MOA



Code: MOA Time Slot/Poster Number: 10:30 - 11:00 am Session: Coherent Raman I

Applications of Raman Scattering in Quantum Technologies
K. F. Reim1; P. Bustard1; K. C. Lee1; J. Nunn1; V. O. Lorenz2; B. J. Sussman3; N. K. Langford1; D. K. Jaksch1; I. A. Walmsley1
1University of Oxford, Oxford, UK; 2University of Delaware, Newark, DE; 3National Research Council, Ottawa, Canada

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Summary
The Raman effect couples light to the electronic ground state of matter. This means that it is possible to utilize the long-lived coherence of the material excitation to control, measure and store optical radiation. This, in turn, enables a number of novel applications, including the generation of broadband light, the distribution of quantum entanglement and the storage and retrieval of quantum light for long-distance communications. We describe three applications of Raman scattering to technologies related to the above goals, using a variety of material excitations: molecular vibrations, bulk phonons in a crystalline solid, and atomic spin waves.

Code: MOA Time Slot/Poster Number: 11:00 - 11:30 am Session: Coherent Raman I

Photoinduced Structural Dynamics of 4-(Dimethylamino)benzonitrile (DMABN) Probed with Femtosecond Stimulated Raman Spectroscopy (FSRS)
Justin Rhinehart; Randy Mehlenbacher; David Mccamant
University of Rochester, Rochester, NY

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Summary
FSRS and transient absorption have been used to probe the photoinduced charge transfer (CT) dynamics of DMABN. FSRS spectra of the quinoidal C=C stretching mode at 1581 cm-1 in the CT state support internal conversion from the locally excited to the charge transfer state in 4 -5 ps and then a subsequent vibrational relaxation within the CT state manifold on a 6 - 8 ps time scale. Dramatic shifting and narrowing of the 1581 cm-1 quinoidal C=C stretch on the ~7 ps time scale indicate that the quinoidal distortion plays an important part in the CT reaction coordinate.

Code: MOA Time Slot/Poster Number: 11:30 - 11:50 am Session: Coherent Raman I

Femtosecond Stimulated Raman Spectroscopy: Theory and Experiments
Soo-Ying Lee1; Kai Niu1; Bin Zhao1; Zhigang Sun2
1School of Physical & Mathematical Sciences, Singapore, Singapore; 2Department of Chemistry, Duke University, Durham, United States of America

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Summary
Femtosecond stimulated Raman spectroscopy is described by eight Feynman dual time-line diagrams where the corresponding third-order polarization expressions can be written down easily. The theory is applied to explain: (a) the resonance FSRS from the ground vibrational state of rhodamine 6G, (b) the inversion symmetry of the CCl3 bending sidebands about the CD stretch in the FSRS spectra of a dynamic wave packet on the ground state surface of CDCl3 which has been created by impulsive Raman scattering, and (c) dispersive lineshapes in the FSRS spectra in the first 500 fs photoisomerization of excited state bacteriorhodopsin.

Code: MOA Time Slot/Poster Number: 11:50 am - 12:10 pm Session: Coherent Raman I

Femtosecond Time-Resolved Observation of Hot Vibrational States in Carotenoides
Vinu Namboodiri; Mahesh Namboodiri; Günter Flachenecker; Arnulf Materny
Jacobs University Bremen, Bremen, Germany

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Summary
Femtosecond time-resolved degenerate four-wave mixing (DFWM) spectroscopy is applied to investigate the intra-molecular dynamics of carotenoides after initial photo excitation. Making use of single and two-photon resonances, within one experiment the internal conversion processes populating and depopulating the excited S1 state can be observed together with the dynamics of hot vibrational states of the ground S0 state. A rate model is used to evaluate the experimental data. The results are compared with results obtained from former experiments, which were using transient gratings as well as coherent anti-Stokes Raman spectroscopy for the characterization of ground and excited state dynamics.

Code: MOA Time Slot/Poster Number: 12:10 - 12:30 pm Session: Coherent Raman I

Spectral Interferences In Femtosecond Stimulated Raman Microscopy
Benjamin Marx1, 2; Evelyn Ploetz1, 2; Peter Gilch1, 2
1Ludwig-Maximilians-Universität München (LMU), München, Germany; 2Heinrich-Heine-Universität Düsseldorf (HHU), Düsseldorf, Germany

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Summary
In femtosecond stimulated Raman microscopy a spectrally narrow pump and a broadband probe pulse interact with a sample at the focus of a microscope. Stimulated Raman scattering causes spectral changes of the probe light from which the Raman spectrum can be retrieved. In addition to the Raman signature sinusoidal modulations of the probe spectrum are observed. These modulations are caused by non-linear broadening of the pump pulse in the sample which is heterodyned by the probe light. The effect occurs for pump pulse intensities differing by many orders of magnitude. Properties and suppression of the effect will be discussed.