Intensity, Wavelength, and Polarization Dependence of Nonphotochemical Laser-Induced Nucleation in Supersaturated Aqueous Urea Solutions

We have measured the intensity dependence of nonphotochemical laser-induced nucleation (NPLIN) in 11.9 M aqueous urea solutions at 532 and 1064 nm, using both linearly and circularly polarized light. In all cases, we observed a nonlinear intensity dependence of the nucleation efficiency with thresholds of approximately 0.02−0.06 GW/cm2. The threshold at the green wavelength is lower than the threshold at the near-infrared wavelength. Moreover, the green nucleation efficiency is greater than the near-infrared efficiency at the same intensity. We attribute these differences to the greater absorption coefficient of water at 1064 nm compared to that at 532 nm. At both 532 and 1064 nm, the threshold for NPLIN is lower, and the efficiency of NPLIN at a given intensity is higher for linear polarization than for circular polarization. These differences are consistent with an optical Kerr effect mechanism for NPLIN.

[1]  D. Oxtoby Materials chemistry: Crystals in a flash , 2002, Nature.

[2]  G. M. Hale,et al.  Optical Constants of Water in the 200-nm to 200-microm Wavelength Region. , 1973, Applied optics.

[3]  J. Katz,et al.  Photoinduced nucleation of supersaturated vapors in the presence of carbon disulfide , 1982 .

[4]  P. Vekilov,et al.  Dense Liquid Precursor for the Nucleation of Ordered Solid Phases from Solution, Crystal Growth and Design , 2004 .

[5]  Hiroshi Haneda,et al.  Laser-induced crystal growth and morphology control of benzopinacol produced from benzophenone in ethanol/water mixed solution , 2004 .

[6]  J. D. Shore,et al.  Simulations of the nucleation of AgBr from solution , 2000 .

[7]  F. Leusen Ab initio prediction of polymorphs , 1996 .

[8]  Joanna Aizenberg,et al.  Direct Fabrication of Large Micropatterned Single Crystals , 2003, Science.

[9]  T. Aushev,et al.  Radiative B meson decays into Kπγ and Kππγ final states , 2002 .

[10]  I. Weissbuch,et al.  Tailor-made and charge-transfer auxiliaries for the control of the crystal polymorphism of glycine , 1994 .

[11]  K. Mikkelsen,et al.  Polarizability of molecular clusters as calculated by a dipole interaction model , 2002 .

[12]  B. A. Garetz,et al.  Nonphotochemical, laser-induced nucleation of supersaturated aqueous glycine produces unexpected γ-polymorph , 2001 .

[13]  A. Myerson,et al.  Polarization switching of crystal structure in the nonphotochemical light-induced nucleation of supersaturated aqueous glycine solutions. , 2002, Physical review letters.

[14]  C. Alexander,et al.  Directed nucleation of calcite at a crystal-imprinted polymer surface , 1999, Nature.

[15]  Hiroaki Horiuchi,et al.  Laser-Induced Morphology Control and Epitaxy of Dipara-anthracene Produced from the Photochemical Reaction of Anthracene , 2005 .

[16]  R. Popovitz‐Biro,et al.  Understanding and control of nucleation, growth, habit, dissolution and structure of two‐ and three‐dimensional crystals using `tailor‐made' auxiliaries , 1995 .

[17]  Young,et al.  Nonphotochemical, Polarization-Dependent, Laser-Induced Nucleation in Supersaturated Aqueous Urea Solutions. , 1996, Physical review letters.