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David M Jonas

Publications and source records attributed to David M Jonas.

7 recordsLinked to original sources
PubMed2005

Response functions for dimers and square-symmetric molecules in four-wave-mixing experiments with polarized light.

Four-wave-mixing nonlinear-response functions are given for intermolecular and intramolecular vibrations of a perpendicular dimer and intramolecular vibrations of a square-symmetric molecule containing a doubly degenerate state. A two-dimensional particle-in-a-box model is used to approximate the electronic wave functions and obtain harmonic potentials for nuclear motion. Vibronic interactions due to symmetry-lowering distortions along Jahn-Teller active normal modes are discussed. Electronic dephasing due to nuclear motion along both symmetric and asymmetric normal modes is included in these response functions, but population transfer between states is not. As an illustration, these response functions are used to predict the pump-probe polarization anisotropy in the limit of impulsive excitation.

Anisotropy↗
PubMed2005

2D correlation analysis of the continuum in single molecule surface enhanced Raman spectroscopy.

The role and the nature of the continuum in Surface Enhanced Raman Spectroscopy (SERS) are unclear. Here, two-dimensional (2D) covariance and correlation analysis is applied to single molecule SERS spectra on silver colloids with and without rhodamine 6G (native colloid). The resulting 2D covariance and correlation maps show that the sharp molecular Raman peaks from rhodamine 6G and the molecule responsible for the SERS peaks from the native colloid are correlated to different continua even though both continua are present in each data set. This suggests that two distinct active sites on the silver colloids produce the two different continua, and that each site has some molecular specificity.

Journal Article↗
PubMed2005

Mid-infrared electric field characterization using a visible charge-coupled-device-based spectrometer.

We characterize ultrashort mid-infrared pulses through upconversion by using the stretched pulses obtained from the uncompressed output of a chirped-pulse amplifier. The power spectrum thus translated into the visible region can be readily measured with a standard silicon CCD camera-based spectrometer. The spectral phase is also characterized by a variant of zero-added-phase spectral phase interferometry for direct electric field reconstruction. This is a general method that provides a multiplex advantage over conventional infrared detector array-based methods.

Journal Article↗
PubMed2004

Fourier algorithm for four-wave-mixing signals from optically dense systems with memory.

A triple Fourier-transform algorithm for generating and propagating femtosecond four-wave-mixing signals in optically thick samples is demonstrated. The algorithm has a dynamic range that is useful for tests of theory and simulations of experiments with an arbitrary nonlinear response. Although two-pulse echoes decay faster as optical density increases for a Bloch model, we find that systems with memory exhibit the opposite trend.

Journal Article↗
PubMed2002

Two-dimensional femtosecond spectroscopy.

The simplest two-dimensional (2D) spectra show how excitation with one (variable) frequency affects the spectrum at all other frequencies, thus revealing the molecular connections between transitions. Femtosecond 2D Fourier transform (2D FT) spectra are more flexible and share some of the remarkable properties of their conceptual parent, 2D FT nuclear magnetic resonance. When 2D FT spectra are experimentally separated into real absorptive and imaginary refractive parts, the time resolution and frequency resolution can both reach the uncertainty limit set for each resonance by the sample itself. Coherent four-level contributions to the signal provide new molecular phase information, such as relative signs of transition dipoles. The nonlinear response can be picked apart by selecting a single coherence pathway (e.g., specifying the relative signs of energy level difference frequencies during different time intervals as in the photon echo). Because molecules are frozen on the femtosecond timescale, femtosecond 2D FT experiments can separate a distribution of instantaneous molecular environments and intramolecular geometries as inhomogeneous broadening. This review provides an introduction to two-dimensional Fourier transform experiments exploiting second- and third-order vibrational and electronic nonlinearities.

Journal Article↗