Presentation on theme: "Forecasting two-photon absorption based on one-photon properties"— Presentation transcript:
1Forecasting two-photon absorption based on one-photon properties Nikolay Makarov,Department of Physics, Montana State UniversityMikhail Drobizhev, Zhiyong Suo, Aleks RebaneE. Scott Tarter, Benjamin D. Reeves, Brenda SpanglerFanqing Meng, Charles W. SpanglerCraig J. Wilson, Harry L. AndersonDepartment of Physics, Montana State University, Bozeman, MTSensopath Technologies, Inc., Bozeman, MTMPA Technologies, Inc., Bozeman, MTDepartment of Chemistry, University of Oxford, Mansfield, Oxford, UK
3Motivation: Why to predict? lNHClNCHNNCWhich one is better? Why?
4Motivation: What can quantum chemistry do? m, Em, mC. Katan, S. Tretiak, M.H.V. Werts, A.J. Bain, R.J. Marsh, N. Leonczek, N. Nicolaou, E. Badaeva, O. Mongin, M. Blanchard-Desce,“Two-photon transitions in quadrupolar and branched chromophores: experiment and theory”, J. Phys. Chem. B 2007, 111,
5Experiments: Setup Jobin Yvon Triax 550 sample Laser system L2 USB Coherent VERDI 64W CW 532nmL2Coherent MIRA 9000.5W 795nm 150fsWavelength controlHamamatsu Streak Camera C5680Coherent LEGENDRegen. Amplifier1.1W 1kHz 795nm 150fsIntensity controlTOPAS-C0.3W 1kHz 125fsUSBSerialDigital OscilloscopeRef. Channel DAQGPIBCCD cameracontrol and DAQPCLabViewFilterwheelCorre-latorRef. detectorFROGOSAL1Pulse characterizationLNCCDsample3006001200l/mm-1F1M1Jobin Yvon Triax 550Perkin-Elmer Lambda900SpectrophotometerPerkin-Elmer LS 50BLuminescence Spectrometer
7Second order perturbation theory: Calculations: How to?Second order perturbation theory:1Local field factors:LorentzOnsagerDipole moments:SolvatochromicshiftsLinear absorption,fluorescenceMolecule densityFluorescence anisotropy
8Calculations: Results 1002003007211691854312102, GM1002003002, GM11212105416978314R2For molecule density (=1)For anisotropy2(a)2(b)fL0.83.31.4fO0.61.80.9
9Conclusions Acknowledgements See poster for details We show that the perturbation theory applied for two-level system quantitatively predicts the 2PA cross sections in dipolar molecules, provided that the necessary molecular parameters such as transition- and permanent dipole moments are independently measured.In most cases, the discrepancy between theory and experiment was less than 20%, and always less than 50%. This is the first time that such direct quantitative correspondence is demonstrated for a wide range of dipolar molecules.The overall significance of this work demonstrates a practical way how a set of relatively straightforward linear spectroscopic measurements can be used to study and predict nonlinear 2PA properties.AcknowledgementsThe work was supported by AFOSR.See poster for details