[Show abstract][Hide abstract] ABSTRACT: Steering the electrons during an ultrafast photo-induced process in a molecule influences the chemical behavior of the system, opening the door to the control of photochemical reactions and photobiological processes. Electrons can be efficiently localized using a strong laser field with a well-designed temporal shape of the electric component. Consequently, many experiments have been performed with laser sources in the near-infrared region (800 nm) in the interest of studying and enhancing the electron localization. However, due to its limited accessibility, the mid-infrared (MIR) range has barely been investigated, although it allows to efficiently control small molecules and even more complex systems. To push further the manipulation of basic chemical mechanisms, we used a MIR two-color (1800 and 900 nm) laser field to ionize H2 and D2 molecules and to steer the remaining electron during the photo-induced dissociation. The study of this prototype reaction led to the simultaneous control of four fragmentation channels. The results are well reproduced by a theoretical model solving the time-dependent Schrödinger equation for the molecular ion, identifying the involved dissociation mechanisms. By varying the relative phase between the two colors, asymmetries (i.e., electron localization selectivity) of up to 65% were obtained, corresponding to enhanced or equivalent levels of control compared to previous experiments. Experimentally easier to implement, the use of a two-color laser field leads to a better electron localization than carrier-envelope phase stabilized pulses and applying the technique in the MIR range reveals more dissociation channels than at 800 nm.
Full-text · Article · Jan 2016 · Journal of Physics B Atomic Molecular and Optical Physics
[Show abstract][Hide abstract] ABSTRACT: Osteochondrosis is an ischemic chondronecrosis of epiphyseal growth cartilage that results in focal failure of endochondral ossification and osteochondritis dissecans at specific sites in the epiphyses of humans and animals, including horses. The upstream events leading to the focal ischemia remain unknown. The epiphyseal growth cartilage matrix is composed of proteoglycan and collagen macromolecules and encases its vascular tree in canals. The matrix undergoes major dynamic changes in early life that could weaken it biomechanically and predispose it to focal trauma and vascular failure. Subregions in neonatal foal femoral epiphyses (n = 10 osteochondrosis predisposed; n = 6 control) were assessed for proteoglycan and collagen structure/content employing 3T quantitative MRI (3T qMRI: T1ρ & T2 maps). Site-matched validations were made with histology, immunohistochemistry and second-harmonic microscopy. Growth cartilage T1ρ and T2 relaxation times were significantly increased (p < 0.002) within the proximal third of the trochlea, a site predisposed to osteochondrosis, when compared with other regions. However this was observed in both control and osteochondrosis predisposed specimens. Microscopic evaluation of this region revealed an expansive area with low proteoglycan content and a hypertrophic-like appearance on second-harmonic microscopy. We speculate that this matrix structure and composition, though physiological, may weaken the epiphyseal growth cartilage biomechanically in focal regions and could enhance the risk of vascular failure with trauma leading to osteochondrosis. However additional investigations are now required to confirm this. 3T qMRI will be useful for future non-invasive longitudinal studies to track the osteochondrosis disease trajectory in animals and humans. This article is protected by copyright. All rights reserved
No preview · Article · Jan 2016 · Journal of Orthopaedic Research
[Show abstract][Hide abstract] ABSTRACT: In this work, we report the implementation of interferometric second harmonic generation (SHG) microscopy with femtosecond pulses. As a proof of concept, we imaged the phase distribution of SHG signal from the complex collagen architecture of juvenile equine growth cartilage. The results are analyzed in respect to numerical simulations to extract the relative orientation of collagen fibrils within the tissue. Our results reveal large domains of constant phase together with regions of quasi-random phase, which are correlated to respectively high- and low-intensity regions in the standard SHG images. A comparison with polarization-resolved SHG highlights the crucial role of relative fibril polarity in determining the SHG signal intensity. Indeed, it appears that even a well-organized noncentrosymmetric structure emits low SHG signal intensity if it has no predominant local polarity. This work illustrates how the complex architecture of noncentrosymmetric scatterers at the nanoscale governs the coherent building of SHG signal within the focal volume and is a key advance toward a complete understanding of the structural origin of SHG signals from tissues.
Full-text · Article · Dec 2015 · Biophysical Journal
[Show abstract][Hide abstract] ABSTRACT: The band structure of matter determines its properties. In solids, it is typically mapped with angle-resolved photoemission spectroscopy, in which the momentum and the energy of incoherent electrons are independently measured. Sometimes, however, photoelectrons are difficult or impossible to detect. Here we demonstrate an all-optical technique to reconstruct momentum-dependent band gaps by exploiting the coherent motion of electron-hole pairs driven by intense midinfrared femtosecond laser pulses. Applying the method to experimental data for a semiconductor ZnO crystal, we identify the split-off valence band as making the greatest contribution to tunneling to the conduction band. Our new band structure measurement technique is intrinsically bulk sensitive, does not require a vacuum, and has high temporal resolution, making it suitable to study reactions at ambient conditions, matter under extreme pressures, and ultrafast transient modifications to band structures.
Full-text · Article · Nov 2015 · Physical Review Letters
[Show abstract][Hide abstract] ABSTRACT: By employing pulse compression with a stretched hollow-core fiber, we generated 2-cycle pulses at 1.8 μm (12 fs) carrying 5 mJ of pulse energy at 100 Hz repetition rate. This energy scaling in the mid-infrared spectral range was achieved by lowering the intensity in a loose focusing condition, thus suppressing the ionization induced losses. The correspondingly large focus was coupled into a hollow-core fiber of 1 mm inner diameter, operated with a pressure gradient to further reduce detrimental nonlinear effects. The required amount of self-phase modulation for spectral broadening was obtained over 3 m of propagation distance.
Full-text · Article · Nov 2015 · Applied Physics Letters
[Show abstract][Hide abstract] ABSTRACT: The influence of cyclic electron delocalization associated with aromaticity on the high-order-harmonic generation (HHG) process is investigated in organic molecules. We show that the aromatic molecules benzene (C6H6) and furan (C4H4O) produce high-order harmonics more efficiently than nonaromatic systems having the same ring structure. We also demonstrate that the relative strength of plateau harmonics is sensitive to the aromaticity in five-membered-ring molecules using furan, pyrrole (C4H4NH), and thiophene (C4H4S). Numerical time-dependent Schrödinger equation simulations of total orientation-averaged strong-field ionization yields show that the HHG from aromatic molecules comes predominantly from the two highest π molecular orbitals, which contribute to the aromatic character of the systems.
Full-text · Article · Oct 2015 · Physical Review A
[Show abstract][Hide abstract] ABSTRACT: 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.
Full-text · Article · Sep 2015 · Journal of Biophotonics
[Show abstract][Hide abstract] ABSTRACT: When intense light interacts with an atomic gas, recollision between an ionizing electron and its parent ion creates high-order harmonics of the fundamental laser frequency. This sub-cycle effect generates coherent soft X-rays and attosecond pulses, and provides a means to image molecular orbitals. Recently, high harmonics have been generated from bulk crystals, but what mechanism dominates the emission remains uncertain. To resolve this issue, we adapt measurement methods from gas-phase research to solid zinc oxide driven by mid-infrared laser fields of 0.25 volts per ångström. We find that when we alter the generation process with a second-harmonic beam, the modified harmonic spectrum bears the signature of a generalized recollision between an electron and its associated hole. In addition, we find that solid-state high harmonics are perturbed by fields so weak that they are present in conventional electronic circuits, thus opening a route to integrate electronics with attosecond and high-harmonic technology. Future experiments will permit the band structure of a solid to be tomographically reconstructed.
[Show abstract][Hide abstract] ABSTRACT: Electric breakdown in air occurs for electric fields exceeding 34 kV/cm and results in a large current surge that propagates along unpredictable trajectories. Guiding such currents across specific paths in a controllable manner could allow protection against lightning strikes and high-voltage capacitor discharges. Such capabilities can be used for delivering charge to specific targets, for electronic jamming, or for applications associated with electric welding and machining. We show that judiciously shaped laser radiation can be effectively used to manipulate the discharge along a complex path and to produce electric discharges that unfold along a predefined trajectory. Remarkably, such laser-induced arcing can even circumvent an object that completely occludes the line of sight.
[Show abstract][Hide abstract] ABSTRACT: Here we introduce a high sensitive side-polished fiber optic based surface plasmon resonance (SPR) sensor for refractometry in liquids for 1.32–1.37 Refractive Index Unit (RIU). In fabrication, a Controllable Hybrid Polishing Method (CHPM) was used to make high quality D-shaped fibers. For characterization, a super continuum (SC) light source was used in the measurement setup. The sensor has a spectral sensitivity of 5200 nm/RIU with a Limit of Detection (LOD) of 5.8 × 10−6 RIU. Also, we have demonstrated that by reducing the intensity noise in our light source, a Signal-to-Noise Ratio (SNR) of 12.6 dB and a Limit of Detection (LOD) of 3.7 × 10−6 RIU is achievable in an intensiometric approach.
No preview · Article · Jun 2015 · Sensors and Actuators A Physical
[Show abstract][Hide abstract] ABSTRACT: We propose a novel Surface Plasmon Resonance (SPR)-based sensor that detects dew formation in optical fiber-based smart textiles. The proposed SPR sensor facilitates the observation of two phenomena: condensation of moisture and evaporation of water molecules in air. This sensor detects dew formation in less than 0.25 s, and determines dew point temperature with an accuracy of 4%. It can be used to monitor water layer depth changes during dew formation and evaporation in the range of a plasmon depth probe, i.e., 250 nm, with a resolution of 7 nm. Further, it facilitates estimation of the relative humidity of a medium over a dynamic range of 30% to 70% by measuring the evaporation time via the plasmon depth probe.
[Show abstract][Hide abstract] ABSTRACT: We investigate the behavior of resonant-induced harmonics from tin using driving lasers with tunable wavelengths. The intensity of the resonant harmonic is suppressed by the tuning laser wavelength around 1.8µm to understand the interaction dynamics of continuum electron with the autoionizing state.
[Show abstract][Hide abstract] ABSTRACT: Carbon molecules are used to generate intense high-order harmonics using driving lasers with 0.8 µm - 1.71 µm wavelengths. By driving plasma of reduced size (~200µm) with 1.71µm laser, we could extend the cutoff to ~70eV, while reducing the peak intensity by only ~31%.