Dan Oron

Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy

Molecular vibrations have oscillation periods that reflect the molecular structure, and are hence being used as a spectroscopic fingerprint for detection and identification. At present, all nonlinear spectroscopy schemes use two or more laser beams to measure such vibrations. The availability of ultrashort (femtosecond) optical pulses with durations shorter than typical molecular vibration periods has enabled the coherent excitation of molecular vibrations using a single pulse. Here we perform single-pulse vibrational spectroscopy on several molecules in the liquid phase, where both the excitation and the readout processes are performed by the same pulse. The main difficulty with single-pulse spectroscopy is that all vibrational levels with energies within the pulse bandwidth are excited. We achieve high spectral resolution, nearly two orders of magnitude better than the pulse bandwidth, by using quantum coherent control techniques. By appropriately modulating the spectral phase of the pulse we are able to exploit the quantum interference between multiple paths to selectively populate a given vibrational level, and to probe this population using the same pulse. This scheme, using a single broadband laser source, is particularly attractive for nonlinear microscopy applications, as we demonstrate by constructing a coherent anti-Stokes Raman (CARS) microscope operating with a single laser beam.

Scanningless depth-resolved microscopy.

The ability to perform optical sectioning is one of the great advantages of laser-scanning microscopy. This introduces, however, a number of difficulties due to the scanning process, such as lower frame rates due to the serial acquisition process. Here we show that by introducing spatiotemporal pulse shaping techniques to multiphoton microscopy it is possible to obtain full-frame depth resolved imaging completely without scanning. Our method relies on temporal focusing of the illumination pulse. The pulsed excitation field is compressed as it propagates through the sample, reaching its shortest duration at the focal plane, before stretching again beyond it. This method is applied to obtain depth-resolved twophoton excitation fluorescence (TPEF) images of drosophila egg-chambers with nearly 105 effective pixels using a standard Ti:Sapphire laser oscillator.

Built-in Quantum Dot Antennas in Dye-Sensitized Solar Cells

A new design of dye-sensitized solar cells involves colloidal semiconductor quantum dots that serve as antennas, funneling absorbed light to the charge separating dye molecules via nonradiative energy transfer. The colloidal quantum dot donors are incorporated into the solid titania electrode resulting in high energy transfer efficiency and significant improvement of the cell stability. This design practically separates the processes of light absorption and charge carrier injection, enabling us to optimize each of these separately. Incident photon-to-current efficiency measurements show a full coverage of the visible spectrum despite the use of a red absorbing dye, limited only by the efficiency of charge injection from the dye to the titania electrode. Time resolved luminescence measurements clearly relate this to Forster resonance energy transfer from the quantum dots to the dye. The presented design introduces new degrees of freedom in the utilization of quantum dot sensitizers for photovoltaic cells. In particular, it opens the way toward the utilization of new materials whose band offsets do not allow direct charge injection.

Multiphoton plasmon-resonance microscopy

A novel method for detection of noble-metal nanoparticles by their nonlinear optical properties is presented and applied for specific labeling of cellular organelles. When illuminated by laser light in resonance with their plasmon frequency these nanoparticles generate an enhanced multiphoton signal. This enhanced signal is measured to obtain a depth-resolved image in a laser scanning microscope setup. Plasmon-resonance images of both live and fixed cells, showing specific labeling of cellular organelles and membranes, either by two-photon autofluorescence or by third-harmonic generation, are presented.

Dimensionality dependence of the Rayleigh-Taylor and Richtmyer-Meshkov instability late-time scaling laws

The late-time nonlinear evolution of the three-dimensional (3D) Rayleigh–Taylor (RT) and Richtmyer–Meshkov (RM) instabilities for random initial perturbations is investigated. Using full 3D numerical simulations, a statistical mechanics bubble-competition model, and a Layzer-type drag-buoyancy model, it is shown that the RT scaling parameters, αB and αS, are similar in two and three dimensions, but the RM exponents, θB and θS are lower by a factor of 2 in three dimensions. The similarity parameter hB/〈λ〉 is higher by a factor of 3 in the 3D case compared to the 2D case, in very good agreement with recent Linear Electric Motor (LEM) experiments. A simple drag-buoyancy model, similar to that proposed by Youngs [see J. C. V. Hanson et al., Laser Part. Beams 8, 51 (1990)], but using the coefficients from the A=1 Layzer model, rather than phenomenological ones, is introduced.

Single-pulse coherent anti-Stokes Raman spectroscopy in the fingerprint spectral region

Quantum coherent control techniques are applied to achieve high spectral resolution nonlinear vibrational spectroscopy using a single ultrashort laser source. By controlling the spectral phase of ∼10 fs pulses, we are able to obtain detailed coherent anti-Stokes Raman (CARS) spectra in the important fingerprint spectral region, which reflects the structural chemical information. A full theoretical analysis and an experimental demonstration of two alternative schemes leading to spectral resolution two orders of magnitude better than the pulse bandwidth are presented. The first involves selective excitation of vibrational levels within the pulse bandwidth by periodic modulation of the spectral phase of the pulse. In the second scheme an effective narrow probing of the vibrational level has been achieved by phase shifting of a narrow spectral band. Single-pulse CARS offers an attractive alternative to conventional multibeam nonlinear vibrational spectroscopy techniques.

Patterned two-photon illumination by spatiotemporal shaping of ultrashort pulses

Multiphoton excitation by temporally focused pulses can be combined with spatial Fourier-transform pulse shaping techniques to enhance spatial control of the excitation volume. Here we propose and demonstrate an optical system for the generation of such spatiotemporally engineered light pulses using a combination of spatial control by a two-dimensional reconfigurable light modulator, with a dispersive optical setup for temporal focusing. We show that although the properties of a holographic beam significantly differ from those of plane-wave illumination used in previous temporal focusing realizations, this leads only to a slightly reduced axial resolution. We show that the system can provide scanningless, arbitrarily shaped, depth resolved excitation patterns that offer new perspectives for multiphoton photoactivation and optical lithography applications.

Improved depth resolution in video-rate line-scanning multiphoton microscopy using temporal focusing

By introducing spatiotemporal pulse shaping techniques to multiphoton microscopy it is possible to obtain video-rate images with depth resolution similar to point-by-point scanning multiphoton microscopy while mechanically scanning in only one dimension. This is achieved by temporal focusing of the illumination pulse: The pulsed excitation field is compressed as it propagates through the sample, reaching its shortest duration (and highest peak intensity) at the focal plane before stretching again beyond it. This method is applied to produce, in a simple and scalable setup, video-rate two-photon excitation fluorescence images of Drosophila egg chambers with nearly 100,000 effective pixels and 1.5 microm depth resolution.

Depth-resolved structural imaging by third-harmonic generation microscopy

Third harmonic generation microscopy is shown to be a robust method for obtaining structural information on a variety of biological specimens. Its nature allows depth-resolved imaging of inhomogeneities with virtually no background from surrounding homogeneous media. With an appropriate illumination geometry, third harmonic generation microscopy is shown to be particularly suitable for imaging of biogenic crystals, enabling extraction of the crystal orientation.

Second‐Harmonic Generation from a Single Core/Shell Quantum Dot

Nanoparticles emitting two-photon luminescence are broadly used as photostable emitters for nonlinear microscopy. Second-harmonic generation (SHG) as another two-photon mechanism offers complementary optical properties but the reported sizes of nanoparticles are still large, of a few tens of nanometers. Herein, coherent SHG from single core/shell CdTe/CdS nanocrystals with a diameter of 10 to 15 nm is reported. The nanocrystal excitation spectrum reveals resonances in the nonlinear efficiency with an overall maximum at about 970 nm. Polarization analysis of the second-harmonic emission confirms the expected zinc blende symmetry, and allows extraction of the three-dimensional nanocrystal orientation. The small size of these nonlinearly active quantum dots, together with the intrinsic coherence and orientation sensitivity of the SHG process, are well adapted for ultrafast probing of optical near-fields with high resolution as well as for orientation tracking for bioimaging applications.