Conjugatged Oligomeric Coordinated Silver Phenylacetylide Derivatives With Ultrafast Optical Kerr Effect
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Conjugatged Oligomeric Coordinated Silver Phenylacetylide Derivatives With Ultrafast Optical Kerr Effect Y. H. Xu1, B. K.Teo1, H.M.Wu2, S.L.Guo2, Y.K.He2, H.Y.Chen2,*,W. Qian3,S.J.Wu3, Y.H.Zuo3 1
Department of Chemistry, University of Illinois at Chicago, Chicago, IL 60607 College of Chemistry and Molecular Engineering, Peking Univ., Beijing 100871, P.R. China 3 Department of Physics, Peking Univ., Beijing 100871, P.R. China 2
ABSTRACT Silver phenylacetylide prepared by one-step process was characterized as a linear coordinated polymeric compound by matrix-assisted laser desorption/ionization time-of-flight (MALDI-TOF) mass spectroscopy. Its prominent third-order optical nonlinearity was detected by heterodyned ultrafast optical Kerr effect (OHD-OKE) measurement. The second-order hyperpolarizability was enhanced by 2 orders of magnitude by means of incorporation of proper electron-pushing groups. The structure status was further investigated by quantum chemical calculation and molecular modeling. INTRODUCTION Special attention has been focused on conjugated organic polymers for their promising potentials of designing various advanced materials [1-3]. In recent ten years, investigations of functionalized transition metal compounds with organic ligands have been greatly intensified due to the presence of d-electrons incorporated in the conjugated system, which are expected to enhance the hyperpolarizability and nonlinear susceptibilities [4,5]. Silver phenylacetylide is actually a polymeric conjugated compound, thus it is naturally to be expected to exhibit optical nonlinear response. The prominent third-order nonlinear optical (NLO) properties of metal phenylacetylide compounds were really observed through OHD-OKE measurement as described in our previous letter [6]. Here we report the strategy to enhance the NLO properties of silver phenylacetylides through structure-property relationship study. The structure status of silver phenylacetylide and its derivatives were further investigated by quantum chemical method and molecular modeling. EXPERIMENTS Phenylacetylene (ACROS, 98%) was redistilled just prior to reaction or polymerization. Micro FT-IR spectra were recorded by Nicolet Magna 750. UV-vis spectra were taken by Shimadzu 2100. Silver content was determined by inductively coupled plasma-atomic emission spectrometry (IRIS AP) in Institute of Physics, Chinese Academy of Sciences. Differential scanning calorimetry (DSC) analysis was done by TA DSC-2010. MALDI-TOF MS analysis were performed using a BRUKER BIFLEXTMIII, with 1,8,9-anthracenetriol (99%, Aldrich) as matrix and data collected by linear scan or reflected mode in Institute of Chemistry, Chinese Academy of Sciences. The OHD-OKE measurements were performed by using ultrashort laser pulses generated from a Satori Model 774 ultrafast dye laser. One-step preparation of silver phenylacetylide [AgC≡CPh]n (APA): 6.15 mmol of silver nitrate, 18.45 mmol of phenylacetylene and 18.45 mmol of triethylamine were reacted in 70 mL acetonitrile with stirring. Then the pro
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