Lora Ramunno

Polarization-dependent femtosecond laser ablation of poly-methyl methacrylate

We show that ablation features in poly-methyl methacrylate (PMMA) induced by a single femtosecond laser pulse are imposed by light polarization. The ablation craters are elongated along the major axis of the polarization vector and become increasingly prominent as the pulse energy is increased above the threshold energy. We demonstrate 40% elongation for linearly and elliptically polarized light in the fluence range of 4-20Jcm 2 , while circularly polarized light produced near circular ablation craters irrespective of pulse energies. We also show that irradiation with multiple pulses erases the polarization-dependent elongation of the ablation craters. However, for line ablation the orientation of the electric field vector is imprinted in the form of quasi-periodic structures inside the ablated region. Theoretically, we show that the polarization dependence of the ablation features arises from a local field enhancement during light-plasma interaction. Simulations also show that in materials with high nonlinearities such as doped PMMA, in addition to conventional explosive boiling, sub-surface multiple filamentation can also give rise to porosity.

Intense VUV laser cluster interaction in the strong coupling regime

The interaction of noble gas clusters with intense, VUV radiation is investigated by molecular dynamics simulations. It is shown that the free-electron laser cluster interaction creates a strongly coupled plasma. A new heating mechanism is identified that is more efficient than inverse Bremsstrahlung heating and explains the observation of unusually high charge states in recent experiments at DESY. The heating mechanism is a consequence of the strongly coupled plasma dynamics, in which collisional processes are strongly modified. Energy absorption takes place in the following cycle: many-body collisions, resulting in an enhanced recombination of free electrons to exited states, and subsequent reionization.

Imaging and modeling collagen architecture from the nano to micro scale

The collagen meshwork plays a central role in the functioning of a range of tissues including cartilage, tendon, arteries, skin, bone and ligament. Because of its importance in function, it is of considerable interest for studying development, disease and regeneration processes. Here, we have used second harmonic generation (SHG) to image human tissues on the hundreds of micron scale, and developed a numerical model to quantitatively interpret the images in terms of the underlying collagen structure on the tens to hundreds of nanometer scale. Focusing on osteoarthritic changes in cartilage, we have demonstrated that this combination of polarized SHG imaging and numerical modeling can estimate fibril diameter, filling fraction, orientation and bundling. This extends SHG microscopy from a qualitative to quantitative imaging technique, providing a label-free and non-destructive platform for characterizing the extracellular matrix that can expand our understanding of the structural mechanisms in disease.

Image formation in CARS and SRS: effect of an inhomogeneous nonresonant background medium

We investigate the role of a spatially inhomogenous nonresonant background medium on several Raman-based imaging modalities. In particular, we consider a small resonant bead submerged in a spatially heterogeneous nonresonant χ(3) background. Using detailed 3D electrodynamic simulations, we compare coherent anti-Stokes Raman scattering (CARS), frequency-modulated CARS, amplitude-modulated stimulated Raman scattering (SRS), and frequency-modulated SRS. We find that only FM-SRS is background-free.

Steplike intensity threshold behavior of extreme ionization in laser-driven xenon clusters.

The generation of highly charged Xe(q+) ions up to q=24 is observed in Xe clusters embedded in helium nanodroplets and exposed to intense femtosecond laser pulses (λ=800  nm). Laser intensity resolved measurements show that the high-q ion generation starts at an unexpectedly low threshold intensity of about 10(14)  W/cm2. Above threshold, the Xe ion charge spectrum saturates quickly and changes only weakly for higher laser intensities. Good agreement between these observations and a molecular dynamics analysis allows us to identify the mechanisms responsible for the highly charged ion production and the surprising intensity threshold behavior of the ionization process.

Self-controlled formation of microlenses by optical breakdown inside wide-band-gap materials

By repeatedly illuminating fused silica slabs with focused femtosecond pulses, we permanently decrease the local refractive index without increasing the linear absorption or scattering. This progressively forms a biconvex lens in the prefocal region. With linearly polarized light, the index change reaches several percent and is associated with the formation of an array of planar nanocracks. We analyze the polarization-dependent focusing power of the subwavelength periodic structure. While the detailed material modification changes, spontaneous defocusing lens formation is a common feature of every wide-band-gap transparent materials that we have studied (SiO2, BK7, LiF, sapphire, and mica).

Analysis of forward and backward Second Harmonic Generation images to probe the nanoscale structure of collagen within bone and cartilage

Collagen ultrastructure plays a central role in the function of a wide range of connective tissues. Studying collagen structure at the microscopic scale is therefore of considerable interest to understand the mechanisms of tissue pathologies. Here, we use second harmonic generation microscopy to characterize collagen structure within bone and articular cartilage in human knees. We analyze the intensity dependence on polarization and discuss the differences between Forward and Backward images in both tissues. Focusing on articular cartilage, we observe an increase in Forward/Backward ratio from the cartilage surface to the bone. Coupling these results to numerical simulations reveals the evolution of collagen fibril diameter and spatial organization as a function of depth within cartilage.

Image formation in CARS microscopy: effect of the Gouy phase shift

Image formation in Coherent Anti-Stokes Raman Scattering (CARS) microscopy of sub-wavelength objects is investigated via a combined experimental, numerical and theoretical study. We consider a resonant spherical object in the presence of a nonresonant background, using tightly focused laser pulses. When the object is translated along the laser propagation axis, we find the CARS signal to be asymmetric about the laser focal plane. When the object is located before the focus, there is a distinct shadow within the image, whereas the brightest signal is obtained when the object is behind the focus. This behaviour is caused by interference between resonant and nonresonant signals, and the Gouy phase shift is responsible for the observed asymmetry within the image.

Imaging the noncentrosymmetric structural organization of tendon with Interferometric Second Harmonic Generation microscopy.

We image the relative orientation of organized groups of noncentrosymmetric molecules (like collagen or myosin) at the micron scale in biological tissues by combining interferometry and Second Harmonic Generation (SHG) microscopy.

Laser-induced plasmonic colours on metals

The use of metal nanostructures for colourization has attracted a great deal of interest with the recent developments in plasmonics. However, the current top-down colourization methods based on plasmonic concepts are tedious and time consuming, and thus unviable for large-scale industrial applications. Here we show a bottom-up approach where, upon picosecond laser exposure, a full colour palette independent of viewing angle can be created on noble metals. We show that colours are related to a single laser processing parameter, the total accumulated fluence, which makes this process suitable for high throughput industrial applications. Statistical image analyses of the laser irradiated surfaces reveal various distributions of nanoparticle sizes which control colour. Quantitative comparisons between experiments and large-scale finite-difference time-domain computations, demonstrate that colours are produced by selective absorption phenomena in heterogeneous nanoclusters. Plasmonic cluster resonances are thus found to play the key role in colour formation.Plasmonic resonances in metallic nanoparticles have been used since antiquity to colour glasses. The use of metal nanostructures for surface colourization has attracted considerable interest following recent developments in plasmonics. However, current top-down colourization methods are not ideally suited to large-scale industrial applications. Here we use a bottom-up approach where picosecond laser pulses can produce a full palette of non-iridescent colours on silver, gold, copper and aluminium. We demonstrate the process on silver coins weighing up to 5 kg and bearing large topographic variations (∼1.5 cm). We find that colours are related to a single parameter, the total accumulated fluence, making the process suitable for high-throughput industrial applications. Statistical image analyses of laser-irradiated surfaces reveal various nanoparticle size distributions. Large-scale finite-difference time-domain computations based on these nanoparticle distributions reproduce trends seen in reflectance measurements, and demonstrate the key role of plasmonic resonances in colour formation.