Gregory Walker

High-performance photorefractive polymer operating at 1550 nm with near-video-rate response time

The development of a high-performance photorefractive polymer composite operating at 1550 nm is reported. We show 40% internal diffraction efficiency with response time of 35 ms and a net gain of 20cm−1 in four-wave mixing and two-beam coupling experiments, respectively. This is more than an order of magnitude improvement in the diffraction efficiency and net two beam coupling gain and two orders of magnitude in the response time than the previously reported photorefractive polymer operating at this technologically important wavelength. The improvement in photorefractive characteristics is accomplished by an enhanced orientation of the nonlinear optical chromophore in the present composite.

High-performance photorefractive polymer operating at 975 nm

A family of photorefractive polymer composites has been developed that enable high-performance device operation at a wavelength of 975nm. This constitutes a major extension into the near-infrared spectral region for the operation of all-organic photorefractive devices. Utilizing our photorefractive materials, we demonstrate large net two-beam coupling gain of more than 100cm−1, 60% diffraction efficiency in four-wave mixing experiments, and a fast response time of 33ms, at an irradiance of 1W∕cm2.

Video-rate compatible photorefractive polymers with stable dynamic properties under continuous operation

We report on photorefractive polymer composites that exhibit stable dynamic properties under continuous operation. These materials are based on a bis-triarylamine side-chain polymer matrix with a low ionization potential. The evolution of the response time for exposures up to 4kJ∕cm2 was studied and compared with that obtained in poly(n-vinylcarbazole) (PVK) based composites. In the composites, operational stability is combined with video-rate compatible dynamics, large dynamic range at moderate fields, and long shelf lifetimes.

Direct imaging through scattering media by use of efficient third-harmonic generation in organic materials

We report on real-time, time-gated, direct imaging through scattering media with an attenuation of 14 mean-free paths by use of third-harmonic generation in the eye-safe and telecommunication-compatible near-IR spectral region (1550 nm).

Characterisation of a dipolar chromophore with third-harmonic generation applications in the near-IR

E-2-Tricyanovinyl-3-n-hexyl-5-[4-{bis(4-n-butylphenyl)amino}-2-methoxystyryl]-thiophene, 1, has previously been used to demonstrate applications relying on frequency tripling of 1.55 μm light. Here we report the synthesis and chemical characterisation of 1, along with quantum-chemical calculations and additional experimental investigations of its third-order nonlinear properties that give more insight into its frequency tripling properties. Although 1 can be processed into amorphous films, crystals can also be grown by slow evaporation of solutions; the crystal structure determined by X-ray diffraction shows evidence of significant contributions from zwitterionic resonance forms to the ground-state structure, and reveals centrosymmetric packing exhibiting π–π and C–H⋯NC interactions. Both solutions and films of 1 exhibit near-infrared two-photon absorption into the low-lying one-photon-allowed state with a peak two-photon cross-section of ca. 290 GM (measured using the white-light continuum method with a pump wavelength of 1800 nm) at a transition energy equivalent to degenerate two-photon absorption at ca. 1360 nm; two related chromophores are also found to show comparable near-IR two-photon cross-sections. Closed-aperture Z-scan measurements and quantum-chemical calculations indicate that the nonlinear refractive index and third-harmonic generation properties of 1 are strongly dependent on frequency in the telecommunications range, due the aforementioned two-photon resonance.

Photorefractive polymers based on bis-triarylamine side-chain polymers

We report on the photorefractive properties of two polymer composites that utilize a new bis-triarylamine side-chain polymer matrix. Correctly locating the frontier orbitals of the new transport manifold with respect to the HOMO levels of chromophores, allows stable continuous operation over exposure levels of more that 4 kJ/cm2 when samples are electrically biased at 57 V/μm. This operational stability is combined with video-rate compatible grating build-up times and a dynamic range that allows index modulations of 3 x 10-3 and gain coefficients on the order of 100 cm-1 at moderate fields. The thermal stability of one of the composites reported is excellent, showing no signs of phase separation even after one week at 60°C. A comparison with the stability of composites where the new matrix was replaced by PVK is also presented.

Time-gated imaging through scattering media by using efficient THG in organic films

We report on efficient third-harmonic generation (THG) with large spectral and angular bandwidths in polymer thin films doped with conjugated organic molecules. Using the efficient THG exhibited by these organic films, we demonstrate real-time, time-gated, direct imaging of objects immersed in highly scattering media by using femtosecond pulses tuned at the eye-safe and telecommunication-compatible near-infrared spectral region (1550 nm). By using a low cost detection system we resolved THG time-gated images of objects immersed in media with a scattering attenuation of 14 mean-free paths, equivalent to an attenuation of six optical densities.