Excitable dynamics in high-Lewis number premixed gas combustion at normal and microgravity

Freely-propagating, premixed gas flames in high-Lewis (Le) number, quiescent mixtures are studied experimentally in tubes of various diameter at normal (lg) and microgravity (mu g). A premixture of lean butane and oxygen diluted with helium, argon, neon, nitrogen or a mixture of multiple diluents is examined such that the thermal diffusivity of the mixture (and to a lesser extent, the mass diffusivity of the rate-limiting component) is systematically varied. In effect, different diluents allow variation of the Le without changing the chemistry. The flames are recorded with high speed cinematography and their stability is visually assessed. Different modes of propagation were observed depending on the diameter of the tubes (different conductive heat loss), the composition of the mixture and the g-level. At 1g, four modes of propagation were observed in small and intermediate diameter tubes (large conductive heat loss): (1) steadily propagating flames, (2) radial and longitudinal pulsating flames, (3) 'wavering' flames, and (4) rotating spiral flames. As the diameter of the tube increases, the radial modes become more pronounced while the longitudinal modes systematically disappear. Also, multiple, simultaneous, spatially-separated 'pacemaker' sites are observed in intermediate and large diameter tubes. Each site starts as a small region of high luminosity and develops into a flamelet which assumes the form of one of the fore mentioned modes. These flamelets eventually interact, annihilate each other in their regions of intersection and merge at their newly created free-ends. For very large tubes, radially-propagating wave-trains (believed to be 'trigger waves') are observed. These are analogous to the radial pulsations observed in the smaller diameter tubes. At mu g, three modes of propagation have been observed: (1) steadily propagating flames, (2) radial and longitudinal pulsating flames, and (3) multi-armed, rotating flames. Since the pulsating mode exists at mu g and 1g, buoyant flicker is not the mechanism which drives the pulsations. Moreover, all of the instabilities at 1g and mu g have characteristic frequencies on the O(100Hz). This value is lower than the fundamental, longitudinal acoustic frequencies of the tubes which suggests that the instabilities are not acoustically driven. The patterns formed by this reaction bear remarkable similarities with the patterns formed in most excitable media when the behavior of the system is driven by couplings between chemical reaction and diffusion (e.g., Belousov-Zhabotinsky reaction, Patterns in slime molds, spiral waves in the retina of a bird's eye). While it is recognized that the chemical mechanism associated with this premixed gas reaction is exponentially sensitive to temperature and undoubtedly different from those which govern previously observed excitable media (most are isothermal, or weakly exothermic, liquid phase reactions), similar spatial and temporal patterns should not come as a complete surprise considering heat and mass diffusion are self similar. It is concluded that this premixed gas system is a definitive example of a diffusive-thermal, gas-phase oscillator based on these experimental results and their favorable comparison with theory.