Observation of stimulated Raman scattering in polar tetragonal crystals of barium antimony tartrate trihydrate, Ba[Sb₂((+)C₄H₂O₆)₂]·3H₂O

Abstract

The non-centrosymmetric polar tetragonal (P4 1 ) barium antimony tartrate trihydrate, Ba[Sb 2 ((+)C 4 H 2 O 6 ) 2 ]·3H 2 O, was found to be an attractive novel semi-organic crystal manifesting numerous χ (2) -and χ (3) -nonlinear optical interactions. In particular, with picosecond single-and dualwavelength pumping SHG and THG via cascaded parametric four-wave processes were observed. High-order Stokes and anti-Stokes lasing related to two SRS-promoting vibration modes of the crystal, with ω SRS1 575 cm −1 and ω SRS2 2940 cm −1 , takes place. Basing on a spontaneous Raman investigation an assignment of the two SRS-active vibration modes is discussed.

Cocrystals of 2-Aminopyrimidine with Boric Acid—Crystal Engineering of a Novel Nonlinear Optically (NLO) Active Crystal

“…Second harmonic generation (SHG) measurements of (2-AMP) 3 (H 3 BO 3 ) 2 were performed using the modified Kurtz-Perry powder method [15]. The samples were irradiated with 160 fs laser pulses generated at an 82 MHz repetition rate by a Ti:sapphire laser (MaiTai, Spectra Physics, Santa Clara, CA, USA) at 800 nm.…”

“…(2-AMP) 3 (H 3 BO 3 ) 2 cocrystals were prepared by slow evaporation at room temperature of the aqueous solution of 2-aminopyrimidine and boric acid mixed in a 1:1 molar ratio. The resulting colorless crystals were filtered off and dried in air.…”

“…The basic crystallographic data, measurement, and refinement details are summarized in Table 1. The crystallographic data of (2-AMP) 3 (H 3 BO 3 ) 2 and 2-AMP(H 3 BO 3 ) 2 were deposited at the Cambridge Crystallographic Data Centre as supplementary publications CCDC 1586908 and CCDC 1586909, respectively. A copy of the data is available free of charge from CCDC, 12 Union Road, Cambridge CG21, EZ, UK (fax: +44 1223 336033; e-mail: deposit@ccdc.cam.ac.uk).…”

“…Considering these properties, crystal engineering has two main objectives-to incorporate the 2-aminopyrimidine moiety into molecular crystals with proper symmetry and to preserve it preferably as a neutral molecule. Moreover, several organic molecular crystals and "semi-organic" materials are promising as stimulated Raman scattering (SRS)-active materials, which could also exhibit various χ (2) and χ (3) NLO effects including third harmonic generation and cascaded self-frequency doubling and tripling [2,3].…”

“…In this paper, we report the preparation, crystal structure determination, and spectroscopic and optical properties of two molecular cocrystals of 2-aminopyrimidine with boric acid, i.e., trigonal 2-aminopyrimidine-boric acid (3/2), (2-AMP) 3 (H 3 BO 3 ) 2 , and monoclinic 2-aminopyrimidine-boric acid (1/2), 2-AMP(H 3 BO 3 ) 2 . These hydrogen-bonded materials were isolated within a crystal engineering study employing promising inorganic and organic molecular carriers of NLO properties.…”