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Núria Crivillers

Publications and source records attributed to Núria Crivillers.

5 recordsLinked to original sources

Polariton-polariton coherent coupling in a molecular spin-superconductor chip

The ability to establish coherent communication channels is key for scaling up quantum devices. Here, we engineer interactions between distant polaritons, hybrid spin-photon excitations formed at different lumped-element superconducting resonators within a chip. The chip consists of several resonator pairs, slightly detuned in frequency to make them addressable, capacitively coupled within each pair and inductively coupled to a common readout line. They interact locally with samples of PTMr and Tripak$^{-}$ organic free radicals, deposited onto their inductors, which provide model $S = 1/2$, $g \simeq 2$ spin ensembles. Frequency-dependent microwave transmission experiments, performed at very low temperatures, measure polariton frequencies as a function of magnetic field in different scenarios. When only one resonator within a pair hosts a molecular sample, the results evidence that spins couple remotely to the empty LER as well as to the local cavity mode. If both resonators interact with a spin ensemble, the magnetic field tunes the polariton frequencies relative to each other, on account of the different spin-photon interactions at each LER. When polaritons are brought into mutual resonance, an avoided level crossing emerges that gives direct spectroscopic evidence for a coherent polariton-polariton interaction mediated by the circuit. Pump-probe experiments reveal that the excitation of a polariton within a connected pair is felt, thus it can be read out, by the other one. These observations, backed by model calculations, illustrate the control and detection of distant photon-photon and spin-spin correlations and entanglement in a scalable modular chip.

quant-ph↗

Optimizing magnetic coupling in lumped element superconducting resonators for molecular spin qubits

We engineer lumped-element superconducting resonators that maximize magnetic coupling to molecular spin qubits, achieving record single-spin couplings up to $100$ kHz and collective couplings exceeding $10$ MHz. The resonators interact with PTMr organic free radicals, model spin systems with $S=1/2$ and a quasi-isotropic $g \simeq 2$, dispersed in polymer matrices. The highest collective spin-photon coupling strengths are attained with resonators having large inductors, which therefore interact with most spins in the molecular ensemble. By contrast, the coupling of each individual spin $G_{1}$ is maximized in resonators having a minimum size inductor, made of a single wire. The same platform has been used to study spin relaxation and spin coherent dynamics in the dispersive regime, when spins are energetically detuned from the resonator. We find evidences for the Purcell effect, i.e. the photon induced relaxation of those spins that are most strongly coupled to the circuit. The rate of this process gives access to the distribution of single spin photon couplings in a given device. For resonators with a $50$ nm wide constriction at the inductor center, single maximum $G_{1}$ values reach $\sim 100$ kHz. Pumping the spins with strong pulses fed through an independent transmission line induces coherent Rabi oscillations. The spin excitation then proceeds via either direct resonant processes induced by the main pulse frequency or, in the case of square-shaped pulses, via the excitation of the cavity by sideband frequency components. The latter process measures the cavity mode hybridization with the spins and can be eliminated by using Gaussian shaped pulses. These results establish a scalable route toward integrated molecular-spin quantum processors.

quant-ph↗

Interaction of Luminescent Defects in Carbon Nanotubes with Covalently Attached Stable Organic Radicals

The functionalization of single-walled carbon nanotubes (SWCNTs) with luminescent sp$^{3}$ defects has greatly improved their performance in applications such as quantum light sources and bioimaging. Here, we report the covalent functionalization of purified semiconducting SWCNTs with stable organic radicals (perchlorotriphenylmethyl, PTM) carrying a net spin. This model system allows us to use the near-infrared photoluminescence arising from the defect-localized exciton as a highly sensitive probe for the short-range interaction between the PTM radical and the SWCNT. Our results point toward an increased triplet exciton population due to radical-enhanced intersystem crossing, which could provide access to the elusive triplet manifold in SWCNTs. Furthermore, this simple synthetic route to spin-labeled defects could enable magnetic resonance studies complementary to in vivo fluorescence imaging with functionalized SWCNTs and facilitate the scalable fabrication of spintronic devices with magnetically switchable charge transport.

cond-mat.mtrl-sci↗

Stability of radical-functionalized gold surfaces by self-assembly and on-surface chemistry

We have investigated the radical functionalization of gold surfaces with a derivative of the perchlorotriphenylmethyl (PTM) radical, using two methods: by chemisorption from the radical solution and by on surface chemical derivatization from a precursor. We have investigated the obtained self-assembled monolayers by photon-energy dependent X-ray photoelectron spectroscopy. Our results show that the molecules were successfully anchored on the surfaces. The monolayers are characterized by air and beam stability unprecedented for films of organic radicals. Over very long beam exposure we observed a dynamic nature of the radical-Au complex. The results clearly indicate that (mono)layers of PTM; radical derivatives have the necessary stability to stand device applications.

cond-mat.mtrl-sci↗

Robust organic radical molecular junctions using acetylene terminated groups for C-Au bond formation

Organic paramagnetic and electroactive molecules are attracting interest as core components of molecular electronic and spintronic devices. Currently, further progress is hindered by the modest stability and reproducibility of the molecule/electrode contact. We report the synthesis of a persistent organic radical bearing one and two terminal alkyne groups to form Au-C σ bonds. The formation and stability of self-assembled monolayers and the electron transport through single-molecule junctions at room temperature have been studied. The combined analysis of both systems demonstrates that this linker forms a robust covalent bond with gold and a better-defined contact when compared to traditional sulfur-based linkers. Density functional theory and quantum transport calculations support the experimental observation highlighting a reduced variability of conductance values for the C-Au based junction. Our findings advance the quest for robustness and reproducibility of devices based on electroactive molecules.

cond-mat.mes-hall↗