are achieved, giving a highest energy conversion efficiency of 6.16%. The superior device performance and the low band-gap render this new polymer highly promising for the construction of efficient polymer-based tandem solar cells.
In this work, a nonaqueous method is used to fabricate thin TiO2 layers. In contrast to the common aqueous sol-gel approach, our method yields layers of anatase nanocrystallites already at low temperature. Raman spectroscopy, electron microscopy and charge extraction by linearly increasing voltage are employed to study the effect of sintering temperature on the structural and electronic properties of the nanocrystalline TiO2 layer. Raising the sintering temperature from 120 to 600 A degrees C is found to alter the chemical composition, the layer's porosity and its surface but not the crystal phase. The room temperature mobility increases from 2 x 10(-6) to 3 x 10(-5) cm(2)/Vs when the sinter temperature is increased from 400 to 600 A degrees C, which is explained by a better interparticle connectivity. Solar cells comprising such nanoporous TiO2 layers and a soluble derivative of cyclohexylamino-poly(p-phenylene vinylene) were fabricated and studied with regard to their structural and photovoltaic properties. We found only weak polymer infiltration into the oxide layer for sintering temperatures up to 550 A degrees C, while the polymer penetrated deeply into titania layers that were sintered at 600 A degrees C. Best photovoltaic performance was reached with a nanoporous TiO2 film sintered at 550 A degrees C, which yielded a power conversion efficiency of 0.5 %. Noticeably, samples with the TiO2 layer dried at 120 A degrees C displayed short-circuit currents and open circuit voltages only about 15-20 % lower than for the most efficient devices, meaning that our nonaqueous route yields titania layers with reasonable transport properties even at low sintering temperatures.
We excite an epitaxial SrRuO3 thin film transducer by a pulse train of ultrashort laser pulses, launching coherent sound waves into the underlying SrTiO3 substrate. Synchrotron-based x-ray diffraction (XRD) data exhibiting separated sidebands to the substrate peak evidence the excitation of a quasi-monochromatic phonon wavepacket with sub-THz central frequency. The frequency and bandwidth of this sound pulse can be controlled by the optical pulse train. We compare the experimental data to combined lattice dynamics and dynamical XRD simulations to verify the coherent phonon dynamics. In addition, we observe a lifetime of 130 ps of such sub-THz phonons in accordance with the theory.
Single-particle tracking has become a standard tool for the investigation of diffusive properties, especially in small systems such as biological cells. Usually the resulting time series are analyzed in terms of time averages over individual trajectories. Here we study confined normal as well as anomalous diffusion, modeled by fractional Brownian motion and the fractional Langevin equation, and show that even for such ergodic systems time-averaged quantities behave differently from their ensemble-averaged counterparts, irrespective of how long the measurement time becomes. Knowledge of the exact behavior of time averages is therefore fundamental for the proper physical interpretation of measured time series, in particular, for extraction of the relaxation time scale from data.
In this work, we show how Gibbs or thermal states appear dynamically in closed quantum many-body systems, building on the program of dynamical typicality. We introduce a novel perturbation theorem for physically relevant weak system-bath couplings that is applicable even in the thermodynamic limit. We identify conditions under which thermalization happens and discuss the underlying physics. Based on these results, we also present a fully general quantum algorithm for preparing Gibbs states on a quantum computer with a certified runtime and error bound. This complements quantum Metropolis algorithms, which are expected to be efficient but have no known runtime estimates and only work for local Hamiltonians.
A Bose-Hubbard model on a dynamical lattice was introduced in previous work as a spin system analogue of emergent geometry and gravity. Graphs with regions of high connectivity in the lattice were identified as candidate analogues of spacetime geometries that contain trapped surfaces. We carry out a detailed study of these systems and show explicitly that the highly connected subgraphs trap matter. We do this by solving the model in the limit of no back-reaction of the matter on the lattice, and for states with certain symmetries that are natural for our problem. We find that in this case the problem reduces to a one-dimensional Hubbard model on a lattice with variable vertex degree and multiple edges between the same two vertices. In addition, we obtain a (discrete) differential equation for the evolution of the probability density of particles which is closed in the classical regime. This is a wave equation in which the vertex degree is related to the local speed of propagation of probability. This allows an interpretation of the probability density of particles similar to that in analogue gravity systems: matter inside this analogue system sees a curved spacetime. We verify our analytic results by numerical simulations. Finally, we analyze the dependence of localization on a gradual, rather than abrupt, falloff of the vertex degree on the boundary of the highly connected region and find that matter is localized in and around that region.
We study phase synchronization in a network motif with a starlike structure in which the central node's (the hub's) frequency is strongly detuned against the other peripheral nodes. We find numerically and experimentally a regime of remote synchronization (RS), where the peripheral nodes form a phase synchronized cluster, while the hub remains free with its own dynamics and serves just as a transmitter for the other nodes. We explain the mechanism for this RS by the existence of a free amplitude and also show that systems with a fixed or constant amplitude, such as the classic Kuramoto phase oscillator, are not able to generate this phenomenon. Further, we derive an analytic expression which supports our explanation of the mechanism.
We present ultrafast X-ray diffraction (UXRD) experiments which sensitively probe impulsively excited acoustic phonons propagating in a SrRuO3/SrTiO3 superlattice and further into the substrate. These findings are discussed together with previous UXRD results (Herzog et al. in Appl. Phys. Lett. 96, 161906, 2010; Woerner et al. in Appl. Phys. A 96, 83, 2009; v. Korff Schmising in Phys. Rev. B 78, 060404(R), 2008 and in Appl. Phys. B 88, 1, 2007) using a normal-mode analysis of a linear-chain model of masses and springs, thus identifying them as linear-response phenomena. We point out the direct correspondence of calculated observables with X-ray signals. In this framework the complex lattice motion turns out to result from an interference of vibrational eigenmodes of the coupled system of nanolayers and substrate. UXRD in principle selectively measures the lattice motion occurring with a specific wavevector, however, each Bragg reflection only measures the amplitude of a delocalized phonon mode in a spatially localized region, determined by the nanocomposition of the sample or the extinction depth of X-rays. This leads to a decay of experimental signals although the excited modes survive.
On 27 February 2010 the M-w 8.8 Maule earthquake in Central Chile ruptured a seismic gap where significant strain had accumulated since 1835. Shortly after the mainshock a dense network of temporary seismic stations was installed along the whole rupture zone in order to capture the aftershock activity. Here, we present the aftershock distribution and first motion polarity focal mechanisms based on automatic detection algorithms and picking engines. By processing the seismic data between 15 March and 30 September 2010 from stations from IRIS, IPGP, GFZ and University of Liverpool we determined 20,205 hypocentres with magnitudes M-w between 1 and 5.5. Seismic activity occurs in six groups: 1.) Normal faulting outer rise events 2.) A shallow group of plate interface seismicity apparent at 25-35 km depth and 50-120 km distance to the trench with some variations between profiles. Along strike, the aftershocks occur largely within the zone of coseismic slip but extend similar to 50 km further north, and with predominantly shallowly dipping thrust mechanisms. Along dip, the events are either within the zone of coseismic slip, or downdip from it, depending on the coseismic slip model used. 3.) A third band of seismicity is observed further downdip at 40-50 km depth and further inland at 150-160 km trench perpendicular distance, with mostly shallow dipping (similar to 28 degrees) thrust focal mechanisms indicating rupture of the plate interface significantly downdip of the coseismic rupture, and presumably above the intersection of the continental Moho with the plate interface. 4.) A deep group of intermediate depth events between 80 and 120 km depth is present north of 36 degrees S. Within the Maule segment, a large portion of events during the inter-seismic phase originated from this depth range. 5.) The magmatic arc exhibits a small amount of crustal seismicity but does not appear to show significantly enhanced activity after the M-w 8.8 Maule 2010 earthquake. 6.) Pronounced crustal aftershock activity with mainly normal faulting mechanisms is found in the region of Pichilemu (similar to 34.5 degrees S). These crustal events occur in a similar to 30 km wide region with sharp inclined boundaries and oriented oblique to the trench. The best-located events describe a plane dipping to the southwest, consistent with one of the focal planes of the large normal-faulting aftershock (M-w = 6.9) on 11 March 2010.
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.