Abstract
High‐performance
ultraviolet
(UV)
nonlinear
optical
(NLO)
crystals
must
exhibit
three
critical
properties:
a
large
second‐harmonic
generation
(SHG)
response,
adequate
birefringence,
and
short
UV
cutoff
edge.
However,
these
key
characteristics
are
often
interdependent
challenging
to
achieve
simultaneously
within
single
crystal.
In
this
study,
novel
non‐centrosymmetric
compound,
K[NH
2
(CH
COO)
]
is
introduced,
synthesized
from
the
innovative
flexible
π‐conjugated
group
[NH
−
.
Benefiting
excellent
microscopic
properties
of
groups,
despite
suboptimal
arrangement
groups
still
demonstrates
remarkable
balance
in
its
linear
performance.
This
includes
strong
SHG
response
3
times
that
KDP,
suitable
birefringence
0.088@1064
nm,
edge
at
208
nm.
Emphatically,
high‐quality,
inch‐sized
(up
60
×
46
30
mm
)
successfully
grown
using
water
solution
technique,
paving
way
for
practical
applications
promising
material.
Accounts of Chemical Research,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Dec. 12, 2024
ConspectusThe
invention
of
the
laser
marked
a
milestone
in
modern
science
and
technology.
Inorganic
second-order
nonlinear
optical
(NLO)
crystals,
with
their
unique
frequency
conversion
capabilities,
play
critical
role
extending
wavelength
ranges.
These
materials
are
indispensable
science,
information
transmission,
other
fields
such
as
industrial
Internet.
As
Moore's
Law
drives
demand
for
shorter
wavelengths
higher-precision
sources,
development
high-performance
short-wave
ultraviolet
(UV)
(<300
nm)
NLO
UV
solid-state
lasers
has
become
increasingly
important.
While
researchers
have
synthesized
variety
discovery
largely
relied
on
trial-and-error
approaches,
which
not
only
time-consuming
but
also
serendipitous
rather
than
based
rational
design
principles.
Moreover,
complexity
designing
these
is
compounded
by
need
to
meet
several
strict
functional
criteria,
including
short
cutoff
edge,
strong
second-harmonic
generation
(SHG)
effect,
moderate
birefringence,
all
hinder
efficient
synthesis.
The
controlled
synthesis
therefore,
remains
significant
scientific
challenge.In
this
Account,
we
propose
three-step
strategy
address
challenge:
(1)
Rational
screening
highly
polar
groups,
particularly
new
NLO-active
groups
novel
bonding
characteristics
(π-localized
distorted
[O
Chemical Science,
Journal Year:
2024,
Volume and Issue:
15(21), P. 8071 - 8079
Published: Jan. 1, 2024
A
universal
synthesis
method
for
polyfluoroantimonites
has
been
developed.
Polar
[(C
5
H
6
N
2
)
H](Sb
4
F
13
was
achieved
by
polyfluoroantimonite
strategy.
It
features
a
strong
SHG
effect,
large
birefringence
and
high
LIDT
value.
Chemical Science,
Journal Year:
2024,
Volume and Issue:
15(26), P. 10193 - 10199
Published: Jan. 1, 2024
[LiNO
3
·H
2
O·
o
-C
5
H
NO]·
NO
and
[Mg(NO
)
·6H
O]·(
NO)
,
with
giant
birefringence,
large
bandgaps,
good
growth
habits,
were
designed
using
a
cocrystal
strategy.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Dec. 15, 2024
Abstract
Nonlinear
optics,
signifying
a
revolutionary
paradigm
change
within
the
realm
of
has
ushered
in
transformative
era
by
employing
nonlinear
optical
crystals
to
manipulate
and
harness
laser
power
for
at
least
six
decades.
The
most
exciting
aspects
(NLO)crystal
is
repercussions
bonding
over
extended
functionalized
units
external
force
how
slight
alterations
atomic
scale
can
result
huge
changes
macroscopic
properties.
However,
date,
precisely
controlling
unit
its
potential
induce
directed
property
is,
yet,
not
fully
realized.
Here,
NLO
are
explored
prospected
from
viewpoint
unit,
with
an
emphasis
on
application
material
design
control
regulate
key
properties
start
regulating
their
functions.
An
introduction
anionic
group
theory
started
here,
which
considers
functional
be
primary,
then
turns
discussion
modification
through
emerging
strategies
this
facilitates
new
materials.
Additional
breakthroughs
rational
strategy
functionalize
groups
covered,
including
integration,
preferential
arrangement
induction,
microcosmic
performance
maximization
as
well
supports
these
materials
discovery
theoretical
method.
Beyond
gratifying
achievements
made,
some
future
perspectives
move
step
forward
finally
provided.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(38)
Published: June 26, 2024
Abstract
Birefringent
crystals
have
essential
applications
in
optical
communication
areas.
Low‐dimensional
structures
with
inherited
structural
anisotropy
are
potential
systems
for
investigating
birefringent
materials
large
birefringence.
In
this
work,
the
zero‐dimensional
(0D)
[(
p
‐C
5
H
NO)
2
ZnCl
]
(
1
)
and
[
6
NO]
[ZnCl
4
were
obtained
by
introducing
π‐conjugated
NO
(4HP)
into
three‐dimensional
(3D)
.
Remarkably,
exhibits
a
giant
birefringence
of
0.482@546
nm,
which
is
largest
among
Zn‐based
ultraviolet
(UV)
compounds
160
times
that
According
to
theoretical
calculation
analyses,
polarizability,
high
spatial
density,
ideal
distribution
[(4HP)
0
cluster,
low
dimension
result
dramatically
increased
compared
This
work
will
provide
valid
route
accelerating
design
synthesis
excellent
low‐dimensional
systems.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(44)
Published: July 10, 2024
Anisotropy
is
crucial
for
birefringence
(Δn)
in
optical
materials,
but
optimizing
it
remains
a
formidable
challenge
(Δn
>0.3).
Supramolecular
frameworks
incorporating
π-conjugated
components
are
promising
achieving
enhanced
because
of
their
structural
diversity
and
inherent
anisotropy.
Herein,
we
first
synthesized
(C
Advanced Optical Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 17, 2025
Abstract
The
hydrothermal
synthesis
and
characterization
of
a
novel
bismuth
molybdenum
selenite
material,
Bi
2
F
(MoO
3
)
(SeO
·H
O,
designed
using
chemical
substitution‐based
approach,
is
reported.
This
material
represents
the
first
example
its
kind
in
Bi–Mo–Se
system,
providing
new
insights
into
noncentrosymmetric
(NCS)
crystal
engineering.
compound
exhibits
outstanding
nonlinear
optical
(NLO)
properties,
including
second‐harmonic
generation
(SHG)
efficiency
1.2
times
that
KTiOPO₄
birefringence
0.118
at
546.1
nm.
Additionally,
it
demonstrates
wide
transparency
range
(0.36–10
µm),
making
promising
candidate
for
advanced
NLO
applications.
Structural
computational
analyses
show
remarkable
SHG
response
driven
by
highly
distorted
MoO₆
octahedra,
strong
interatomic
interactions
within
1D
chains,
polarizable
⁺
SeO₃
groups.
Furthermore,
thermally
stable
after
dehydration
affinity
occupying
void
space
5‐membered
ring
(5‐MR).
These
findings
open
avenues
design
NCS
materials
with
enhanced
functionalities,
offering
significant
potential
development
solid‐state
materials.
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Oct. 7, 2024
The
precise
modulation
of
the
spatial
orientations
and
connection
modes
primitives
is
vital
for
certain
critically
important
optical
functions
nonlinear
(NLO)
materials
(specifically,
second-harmonic
generation
(SHG)
bandgap);
however,
we
are
yet
to
achieve
a
sufficient
level
control
designed
construction
efficient
broadband
NLO
materials.
Exploiting
changes
in
microscopic
polarization
that
may
result
from
dimensional
increase,
propose
herein
zero-dimensional
(0D)-to-three-dimensional
(3D)
dimensionality-increase
strategy
realize
strong
SHG
responses
first
time.
novel
3D
pseudo
diamond-like
Zn(SCN)2
has
been
synthesized
by
removing
SHG-inactive
[NH4]+
counter
cations
H2O
molecules
located
between
adjacent
discrete
[Zn(SCN)4]
building
blocks
within
0D
(NH4)2Zn(SCN)4·3H2O.
0D-to-3D
dimensionality
engineering,
proceeding
(NH4)2Zn(SCN)4·3H2O
Zn(SCN)2,
results
significantly
enhanced
activity
(8
×
KH2PO4
@
1064
nm,
4.18
eV
bandgap
former
c.f.
2
β-BaB2O4
380
30
KTiOPO4
2100
4.78
latter)
UV
NIR
regions
(SHG@300–1050
nm).
Theoretical
calculations
crystal
structure
analyses
reveal
coordination-bond-connected
responsible
its
giant
responses.