Broadband negative group velocity dispersion in all-dielectric metamaterial and its role in supercontinuum generation.

All-dielectric metamaterials conforming to an optical reflectionless potential (ORP) offer broadband, omni-directional suppression of reflection. Though they are predicted to possess broadband negative group velocity dispersion (GVD), ultrashort pulse propagation through such materials has not been studied so far, to the best of our knowledge. In this work, we demonstrate negative GVD and group delay dispersion over broadband covering visible to near-infrared wavelengths. We investigate the role of ORP in supercontinuum generation (SC), which is observed to be polarization independent. The negative GVD in ORPs is interesting for pulse compression, phase compensation, dispersion engineering, and controlled SC generation.

Ultrafast dynamics of hemin aggregates.

The effects of solvents on the conformation of hemin and their implications on the dynamics of the complex have been studied using the time-resolved optical Kerr effect (OKE) with 35 fs laser pulses (at a central wavelength of 800 nm). The OKE enabled estimation to be made of the third-order nonlinear electronic susceptibility (χ(3)) of hemin solutions: it was found to be significantly smaller than that in hemin thin films. The real and imaginary components of χ(3) were negative in both the solvents, suggesting that one-photon as well as two-photon absorption processes contribute to the nonlinear electronic susceptibility of hemin. Our study of the ultrafast heme dynamics not only unveils the instantaneous electronic response related to electronic susceptibility but also brings to the fore a novel libration process that has hitherto remained undetected. The hindered rotation in the femtosecond domain that may be responsible for this libration process possibly stems from π-π hemin oligomers formed in aqueous solution. The present results provide new insights into the conformational dynamics in the self-assembly of heme oligomers that may also be significant in certain pathogenic conditions where free heme is formed in biological systems.

Inscription of type I and depressed cladding waveguides in lithium niobate using a femtosecond laser.

We describe two types of waveguides (type I and depressed cladding) inscribed in lithium niobate using a variable repetition rate (200 kHz-25 MHz), 270 fs duration fiber laser. The type I modification-based waveguides have propagation losses in the range from 1.2 to 10 dB/cm at 1550 nm, depending on experimental parameters. These waveguides are not permanent; they deteriorate over time. Such deterioration of waveguides can be slowed down from 30 days to 100 days by pre-annealing the samples and by writing at a 720 kHz laser repetition rate. The propagation losses measured at 1550 nm show significant improvement for pre-annealed samples. The depressed cladding-inscribed waveguides are permanent, but the propagation loss depends on the number of damage tracks. A track separation of ∼1 µm between adjacent damage tracks yields the lowest propagation loss of 0.5 dB/cm at 1550 nm for a 40 µm diameter waveguide. We observe multimode guidance for sizes in the range of 20-80 µm in these waveguide structures at 1550 nm. Their crystalline nature is found to remain intact, as inferred from second-harmonic generation within the waveguide region.

Femtosecond supercontinuum generation in water in the vicinity of absorption bands.

We show that it is possible to overcome the perceived limitations caused by absorption bands in water so as to generate supercontinuum (SC) spectra in the anomalous dispersion regime that extend well beyond 2000 nm wavelength. By choosing a pump wavelength within a few hundred nanometers above the zero-dispersion wavelength of 1048 nm, initial spectral broadening extends into the normal dispersion regime and, in turn, the SC process in the visible strongly benefits from phase-matching and matching group velocities between dispersive radiation and light in the anomalous dispersion regime. Some of the SC spectra are shown to encompass two and a half octaves.

Influencing supercontinuum generation by phase distorting an ultrashort laser pulse.

We show that the spectral distribution of the supercontinuum (SC) generated in barium fluoride is amenable to alteration simply by controlling the second- and third-order phase distortion of incident femtosecond-duration pulses. The second- and third-order phase distortions are controlled by an acoustic-optic programmable dispersive filter (AOPDF). The spectral extent on the blue side of the SC is influenced by independently varying the phase distortion of an ultrashort laser pulse.

Selective breaking of bonds in water with intense, 2-cycle, infrared laser pulses.

One of the holy grails of contemporary science has been to establish the possibility of preferentially breaking one of several bonds in a molecule. For instance, the two O-H bonds in water are equivalent: given sufficient energy, either one of them is equally likely to break. We report bond-selective molecular fragmentation upon application of intense, 2-cycle pulses of 800 nm laser light: we demonstrate up to three-fold enhancement for preferential bond breaking in isotopically substituted water (HOD). Our experimental observations are rationalized by means of ab initio computations of the potential energy surfaces of HOD, HOD(+), and HOD(2+) and explorations of the dissociation limits resulting from either O-H or O-D bond rupture. The observations we report present a formidable theoretical challenge that need to be taken up in order to gain insights into molecular dynamics, strong field physics, chemical physics, non-adiabatic processes, mass spectrometry, and time-dependent quantum chemistry.

DNA damage by OH radicals produced using intense, ultrashort, long wavelength laser pulses.

We probe femtosecond laser induced damage to aqueous DNA, relying on strong-field interaction with water wherein electrons and free radicals are generated in situ; these, in turn, interact with DNA plasmids under physiological conditions, producing nicks. Exposure to intense femtosecond pulses of 1350 and 2200 nm light induces single strand breaks and double strand breaks (DSBs) in DNA. At the longer wavelength (and at higher intensities), rotationally hot OH radicals induce DSBs, producing linear DNA. Strand breaks occur due to single or multiple OH hits on DNA. With 2200 nm light, DSBs are formed mostly by the action of two OH radicals; use of OH scavengers establishes that the probability of a two-hit event reduces much faster than a one-hit event as scavenger concentration is increased. Thermal effects do not induce DSBs with 2200 nm light.

Carrier-envelope-phase effects in ultrafast strong-field ionization dynamics of multielectron systems: Xe and CS2.

Carrier-envelope-phase- (CEP) stabilized 5 and 22 fs pulses of intense 800 nm light are used to probe the strong-field ionization dynamics of xenon and carbon disulfide. We compare ion yields obtained with and without CEP stabilization. With 8-cycle (22 fs) pulses, Xe(6+) yields are suppressed (relative to Xe(+)) by 30%-50%, depending on phase, reflecting the phase dependence of nonsequential ionization and its contribution to the formation of higher charge states. Ion yields for Xe(q+) (q = 2-4) with CEP-stabilized pulses are enhanced (by up to 50%) compared to those with CEP-unstabilized pulses. Such enhancement is particularly pronounced with 2-cycle (5 fs) pulses and is distinctly phase dependent. Orbital shape and symmetry affect how CS(2) responds to variations in optical field that are effected as CEP is altered, keeping intensity constant. Molecular fragmentation is found to depend on field strength (not intensity); the relative enhancement of fragmentation when CEP-stabilized 2-cycle pulses are used is found to be at the expense of molecular ionization.

Optical trapping in an absorbing medium: from optical tweezing to thermal tweezing.

We report on optical trapping in a weakly absorbing medium, hemin, an iron-containing porphyrin that is an important component of hemoglobin. By altering the hemin concentration we are able to control the amount of optical energy that is absorbed; changing the hemin concentration from <12 mg/ml to >45 mg/ml enables the onset of thermal trapping to be observed. By estimating the trap strength using two different methods we are readily able to differentiate between the optical trapping and thermal trapping regimes. We also deduce the rise in temperature that occurs within the laser focal volume: temperature changes of 5-24 K are observed for laser power values of 10-90 mW for hemin concentrations of 0-50 mg/ml.

Intense two-cycle laser pulses induce time-dependent bond hardening in a polyatomic molecule.

A time-dependent bond-hardening process is discovered in a polyatomic molecule (tetramethyl silane, TMS) using few-cycle pulses of intense 800 nm light. In conventional mass spectrometry, symmetrical molecules such as TMS do not exhibit a prominent molecular ion (TMS(+)) as unimolecular dissociation into [Si(CH(3))(3)](+) proceeds very fast. Under a strong field and few-cycle conditions, this dissociation channel is defeated by time-dependent bond hardening: a field-induced potential well is created in the TMS(+) potential energy curve that effectively traps a wave packet. The time dependence of this bond-hardening process is verified using longer-duration (≥100 fs) pulses; the relatively slower falloff of optical field in such pulses allows the initially trapped wave packet to leak out, thereby rendering TMS(+) unstable once again.

Effect of intense, ultrashort laser pulses on DNA plasmids in their native state: strand breakages induced by in situ electrons and radicals.

Single strand breaks are induced in DNA plasmids, pBR322 and pUC19, in aqueous media exposed to strong fields generated using ultrashort laser pulses (820 nm wavelength, 45 fs pulse duration, 1 kHz repetition rate) at intensities of 1-12 TW cm(-2). The strong fields generate, in situ, electrons and radicals that induce transformation of supercoiled DNA into relaxed DNA, the extent of which is quantified. Introduction of electron and radical scavengers inhibits DNA damage; results indicate that OH radicals are the primary (but not sole) cause of DNA damage.

Optical-tweezer-induced microbubbles as scavengers of carbon nanotubes.

A modified optical tweezers set-up has been used to generate microbubbles in flowing, biologically relevant fluids and human whole blood that contains carbon nanotubes (CNTs) using low power (< or =5 mW), infrared (1064 nm wavelength), continuous wave laser light. Temperature driven effects at the tweezers' focal point help to optically trap these microbubbles. It is observed that proximate CNTs are driven towards the focal spot where, on encountering the microbubble, they adhere to it. Such CNT-loaded microbubbles can be transported both along and against the flow of surrounding fluid, and can also be exploded to cause fragmentation of the bundles. Thus, microbubbles may be used for scavenging, transporting and dispersal of potentially toxic CNTs in biologically relevant environments.

Bright visible emission from carbon nanotubes spatially constrained on a micro-bubble.

We report emission of broadband light in the spectral range 500 nm - 900 nm from single walled carbon nanotubes (SWNTs) in a liquid environment upon irradiance by a very low power (typically <5 mW), continuous-wave laser source in a tweezers setup. We show (i) formation of micro-bubbles upon irradiation of fluids containing bundles of SWNTs, (ii) optical trapping of such micro-bubbles, (iii) adhesion of SWNTs on the surface of such micro-bubbles, and (iv) bright emission of white light due to tweezer-induced localized heating of spatially-constrained SWNTs.

Strong fields induce ultrafast rearrangement of H atoms in H2O.

H atoms in H(2)O are rearranged by strong optical fields generated by intense 9.3 fs laser pulses to form H(2)(+). This atomic rearrangement is ultrafast: It occurs within a single laser pulse. Quantum-chemical calculations reveal that H(2)(+) originates in the (1)A state of H(2)O(2+) when the O-H bond elongates to 1.15 a.u. and the H-O-H angle becomes 120 degrees. Bond formation on the ultrafast time scale of molecular vibrations (10 fs for H(2)(+)) and in strong fields has hitherto not been reported.

Polarization and energy stability of filamentation-generated few-cycle pulses.

Polarization properties and energy stability are measured for few-cycle pulses that are generated by filamentation in dual Ar-filled tubes in tandem. The dual-tube geometry enhances the contribution of self-phase modulation to spectral broadening. The polarization extinction ratio (I(perpendicular)/I(parallel) is improved for the beam transmitted through the second tube compared to the first tube and of the incident laser beam. Polarization control of few-cycle pulses is realized in simple fashion by a half-wave plate placed prior to the dual-tube assembly. We show that intensity clamping in the filament affords a major advantage in accomplishing a significant reduction in energy fluctuations compared to those inherent in the incident laser beam.

Euler buckling-induced folding and rotation of red blood cells in an optical trap.

We investigate the physics of an optically driven micromotor of biological origin. When a single, live red blood cell (RBC) is placed in an optical trap, the normal biconcave disc shape of the cell is observed to fold into a rod-like shape. If the trapping laser beam is circularly polarized, the folded RBC rotates. A model based on geometric considerations, using the concept of buckling instabilities, captures the folding phenomenon; the rotation of the cell is rationalized using the Poincaré sphere. Our model predicts that (i) at a critical power of the trapping laser beam the RBC shape undergoes large fluctuations, and (ii) the torque that is generated is proportional to the power of the laser beam. These predictions are verified experimentally. We suggest a possible mechanism for the emergence of birefringent properties in the RBC in the folded state.

Femtosecond laser written channel waveguides in tellurite glass.

We have made and characterized a new, erbium-doped tellurite glass that has high glass transition temperature. Addition of phosphate is found to increase the phonon energy. The peak emission cross section is 6 x 10(-21) cm(2) at 1537 nm and the fluorescence lifetime of the (4)I(13/2)-(4)I(15/2) transition is 4.1 ms. We have written 2-D channel waveguides in this glass using focused, 45-fs pulses from an amplified Ti:sapphire laser at different laser energies and writing speeds. Migration of atoms towards the periphery of the waveguides occurs, leading to refractive index changes. Channels show waveguiding at 1310 nm which is promising for the fabrication of integrated lasers and broadband amplifiers.

Optical control of filamentation-induced damage to DNA by intense, ultrashort, near-infrared laser pulses.

We report on damage to DNA in an aqueous medium induced by ultrashort pulses of intense laser light of 800 nm wavelength. Focusing of such pulses, using lenses of various focal lengths, induces plasma formation within the aqueous medium. Such plasma can have a spatial extent that is far in excess of the Rayleigh range. In the case of water, the resulting ionization and dissociation gives rise to in situ generation of low-energy electrons and OH-radicals. Interactions of these with plasmid DNA produce nicks in the DNA backbone: single strand breaks (SSBs) are induced as are, at higher laser intensities, double strand breaks (DSBs). Under physiological conditions, the latter are not readily amenable to repair. Systematic quantification of SSBs and DSBs at different values of incident laser energy and under different external focusing conditions reveals that damage occurs in two distinct regimes. Numerical aperture is the experimental handle that delineates the two regimes, permitting simple optical control over the extent of DNA damage.

Depolarization of white light generated by ultrashort laser pulses in optical media.

We report measurements of the extinction ratio (ER) of white light generated upon irradiation of BK7 glass by ultrashort (36 fs) laser pulses with incident power approximately 10(3) times larger than the critical power for self-focusing. At low incident powers, the continuum is symmetric about the incident laser wavelength; at high powers it becomes broader and distinctly asymmetric towards the blue side. We observe that ER degrades by 100-fold after the onset of multiphoton-induced free-electron generation (at incident intensity approximately 2 TW cm-2), which also corresponds to the onset of asymmetry in white-light spectra.

High-contrast interference pattern of amplified spontaneous emission from dyes under transient grating excitation.

We demonstrate a high-contrast interference fringe pattern formed by amplified spontaneous emission (ASE) in a noncollinear two-beam self-diffraction setup by use of dyes. In the presence of a transient grating a stable interference pattern is observed in ASE induced by one- and two-photon absorption. The fringe visibility varies from 0.2 to 0.65 with a temporal delay in the two beams. The variation of the angle between the two exciting beams at the temporal overlap shows an increase in the fringe visibility with an increase in the angle.