• θ-TaN achieves a room-temperature thermal conductivity of ~1100 W·m⁻¹·K⁻¹, nearly three times that of copper, shattering the long-standing limit for metals.
• The ultrahigh thermal conductivity is phonon-dominated, enabled by a large acoustic-optical phonon gap and acoustic phonon bunching that suppress phonon-phonon scattering.
• High-quality single crystals of metastable θ-TaN were synthesized via a flux-assisted metathesis reaction, overcoming challenges of conventional high-pressure routes.
• This discovery validates theoretical predictions and opens new avenues for thermal management in high-power electronics and other applications.
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