Color rendition, luminous efficacy and reliability are three key technical parameters for white light-emitting diodes (wLEDs) that are dominantly determined by down-conversion phosphors. However, there is usually an inevitable trade-off between color rendition and luminescence efficacy because the spectrum of red phosphor (that is, spectral broadness and position) cannot satisfy them simultaneously. In this work, we report a very promising red phosphor that can minimize the aforementioned trade-off via structure and band-gap engineering, achieved by introducing isostructural LiSi2N3 into CaAlSiN3:Eu2+. The solid solution phosphors show both substantial spectra broadening (88→117 nm) and blueshift (652→642 nm), along with a significant improvement in thermal quenching (only a 6% reduction at 150 °C), which are strongly associated with electronic and crystal structure evolutions. The broadband and robust red phosphor thus enables fabrication of super-high color rendering wLEDs (Ra=95 and R9=96) concurrently with the maintenance of a high-luminous efficacy (101 lm W−1), validating its superiority in high-performance solid state lightings over currently used red phosphors.
The
oxidation state of an element influences its chemical behavior
of reactivity and bonding. Finding unusual oxidation state of elements
is a theme of eternal pursuit. As labeled by an alkali-earth metal,
barium (Ba) invariably exhibits an oxidation state of +2 by a loss
of two 6s valence electrons while its inner 5p closed shell is known
to remain intact. Here, we show through the reaction with fluorine
(F) at high pressure that Ba exhibits a hitherto unexpected high oxidation
state greater than +2 in three pressure-stabilized F-rich compounds
BaF3, BaF4, and BaF5, where Ba takes
on the role of a 5p element by opening up its inert 5p shell. Interestingly
enough, these pressure-stabilized Ba fluorides share common structural
features of Ba-centered polyhedrons but exhibit a diverse variety
of electronic properties showing semiconducting, metallic, and even
magnetic behaviors. Our work modifies the traditional knowledge on
the chemistry of alkali-earth Ba element established at ambient pressure
and highlights the major role of pressure played in tuning the oxidation
state of elements.
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