Sharly Fleischer

Efficient frequency doubling of a femtosecond fiber laser

We report optimization of a stretched-pulse erbium-doped fiber laser for second-harmonic generation and the evaluation of several nonlinear crystals for this application. With compressed fundamental pulse energies of 2.7 nJ at 31.8 MHz, we achieved 10% conversion efficiency and 86-fs, 771-nm pulses with energies of 270 pJ. Frequency-resolved optical gating was used to analyze both the fundamental and the frequencydoubled pulses.

A review of non-linear terahertz spectroscopy with ultrashort tabletop-laser pulses

Over the past decade, breakthroughs in the generation and control of ultrafast high-field terahertz (THz) radiation have led to new spectroscopic methodologies for the study of light-matter interactions in the strong-field limit. In this review, we will outline recent experimental demonstrations of non-linear THz material responses in materials ranging from molecular gases, to liquids, to varieties of solids – including semiconductors, nanocarbon, and correlated electron materials. New insights into how strong THz fields interact with matter will be discussed in which a THz field can act as either a non-resonant electric field or a broad bandwidth pulse driving specific resonances within it. As an emerging field, non-linear THz spectroscopy shows promise for elucidating dynamic problems associated with next generation electronics and optoelectronics, as well as for demonstrating control over collective material degrees of freedom.

Controlling the sense of molecular rotation

We introduce a new scheme for controlling the sense of molecular rotation. By varying the polarization and the delay between two ultrashort laser pulses, we induce unidirectional molecular rotation, thereby forcing the molecules to rotate clockwise/counterclockwise under field-free conditions. We show that unidirectionally rotating molecules are confined to the plane defined by the two polarization vectors of the pulses, which leads to a permanent anisotropy in the molecular angular distribution. The latter may be useful for controlling collisional cross-sections and optical and kinetic processes in molecular gases. We discuss the application of this control scheme to individual components within a molecular mixture in a selective manner.

Nonlinear two-dimensional terahertz photon echo and rotational spectroscopy in the gas phase

Significance Molecular rotations of small molecules provide a useful testbed for examining light−matter interactions with quantum mechanical systems, but the methods of modern spectroscopy have been largely unavailable in the terahertz frequency range where most of the rotational states that are thermally populated at ordinary temperatures absorb light. Applying a pair of strong terahertz pulses, we excite molecular rotations coherently, interrogate thermally populated rotational states, manipulate the rotational motions nonlinearly, and observe connections between different rotational states spectroscopically. The method is applicable to polar molecules in flames and other reactive conditions, and it enables enhanced control over molecular motion with light. Ultrafast 2D spectroscopy uses correlated multiple light−matter interactions for retrieving dynamic features that may otherwise be hidden under the linear spectrum; its extension to the terahertz regime of the electromagnetic spectrum, where a rich variety of material degrees of freedom reside, remains an experimental challenge. We report a demonstration of ultrafast 2D terahertz spectroscopy of gas-phase molecular rotors at room temperature. Using time-delayed terahertz pulse pairs, we observe photon echoes and other nonlinear signals resulting from molecular dipole orientation induced by multiple terahertz field−dipole interactions. The nonlinear time domain orientation signals are mapped into the frequency domain in 2D rotational spectra that reveal J-state-resolved nonlinear rotational dynamics. The approach enables direct observation of correlated rotational transitions and may reveal rotational coupling and relaxation pathways in the ground electronic and vibrational state.

Selective control of molecular rotation

We demonstrate selective control over rotational motion of small, linear molecules. By means of sequential excitation of the rotational motion by ultrashort pulses, we first prepare transiently aligned molecules with periodically revived angular distribution. Upon further, properly timed excitation, the rotational energy can be increased or decreased, depending on the exact timing of the second pulse. We show how this approach can be applied for selective rotational control of a single component in a molecular mixture. We discuss this selectivity in the context of molecular isotopes (14N2, 15N2), where the difference in isotopic mass gives rise to different rotational revival times. We further apply the method to the selective addressing of molecular spin isomers (para, ortho15N2) in a mixture, where wavefunction symmetry differences replace the mass differences as the origin of the selectivity. In both cases the method is demonstrated experimentally and the results are analysed theoretically.

Rotational Control of Asymmetric Molecules: Dipole- versus Polarizability-Driven Rotational Dynamics

We experimentally study the optical- and terahertz-induced rotational dynamics of asymmetric molecules in the gas phase. Terahertz and optical fields are identified as two distinct control handles over asymmetric molecules, as they couple to the rotational degrees of freedom via the molecular dipole and polarizability selectively. The distinction between those two rotational handles is highlighted by different types of quantum revivals observed in long-duration (>100  ps) field-free rotational evolution. The experimental results are in excellent agreement with random phase wave function (RPWF) simulations [Phys. Rev. A 91, 063420 (2015)] and provide verification of the RPWF as an efficient method for calculating asymmetric molecular dynamics at ambient temperatures, where exact calculation methods are practically not feasible. Our observations and analysis pave the way for orchestrated excitations by both optical and terahertz fields as complementary rotational handles that enable a plethora of new possibilities in three-dimensional rotational control of asymmetric molecules.

A novel experimental method for the local mechanical testing of human coronal dentin

OBJECTIVES The small volume of human dentin available for sample preparation and the local variations in its microstructure present a real challenge in the determination of their mechanical properties. The main purpose of the present study was to develop a new procedure for the preparation and mechanical testing of small-scale specimens of biomaterials such as dentin, so as to probe local mechanical properties as a function of microstructure. METHODS Ultra short laser pulses were used to mill a block of dentin into an array of 16 microm size dentin pillars. These could then be individually tested in compression with an instrumented nanoindenter fitted with a 30 microm wide flat punch. RESULTS The laser-based pillar preparation procedure proved effective and reliable. Data was produced for the mechanical properties of a first set of dry dentin micro-pillars. SIGNIFICANCE This novel experimental approach enables the preparation and compression of micron-scale samples with well-defined microstructure. For dentin, this means samples containing a relatively small number of well-defined parallel tubules, with a distinct orientation relative to the applied load. The ability to isolate the separate effects of microstructural parameters on the mechanical properties is of major significance for future substantiation of theoretical models.

Spinning molecules selectively : laser control of isotopes and nuclear spin isomers

Following excitation by a strong ultra-short laser pulse, molecules develop coordinated rotational motion, exhibiting transient alignment along the direction of the laser electric field, followed by periodic full and fractional revivals that depend on the molecular rotational constants. In mixtures, the different species undergo similar rotational dynamics, all starting together but evolving differently with each demonstrating its own periodic revival cycles. For a bimolecular mixture of linear molecules, at predetermined times, one species may attain a maximally aligned state while the other is anti-aligned (i.e. molecular axes are confined in a plane perpendicular to the laser electric field direction). By a properly timed second laser pulse, the rotational excitation of the undesired species may be almost completely removed leaving only the desired species to rotate and periodically realign, thus facilitating further selective manipulations by polarized light. In this paper, such double excitation schemes are demonstrated for mixtures of molecular isotopes (isotopologues) and for nuclear spin isomers.

Coherent Radiative Decay of Molecular Rotations: A Comparative Study of Terahertz-Oriented versus Optically Aligned Molecular Ensembles

The decay of field-free rotational dynamics is experimentally studied by two complementary methods: laser-induced molecular alignment and terahertz-field-induced molecular orientation. A comparison between the decay rates of different molecular species at various gas pressures reveals that oriented molecular ensembles decay faster than aligned ensembles. The discrepancy in decay rates is attributed to the coherent radiation emitted by the transiently oriented ensembles and is absent from aligned molecules. The experimental results reveal the dramatic contribution of coherent radiative emission to the observed decay of rotational dynamics and underline a general phenomenon expected whenever field-free coherent dipole oscillations are induced.

Compressive Response of Dentin Micro-Pillars

We propose a new experimental approach for the study of Young’s modulus and the strength of dentin, using micro sized pillar-like specimens tested under compression using a nanoindenter apparatus fitted with a flat punch indenter. Dentin micro pillars were prepared by ablation with ultra short laser pulses, and subsequently compressed with a 30 μm diameter flat punch. Tubule orientation is found to affect the compression behavior of dry dentine in air, more so for Young’s modulus than for strength. We propose to fit these results with adaptations of fiber composite theoretical models.