4D spatiotemporal evolution of liquid spray using kilohertz-rate x-ray computed tomography.

Four-dimensional (x,y,z,t) x-ray computed tomography was demonstrated in an optically complex spray using an imaging system consisting of three x-ray sources and three high-speed detectors. The x-ray sources consisted of high-flux rotating anode x-ray tube sources that illuminated the spray from three lines of sight. The absorption, along each absorption path, was collected using a CsI phosphor plate and imaged by a high-speed intensified CMOS camera at 20 kHz. The radiographs were converted to a quantitative equivalent path length (EPL) of liquid using a variable attenuation coefficient to account for beam hardening. The EPL data were then reconstructed using the algebraic reconstruction technique into high-speed time sequences of the three-dimensional liquid mass distribution.

Two-color volumetric laser-induced fluorescence for 3D OH and temperature fields in turbulent reacting flows.

Single-shot, two-color, volumetric laser-induced fluorescence was demonstrated for three-dimensional (3D), tomographic imaging of the structural properties of the OH radical and temperature field in a turbulent hydrogen-air flame. Two narrowband laser sources were tuned to the Q1(5) and Q1(14) transitions of the (1,0) band in the A2Σ←X2Π system and illuminated a volumetric region of the flame. Images from eight unique perspectives collected simultaneously from each of the two transitions were used to reconstruct overlapping OH fields with different Boltzmann fractions and map the 3D temperature distribution with nanosecond precision. Key strategies for minimizing sources of error, such as detector sensitivity and spatial overlap of the two fields, are discussed.

Towards elucidating the photochemistry of the sunscreen filter ethyl ferulate using time-resolved gas-phase spectroscopy.

Ultrafast time-resolved ion yield (TR-IY) and velocity map imaging spectroscopies are employed to reveal the relaxation dynamics after photoexcitation in ethyl 4-hydroxy-3-methoxycinnamate (ethyl ferulate, EF), an active ingredient in commercially available sunscreens. In keeping with a bottom-up strategy, the building blocks of EF, 2-methoxy-4-vinylphenol (MVP) and 4-hydroxy-3-methoxycinnamyl alcohol (coniferyl alcohol, ConA), were also studied to assist in our understanding of the dynamics of EF as we build up in molecular complexity. In contrast to the excited state dynamics of MVP and ConA, which are described by a single time constant (>900 ps), the dynamics of EF are described by three time constants (15 ± 4 ps, 148 ± 47 ps, and >900 ps). A mechanism is proposed involving internal conversion (IC) between the initially excited S1(11ππ*) and S2(11nπ*) states followed by intramolecular vibrational redistribution (IVR) on both states, in competition with intersystem crossing onto neighbouring triplet states (15 ± 4 ps). IVR and IC within the triplet manifold then ensues (148 ± 47 ps) to populate a low-lying triplet state (>900 ps). Importantly, the fluorescence spectrum of EF at the S1 origin, along with the associated lifetime (6.9 ± 0.1 ns), suggests that population is trapped, during initial IVR, on the S1(11ππ*) state. This serves to demonstrate the complex, competing dynamics in this sunscreen filter molecule.

One-dimensional single-shot thermometry in flames using femtosecond-CARS line imaging.

We report single-laser-shot one-dimensional thermometry in flames using femtosecond coherent anti-Stokes Raman scattering (fs-CARS) line imaging. Fs-CARS enables high-repetition-rate (1-10 kHz), nearly collision-free measurement of temperature and species concentration in reacting flows. Two high-power 800 nm beams are used as the pump and probe beams and a 983 nm beam is used as the Stokes beam for CARS signal generation from the N2Q-branch transitions at ∼2330 cm(-1). The probe beam is frequency-chirped for single-laser-shot imaging. All three laser beams are formed into sheets and crossed in a line which forms the probe region. The resulting 1D line-CARS signal at ∼675 nm is spatially and spectrally resolved and recorded as a two-dimensional (2D) image. Single-shot temperature measurements are demonstrated in flat-field flames up to temperatures exceeding 2000 K, demonstrating the potential of fs-CARS line imaging for high-repetition-rate thermometry in turbulent flames. Such measurements can provide valuable data to validate complex turbulent-combustion models as well as increase the understanding of the spatio-temporal instabilities in practical combustion devices such as modern gas-turbine combustors and augmentors.

Energy deposition during electron-induced dissociation.

We report studies of the internal energy deposited during activation of mass-selected ions through electron-ion collisions. Characteristic fragmentations of the molecular ion of limonene and W(CO) (n/+) (n = 1-6) indicate that electron-induced dissociation in a Fourier transform ion cyclotron resonance mass spectrometer proceeds via multiple collisions and that the average internal energy deposited during the activation process can be selected to be similar to that associated with electron-impact ionization. Control of the degree of ion excitation through selection of the electron energy, flux, and interaction time with the ions of interest is demonstrated, and advantages of this promising activation technique are discussed.