Using high-level ab initio many-body theory, we theoretically propose that the Dy and the Ni atoms in the [Dy2Ni2(L)4(NO3)2(DMF)2] real molecular magnet as well as in its core, that is, the [Dy2Ni2O6] system, act as two-level qubit systems. Despite their spatial proximity we can individually control each qubit in this highly correlated real magnetic system through specially designed laser-pulse combinations. This allows us to prepare any desired two-qubit state and to build several classical and quantum logic gates, such as the two-qubit (binary) CNOT gate with three distinct laser pulses. Other quantum logic gates include the single-qubit (unary) quantum X, Y, and Z Pauli gates; the Hadamard gate (which necessitates the coherent quantum superposition of two many-body electronic states); and the SWAP gate (which plays an important role in Shor’s algorithm for integer factorization). Finally, by sequentially using the achieved CNOT and Hadamard gates we are able to obtain the maximally entangled Bell states, for example, ( )­(|00⟩ + |11⟩).

Invited for this month's cover picture are the groups of Wolfgang Hübner (TU Kaiserslautern, Germany), Annie Powell (Karlsruhe Institut of Technology, Germany), and Andreas‐Neil Unterreiner (Karlsruhe Institut of Technology, Germany). The cover picture shows the Dy2Ni2‐molecular magnet being excited with a UV/Vis laser pulse, together with its time‐resolved spectrum after the pulse. The comparison of the theoretical and the experimental spectra together with both the observed and the calculated relaxation times reveal, among others, three key points: the intermediate states participating in the laser‐induced dynamics, the partial metal‐to‐oxygen charge‐transfer excitations, and the order of magnitude of the coupling of the molecular magnet to the thermal bath of the environment. Read the full text of their Full Paper at 10.1002/open.202100153.

The two new mononuclear complexes Cu­(tdp)­Cl2·MeCN (1·MeCN, tdp = 2,2′-(1H-1,2,3-triazole-1,4-diyl)­dipyridine) and Cu­(tdp)­Cl2 (1) have been synthesized. Each compound can undergo a reversible SCSC transformation via the sorption/desorption of lattice MeCN molecules to afford the other compound. During the transformation of 1·MeCN to 1, the space group changed from C2/c to P21/n involving a variation in the molecular stacking fashions, leading to a change in magnetic exchange couplings. Using a fully ab initio description of the electronic and magnetic properties of both geometries, we qualitatively explain the difference in the magnetic susceptibilities of the two structures and theoretically calculate their easy and hard axes.

We present a combined experimental and theoretical study of the ultrafast transient absorption spectroscopy results of a {Ni2Dy2}‐compound in DMF, which can be considered as a prototypic molecule for single molecule magnets. We apply state‐of‐the‐art ab initio quantum chemistry to quantitatively describe the optical properties of an inorganic complex system comprising ten atoms to form the chromophoric unit, which is further stabilized by surrounding ligands. Two different basis sets are used for the calculations to specifically identify two dominant peaks in the ground state. Furthermore, we theoretically propagate the compound's correlated many‐body wavefunction under the influence of a laser pulse as well as relaxation processes and compare against the time‐resolved absorption spectra. The experimental data can be described with a time constant of several hundreds of femtoseconds attributed to vibrational relaxation and trapping into states localized within the band gap. A second time constant is ascribed to the excited state while trap states show lifetimes on a longer timescale. The theoretical propagation is performed with the density‐matrix formalism and the Lindblad superoperator, which couples the system to a thermal bath, allowing us to extract relaxation times from first principles.

The Front Cover shows the Dy2Ni2‐molecular magnet being excited with a UV/Vis laser pulse, together with its time‐resolved spectrum after the pulse. The comparison of the theoretical and the experimental spectra together with both the observed and the calculated relaxation times provides evidence on: the intermediate states participating in the laser‐induced dynamics, the partial metal‐to‐oxygen charge‐transfer excitations, and the order of magnitude of the coupling of the molecular magnet to the thermal bath of the environment. More information can be found in the Full Paper by Stefan Sold et al.