Nonlinear analytical flame models with amplitude-dependent time-lag distributions

In the present work, we formulate a new method to represent a given Flame Describing Function by analytical expressions. The underlying idea is motivated by the observation that different types of perturbations in a burner travel with different speeds and that the arrival of a perturbation at the flame is spread out over time. We develop an analytical model for the Flame Describing Function, which consists of a superposition of several Gaussians, each characterised by three amplitude-dependent quantities: central time-lag, peak value and standard deviation. These quantities are treated as fitting parameters, and they are deduced from the original Flame Describing Function by using error minimisation and nonlinear optimisation techniques. The amplitude-dependence of the fitting parameters is also represented analytically (by linear or quadratic functions). We test our method by using it to make stability predictions for a burner with well-documented stability behaviour (Noiray's matrix burner). This is done in the time-domain with a tailored Green's function approach

Initial coupling and reaction progression of directly deposited biradical graphene nanoribbon monomers on iodine-passivated versus pristine Ag(111)

The development of widely applicable methods for the synthesis of C-C-bonded nanostructures on inert and insulating surfaces is a challenging yet rewarding milestone in the field of on-surface synthesis. This would enable studies of nearly unperturbed covalent nanostructures with unique electronic properties as graphene nanoribbons (GNR) and π-conjugated 2D polymers. The prevalent Ullmann-type couplings are almost exclusively carried out on metal surfaces to lower the temperature required for initial dehalogenation well below the desorption threshold. To overcome the necessity for the activation of monomers on the target surface, we employ a recently developed Radical Deposition Source (RaDeS) for the direct deposition of radicals onto inert surfaces for subsequent coupling by addition reactions. The radicals are generated en route by indirect deposition of halogenated precursors through a heated reactive tube, where the dehalogenation reaction proceeds. Here, we use the ditopic 6,11-diiodo-1,2,3,4-tetraphenyltriphenylene (DITTP) precursor that afforded chevron-like GNR on Au(111) via the usual two-staged reaction comprised of monomer-coupling into covalent polymers and subsequent formation of an extended GNR by intramolecular cyclodehydrogenation (CDH). As a model system for inert surfaces, we use Ag(111) passivated with a closed monolayer of chemisorbed iodine that behaves in an inert manner with respect to dehalogenation reactions and facilitates the progressive coupling of radicals into extended covalent structures. We deposit the DITTP-derived biradicals onto both iodine-passivated and pristine Ag(111) surfaces. While on the passivated surface, we directly observe the formation of covalent polymers, on pristine Ag(111) organometallic intermediates emerge instead. This has decisive consequences for the further progression of the reaction: heating the organometallic chain directly on Ag(111) results in complete desorption, whereas the covalent polymer on iodine-passivated Ag(111) can be transformed into the GNR. Yet, the respective CDH proceeds directly on Ag(111) after thermal desorption of the iodine passivation. Accordingly, future work is aimed at the further development of approaches for the complete synthesis of GNR on inert surfaces

Instabilities and disorder of the domain patterns in the systems with competing interactions

The dynamics of the domains is studied in a two-dimensional model of the microphase separation of diblock copolymers in the vicinity of the transition. A criterion for the validity of the mean field theory is derived. It is shown that at certain temperatures the ordered hexagonal pattern becomes unstable with respect to the two types of instabilities: the radially-nonsymmetric distortions of the domains and the repumping of the order parameter between the neighbors. Both these instabilities may lead to the transformation of the regular hexagonal pattern into a disordered pattern.Comment: ReVTeX, 4 pages, 3 figures (postscript); submitted to Phys. Rev. Let

Transmission-dominated mid-infrared supermirrors with finesse exceeding 200 000

We fabricate and characterize substrate-transferred single-crystal mirror coatings with 9.33 $\pm$ 0.17 ppm of transmittance and 4.27 $\pm$ 0.52 ppm of excess optical loss, corresponding to a transmission-loss dominated reflectance of 99.9986% at 4.45 $\mu$m. For the first time, a cavity finesse > 200 000 is achieved in the mid-infrared.Comment: Sept 21: Minor revisions to conform to 2-page length requirement including abbr. refs.; Figure font sizes increase

Aeroacoustic response of an array of tubes with and without bias-flow

Heat exchangers, consisting of tube arrays in a cross-flow are a vital component of power generation systems. They are of interest from an acoustic point of view, because they can reflect, transmit and absorb an incident sound wave; in other words, they have the potential to act as a sound absorber and even as a passive control device to prevent a thermoacoustic instability in the power generation system. This paper presents a fundamental study of the aeroacoustic response of a tube array with and without bias-flow (also called cross-flow). The study has a theoretical and experimental side. On the theoretical side, a new model, based on the assumption of quasi-steady flow, was developed to predict the acoustic reflection and transmission coefficient of a tube array with bias-flow. Also, the model by Huang and Heckl (Huang and Heckl, 1993, Acustica 78, 191–200) for the case without bias-flow was evaluated. On the experimental side, flow-duct experiments using a multi-microphone technique were performed to validate the predictions from both models. The agreement was found to be very good for low frequencies. The measurements revealed the limit of validity of the quasi-steady model in terms of the Strouhal number. Although this limit is quite low, our quasi-steady model can serve as a valuable tool for designers of heat exchangers

High harmonic generation in a gas-filled hollow-core photonic crystal fiber

High harmonic generation (HHG) of intense infrared laser radiation (Ferray et al., J. Phys. B: At. Mol. Opt. Phys. 21:L31, 1988; McPherson et al., J. Opt. Soc. Am. B 4:595, 1987) enables coherent vacuum-UV (VUV) to soft-X-ray sources. In the usual setup, energetic femtosecond laser pulses are strongly focused into a gas jet, restricting the interaction length to the Rayleigh range of the focus. The average photon flux is limited by the low conversion efficiency and the low average power of the complex laser amplifier systems (Keller, Nature 424:831, 2003; Südmeyer et al., Nat. Photonics 2:599, 2008; Röser et al., Opt. Lett. 30:2754, 2005; Eidam et al., IEEE J. Sel. Top. Quantum Electron. 15:187, 2009) which typically operate at kilohertz repetition rates. This represents a severe limitation for many experiments using the harmonic radiation in fields such as metrology or high-resolution imaging. Driving HHG with novel high-power diode-pumped multi-megahertz laser systems has the potential to significantly increase the average photon flux. However, the higher average power comes at the expense of lower pulse energies because the repetition rate is increased by more than a thousand times, and efficient HHG is not possible in the usual geometry. So far, two promising techniques for HHG at lower pulse energies were developed: external build-up cavities (Gohle et al., Nature 436:234, 2005; Jones et al., Phys. Rev. Lett. 94:193, 2005) and resonant field enhancement in nanostructured targets (Kim et al., Nature 453:757, 2008). Here we present a third technique, which has advantages in terms of ease of HHG light extraction, transverse beam quality, and the possibility to substantially increase conversion efficiency by phase-matching (Paul et al., Nature 421:51, 2003; Ren et al., Opt. Express 16:17052, 2008; Serebryannikov et al., Phys. Rev. E (Stat. Nonlinear Soft Matter Phys.) 70:66611, 2004; Serebryannikov et al., Opt. Lett. 33:977, 2008; Zhang et al., Nat. Phys. 3:270, 2007). The interaction between the laser pulses and the gas occurs in a Kagome-type Hollow-Core Photonic Crystal Fiber (HC-PCF) (Benabid et al., Science 298:399, 2002), which reduces the detection threshold for HHG to only 200nJ. This novel type of fiber guides nearly all of the light in the hollow core (Couny et al., Science 318:1118, 2007), preventing damage even at intensities required for HHG. Our fiber guided 30-fs pulses with a pulse energy of more than 10μJ, which is more than five times higher than for any other photonic crystal fiber (Hensley et al., Conference on Lasers and Electro-Optics (CLEO), IEEE Press, New York, 2008

Origin of solvent-induced polymorphism in self-assembly of trimesic acid monolayers at solid-liquid interfaces

Encoding information in the chemical structure of tectons is the pivotal strategy in self-assembly for the realization of targeted supramolecular structures. However, frequently observed polymorphism in supramolecular monolayers provides experimental evidence for a decisive additional influence of environmental parameters, such as solute concentration or type of solvent, on structure selection. While concentration-induced polymorphism is comparatively well understood, the thermodynamical and molecular origins of solvent-induced polymorphism remain elusive. To shed light on this fundamental aspect of self-assembly, we explore the solvent-induced polymorphism of trimesic acid (TMA) monolayers on graphite as prototypical example. Using the homologous series of fatty acids as solvents, TMA self-assembles into the anticipated chickenwire polymorph for longer chain fatty acids, whereas the more densely packed, but still porous flower polymorph emerges in shorter chain fatty acids. According to our initial working hypothesis, the origin of this solvent-induced polymorphism lies in a solvent-dependence of the free energy gain. Utilizing an adapted Born-Haber cycle constructed from measured TMA sublimation and dissolution enthalpies as well as Density Functional Theory calculated monolayer binding energies, we quantitatively assessed the self-assembly thermodynamics of both polymorphs in hexanoic, heptanoic, and nonanoic acid. Yet, in contrast to the experimental findings, these results suggest superior thermodynamical stability of the chickenwire polymorph in all solvents. On the other hand, additional experiments comprising variable temperature Scanning Tunneling Microscopy corroborate that the flower polymorph is thermodynamically most stable in hexanoic acid. To resolve this apparent contradiction, we propose a thermodynamical stabilization of the flower polymorph in hexanoic acid through the stereochemically specific co-adsorption of shape-matched solvent molecules in its unique smaller elongated pores. This alternative explanation gains further support from experiments with side-substituted hexanoic acid solvents. Combination of a quantitative thermodynamic analysis and studies with systematic variations of the solvent’s molecular structure holds great promise to enhance the understanding of thus far underexplored solvent effects

A Phase-Field Model of Spiral Dendritic Growth

Domains of condensed-phase monolayers of chiral molecules exhibit a variety of interesting nonequilibrium structures when formed via pressurization. To model these domain patterns, we add a complex field describing the tilt degree of freedom to an (anisotropic) complex-phase-field solidification model. The resulting formalism allows for the inclusion of (in general, non-reflection symmetric) interactions between the tilt, the solid-liquid interface, and the bond orientation. Simulations demonstrate the ability of the model to exhibit spiral dendritic growth.Comment: text plus Four postscript figure file