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Abstract In this work, we report the development and assessment of the nonadiabatic molecular dynamics approach with the electronic structure calculations based on the linearly scaling subsystem density functional method. The approach is implemented in an open-source embedded Quantum Espresso/Libra software specially designed for nonadiabatic dynamics simulations in extended systems. As proof of the applicability of this method to large condensed-matter systems, we examine the dynamics of nonradiative relaxation of excess excitation energy in pentacene crystals with the simulation supercells containing more than 600 atoms. We find that increased structural disorder observed in larger supercell models induces larger nonadiabatic couplings of electronic states and accelerates the relaxation dynamics of excited states. We conduct a comparative analysis of several quantum-classical trajectory surface hopping schemes, including two new methods proposed in this work (revised decoherence-induced surface hopping and instantaneous decoherence at frustrated hops). Most of the tested schemes suggest fast energy relaxation occurring with the timescales in the 0.7–2.0 ps range, but they significantly overestimate the ground state recovery rates. Only the modified simplified decay of mixing approach yields a notably slower relaxation timescales of 8–14 ps, with a significantly inhibited ground state recovery. 

We present the design, fabrication and characterization of high quality factor silicon nitride nanobeam PhC cavities at visible wavelengths for coupling to diamond color centers in a cavity QED system. We demonstrate devices with a quality factor of ∼24, 000 (±250) around the zero-phonon line of the germanium-vacancy center in diamond. We also present an efficient fiber-to-waveguide coupling platform for suspended nanophotonics. By gently changing the corresponding effective indices at the fiber-waveguide interface, we achieve a coupling efficiency of ∼96% (±2%) at the cavity resonance.