0000000001302465
AUTHOR
Aman Ullah
Spectroscopic analysis of vibronic relaxation pathways in molecular spin qubit [Ho(W5O18)2]9−: sparse spectra are key
Molecular vibrations play a key role in magnetic relaxation processes of molecular spin qubits as they couple to spin states, leading to the loss of quantum information. Direct experimental determination of vibronic coupling is crucial to understand and control the spin dynamics of these nano-objects, which represent the limit of miniaturization for quantum devices. Herein, we measure the vibrational properties of the molecular spin qubit $[$Ho(W$_5$O$_{18}$)$_2]^{9-}$ by means of magneto-infrared spectroscopy. Our results allow us to unravel the vibrational decoherence pathways in combination with $ab$ $initio$ calculations including vibronic coupling. We observe field-induced spectral cha…
Electrical two-qubit gates within a pair of clock-qubit magnetic molecules
Enhanced coherence in HoW$_{10}$ molecular spin qubits has been demonstrated by use of Clock Transitions (CTs). More recently it was shown that, while operating at the CTs, it was possible to use an electrical field to selectively address HoW$_{10}$ molecules pointing in a given direction, within a crystal that contains two kinds of identical but inversion-related molecules. Herein we theoretically explore the possibility of employing the electric field to effect entangling two-qubit quantum gates among two neighbouring CT-protected HoW$_{10}$ qubits within a diluted crystal. We estimate the thermal evolution of $T_1$, $T_2$, find that CTs are also optimal operating points from the point of…
Insights on the coupling between vibronically active molecular vibrations and lattice phonons in molecular nanomagnets
Spin-lattice relaxation is a key open problem to understand the spin dynamics of single-molecule magnets and molecular spin qubits. While modelling the coupling between spin states and local vibrations allows to determine the more relevant molecular vibrations for spin relaxation, this is not sufficient to explain how energy is dissipated towards the thermal bath. Herein, we employ a simple and efficient model to examine the coupling of local vibrational modes with long-wavelength longitudinal and transverse phonons in the clock-like spin qubit [Ho(W$_5$O$_{18}$)$_2$]$^{9-}$. We find that in crystals of this polyoxometalate the vibrational mode previously found to be vibronically active at …
Quantum coherent spin-electric control in a molecular nanomagnet at clock transitions
Electrical control of spins at the nanoscale offers significant architectural advantages in spintronics, because electric fields can be confined over shorter length scales than magnetic fields1–5. Thus, recent demonstrations of electric-field sensitivities in molecular spin materials6–8 are tantalizing, raising the viability of the quantum analogues of macroscopic magneto-electric devices9–15. However, the electric-field sensitivities reported so far are rather weak, prompting the question of how to design molecules with stronger spin–electric couplings. Here we show that one path is to identify an energy scale in the spin spectrum that is associated with a structural degree of freedom with…
In Silico Molecular Engineering of Dysprosocenium-Based Complexes to Decouple Spin Energy Levels from Molecular Vibrations
Molecular nanomagnets hold great promise for spintronics and quantum technologies, provided that their spin memory can be preserved above liquid-nitrogen temperatures. In the past few years, the magnetic hysteresis records observed for two related dysprosocenium-type complexes have highlighted the potential of molecular engineering to decouple vibrational excitations from spin states and thereby enhance magnetic memory. Herein, we study the spin-vibrational coupling in [(CpiPr5)Dy(Cp*)]+ (CpiPr5 = pentaisopropylcyclopentadienyl, Cp* = pentamethylcyclopentadienyl), which currently holds the hysteresis record (80 K), by means of a computationally affordable methodology that combines first-pri…
Binding Sites, Vibrations and Spin-Lattice Relaxation Times in Europium(II)-Based Metallofullerene Spin Qubits.
Abstract To design molecular spin qubits with enhanced quantum coherence, a control of the coupling between the local vibrations and the spin states is crucial, which could be realized in principle by engineering molecular structures via coordination chemistry. To this end, understanding the underlying structural factors that govern the spin relaxation is a central topic. Here, we report the investigation of the spin dynamics in a series of chemically designed europium(II)‐based endohedral metallofullerenes (EMFs). By introducing a unique structural difference, i. e. metal‐cage binding site, while keeping other molecular parameters constant between different complexes, these manifest the ke…
Quantum coherent manipulation of spin information in molecular nanomagnets
Los sistemas cuánticos de dos niveles basados en estados de espín, conocidos como ``qubits de espín'', son bloques prometedores para el desarrollo de tecnologías cuánticas. Entre las distintas plataformas físicas, los qubits de espín definidos en imanes de molécula única (SMM) son candidatos prometedores porque su estructura electrónica puede ajustarse fácilmente mediante ingeniería química (es decir, el Hamiltoniano de espín molecular puede modificarse con facilidad). Sin embargo, los qubits moleculares de espín generados en SMM se enfrentan a varios retos: coherencia cuántica frágil, control coherente insuficiente de los estados de espín y generación de entrelazamiento entre los qubits de…
CSD 2036360: Experimental Crystal Structure Determination
Related Article: Junjie Liu, Jakub Mrozek, Aman Ullah, Yan Duan, Jos�� J. Baldov��, Eugenio Coronado, Alejandro Gaita-Ari��o, Arzhang Ardavan|2021|Nat.Phys.|17|1205|doi:10.1038/s41567-021-01355-4
CSD 2036359: Experimental Crystal Structure Determination
Related Article: Junjie Liu, Jakub Mrozek, Aman Ullah, Yan Duan, Jos�� J. Baldov��, Eugenio Coronado, Alejandro Gaita-Ari��o, Arzhang Ardavan|2021|Nat.Phys.|17|1205|doi:10.1038/s41567-021-01355-4
CSD 2036358: Experimental Crystal Structure Determination
Related Article: Junjie Liu, Jakub Mrozek, Aman Ullah, Yan Duan, Jos�� J. Baldov��, Eugenio Coronado, Alejandro Gaita-Ari��o, Arzhang Ardavan|2021|Nat.Phys.|17|1205|doi:10.1038/s41567-021-01355-4
Quantum coherent spin-electric control in a molecular nanomagnet at clock transitions. Open data set
Data supporting the related publication.