Unexpected Photodriven Linker-to-Node Hole Transfer in a Zirconium-Based Metal-Organic Framework.

Zr(μ-O)(μ-OH) node cores are indispensable building blocks for almost all zirconium-based metal-organic frameworks. Consistent with the insulating nature of zirconia, they are generally considered electronically inert. Contrasting this viewpoint, we present spectral measurements and calculations indicating that emission from photoexcited NU-601, a six-connected Zr-based MOF, comes from both linker-centric locally excited and linker-to-node charge-transfer (CT) states.

Mixed quantum-classical modeling of exciton-phonon scattering in solids: Application to optical linewidths of monolayer MoS2.

We present a mixed quantum-classical framework for the microscopic and non-Markovian modeling of exciton-phonon scattering in solid-state materials and apply it to calculate the optical linewidths of monolayer MoS2. Within this framework, we combine reciprocal-space mixed quantum-classical dynamics with models for the quasiparticle band structure as well as the electron-hole and carrier-phonon interactions, parametrized against ab initio calculations, although noting that a direct interfacing with ab initio calculations is straightforward in principle. We introduce various parameters for truncating the Brillouin zone to select regions of interest.

Dark State Concentration Dependent Emission and Dynamics of CdSe Nanoplatelet Exciton-Polaritons.

The recent surge of interest in polaritons has prompted fundamental questions about the role of dark states in strong light-matter coupling phenomena. Here, we systematically vary the relative number of dark states by controlling the number of stacked CdSe nanoplatelets confined in a Fabry-Pérot cavity. We find the emission spectrum to change significantly with an increasing number of nanoplatelets, with a gradual shift of the dominant emission intensity from the lower polariton branch to a manifold of dark states.

Mixed Quantum-Classical Dynamics under Arbitrary Unitary Basis Transformations.

A common approach to minimizing the cost of quantum computations is by unitarily transforming a quantum system into a basis that can be optimally truncated. Here, we derive classical equations of motion subjected to similar unitary transformations and propose their integration into mixed quantum-classical dynamics, allowing this class of methods to be applied within arbitrary bases for both the quantum and classical coordinates. To this end, canonical positions and momenta of the classical degrees of freedom are combined into a set of complex-valued coordinates amenable to unitary transformations.