Jonathan V. Thompson

Dual Raman-Brillouin Microscope for Chemical and Mechanical Characterization and Imaging

We present a unique confocal microscope capable of measuring the Raman and Brillouin spectra simultaneously from a single spatial location. Raman and Brillouin scattering offer complementary information about a materials chemical and mechanical structure, respectively, and concurrent monitoring of both of these spectra would set a new standard for material characterization. We achieve this by applying recent innovations in Brillouin spectroscopy that reduce the necessary acquisition times to durations comparable to conventional Raman spectroscopy while attaining a high level of spectral accuracy. To demonstrate the potential of the system, we map the Raman and Brillouin spectra of a molded poly(ethylene glycol) diacrylate (PEGDA) hydrogel sample in cyclohexane to create two-dimensional images with high contrast at microscale resolutions. This powerful tool has the potential for very diverse analytical applications in basic science, industry, and medicine.

Stimulated Brillouin Scattering Microscopic Imaging

Two-dimensional stimulated Brillouin scattering microscopy is demonstrated for the first time using low power continuous-wave lasers tunable around 780 nm. Spontaneous Brillouin spectroscopy has much potential for probing viscoelastic properties remotely and non-invasively on a microscopic scale. Nonlinear Brillouin scattering spectroscopy and microscopy may provide a way to tremendously accelerate the data aquisition and improve spatial resolution. This general imaging setup can be easily adapted for specific applications in biology and material science. The low power and optical wavelengths in the water transparency window used in this setup provide a powerful bioimaging technique for probing the mechanical properties of hard and soft tissue.

Optimization of focusing through scattering media using the continuous sequential algorithm

The ability to control the propagation of light through scattering media is essential for atmospheric optics, astronomy, biomedical imaging, and remote sensing. The optimization of focusing light through a scattering medium is of particular interest for the case of highly scattering materials. Optical wavefront beam-shaping plays a critical role in optimizing such a propagation; however, an enormous field of adjustable parameters makes the overall task complicated. Here, we propose and experimentally evaluate several variations on the standard continuous sequential algorithm (CSA) that hold a promise of revealing new, faster, and more efficient optimization algorithms for selecting an optical wavefront to focus light through a scattering medium. We demonstrate that the order in which pixels are chosen in the CSA can lead to a two-fold decrease in the number of iterations required to reach a given enhancement.

Wavefront shaping enhanced Raman scattering in a turbid medium

Spontaneous Raman scattering is a powerful tool for chemical sensing and imaging but suffers from a weak signal. In this Letter, we present an application of adaptive optics to enhance the Raman scattering signal detected through a turbid, optically thick material. This technique utilizes recent advances in wavefront shaping techniques for focusing light through a turbid media and applies them to chemical detection to achieve a signal enhancement with little sacrifice to the overall simplicity of the experimental setup. With this technique, we demonstrate an enhancement in the Raman signal from titanium dioxide particles through a highly scattering material. This technique may pave the way to label-free tracking using the optical memory effect.

Enabling time resolved microscopy with random Raman lasing

Optical imaging of fast events and processes is essential for understanding dynamics of complex systems. A bright flash of illuminating light is required to acquire sufficient number of photons for superior image quality. Laser pulses can provide extreme brightness and are typically employed to achieve high temporal resolution; however, the high degree of coherence associated with the lasing process degrades the image quality with speckle formation. Random lasers are low-coherence sources of stimulated emission and do not suffer from speckle, but are rather broadband and have a relatively low output power limiting the scope of their potential applications. In this report, we demonstrate the use of random Raman lasing as a novel imaging light source with unprecedented brightness for a speckle-free and narrowband light source. We showcase the advantages of a random Raman laser to image the nanosecond scale dynamics of cavitation formation in water and quantitatively compare these images to those taken with incoherent fluorescent emission and coherent laser light as illumination source.

Amplitude concentration in a phase-modulated spectrum due to femtosecond filamentation

We present a method by which the spectral intensity of an ultrafast laser pulse can be accumulated at selected frequencies by a controllable amount. Using a 4-f pulse shaper we modulate the phase of the frequency components of a femtosecond laser. By inducing femtosecond filamentation with the modulated pulse, we can concentrate the spectral amplitude of the pulse at various frequencies. The phase mask applied by the pulse shaper determines the frequencies for which accumulation occurs, as well as the intensity of the spectral concentration. This technique provides a way to obtain pulses with adjustable amplitude using only phase modulation and the nonlinear response of a medium. This provides a means whereby information which is encoded into spectral phase jumps may be decoded into measurable spectral intensity spikes.

Enhanced coupling of light into a turbid medium through microscopic interface engineering

Significance Optical scattering severely limits the range and sensitivity of detection techniques within/through turbid media, such as biological samples and security-related materials. In this article, we demonstrate a method to enhance the coupling of light into a highly scattering medium. This enhanced coupling results in higher optical sensitivity to particles within the medium, as well as enhanced optical transmission through the medium. These results pave the way for enhanced spectroscopy in biological and other turbid media. There are many optical detection and sensing methods used today that provide powerful ways to diagnose, characterize, and study materials. For example, the measurement of spontaneous Raman scattering allows for remote detection and identification of chemicals. Many other optical techniques provide unique solutions to learn about biological, chemical, and even structural systems. However, when these systems exist in a highly scattering or turbid medium, the optical scattering effects reduce the effectiveness of these methods. In this article, we demonstrate a method to engineer the geometry of the optical interface of a turbid medium, thereby drastically enhancing the coupling efficiency of light into the material. This enhanced optical coupling means that light incident on the material will penetrate deeper into (and through) the medium. It also means that light thus injected into the material will have an enhanced interaction time with particles contained within the material. These results show that, by using the multiple scattering of light in a turbid medium, enhanced light–matter interaction can be achieved; this has a direct impact on spectroscopic methods such as Raman scattering and fluorescence detection in highly scattering regimes. Furthermore, the enhanced penetration depth achieved by this method will directly impact optical techniques that have previously been limited by the inability to deposit sufficient amounts of optical energy below or through highly scattering layers.

Directional coherent light via intensity-induced sideband emission

We introduce a unique technique for generating directional coherent emissions that could be utilized to create coherent sources in a wide range of frequencies from the extreme ultraviolet (XUV) to the deep infrared. This is accomplished without population inversion by pumping a two-level system with a far-detuned strong optical field that induces the splitting of the two-level system. A nonlinear process of four-wave mixing then occurs across the split system, driving coherent emission at sidebands both red- and blue-detuned from the pump frequency, and propagates both forward and backward along the pump beam path. We observed this phenomenon in dense rubidium vapor along both the D1 and D2 transitions. The sideband emission exhibits a short pulse duration (<1 ns) with threshold-like behavior dependent on both the pump intensity and Rb vapor density. This technique offers a new capability for manipulating the emission frequency simply through intensity-induced atomic modulation that can be scaled to most frequency regimes using various atomic/molecular ensembles and pump energies.

Evidence of Anderson localization effects in random Raman lasing

Anderson localization, also known as strong localization, is the absence of diffusion in turbid media resulting from wave interference. The effect was originally predicted for electron motion, and is widely known to exist in systems of less than 3 dimensions. However, Anderson localization of optical photons in 3 dimensional systems remains an elusive and controversial topic. Random Raman lasing offers the unique combination of large gain and virtually zero absorption. The lack of absorption makes long path length, localized modes preferred. The presence of gain offsets what little absorption is present, and preferentially amplifies localized modes due to their large Q factors compared with typical low Q modes present in complex media. Random Raman lasers exhibit several experimentally measured properties that diverge from classical, particle-like, diffusion. First, the temporal width of the emission being 1 to a few nanoseconds in duration when it is pumped with a 50 ps laser is a full order of magnitude longer than is predicted by Monte Carlo simulations. Second, the random Raman laser emission is highly multi-mode, consisting of hundreds of simultaneous lasing modes. This is in contrast to early theoretical results and back of the envelope arguments that both suggest that only a few modes should be present. We will present the evidence that suggests a divergence from classical diffusion theory. One likely explanation, that is consistent with all of these anomalies, is the presence of high-Q localized modes consistent with Anderson localization.

Pulsed cooperative backward emissions from non-degenerate atomic transitions in sodium

We study backward cooperative emissions from a dense sodium atomic vapor. Ultrashort pulses produced from a conventional amplified femtosecond laser system with an optical parametric amplifier are used to excite sodium atoms resonantly on the two-photon 3S?4S transition. Backward superfluorescent emissions (BSFEs), both on the 4S?3P and 4S?3P transitions, are observed. The picosecond temporal characteristics of the BSFE are observed using an ultrafast streak camera. The power laws for the dependencies of the average time delay and the intensity of the BSFEs on input power are analyzed in the sense of cooperative emission from nonidentical atomic species. As a result, an absolute (rather than relative) time delay and its fluctuations (free of any possible external noise) are determined experimentally. The possibility of a backward swept-gain superfluorescence as an artificial laser guide star in the sodium layer in the mesosphere is also discussed.