J. A. Dharmadhikari

Measuring erythrocyte deformability with fluorescence, fluid forces, and optical trapping

A laser-based method has been developed for experimentally probing single red blood cell (RBC) buckling and determining RBC membrane rigidity. Our method combines a liquid flow cell, fluorescence microscopy, and an optical-trap to facilitate simple measurements of the shear modulus and buckling properties of single RBCs, under physiological conditions. The efficacy of the method is illustrated by studying buckling behavior of normal and Plasmodium-infected RBCs, and the effect of Plasmodium falciparum-conditioned medium on normal, uninfected cells. Our simple method, which quantifies single-RBC deformability, may ease detection of RBC hematological disorders.

Shape anisotropy induces rotations in optically trapped red blood cells

A combined experimental and theoretical study is carried out to probe the rotational behavior of red blood cells (RBCs) in a single beam optical trap. We induce shape changes in RBCs by altering the properties of the suspension medium in which live cells float. We find that certain shape anisotropies result in the rotation of optically trapped cells. Indeed, even normal (healthy) RBCs can be made to rotate using linearly polarized trapping light by altering the osmotic stress the cells are subjected to. Hyperosmotic stress is found to induce shape anisotropies. We also probe the effect of the mediums viscosity on cell rotation. The observed rotations are modeled using a Langevin-type equation of motion that takes into account frictional forces that are generated as RBCs rotate in the medium. We observe good correlation between our measured data and calculated results.

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.

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.

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.

On the birefringence of healthy and malaria-infected red blood cells

Abstract. The birefringence of a red blood cell (RBC) is quantitatively monitored as it becomes infected by a malarial parasite. Large changes occur in the cell’s refractive index at different stages of malarial infection. The observed rotation of an optically trapped, malaria-infected RBC is not a simple function of shape distortion: the malarial parasite is found to itself exercise a profound influence on the rotational dynamics by inducing stage-specific birefringence. Our measurements shed new light on the competition between shape- and form-birefringence in RBCs. We demonstrate the possibility of using birefringence to establish very early stages of infected parasites and of assessing various factors that contribute to birefringence in normal and infected cells. Our results have implications for the development and use of noninvasive techniques of quantifying changes in cell properties induced by malaria disease pathology.

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.

Generation of stable colloidal gold nanoparticles by ultrashort laser-induced melting and fragmentation

We report on generation of stable colloidal gold nanoparticles by ultrashort laser-induced melting and fragmentation. Irradiation of colloidal gold nanoparticles (of initial size larger than 25 nm) by 56 fs long, near-IR pulses of moderate fluence (1.3–5.3 J cm−2) generates very small (2.5 nm) nanoparticles with a narrow size distribution (±0.5 nm). Systematic measurements show the final size of fragmented nanoparticles to be (i) very weakly dependent on the original size and particle shape as well as of pump laser wavelength (800 nm, 1200 nm and 1350 nm), but (ii) strongly dependent on laser parameters; moreover, fragmentation is effectively controllable by pulse fluence and irradiation time. The fragmented particles appear to be contaminant free and have high crystalline quality. We find that the fragmented particles are stable over a time period of more than three months. Stable, contaminant-free, crystalline colloidal gold nanoparticles of sizes around 3 nm, with very narrow size distribution, have potential utility in diverse nanotechnological applications, ranging from biologically relevant imaging to nanoscopic generators of high-frequency mechanical vibrations in the GHz range.

Seventh-harmonic generation from tightly focused 2 μm ultrashort pulses in air.

We report generation of third, fifth and seventh harmonics from air by using tightly focused, ultrashort pulses of short-wave infrared (2 μm) radiation. We have measured the third- and fifth-harmonic efficiencies to be 5×10(-5) and ~1.4×10(-5), respectively, with the ratio of fifth-to-third-harmonic efficiency being close to 0.28. Our experimental results provide confirmation of expectations of the higher-order Kerr effect model.

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.