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The use of d -level qudits instead of two-level qubits can largely increase the power of quantum logic for many applications, ranging from quantum simulations to quantum error correction. Magnetic molecules are ideal spin systems to realize these large-dimensional qudits. Indeed, their Hamiltonian can be engineered to an unparalleled extent and can yield a spectrum with many low-energy states. In particular, in the past decade, intense theoretical, experimental, and synthesis efforts have been devoted to develop quantum simulators based on molecular qubits and qudits. However, this remarkable potential is practically unexpressed, because no quantum simulation has ever been experimentally demonstrated with these systems. Here, we show the first prototype quantum simulator based on an ensemble of molecular qudits and a radiofrequency broadband spectrometer. To demonstrate the operativity of the device, we have simulated quantum tunneling of the magnetization and the transverse-field Ising model, representative of two different classes of problems. These results represent an important step toward the actual use of molecular spin qudits in quantum technologies.

We demonstrate by use of continuous wave- and pulse-electron paramagnetic resonance spectroscopy on oriented single crystals of magnetically dilute Yb III ions in Yb 0.01 Lu 0.99 (trensal) that molecular entangled two-qubit systems can be constructed by exploiting dipolar interactions between neighboring Yb III centers. Furthermore, we show that the phase memory time and Rabi frequencies of these dipolar-interaction-coupled entangled two-qubit systems are comparable to the ones of the corresponding single qubits.

Multifrequency electron paramagnetic resonance spectroscopy on oriented single crystals of magnetically dilute Gd(III) ions in Gd 0.004 Y 0.996 (trensal) is used to determine the Hamiltonian parameters of the ground 8 S 7/2 term and its phase memory time, T m , characterizing its coherent spin dynamics. The vanishing orbital angular momentum of the 8 S 7/2 term makes it relatively insensitive to spin-lattice relaxation mediated by magnetoelastic coupling and leads to a T m of 12 μs at 3 K, which is not limited by spin-lattice relaxation.

We report the synthesis, characterization, and magnetic properties of eight neutral functionalized trigonal lanthanide coordination complexes LnL with Ln = Gd ( 1 ), Tb ( 2 ), Dy ( 3 ), Ho ( 4 ), Er ( 5 ), Tm ( 6 ), Yb ( 7 ), Lu ( 8 ). These were prepared through a one-pot synthesis where, first, the ligand H 3 L was synthesized in situ through a Schiff base reaction of tris(2-aminoethyl)amine with 2,6-diformyl- p -cresol. Following addition of Ln(OTf) 3 · x H 2 O and base, LnL was obtained. Powder X-ray diffraction confirms that all complexes are isostructural. LnL contain pendant, noncoordinating carbonyl functions that are reactive and represent direct anchoring points to appropriately functionalized surfaces. Furthermore, these reactive carbonyl functions can be used to postfunctionalize LnL: for example, with aromatic π systems. We present herein the Schiff base condensation of 7 with benzylamine to yield 9 as well as the characterization and magnetic properties of 9 . Our study establishes LnL as a truly versatile module for the surface deposition of Ln-based single-ion magnets.