title: Pb2Ba3(BO3)3Cl: A Material with Large SHG Enhancement Activated by Pb-Chelated BO3 Groups.
abstract: Pb(II) has long been associated with lone pair activity and is often substituted in alkali earth metal borates to create new nonlinear optical (NLO) materials with enhanced second harmonic generation (SHG) capabilities. However, large enhancement in isomorphic Pb-free analogues is rare. Here we report a new NLO material Pb2Ba3(BO3)3Cl with a phase-matching SHG response approximately 3.2× that of KDP and 6× higher than its isomorphic compound Ba5(BO3)3Cl. We show that the enhanced SHG response originates from a unique edge-sharing connection between lead-oxygen polyhedra and boron-oxygen groups, making the dielectric susceptibility more easily affected by the external electric field of an incident photon. This understanding provides a route to identify systems that would benefit from SHG-active cation substitution in isomorphic structures that exhibit weak or null SHG responses.
authors.affiliation: ‡Engineering Department of Chemistry and Environment, Xinjiang Institute of Engineering, 236 Nanchang Road, Urumqi 830091, China.
authors.forename: Xiaoyu
authors.initials: X
authors.lastname: Dong
authors.forename: Qun
authors.initials: Q
authors.lastname: Jing
authors.affiliation: ‡Engineering Department of Chemistry and Environment, Xinjiang Institute of Engineering, 236 Nanchang Road, Urumqi 830091, China.
authors.forename: Yunjing
authors.initials: Y
authors.lastname: Shi
authors.forename: Zhihua
authors.initials: Z
authors.lastname: Yang
authors.forename: Shilie
authors.initials: S
authors.lastname: Pan
authors.affiliation: §Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States.
authors.forename: Kenneth R
authors.initials: KR
authors.lastname: Poeppelmeier
authors.affiliation: ∥Department of Materials Science and Engineering, Drexel University, 3141 Chestnut Street, Philadelphia, Pennsylvania 19104-2816, United States.
authors.forename: Joshua
authors.initials: J
authors.lastname: Young
authors.affiliation: ⊥Department of Materials Science and Engineering, Northwestern University, 2220 Campus Drive, Evanston, Illinois 60208-0893, United States.
authors.forename: James M
authors.initials: JM
authors.lastname: Rondinelli