Matthew Reichert

Dual-arm Z-scan technique to extract dilute solute nonlinearities from solution measurements

We present a technique in which small solute nonlinearities may be extracted from large solvent signals by performing simultaneous Z-scans on two samples (solvent and solution). By using a dual-arm Z-scan apparatus with identical arms, fitting error in determining the solute nonlinearity is reduced because the irradiance fluctuations are correlated for both the solvent and solution measurements. To verify the sensitivity of this technique, the dispersion of nonlinear refraction of a squaraine molecule is measured. Utilizing this technique allows for the effects of the solvent n2 to be effectively eliminated, thus overcoming a longstanding problem in nonlinear optical characterization of organic dyes.

Beam deflection measurement of time and polarization resolved ultrafast nonlinear refraction

We modify the well-known photothermal beam deflection technique to study ultrafast nonlinearities. Using phase-sensitive detection we directly measure the temporal and polarization dynamics of nonlinear refraction (NLR) with sensitivity to optically induced phase changes of approximately λ/20,000. We use the relative polarization dependence of excitation and probe to separate the isotropic and reorientational components of the NLR.

Beam deflection measurement of bound-electronic and rotational nonlinear refraction in molecular gases.

A polarization-resolved beam deflection technique is used to separate the bound-electronic and molecular rotational components of nonlinear refractive transients of molecular gases. Coherent rotational revivals from N(2), O(2), and two isotopologues of carbon disulfide (CS(2)), are identified in gaseous mixtures. Dephasing rates, rotational and centrifugal distortion constants of each species are measured. Polarization at the magic angle allows unambiguous measurement of the bound-electronic nonlinear refractive index of air and second hyperpolarizability of CS(2). Agreement between gas and liquid phase second hyperpolarizability measurements is found using the Lorentz-Lorenz local field correction.

Quasi-three-level model applied to measured spectra of nonlinear absorption and refraction in organic molecules

Materials with a large nonlinear refractive index (n2) and relatively small linear and nonlinear absorption losses, namely, two-photon absorption (2PA, of coefficient α2), have long been sought after for applications such as all-optical switching (AOS). Here we experimentally determine the linear and 2PA properties of several organic molecules, which we approximate as centrosymmetric, and use a simplified essential-state model (quasi-three-level model) to predict the dispersion of n2. We then compare these predictions with experimental measurements of n2 and find good agreement. Here “quasi”-three-level means using a single one-photon allowed intermediate state and multiple (here two) two-photon allowed states. This also allows predictions of the figure-of-merit (FOM), defined as the ratio of nonlinear refractive phase shift to the 2PA fractional loss, that determines the viability for such molecules to be used in device applications. The model predicts that the optimized wavelength range for a large FOM lies near the short wavelength linear absorption edge for cyanine-like dyes where the magnitude of n2 is quite large. However, 2PA bands lying close to the linear absorption edge in certain classes of molecules can greatly reduce this FOM. We identify two molecules having a large FOM for AOS. We note that the FOM is often defined as the ratio of real to imaginary parts of the third-order susceptibility (χ(3)) with multiple processes leading to both components. As explained later in this paper, such definitions require care to only include the 2PA contribution to the imaginary part of χ(3) in regions of transparency.

Dispersion of nondegenerate nonlinear refraction in semiconductors

We use our recently developed beam-deflection technique to measure the dispersion of the nondegenerate nonlinear refraction (NLR) of direct-gap semiconductors. The magnitude and sign of the NLR coefficient n2(ωa; ωb) are determined over a broad spectral range for different values of nondegeneracy. In the extremely nondegenerate case, n2(ωa; ωb) is positively enhanced near the two-photon absorption (2PA) edge and is significantly larger than its degenerate counterpart, suggesting applications for nondegenerate all-optical switching. At higher photon energies within the 2PA regime, n2(ωa; ωb) switches sign to negative over a narrow wavelength range. This strong anomalous nonlinear dispersion provides large phase modulation of a femtosecond pulse with bandwidth centered near the zero-crossing frequency. The measured nondegenerate dispersion closely follows our earlier predictions based on nonlinear Kramers-Kronig relations [Sheik-Bahae et. al, IEEE J. Quant. Electron. 30, 249 (1994)].

Quality of spatial entanglement propagation

We explore, both experimentally and theoretically, the propagation dynamics of spatially entangled photon pairs (biphotons). Characterization of entanglement is done via the Schmidt number, which is a universal measurement of the degree of entanglement directly related to the nonseparability of the state into its subsystems. We develop expressions for the terms of the Schmidt number that depend on the amplitude and phase of the commonly used double-Gaussian approximation for the biphoton wave function, and demonstrate migration of entanglement between amplitude and phase upon propagation. We then extend this analysis to incorporate both phase curvature in the pump beam and higher spatial frequency content of more realistic non-Gaussian wave functions. Specifically, we generalize the classical beam quality parameter

Nonlinear refraction dynamics of solvents and gases

{M}^{2}

Observation of Nondegenerate Two-Photon Gain in GaAs

to the biphotons, allowing the description of more information-rich beams and more complex dynamics. Agreement is found with experimental measurements using direct imaging and Fourier optics.

Massively Parallel Coincidence Counting of High-Dimensional Entangled States

We present measurements of the temporal and polarization dependence of the nonlinear optical (NLO) response of selected organic solvents using our beam deflection (BD) method. These measurements allow us to separately determine the bound-electronic and nuclear responses which then determines the NLO response function. With this NLO response function the outcome of other experiments such as Z-scan as a function of pulse-width can be predicted. By performing similar measurements on the gas phase of these solvents we can compare the hyper-polarizabilities in the two phases.

Biphoton transmission through non-unitary objects

Two-photon lasers require materials with large two-photon gain (2PG) coefficients and low linear and nonlinear losses. Our previous demonstration of large enhancement of two-photon absorption in semiconductors for very different photon energies translates directly into enhancement of 2PG. We experimentally demonstrate nondegenerate 2PG in optically excited bulk GaAs via femtosecond pump-probe measurements. 2PG is isolated from other pump induced effects through the difference between measurements performed with parallel and perpendicular polarizations of pump and probe. An enhancement in the 2PG coefficient of nearly 2 orders of magnitude is reported. The results point a possible way toward two-photon semiconductor lasers.