Rational Design of Charge‐Neutral, Near‐Infrared‐Emitting Osmium(II) Complexes and OLED Fabrication

Abstract A new series of charge neutral Os(II) isoquinolyl triazolate complexes ( 1 – 4 ) with both trans and cis arrangement of phosphine donors are synthesized, and their structural, electrochemical and photophysical properties are established. In sharp contrast to the cis ‐arranged complexes 2 – 4 , the trans derivative 1 , which shows a planar arrangement of chromophoric N ‐substituted chelates, offers the most effective extended π ‐delocalization and hence the lowest excited state energy gap. These complexes exhibit phosphorescence with peak wavelengths ranging from 692–805 nm in degassed CH 2 Cl 2 at room temperature. Near‐infrared (NIR)‐emitting electroluminescent devices employing 6 wt % of 1 (or 4 ) doped in Alq 3 host material are successfully fabricated. The devices incorporating 1 as NIR phosphor exhibit fairly intense emission with a peak wavelength at 814 nm. Forward radiant emittance reaches as high as 65.02 µW cm −2 , and a peak EQE of ∼1.5% with devices employing Alq 3 , TPBi and/or TAZ as electron‐transporting/exciton‐blocking layers. Upon switching to phosphor 4 , the electroluminescence blue shifts to 718 nm, while the maximum EQE and radiance increase to 2.7% and 93.26 (μW cm −2 ) respectively. Their performances are optimized upon using TAZ as the electron transporting and exciton‐blocking material. The OLEDs characterized represent the only NIR‐emitting devices fabricated using charge‐neutral and volatile Os(II) phosphors via thermal vacuum deposition.