Strain rate induced crystallization in bulk metallic glass-forming liquid

We report on the solidification of Au49, Ag5.5, Pd2.3, Cu26.9, Si16.3 bulk metallic glass under various strain rates. Using a copper mold casting technique with a low strain rate during solidification, this alloy is capable of forming glassy rods of at least 5 mm in diameter. Surprisingly, when the liquid alloy is splat cooled at much higher cooling rates and large strain rates, the solidified alloy is no longer fully amorphous. Our finding suggests that the large strain rate during splat cooling induces crystallization. The pronounced difference in crystallization behavior cannot be explained by the previously observed strain rate effect on viscosity alone. A strain rate induced phase separation process is suggested as one of the explanations for this crystallization behavior. The strain-rate-dependent critical cooling rate must be considered in order to assess the intrinsic glass forming ability of metallic liquid.     

Kinetic roughening of laser deposited polymer films: crossover from single particle character to continuous growth

The crossover in kinetic roughening of thin films from a particle-character-dominated regime to continuous growth behavior has been observed in this work. This has been accomplished by atomic force microscopy investigations of pulsed laser deposited amorphous organic films with thicknesses ranging from several nanometers to more than 4 microm. The early-stage random-deposition-like processes end once a closed layer is formed, which grows without saturation on the characteristic length scales. In addition, the influence of oblique film deposition has been examined and interpreted.     

Convergence of dynamical zeta functions

I study poles and zeros of zeta functions in one-dimensional maps. Numerical and analytical arguments are given to show that the first pole of one such zeta function is given by the first zero ofanother zeta function: this describes convergence of the calculations of the first zero, which is generally the physically interesting quantity. Some remarks on how these results should generalize to zeta functions of dynamical systems with pruned symbolic dynamics and in higher dimensions follow.     

Deconstructing spatiotemporal chaos using local symbolic dynamics

We find that the global symbolic dynamics of a diffusively coupled map lattice is well approximated by a very small local model for weak to moderate coupling strengths. A local symbolic model is a truncation of the full symbolic model to one that considers only a single element and a few neighbors. Using interval analysis, we give rigorous results for a range of coupling strengths and different local model widths. Examples are presented of extracting a local symbolic model from data and of controlling spatiotemporal chaos.     

Interaction dynamics of elastic waves with a complex nonlinear scatterer through the use of a time reversal mirror

This Letter reports on work performed to locate and interrogate a nonlinear scatterer in a linearly elastic medium through the use of a time reversal mirror in combination with nonlinear dynamics. Time reversal provides the means to spatially and temporally localize elastic energy on a scattering feature while the nonlinear dynamics spectrum allows one to determine whether the scatterer is nonlinear (e.g., mechanical damage). Here elastic waves are measured in a solid and processed to extract the nonlinear elastic response. The processed elastic signals are then time reversed, rebroadcast, and found to focus on the nonlinear scatterer, thus defining a time-reversed nonlinear elastic wave spectroscopy process. Additionally, the focusing process illuminates the complexity of the nonlinear scatterer in both space and time, providing a means to image and investigate the origins and physical mechanisms of the nonlinear elastic response.     

Azobenzene-functionalized alkanethiols in self-assembled monolayers on gold

Self-assembled monolayers (SAMs) of 4-trifluoromethyl-azobenzene-4′-methyleneoxy-alkanethiols (CF₃– C₆H₄–N=N–C₆H₄–O–(CH₂) _n –SH on (111)-oriented poly-crystalline gold films on mica were examined by X-ray photoelectron spectroscopy (XPS) and X-ray absorption spectroscopy (XAS). The spectra are analyzed with the help of density-functional-theory calculations of the isolated molecule. Only one doublet is detected in the sulphur 2p spectra of the investigated SAMs, consistent with a thiolate bond of the molecule to the gold surface. The C 1s XP spectra and the corresponding XAS π ^* resonance exhibit a rich structure which is assigned to the carbon atoms in the different chemical surroundings. Comparing XPS binding energies of the azobenzene moiety and calculated initial-state shifts reveals comparable screening of all C 1s core holes. While the carbon 1s XPS binding energy lies below the π ^*-resonance excitation-energy, the reversed order is found comparing core ionization and neutral core excitation of the nitrogen 1s core-hole of the azo group. This surprising difference in core-hole binding energies is interpreted as site-dependent polarization screening and charge transfer among the densely packed aromatic moieties. We propose that a quenching of the optical excitation within the molecular layer is thus one major reason for the low trans to cis photo-isomerization rate of azobenzene in aromatic-aliphatic SAMs.     

Water vapor: An extraordinary terahertz wave source under optical excitation

In modern terahertz (THz) sensing and imaging spectroscopy, water is considered a nemesis to be avoided due to strong absorption in the THz frequency range. Here we report the first experimental demonstration and theoretical implications of using femtosecond laser pulses to generate intense broadband THz emission from water vapor. When we focused an intense laser pulse in water vapor contained in a gas cell or injected from a gas jet nozzle, an extraordinarily strong THz field from optically excited water vapor is observed. Water vapor has more than 50% greater THz generation efficiency than dry nitrogen. It had previously been assumed that the nonlinear generation of THz waves in this manner primarily involves a free-electron plasma, but we show that the molecular structure plays an essential role in the process. In particular, we found that THz wave generation from H₂O vapor is significantly stronger than that from D₂O vapor. Vibronic activities of water cluster ions, occurring naturally in water vapor, may possibly contribute to the observed isotope effect along with rovibrational contributions from the predominant monomers.     

Probing noise in flux qubits via macroscopic resonant tunneling

Macroscopic resonant tunneling between the two lowest lying states of a bistable rf SQUID is used to characterize noise in a flux qubit. Measurements of the incoherent decay rate as a function of flux bias revealed a Gaussian-shaped profile that is not peaked at the resonance point but is shifted to a bias at which the initial well is higher than the target well. The rms amplitude of the noise, which is proportional to the dephasing rate 1/tauphi, was observed to be weakly dependent on temperature below 70 mK. Analysis of these results indicates that the dominant source of low energy flux noise in this device is a quantum mechanical environment in thermal equilibrium.     

Observation of anomalous phonon softening in bilayer graphene

The interaction of electron-hole pairs with lattice vibrations exhibits a wealth of intriguing physical phenomena such as the renowned Kohn anomaly. Here we report the observation in bilayer graphene of an unusual phonon softening that provides the first experimental proof for another type of phonon anomaly. Similar to the Kohn anomaly, which is a logarithmic singularity in the phonon group velocity [W. Kohn, Phys. Rev. Lett. 2, 393 (1959)], the observed phonon anomaly exhibits a logarithmic singularity in the optical-phonon energy. Arising from a resonant electron-phonon coupling effect, the anomaly was also expected, albeit not observed, in monolayer graphene. We propose an explanation for why it is easier to observe in bilayer samples.     

Mechanisms of Resonant Infrared Matrix-Assisted Pulsed Laser Evaporation

For the last decade, a variant of pulsed laser ablation, Resonant-Infrared Matrix-Assisted Pulsed Laser Evaporation (RIR-MAPLE), has been studied as a deposition technique for organic and polymeric materials. RIR-MAPLE minimizes photochemical damage from direct interaction with the intense laser beam by encapsulating the polymer in a high infrared-absorption solvent matrix. This review critically examines the thermally-induced ablation mechanisms resulting from irradiation of cryogenic solvent matrices by a tunable free electron laser (FEL). A semi-empirical model is used to calculate temperatures as a function of time in the focal volume and determine heating rates for different resonant modes in two model solvents, based on the thermodynamics and kinetics of the phase transitions induced in the solvent matrices. Three principal ablation mechanisms are discussed, namely normal vaporization at the surface, normal boiling, and phase explosion. Normal vaporization is a highly inefficient polymer deposition mechanism as it relies on collective collisions with evaporating solvent molecules. Diffusion length calculations for heterogeneously nucleated vapor bubbles show that normal boiling is kinetically limited. During high-power pulsed-FEL irradiation, phase explosion is shown to be the most significant contribution to polymer deposition in RIR-MAPLE. Phase explosion occurs when the target is rapidly heated (10⁸ to 10¹⁰ K/s) and the solvent matrix approaches its critical temperature. Spontaneous density stratification (spinodal decay) within the condensed metastable phase leads to rapid homogeneous nucleation of vapor bubbles. As these vapor bubbles interconnect, large pressures build up within the condensed phase, leading to target explosions and recoil-induced ejections of polymer to a near substrate. Phase explosion is a temperature (fluence) threshold-limited process, while surface evaporation can occur even at very low fluences.