arXiv subjects

Michele Sclafani

Publications and source records attributed to Michele Sclafani.

5 recordsLinked to original sources

arXiv2019

Imaging the Renner-Teller effect using laser-induced electron diffraction

Structural information on electronically excited neutral molecules can be indirectly retrieved, largely through pump-probe and rotational spectroscopy measurements with the aid of calculations. Here, we demonstrate the direct structural retrieval of neutral carbonyl disulfide (CS$_2$) in the B$^1$B$_2$ excited electronic state using laser-induced electron diffraction (LIED). We unambiguously identify the ultrafast symmetric stretching and bending of the field-dressed neutral CS$_2$ molecule with combined picometer and attosecond resolution using intrapulse pump-probe excitation and measurement. We invoke the Renner-Teller effect to populate the B$^1$B$_2$ excited state in neutral CS$_2$, leading to bending and stretching of the molecule. Our results demonstrate the sensitivity of LIED in retrieving the geometric structure of CS$_2$, which is known to appear as a two-center scatterer.

physics.chem-ph↗

arXiv2016

Transition from non-sequential to sequential double ionisation in many-electron systems

Obtaining a detailed understanding of strong-field double ionisation of many-electron systems (heavy atoms and molecules) remains a challenging task. By comparing experimental and theoretical results in the mid-IR regime, we have unambiguously identified the transition from non-sequential (e,2e) to sequential double ionisation in Xe and shown that it occurs at an intensity below $10^{14}$ Wcm$^{-2}$. In addition, our data demonstrate that ionisation from the Xe 5s orbital is decisive at low intensities. Moreover, using the acetylene molecule, we propose how sequential double ionisation in the mid-IR can be used to study molecular dynamics and fragmentation on unprecedented few-femtosecond timescales.

physics.atom-ph↗

arXiv2016

An atomically thin matter-wave beamsplitter

Matter-wave interferometry has become an essential tool in studies on the foundations of quantum physics and for precision measurements. Mechanical gratings have played an important role as coherent beamsplitters for atoms, molecules and clusters since the basic diffraction mechanism is the same for all particles. However, polarizable objects may experience van der Waals shifts when they pass the grating walls and the undesired dephasing may prevent interferometry with massive objects. Here we explore how to minimize this perturbation by reducing the thickness of the diffraction mask to its ultimate physical limit, i.e. the thickness of a single atom. We have fabricated diffraction masks in single-layer and bilayer graphene as well as in 1 nm thin carbonaceous biphenyl membrane. We identify conditions to transform an array of single layer graphene nanoribbons into a grating of carbon nanoscrolls. We show that all these ultra-thin nanomasks can be used for high-contrast quantum diffraction of massive molecules. They can be seen as a nanomechanical answer to the question debated by Bohr and Einstein whether a softly suspended double slit would destroy quantum interference. In agreement with Bohr's reasoning we show that quantum coherence prevails even in the limit of atomically thin gratings.

quant-ph↗

arXiv2015

Cavity-assisted manipulation of freely rotating silicon nanorods in high vacuum

Optical control of nanoscale objects has recently developed into a thriving field of research with far-reaching promises for precision measurements, fundamental quantum physics and studies on single-particle thermodynamics. Here, we demonstrate the optical manipulation of silicon nanorods in high vacuum. Initially, we sculpture these particles into a silicon substrate with a tailored geometry to facilitate their launch into high vacuum by laser-induced mechanical cleavage. We manipulate and trace their center-of-mass and rotational motion through the interaction with an intense intra-cavity field. Our experiments show optical forces on nanorotors three times stronger than on silicon nanospheres of the same mass. The optical torque experienced by the spinning rods will enable cooling of the rotational motion and torsional opto-mechanics in a dissipation-free environment.

quant-ph↗

arXiv2015

Strong-field physics with mid-IR fields

Strong-field physics is currently experiencing a shift towards the use of mid-IR driving wavelengths. This is because they permit conducting experiments unambiguously in the quasi-static regime and enable exploiting the effects related to ponderomotive scaling of electron recollisions. Initial measurements taken in the mid-IR immediately led to a deeper understanding of photo-ionization and allowed a discrimination amongst different theoretical models. Ponderomotive scaling of rescattering has enabled new avenues towards time resolved probing of molecular structure. Essential for this paradigm shift was the convergence of two experimental tools: 1) intense mid-IR sources that can create high energy photons and electrons while operating within the quasi-static regime, and 2) detection systems that can detect the generated high energy particles and image the entire momentum space of the interaction in full coincidence. Here we present a unique combination of these two essential ingredients, namely a 160kHz mid-IR source and a reaction microscope detection system, to present an experimental methodology that provides an unprecedented three-dimensional view of strong-field interactions. The system is capable of generating and detecting electron energies that span a six order of magnitude dynamic range. We demonstrate the versatility of the system by investigating electron recollisions, the core process that drives strong-field phenomena, at both low (meV) and high (hundreds of eV) energies. The low energy region is used to investigate recently discovered low-energy structures, while the high energy electrons are used to probe atomic structure via laser-induced electron diffraction. Moreover we present, for the first time, the correlated momentum distribution of electrons from non-sequential double-ionization driven by mid-IR pulses.

physics.atom-ph↗