Solid-State Nonlinear Optical Switch with the Widest Switching Temperature Range Owing to its Continuously Tunable Tc
2020
Interest on the nonlinear
optical (NLO) switches that turn on/off
the second-harmonic generation (SHG) triggered by the external stimulus
(such as heat) have continuously grown, especially on the solid-state
NLO switches showing superior stability, reversibility, and reproducibility.
Herein, we discover (NH4)2PO3F, as
an entirely new solid-state NLO switch showing outstanding switch
contrast and reversibility as well as strong SHG intensity (1.1 ×
KH2PO4 (KDP)) and high laser-induced damage
threshold (2.0 × KDP), undergoes a unique first-order phase transition
that originates from a reversible hydrogen-bond rearrangement and
needs to overcome an energy barrier. Accordingly, we put forward a
strategy to continuously modify such an energy barrier by reducing
the number of hydrogen bonds per unit cell via an isoelectronic replacement
of NH4+ by K+ with a similar size
yet incapability of providing any hydrogen bond. Consequently, Kx(NH4)2–xPO3F (x = 0–0.3) exhibiting
excellent switching performance are obtained. Remarkably, Kx(NH4)2–xPO3F not only realizes a continuously tunable Tc spanning from 270 to 150 K, representing the
widest NLO switching temperature range ever known but also indicates
the first solid-state NLO switch example with continuous Tc. Intrinsically, such a Tc decline depends on the weakening degree of the hydrogen-bonding
interactions in the unit cell. These new insights will shed useful
light on the future material design and open new application possibilities.
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