SearcharxivSearch

arXiv subjects

Borja Cirera

Publications and source records attributed to Borja Cirera.

3 recordsLinked to original sources

Oscillator-driven broadband femtosecond transient microspectroscopy with supercontinuum probes generated in a photonic crystal fiber

We present an oscillator-driven femtosecond transient microspectroscopy system based on supercontinuum generation in a photonic crystal fiber (PCF). The system operates at 80 MHz without pulse amplification, enabling high-sensitivity measurements with a detection sensitivity better than $10^{-4}$ while using low pulse energies suitable for microspectroscopy. Optimization of the PCF length ($\leq 50$ mm) suppresses dispersion-induced chirp, achieving nearly uniform temporal resolution below 100 fs across 450-900 nm. The high-repetition-rate operation allows rapid spectral acquisition and efficient noise reduction. The developed system provides micrometer-scale spatial resolution and supports both reflection and transmission configurations. Ultrafast carrier dynamics in multilayer and monolayer MoS$_2$ are successfully resolved, including spatially dependent relaxation within a single monolayer flake. These results demonstrate a versatile platform for probing local ultrafast dynamics in low-dimensional materials.

physics.optics

Adsorption-Driven Symmetry Lowering in Single Molecules Revealed by Ångstrom-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

Tailoring π-conjugation and vibrational modes to steer on-surface synthesis of pentalene-bridged ladder polymers

The development of synthetic strategies to engineer π-conjugated polymers is of paramount importance in modern chemistry and materials science. Here we introduce a theoretical and experimental synthetic paradigm based on the search for specific vibrational modes through an appropriate tailoring of the π-conjugation of the precursors, in order to increase the attempt frequency of a chemical reaction. First, we on-surface design a 1D π-conjugated polymer with specific π-topology, which is based on bisanthene monomers linked by cumulene bridges that tune specific vibrational modes. In a second step, upon further annealing, such vibrational modes steer the two-fold cyclization reaction between adjacent bisanthene moieties, which gives rise to a long and free-defect pentalene-bridged conjugated ladder polymer featuring a low band gap. In addition, high resolution atomic force microscopy allows us to identify by atomistic insights the resonant form of the polymer, thus confirming the validity of the Glidewell and Lloyd's rules for aromaticity. This on-surface synthetic strategy may stimulate exploiting previously precluded reactions towards novel pi-conjugated polymers with specific structures and properties.

cond-mat.mes-hall