Nonlinear optical (NLO) materials have recently aroused
great interest
owing to their capability of frequency conversion in solid-state lasers.
Herein, we report an acentric zinc germanate K2ZnGe2O6 obtained successfully through spontaneous crystallization
methods. It affords a novel three-dimensional (3D) framework comprised
of [GeO4] and [ZnO4] motifs with K atoms located
in the tunnels. K2ZnGe2O6 displays
a moderate second-harmonic-generation (SHG) intensity (0.73 ×
KDP) with phase-matchable behavior. Optical characterization demonstrated
that it has a UV cutoff edge located at 368 nm with a large energy
band of 3.23 eV, accompanied by a wide transmission window, covering
a 3–5 μm atmospheric window. Moreover, thermal properties
implied that it possesses intriguing thermal stability of 987 °C
and a congruent melting nature. Additionally, first-principles calculations
unveiled that the NLO performance was primarily attributed to the
collective effect of [GeO4] and [ZnO4] building
units. These findings indicate that K2ZnGe2O6 is a potential NLO crystal.
Nonlinear
optical (NLO) crystals have aroused burgeoning interest
in recent years owing to their frequency conversion properties and
versatile optoelectronic applications. Nevertheless, a current challenge
is to excavate NLO crystals with superior overall performance, especially
in configurationally rigid silicates. Herein, a new NLO bismuth silicate,
Cs2Bi2OSi2O7 (CBSO), was
successfully synthesized, which features a 3D structure containing
rare face-sharing [BiO5] pyramids and [SiO4]
groups. The introduction of highly polarized Bi3+ cations
resulted in large induced polarization and an enhanced second harmonic
generation (SHG) intensity of 3.5 KDP. Remarkably, CBSO fully meets
the precedent conditions for NLO applications, including a wide transparent
window, suitable birefringence (0.044 at 1064 nm), good thermal stability
with congruent-melting behavior, and facile crystal growth. Besides,
first-principles calculations were performed to elucidate the structure–property
relationship of CBSO. These observations demonstrate that CBSO is
a promising NLO material and provide new inspiration for designing
novel SHG-active compounds in strongly covalent systems.
A quaternary
nonlinear-optical (NLO) zinc germanate, Rb2ZnGe2O6 (RZGO), was prepared from its stoichiometric
melts, which belongs to the noncentrosymmetric space group C2221 (No. 20) and features a 3D framework formed
by GeO4 tetrahedra, ZnO4 tetrahedra, and Rb+ cations filling into the void space. RZGO displays a good
phase-matchable second-harmonic-generation (SHG) intensity similar
to that of KH2PO4. The UV cutoff edge for RZGO
was found to be approximately 0.37 μm with a broad optical band
gap of 3.22 eV, indicating a large laser-induced damage threshold.
Further characterizations suggested that this compound displays an
excellent thermal stability (1014 °C) and melts congruently.
Besides, theoretical analysis was also implemented to investigate
the electronic structures and effective NLO coefficients as well as
the origin of the observed SHG response for RZGO. The present study
can enrich the diversity of acentric germanate structures and pave
the way for the synthesis of new NLO compounds.
Polymorphism is crucial for unraveling crystallization mechanism, predicting crystal structure and discovering novel materials. A new high-symmetric polymorph of Li2TeMo3O12, α-Li2TeMo3O12, was identified successfully by using a spontaneous crystallization technique,...
The targeted synthesis of ultraviolet (UV) nonlinear optical (NLO) materials with strong second-harmonic generation (SHG) activity and wide transparency window remains a formidable challenge. Herein, a prospective rare-earth borate UV...
Molybdate oxide materials have attracted considerable academic interest owing to their multifunctional optoelectronic properties and applications. However, to date, studies on the intrinsic properties of multiple molybdates have rarely been implemented. Herein, a prospective triple molybdate crystal, Rb 3 LiZn 2 (MoO 4 ) 4 , with high crystalline quality was successfully grown using top-seeded solution growth (TSSG) approaches. Intriguingly, it affords a cage-like structure with the I4̅ 3d space group, analogous to that of Ca 12 Al 14 O 33 (C12A7). The Rb 3 LiZn 2 (MoO 4 ) 4 crystal exhibits excellent thermal stability up to 603 °C, accompanied by a congruent melting nature. Simultaneously, it preserves the optical merits of a large band gap of 4.10 eV and a wide transmission window of 0.29−5.4 μm, which are superior to those of most molybdate crystals. More importantly, Raman spectroscopic measurements demonstrated that the title compound possesses an intense Raman shift located at 925 cm −1 and narrow line width, facilitating a stimulated Raman laser. In addition, first-principles calculations were also implemented to elucidate the structure−property relationships of Rb 3 LiZn 2 (MoO 4 ) 4 . These observations provide an empirical platform for intuitively comprehending the underlying properties of multiple molybdates and pave the way for exploiting Raman crystals.
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