arXiv subjects

Riccardo Montis

Publications and source records attributed to Riccardo Montis.

3 recordsLinked to original sources

arXiv2026

Dense pentacene cocrystal demonstrates room-temperature coherent control

Maximizing the number of addressable spins within a fixed volume can improve ensemble quantum sensor sensitivity, but dense packing usually increases dipolar interactions and excited-state transport, shortening coherence and suppressing optical readout. Here we report a 2:1 cocrystal of 6,13-dihydropentacene and pentacene (DHP/Pc) containing 33.3 mol% pentacene ($3.3\times10^{5}$ ppm; $9.51\times10^{20}$ cm$^{-3}$), a volumetric spin-site density more than two orders of magnitude above previous benchmarks, NV-diamond and pentacene-doped p-terphenyl (PDP). Despite this density, DHP/Pc exhibits microsecond spin coherence, room-temperature optically detected magnetic resonance and coherent control. Time-resolved measurements indicate that the long-lived triplet population is generated predominantly by intersystem crossing and exhibits strong, non-thermal sublevel polarization. Density-functional theory calculations further suggest that the native cocrystal geometry weakens electronic coupling between neighboring pentacenes, while the higher DHP triplet energy creates a barrier to triplet migration. These results identify molecular packing and coformer triplet energetics as complementary design parameters for preserving coherence in high spin-site density systems, demonstrating cocrystallization as a promising route to dense, optically addressable spin materials for room-temperature ensemble quantum sensing.

quant-ph↗

arXiv2024

High sensitivity pressure and temperature quantum sensing in organic crystals

The inherent sensitivity of quantum sensors to their physical environment can make them good reporters of parameters such as temperature, pressure, strain, and electric fields. Here, we present a molecular platform for pressure (P) and temperature (T) sensing using para-terphenyl crystals doped with pentacene. We leverage the optically detected magnetic resonance (ODMR) of the photoexcited triplet electron in the pentacene molecule, that serves as a sensitive probe for lattice changes in the host para-terphenyl due to pressure or temperature variations. We observe maximal ODMR frequency variations of df/dP=1.8 MHz/bar and df/dT=247 kHz/K, which are over 1,200 times and three times greater, respectively, than those seen in nitrogen-vacancy centers in diamond. This results in a >85-fold improvement in pressure sensitivity over best previously reported. The larger variation reflects the weaker nature of the para-terphenyl lattice, with first-principles DFT calculations indicating that even picometer-level shifts in the molecular orbitals due to P, T changes are measurable. The platform offers additional advantages including high levels of sensor doping, narrow ODMR linewidths and high contrasts, and ease of deployment, leveraging the ability for large single crystals at low cost. Overall, this work paves the way for low-cost, optically-interrogated pressure and temperature sensors and lays the foundation for even more versatile sensors enabled by synthetic tunability in designer molecular systems.

quant-ph↗

arXiv2018

Multiple Quintets via Singlet Fission in Ordered Films at Room Temperature

The growing interest in harnessing singlet fission for photovoltaic applications stems from the possibility of generating two excitons from a single photon. Quantum efficiencies above unity have been reported, yet the correlation between singlet fission and intermolecular geometry is poorly understood. To address this, we investigated ordered solid solutions of pentacene in p-terphenyl grown by organic molecular beam deposition. Two classes of dimers are expected from the crystal structure - parallel and herringbone - with intrinsically distinctive electronic coupling. Using electron paramagnetic resonance spectroscopy, we provide compelling evidence for the formation of distinct quintet excitons at room temperature. These are assigned to specific pentacene pairs according to their angular dependence. This work highlights the importance of controlling the intermolecular geometry and the need to develop adequate theoretical models to account for the relationship between structure and electronic interactions in strongly-coupled, high-spin molecular systems.

cond-mat.mtrl-sci↗