Jeanne M. Robinson

Integrated electro-optic lens/scanner in a LiTaO3 single crystal.

We report what we believe to be the first stand-alone integrated electro-optic lens and scanner fabricated on a single crystal of Z-cut LiTaO(3). The independently controlled lens and scanner components consist of lithographically defined domain-inverted regions extending through the thickness of the crystal. A lens power of 0.233 cm(-1) kV(-1) and a deflection angle of 12.68 mrad kV(-1) were observed at the output of the device.

Enhanced optical limiting in derivatized fullerenes

We have observed enhanced optical limiting behavior in solutions of a derivatized fullerene (phenyl-C(61)-butyric acid cholesteryl ester) from 532 to 700 nm. Transient absorption measurements determined the spectral and temporal regions of interest for optical limiting in C(60) and in C(60) derivatives that are due to a reverse saturable absorption mechanism and predicted enhanced limiting at longer wavelengths. Intensity-dependent transmission measurements made at several wavelengths confirmed these results. The increased solubility and the broadened ground-state absorption of the functionalized C(60) make it suitable for use as an optical limiter in the red and the near infrared.

Large-angle electro-optic laser scanner on LiTaO 3 fabricated by in situ monitoring of ferroelectric-domain micropatterning

We report on a horn-shaped electro-optic scanner based on a ferroelectric LiTaO(3) wafer that is capable of scanning 632.8-nm light by an unprecedented 14.88 degrees angle for extraordinary polarized light and by 4.05 degrees for ordinary polarized light. The device concept is based on micropatterning ferroelectric domains in the shape of a series of optimized prisms whose refractive index is electric field tunable through the electro-optic effect. We demonstrate what we believe is a novel technique of using electro-optic imaging microscopy for in situ monitoring of the process of domain micropatterning during device fabrication, thus eliminating imperfect process control based on ex situ monitoring of transient currents.

Cascaded electro-optic scanning of laser light over large angles using domain microengineered ferroelectrics

We present a device concept based on cascaded electro-optic deflection in a domain microengineered ferroelectric chip. In our design, large deflection angles are achieved by cascading several smaller scanners in a single ferroelectric chip, such that each successive scanner stage builds upon the deflection of the previous stage. We demonstrate the basic concept using a two-stage device fabricated in a single crystal wafer of ferroelectric LiTaO3. By operating the device using a specially designed programmable multichannel driver that provides ±1.1 kV per stage, a total scan angle of 25.4° at 5 kHz was demonstrated. Even larger angles of deflection are possible with additional scanner stages.

Integrated high-power electro-optic lens and large-angle deflector

We present a theoretical discussion and experimental demonstration of what to our knowledge is a novel integrated electro-optic lens and beam deflector fabricated in lithium tantalate. The cylindrical lens collimates Gaussian beams as small as 4 mum in diameter, whereas the independently controlled deflector is capable of scanning the collimated beam through an angular range of nearly 20 degrees .

Near-infrared Raman spectroscopy of solid C60. Raman activation of silent modes by 13C and sample disorder

Abstract High-resolution Raman spectra excited from 1.45 to 1.75 eV are presented for solid C 60 films and crystals prepared by four methods. Intersample comparison shows that imperfections introduced in sample preparation can lower symmetries sufficiently to activate silent modes, while oxygen has no observable effect. Unusual resonance and broadening effects observed near 1.6 eV indicate the existence of a weak electronic transition. Explicit calculations for C 60 molecules having one or two 13 C atoms reproduce the observe spectra and show that isotopic symmetry lowering is manifested in lifting of H g degeneracies and activation of silent modes through mixing with nearly Raman-active modes.

Electro-optic coefficients of lithium tantalate at near-infrared wavelengths

The unclamped linear electro-optic coefficients r13 and r33 for lithium tantalate are known at only one wavelength, 632.8 nm, whereas the clamped coefficients are also known at 3.39 μm. In the unclamped mode the effects of mechanical changes caused by piezoelectric and elasto-optic effects are accounted for in the electro-optic coefficient. We demonstrate a novel technique that uses a ferroelectric domain micropatterned electro-optic deflector to measure the unclamped linear electro-optic coefficients r13 and r33 at any wavelength. Using this method, we have determined these values for lithium tantalate at 980, 1330, and 1558 nm.

Femtosecond to nanosecond dynamics in fullerenes: Implications for excitedstate optical nonlinearities

We compared detailed dynamics of the excited-state absorption for C60 in solution, thin films, and entrapped in an inorganic sol-gel glass matrix. Our results demonstrate that the microscopic morphology of the C60 molecules plays a crucial role in determining the relaxation dynamics. This is a key factor for applications in optical limiting for nanosecond pulses using reverse saturable absorption. We find that the dynamics of our C60-glass composites occur on long (ns) timescales, comparable to those in solution; thin film samples, by contrast, show rapid decay (<20 picoseconds). These results demonstrate that C60-sol-gel glass composites contain C60 in a molecular dispersion, and are suitable candidates for solid-state optical limiting. Multispectral analysis of the decay dynamics in solution allows accurate determination of both the intersystem crossing time (600±100ps) and the relative strengths of the singlet and triplet excited-state cross sections as a function of wavelength from 450–950 nm. The triplet excited-state cross section is greater than that for the singlet excited-state over the range from 620–810 nm.

Thermodynamic model of quasiliquid formation on H2O ice: Comparison with experiment

We have developed a new thermodynamic theory of the quasiliquid layer, which has been shown to be effective in modeling the phenomenon in a number of molecular systems. Here we extend our analysis to H(2)O ice, which has obvious implications for environmental and atmospheric chemistry. In the model, the liquid layer exists in contact with an ice defined as a two-dimensional lattice of sites. The system free energy is defined by the bulk free energies of ice I(h) and liquid water and is minimized in the grand canonical ensemble. An additional configurational entropy term arises from the occupation of the lattice sites. Furthermore, the theory predicts that the layer thickness as a function of temperature depends only on the liquid activity. Two additional models are derived, where slightly different approximations are used to define the free energy. With these two models, we illustrate the connection between the quasiliquid phenomenon and multilayer adsorption and the possibility of a two-dimensional phase transition connecting a dilute low coverage phase of adsorbed H(2)O and the quasiliquid phase. The model predictions are in agreement with a subset of the total suite of experimental measurements of the liquid thickness on H(2)O ice as a function of temperature. The theory indicates that the quasiliquid layer is actually equivalent to normal liquid water, and we discuss the impact of such an identification. In particular, observations of the liquid layer to temperatures as low as 200 K indicate the possibility that the quasiliquid is, in fact, an example of deeply supercooled normal water. Finally, we briefly discuss the obvious extension of the pure liquid theory to a thermodynamic theory of interfacial solutions on ice in the environment.

Imaging nanometer-thick patterned self-assembled monolayers via second-harmonic generation microscopy

We have used the inherent surface sensitivity of second-harmonic generation to develop an instrument for nonlinear optical microscopy of surfaces and interfaces. This optical technique is ideal for imaging nanometer-thick, chromophoric self-assembled monolayers (SAMs), which have been patterned using photolithographic techniques. In this paper, we demonstrate the application of second-harmonic generation microscopy to patterned SAMs of the noncentrosymmetric molecule calixarene and discuss the resolution and sensitivity limits of the technique.