arXiv subjects

Luca Moretti

Publications and source records attributed to Luca Moretti.

5 recordsLinked to original sources

arXiv2023

Optical microcavities as platforms for entangled photon spectroscopy

Optical microcavities are often proposed as platforms for spectroscopy in the single- and few-photon regime due to strong light-matter coupling. For classical-light spectroscopies, an empty microcavity simply acts as an optical filter. However, we find that in the single- or few-photon regime treating the empty microcavity as an optical filter does not capture the full effect on the quantum state of the transmitted photons. Focusing on the case of entangled photon-pair spectroscopy, we consider how the propagation of one photon through an optical microcavity changes the joint spectrum of a frequency-entangled photon pair. Using the input-output treatment of a Dicke model, we find that propagation through a strongly coupled microcavity above a certain coupling threshold enhances the entanglement entropy between the signal and idler photons. These results show that optical microcavities are not neutral platforms for quantum-light spectroscopies and their effects must be carefully considered when using change in entanglement entropy as an observable.

quant-ph↗

arXiv2023

Measurement principles for quantum spectroscopy of molecular materials with entangled photons

Nonlinear spectroscopy with quantum entangled photons is an emerging field of research that holds the promise to achieve a superior signal-to-noise ratio and effectively isolate many-body interactions. Photon sources used for this purpose however lack the frequency tunability and spectral bandwidth demanded by contemporary molecular materials. Here, we present design strategies for efficient spontaneous parametric downconversion to generate biphoton states with adequate spectral bandwidth and at visible wavelengths. Importantly, we demonstrate, by suitable design of the nonlinear optical interaction, the scope to engineer the degree of spectral correlations between the photons of the pair. We also present an experimental methodology to effectively characterize such spectral correlations. Importantly, we believe that such a characterization tool can be effectively adapted as a spectroscopy platform to optically probe system-bath interactions in materials.

physics.optics↗

arXiv2018

Pump-Push-Probe for Ultrafast All-Optical Switching: The Case of a Nanographene Molecule

In the last two decades, the three-beams pump-push-probe (PPP) technique has become a well-established tool for investigating the multidimensional configurational space of a molecule, as it permits to disclose precious information about the multiple and often complex deactivation pathways of the excited molecule. From the spectroscopic point of view, such a tool has revealed details about the efficiency of charge pairs generation and conformational relaxation in p-conjugated molecules and macromolecules. In addition, PPP has been effectively utilised for modulating the gain signal in conjugated materials by taking advantage of the spectral overlap between stimulated emission and charge absorption in those systems. However, the relatively low stability of conjugated polymers under intense photoexcitation has been a crucial limitation for their real employment in plastic optical fibres (POFs) and for signal control applications. Here, we highlight the role of PPP for achieving ultrafast all-optical switching in p-conjugated systems. Furthermore, we report new experimental data on optical switching of a newly synthesised graphene molecule, namely dibenzo[hi,st]ovalene (DBOV). The superior environmental and photostability of DBOV and, in general, of graphene nanostructures can represent a great advantage for their effective applications in POFs and information and communications technology.

physics.chem-ph↗

arXiv2017

Near-Infrared Emitting Single Squaraine Dye Aggregate with large Stokes shift

The study of supramolecular interactions and aggregation behaviour of functional materials is of great importance to tune and extend their spectral sensitivity and, hence, improve the optoelectronic response of related devices. In this study, we resolve spatially and spectrally the absorption and emission features of a squaraine aggregate by means of confocal microscopy and absorption/photoluminescence spectroscopy. We observe that the aggregate affords both a broad absorption spectrum (centred at 670 nm), likely originated by a dyes configuration with allowed J- and H- arrangements, and a strong and relatively narrow emission in the near-infrared (NIR) part of the spectrum (centred at 780 nm), with a remarkable Stokes shift of 110 nm that is among the largest exhibited by squaraine dyes. These peculiarities would be beneficial for extending the spectral sensitivity of bot photovoltaic and light-emitting diodes, and extremely appealing for possible applications of these aggregates as NIR fluorescent probes in biomedical applications.

physics.chem-ph↗

arXiv2013

Molecular-Level Switching of Polymer/Nanocrystal Non-Covalent Interactions and Application in Hybrid Solar Cells

Hy brid composites obtained upon blending conjugated polymers and colloidal inorganic semiconductor nanocrystals are regarded as attractive photo-active materials for optoelectronic applications. Here we demonstrate that tailoring nanocrystal surface chemistry permits to exert control on non-covalent bonding and electronic interactions between organic and inorganic components. The pendant moieties of organic ligands at the nanocrystal surface do not merely confer colloidal stability while hindering charge separation and transport, but drastically impact morphology of hybrid composites during formation from blend solutions. The relevance of our approach to photovoltaic applications is demonstrated for composites based on poly(3-hexylthiophene) and Pbs nanocrystals, considered as inadequate before the submission of this manuscript, which enable the fabrication of hybrid solar cells displaying a power conversion efficiency that reaches 3 %. Upon (quasi)steady-state and time-resolved analisys of the photo-induced processes in the nanocomposites and their organic and inorganic components, we ascertained that electron transfer occurs at the hybrid interface yielding long-lived separated charge carriers, whereas interfacial hole transfer appears slow. Here we provide a reliable alternative aiming at gaining control over macroscopic optoelectronic properties of polymer/nanocrystal composites by acting at the molecular-level via ligands' pendant moieties, thus opening new possibilities towards efficient solution-processed hybrid solar cells.

cond-mat.mtrl-sci↗