Aaron D. Slepkov

Generation of large alkali vapor densities inside bare hollow-core photonic band-gap fibers

We demonstrate the ability to generate extremely large rubidium densities in uncoated hollow-core photonic band-gap fibers using light-induced atomic desorption. Once the fiber is exposed to Rb vapor for 1-2 weeks, and this atomic source is removed, the fiber yields large desorbable densities for an extended period of time. We show that optical depths greater than e(-1200) can be created within seconds. Our observed Rb densities are several orders of magnitude larger than any previously reported to be generated optically, and allow for the demonstration of a relatively easy-to-use fiber-based vapor cell capable of producing large optical depths without the need for thermal tuning.

Hyperspectral multimodal CARS microscopy in the fingerprint region

A simple scheme for multimodal coherent anti-Stokes Raman scattering (CARS) microscopy is based on the spectral focusing of ultrafast-oscillator-derived pump/probe light and synchronous photonic crystal fiber (PCF) fiber-generated broadband Stokes light. To date, such schemes allowed rapid hyperspectral imaging throughout the CH/OH high frequency region (2700-4000 cm(-1) ). Here we extend this approach to the middle (1640-3300 cm(-1) ) and fingerprint regions (850-1800 cm(-1) ) of the Raman spectrum. Our simple integrated approach to rapid hyperspectral CARS microscopy in the fingerprint region is demonstrated by applications to label-free multimodal imaging of cellulose and bulk bone, including use of the phosphate resonance at 960 cm(-1) .

Multimodal CARS microscopy of structured carbohydrate biopolymers

We demonstrate the utility of multimodal coherent anti-Stokes Raman scattering (CARS) microscopy for the study of structured condensed carbohydrate systems. Simultaneous second-harmonic generation (SHG) and spectrally-scanned CARS microscopy was used to elucidate structure, alignment, and density in cellulose cotton fibers and in starch grains undergoing rapid heat-moisture swelling. Our results suggest that CARS response of the O-H stretch region (3000 cm−1–3400 cm−1), together with the commonly-measured C-H stretch (2750 cm−1–2970 cm−1) and SHG provide potentially important structural information and contrast in these materials.

Forward-collected simultaneous fluorescence lifetime imaging and coherent anti-Stokes Raman scattering microscopy

We demonstrate the simultaneous collection and separation of femtosecond-laser-based forward-collected coherent anti-Stokes Raman scattering (F-CARS) and two-photon-excitation-induced fluorescence lifetime images (FLIM) using time-correlated single photon counting (TCSPC). We achieve this in a nondescanned geometry using a single multimode fiber without significant loss of light, field of view, and most importantly, TCSPC timing fidelity. In addition to showing the ability to separate CARS images from FLIM images using time gating, we also demonstrate composite multimodal epicollected FLIM imaging with fiber-collected F-CARS imaging in live cells.

Spectroscopy of Rb atoms in hollow-core fibers

Recent demonstrations of light-matter interactions with atoms and molecules confined to hollow waveguides offer great promise for ultralow-light-level applications. The use of waveguides allows for tight optical confinement over interaction lengths much greater than what could be achieved in bulk geometries. However, the combination of strong atom-photon interactions and nonuniformity of guided light modes gives rise to spectroscopic features that must be understood in order to take full advantage of the properties of such systems. We use light-induced atomic desorption to generate an optically dense Rb vapor at room temperature inside a hollow-core photonic band-gap fiber. Saturable-absorption spectroscopy and passive slow-light experiments reveal large ac Stark shifts, power broadening, and transit-time broadening, that are present in this system even at nanowatt powers.

All-optical modulation of four-wave mixing in an Rb-filled photonic bandgap fiber.

We demonstrate efficient all-optical modulation using Rb vapor confined to a hollow-core photonic bandgap fiber. The intensity of a signal field participating in the four-wave-mixing process is modulated using a weak switching field. We observe 3 dB of attenuation in the signal field with only 3600 photons of switching energy, corresponding to 23 photons per atomic cross section lambda(2)/(2pi). Modulation bandwidths as high as 300 MHz are observed.

Single laser source for multimodal coherent anti-Stokes Raman scattering microscopy.

Short laser pulse technology has significantly contributed to biomedical research, especially via nonlinear optical microscopy. Coherent anti-Stokes Raman scattering (CARS) microscopy is a label-free, chemical-selective method that is growing in importance as improved methods and light sources develop. Here we discuss different approaches to laser source development for CARS microscopy and highlight the advantages of a multimodal CARS microscope, illustrated by selected applications in biomedical research.

Spatial-spectral coupling in coherent anti-Stokes Raman scattering microscopy

Coherent anti-Stokes Raman scattering (CARS) microscopy is a third-order nonlinear optical technique which permits label-free, molecule-specific hyperspectral imaging. The interference between coherent resonant and non-resonant terms leads to well known distortions in the vibrational spectrum, requiring the use of retrieval algorithms. It also leads to spatial imaging distortions, largely due to the Gouy phase, when objects are smaller than the Rayleigh range. Here we consider that the focal position and spectral contributions to the nonlinear image formation are intrinsically coupled and cannot be corrected by conventional retrieval methods.

Unraveling the complexity of deep gas accumulations with three-dimensional multimodal CARS microscopy

in deep basins. This requires analysis of gas samples directly tied to specifi c stages of the geologic history of thermally mature basins. Methane-rich hydrocarbon and aqueous fl uid inclusions can provide such samples because they form in fracture-fi lling and diagenetic minerals during the extended history of gas generation, migration, and accumulation (Becker et al., 2010; Mullis et al., 1994; Parris et al., 2003). Unfortunately, inclusions frequently occur in complex, intersecting healed microfractures, often obscuring the less common primary inclusions (Parris et al., 2003), and making it diffi cult to determine the sequence of evolving temperature, pressure, and gas composition. Here we apply molecule-specifi c multimodal threedimensional (3-D) nonlinear microscopy to provide chemically and spatially resolved imaging of assemblages of methane-rich fl uid inclusions and associated crystallographic features, as well as in situ detection of higher hydrocarbons. These observations advance our ability to track gas generation and migration processes within deep basins. METHODS AND SAMPLES

Label-free hyperspectral nonlinear optical microscopy of the biofuel micro-algae Haematococcus Pluvialis

We consider multi-modal four-wave mixing microscopies to be ideal tools for the in vivo study of carotenoid distributions within the important biofuel microalgae Haematococcus pluvialis. We show that hyperspectral coherent anti-Stokes Raman scattering (CARS) microscopy generates non-invasive, quantitative real-time concentrations maps of intracellular carotenoid distributions in live algae.