arXiv subjects

Pablo Merino

Publications and source records attributed to Pablo Merino.

At least 19 recordsLinked to original sources

arXiv2026

Almost sure pointwise convergence for the 2D periodic quintic NLS

We prove probabilistic pointwise convergence to the initial datum for the 2D periodic quintic NLS for data in $H^s(\mathbb T^2)$ with $s > 0$. This is an improvement with respect to the deterministic setting, in which convergence is known to fail if $s < 1/3$. The proof is based on a nonlinear maximal characterization for convergence, Bourgain's linear-nonlinear decomposition and the corresponding nonlinear smoothing for which we employ random tensor estimates.

math.AP↗

arXiv2026

On the almost sure growth of H\"older norms for the 1d periodic fractional BBM equation

We present almost sure polynomial bounds for H\"older norms of solutions of the 1d periodic fractional Benjamin-Bona-Mahony (BBM) equation. Namely, we apply quantitative quasi-invariance of certain Gaussian measures with energy cutoff using the strategy from Tzvetkov (2015) and the globalization argument from Bourgain (1994) in order to extend, almost surely, the $L^2$-based deterministic control to the $L^{\infty}$-based setting.

math.AP↗

arXiv2026

A pathological set regarding the propagation of almost sure properties of Gaussian measures

We provide a complementary result to the quasi-invariance of Gaussian measures supported on Sobolev spaces with high regularity under the dynamics of the three-dimensional periodic defocusing nonlinear wave equation from Gunaratnam-Oh-Tzvetkov-Weber (2022). Namely, given $p$ and $\sigma$ large enough, we prove the existence of dense sets of Sobolev spaces $W^{\sigma,p}(\mathbb{T}^3)$ which do not preserve the regularity $\sigma$ throughout the aforementioned dynamics. This is in sharp contrast with the propagation under the flow of almost sure properties.

math.AP↗

arXiv2026

The Significant Role of Hydrogen in the Formation of Silicon Carbide in Evolved Stars

Cosmic dust is mainly formed in the atmospheres of evolved stars. In carbon rich stars, amorphous carbon along with silicon carbide are the main constituents of dust grains yet the mechanisms involved in the formation of these grains are still poorly understood. Several molecular precursors have been proposed to form silicon carbide grains. Here, we have simulated in the laboratory the formation of silicon carbide dust starting from atomic C, atomic Si and H$_2$ and we have clearly identified SiC$_2$ as a key molecular precursor of nanodust analogues. We show that the interaction of molecular hydrogen with atomic carbon initiates the formation of hydrocarbons, which then react with atomic silicon to produce gas-phase SiC$_2$. In our experiments, the silicon carbide nanodust analogues are partially hydrogenated. Chemical routes for the formation of SiC$_2$ and organosilicon species are discussed on the basis of thermochemical calculations and chemical kinetics modelling. Our findings reveal the central role of molecular hydrogen in the formation of SiC$_2$ and contribute to a deeper understanding of silicon carbide dust formation processes in evolved stars, from atoms to molecules, clusters, and ultimately dust grains.

astro-ph.GA↗

arXiv2026

Adsorption-Driven Symmetry Lowering in Single Molecules Revealed by {\AA}ngstrom-scale Tip-Enhanced Raman Imaging

The vibrational landscape of adsorbed molecules is central to understanding surface interactions at the atomic scale, influencing phenomena from catalysis to molecular electronics. Recent advances in atomic-scale tip-enhanced Raman spectroscopy (TERS) have enabled vibrational mapping of single molecules with sub-nanometer spatial resolution, providing unprecedented insights into molecule-surface interactions by confining light in plasmonic picocavities. Here, we exploit TERS in a cryogenic scanning tunneling microscope junction to perform Raman hyperspectral mapping of single iron phthalocyanine (FePc) molecules in three non-equivalent adsorption configurations on Ag surfaces. We explore the changes in the vibrational modes of FePc molecules adsorbed on two distinct silver crystal terminations with differing symmetry, Ag(111) and Ag(110), revealing how subtle variations in the adsorption geometry due to substrate anisotropy can strongly influence molecular vibrations, lifting the degeneracy of individual normal modes. Our findings not only demonstrate the first use of sub-nanometer TERS mapping across different symmetry configurations but also provide a deeper understanding of how site-specific vibrational properties are intimately linked to local atomic environments. This capability paves the way for precisely tailoring surface interactions and controlling chemical reactions at the atomic scale.

cond-mat.mes-hall↗

arXiv2025

Roadmap for Photonics with 2D Materials

Triggered by the development of exfoliation and the identification of a wide range of extraordinary physical properties in self-standing films consisting of one or few atomic layers, two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and other van der Waals (vdW) crystals currently constitute a wide research field protruding in multiple directions in combination with layer stacking and twisting, nanofabrication, surface-science methods, and integration into nanostructured environments. Photonics encompasses a multidisciplinary collection of those directions, where 2D materials contribute with polaritons of unique characteristics such as strong spatial confinement, large optical-field enhancement, long lifetimes, high sensitivity to external stimuli (e.g., electric and magnetic fields, heating, and strain), a broad spectral range from the far infrared to the ultraviolet, and hybridization with spin and momentum textures of electronic band structures. The explosion of photonics with 2D materials as a vibrant research area is producing breakthroughs, including the discovery and design of new materials and metasurfaces with unprecedented properties as well as applications in integrated photonics, light emission, optical sensing, and exciting prospects for applications in quantum information, and nanoscale thermal transport. This Roadmap summarizes the state of the art in the field, identifies challenges and opportunities, and discusses future goals and how to meet them through a wide collection of topical sections prepared by leading practitioners.

cond-mat.mtrl-sci↗

arXiv2024

Pointwise convergence of the Klein-Gordon flow

We consider the PDEs version of the Carleson problem in the context of the cubic nonlinear Klein-Gordon equation. This means that we aim to establish the lowest regularity class for which one has almost everywhere pointwise convergence of the solutions to the initial data, as $t \to 0$. We prove sharp results for initial data in Sobolev spaces and for their randomized counterparts.

math.AP↗

arXiv2023

Resonant TERS of a Single-Molecule Kondo System

Single-molecule tip-enhanced Raman spectroscopy (TERS) under ultra-high vacuum (UHV) and cryogenic conditions enables exploration of the relations between the adsorption geometry, electronic state, and vibrational fingerprints of individual molecules. TERS capability of reflecting spin states in open-shell molecular configurations is yet unexplored. Here we use the tip of a scanning probe microscope to lift a perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) molecule from a metal surface to bring it into an open-shell spin one-half anionic state. We reveal a correlation between the appearance of a Kondo resonance in the differential conductance spectroscopy and concurrent characteristic changes captured by the TERS measurements. Through a detailed investigation of various adsorbed and tip-contacted PTCDA scenarios, we infer that the Raman scattering on the suspended PTCDA is resonant with a higher excited state. Theoretical simulation of the vibrational spectra enables a precise assignment of the individual TERS peaks to high-symmetry Ag modes, including the fingerprints of the observed spin state. These findings highlight the potential of TERS in capturing complex interactions between charge, spin, and photophysical properties in nanoscale molecular systems, and suggest a pathway for designing spin-optical devices using organic molecules.

cond-mat.mes-hall↗

arXiv2023

PDRs4All III: JWST's NIR spectroscopic view of the Orion Bar

(Abridged) We investigate the impact of radiative feedback from massive stars on their natal cloud and focus on the transition from the HII region to the atomic PDR (crossing the ionisation front (IF)), and the subsequent transition to the molecular PDR (crossing the dissociation front (DF)). We use high-resolution near-IR integral field spectroscopic data from NIRSpec on JWST to observe the Orion Bar PDR as part of the PDRs4All JWST Early Release Science Program. The NIRSpec data reveal a forest of lines including, but not limited to, HeI, HI, and CI recombination lines, ionic lines, OI and NI fluorescence lines, Aromatic Infrared Bands (AIBs including aromatic CH, aliphatic CH, and their CD counterparts), CO2 ice, pure rotational and ro-vibrational lines from H2, and ro-vibrational lines HD, CO, and CH+, most of them detected for the first time towards a PDR. Their spatial distribution resolves the H and He ionisation structure in the Huygens region, gives insight into the geometry of the Bar, and confirms the large-scale stratification of PDRs. We observe numerous smaller scale structures whose typical size decreases with distance from Ori C and IR lines from CI, if solely arising from radiative recombination and cascade, reveal very high gas temperatures consistent with the hot irradiated surface of small-scale dense clumps deep inside the PDR. The H2 lines reveal multiple, prominent filaments which exhibit different characteristics. This leaves the impression of a "terraced" transition from the predominantly atomic surface region to the CO-rich molecular zone deeper in. This study showcases the discovery space created by JWST to further our understanding of the impact radiation from young stars has on their natal molecular cloud and proto-planetary disk, which touches on star- and planet formation as well as galaxy evolution.

astro-ph.GA↗

arXiv2022

Evidence of trion-libron coupling in chirally adsorbed single molecules

Interplay between motion of nuclei and excited electrons in molecules plays a key role both in biological and artificial nanomachines. Here we provide a detailed analysis of coupling between quantized librational modes (librons) and charged excited states (trions) on single phthalocyanine dyes adsorbed on a surface. By means of tunnelling electron-induced electroluminescence, we identify libronic progressions on a {\mu}eV energy range in spectra of chirally adsorbed phthalocyanines, which are otherwise absent from spectra of symmetrically adsorbed species. Experimentally measured libronic spectra match very well the theoretically calculated libron eigenenergies and peak intensities (Franck-Condon factors) and reveal an unexpected depopulation channel for the zero libron of the excited state that can be effectively controlled by tuning the size of the nanocavity. Our results showcase the possibility of characterizing the dynamics of molecules by their low-energy molecular modes using {\mu}eV-resolved tip-enhanced spectroscopy.

cond-mat.mes-hall↗

arXiv2022

PDRs4All: A JWST Early Release Science Program on radiative feedback from massive stars

Massive stars disrupt their natal molecular cloud material through radiative and mechanical feedback processes. These processes have profound effects on the evolution of interstellar matter in our Galaxy and throughout the Universe, from the era of vigorous star formation at redshifts of 1-3 to the present day. The dominant feedback processes can be probed by observations of the Photo-Dissociation Regions (PDRs) where the far-ultraviolet photons of massive stars create warm regions of gas and dust in the neutral atomic and molecular gas. PDR emission provides a unique tool to study in detail the physical and chemical processes that are relevant for most of the mass in inter- and circumstellar media including diffuse clouds, proto-planetary disks and molecular cloud surfaces, globules, planetary nebulae, and star-forming regions. PDR emission dominates the infrared (IR) spectra of star-forming galaxies. Most of the Galactic and extragalactic observations obtained with the James Webb Space Telescope (JWST) will therefore arise in PDR emission. In this paper we present an Early Release Science program using the MIRI, NIRSpec, and NIRCam instruments dedicated to the observations of an emblematic and nearby PDR: the Orion Bar. These early JWST observations will provide template datasets designed to identify key PDR characteristics in JWST observations. These data will serve to benchmark PDR models and extend them into the JWST era. We also present the Science-Enabling products that we will provide to the community. These template datasets and Science-Enabling products will guide the preparation of future proposals on star-forming regions in our Galaxy and beyond and will facilitate data analysis and interpretation of forthcoming JWST observations.

astro-ph.GA↗

arXiv2021

Real space visualization of entangled excitonic states in charged molecular assemblies

Entanglement of excitons holds great promise for the future of quantum computing, which would use individual molecular dyes as building blocks of their circuitry. Even though entangled excitonic eigenstates emerging in coupled molecular assemblies can be detected by far-field spectroscopies, access to the individual modes in real space will bring the much needed insight into the photophysics of these fascinating quantum phenomena. Here we combine tip-enhanced spectromicroscopy with atomic force microscopy to inspect delocalized single-exciton states of charged molecular assemblies engineered from individual perylenetetracarboxylic dianhydride molecules. Hyperspectral mapping of the eigenstates and comparison with calculated many-body optical transitions reveals a second low-lying excited state of the anion monomers and its role in the exciton entanglement within the assemblies. We also demonstrate control over the coupling by switching the assembly charge states. Our results reveal the possibility of tailoring excitonic properties of organic dye aggregates for advanced functionalities and establish the methodology to address them individually at the nanoscale.

physics.atm-clus↗

arXiv2021

Atomic-scale structural fluctuations of a plasmonic cavity

We study fluctuations in plasmonic electroluminescence at the single-atom limit profiting from the precision of a low-temperature scanning tunneling microscope. First, we investigate the influence of a controlled single-atom transfer on the plasmonic properties of the junction. Next, we form a well-defined atomic contact of several quanta of conductance. In contact, we observe changes of the electroluminescence intensity that can be assigned to spontaneous modifications of electronic conductance, plasmonic excitation and optical antenna properties all originating from minute atomic rearrangements at or near the contact. The observations are relevant for the understanding of processes leading to spontaneous intensity variations in plasmon-enhanced atomic-scale spectroscopies.

cond-mat.mes-hall↗

arXiv2020

Gigahertz frame rate imaging of charge-injection dynamics in a molecular light source

Light sources on the scale of single molecules can be addressed and characterized on their proper sub-nanometer scale by scanning tunneling microscopy induced luminescence (STML). Such a source can be driven by defined short charge pulses while the luminescence is detected with sub-nanosecond resolution. We introduce an approach to concurrently image the molecular emitter, which is based on an individual defect, with its local environment along with its luminescence dynamics at a resolution of a billion frames per second. The observed dynamics can be assigned to the single electron capture occurring in the low-nanosecond regime. While the emitter's location on the surface remains fixed, the scanning of the tip modifies the energy landscape for charge injection to the defect. The principle of measurement is extendable to fundamental processes beyond charge transfer like exciton diffusion.

cond-mat.mes-hall↗

arXiv2020

Exciton-trion dynamics of a single molecule in a radio-frequency cavity

Charged optical excitations (trions) generated by charge carrier injection are crucial for emerging optoelectronic technologies as they can be produced and manipulated by electric fields. Trions and neutral excitons can be efficiently induced in single molecules by means of tip-enhanced spectromicroscopic techniques. However, little is known of the exciton-trion dynamics at single molecule level as this requires methods permitting simultaneous sub-nanometer and sub-nanosecond characterization. Here, we investigate exciton-trion dynamics by phase fluorometry, combining radio-frequency modulated scanning tunnelling luminescence with time-resolved single photon detection. We generate excitons and trions in single Zinc Phthalocyanine (ZnPc) molecules on NaCl/Ag(111), determine their dynamics and trace the evolution of the system in the picosecond range with atomic resolution. In addition, we explore dependence of effective lifetimes on bias voltage and propose a conversion of neutral excitons into trions via charge capture as the primary mechanism of trion formation.

physics.atm-clus↗

arXiv2020

Silicon and hydrogen chemistry under laboratory conditions mimicking the atmosphere of evolved stars

Silicon is present in interstellar dust grains, meteorites and asteroids, and to date thirteen silicon-bearing molecules have been detected in the gas-phase towards late-type stars or molecular clouds, including silane and silane derivatives. In this work, we have experimentally studied the interaction between atomic silicon and hydrogen under physical conditions mimicking those at the atmosphere of evolved stars. We have found that the chemistry of Si, H and H$_2$ efficiently produces silane (SiH$_4$), disilane (Si$_2$H$_6$) and amorphous hydrogenated silicon (a-Si:H) grains. Silane has been definitely detected towards the carbon-rich star IRC\,+10216, while disilane has not been detected in space yet. Thus, based on our results, we propose that gas-phase reactions of atomic Si with H and H$_2$ are a plausible source of silane in C-rich AGBs, although its contribution to the total SiH$_4$ abundance may be low in comparison with the suggested formation route by catalytic reactions on the surface of dust grains. In addition, the produced a-Si:H dust analogs decompose into SiH$_4$ and Si$_2$H$_6$ at temperatures above 500 K, suggesting an additional mechanism of formation of these species in envelopes around evolved stars. We have also found that the exposure of these dust analogs to water vapor leads to the incorporation of oxygen into Si-O-Si and Si-OH groups at the expense of SiH moieties, which implies that, if this type of grains are present in the interstellar medium, they will be probably processed into silicates through the interaction with water ices covering the surface of dust grains.

astro-ph.GA↗

arXiv2020

The chemistry of cosmic dust analogues from C, C$_2$, and C$_2$H$_2$ in C-rich circumstellar envelopes

Interstellar carbonaceous dust is mainly formed in the innermost regions of circumstellar envelopes around carbon-rich asymptotic giant branch (AGB) stars. In these highly chemically stratified regions, atomic and diatomic carbon, along with acetylene are the most abundant species after H$_2$ and CO. In a previous study, we addressed the chemistry of carbon (C and C$_2$) with H$_2$ showing that acetylene and aliphatic species form efficiently in the dust formation region of carbon-rich AGBs whereas aromatics do not. Still, acetylene is known to be a key ingredient in the formation of linear polyacetylenic chains, benzene and polycyclic aromatic hydrocarbons (PAHs), as shown by previous experiments. However, these experiments have not considered the chemistry of carbon (C and C$_2$) with C$_2$H$_2$. In this work, by employing a sufficient amount of acetylene, we investigate its gas-phase interaction with atomic and diatomic carbon. We show that the chemistry involved produces linear polyacetylenic chains, benzene and other PAHs, which are observed with high abundances in the early evolutionary phase of planetary nebulae. More importantly, we have found a non-negligible amount of pure and hydrogenated carbon clusters as well as aromatics with aliphatic substitutions, both being a direct consequence of the addition of atomic carbon. The incorporation of alkyl substituents into aromatics can be rationalized by a mechanism involving hydrogen abstraction followed by methyl addition. All the species detected in gas phase are incorporated into the nanometric sized dust analogues, which consist of a complex mixture of sp, sp$^2$ and sp$^3$ hydrocarbons with amorphous morphology.

astro-ph.GA↗

arXiv2019

Tailored Graphenic Structures Directly Grown on Titanium Oxide Boost the Interfacial Charge Transfer

The successful application of titanium oxide-graphene hybrids in the fields of photocatalysis, photovoltaics and photodetection strongly depends on the interfacial contact between both materials. The need to provide a good coupling between the enabling conductor and the photoactive phase prompted us to directly grow conducting graphenic structures on TiO2 crystals. We here report on the direct synthesis of tailored graphenic structures by using Plasma Assisted Chemical Vapour Deposition that present a clean junction with the prototypical titanium oxide (110) surface. Chemical analysis of the interface indicates chemical bonding between both materials. Photocurrent measurements under UV light illumination manifest that the charge transfer across the interface is efficient. Moreover, the influence of the synthesis atmosphere, gas precursor (C2H2) and diluents (Ar, O2), on the interface and on the structure of the as-grown graphenic material is assessed. The inclusion of O2 promotes vertical growth of partially oxidized carbon nanodots/rods with controllable height and density. The deposition with Ar results in continuous graphenic films with low resistivity (6.8x10-6 ohm x m). The synthesis protocols developed here are suitable to produce tailored carbon-semiconductor structures on a variety of practical substrates as thin films, pillars or nanoparticles.

physics.app-ph↗