Laser induced breakdown spectroscopy (LIBS) has become a proven contemporary workhorse for qualitative and quantitative analysis of materials. Recent developments in LIBS have been limited either to signal enhancement strategies or to advances in data analysis techniques that yield better interpretation of LIBS data. Explorations of the initial laser excitation stage of LIBS remain somewhat restricted. In particular, the influence, if any, of the polarization state of excitation laser remains unexplored to a large extent. The current work addresses this lacuna in knowledge by probing the influence of different polarization states of the excitation laser on LIBS spectra of metallic copper. Specifically, we investigate the behaviour of atomic and ionic emission lines with respect to change in polarization state of the incident laser light; our results show distinct polarization dependence. Our observations open up new opportunities of tackling the problem of relatively faint emissions from ionic species in the plasma by adjusting the polarization state of the laser. Our findings also highlight the urgent need for appropriate theoretical study to be undertaken so that proper insights can be developed into the physics that drive the observations that we report here.

Regarded as the most important ion in interstellar chemistry, the trihydrogen cation, H_3^+ , plays a vital role in the formation of water and many complex organic molecules believed to be responsible for life in our universe. Apart from traditional plasma discharges, recent laboratory studies have focused on forming the trihydrogen cation from large organic molecules during their interactions with intense radiation and charged particles. In contrast, we present results on forming H_3^+ from bimolecular reactions that involve only an inorganic molecule, namely water, without the presence of any organic molecules to facilitate its formation. This generation of H_3^+ is enabled by “engineering” a suitable reaction environment comprising water-covered silica nanoparticles exposed to intense, femtosecond laser pulses. Similar, naturally-occurring, environments might exist in astrophysical settings where hydrated nanometer-sized dust particles are impacted by cosmic rays of charged particles or solar wind ions. Our results are a clear manifestation of how aerosolized nanoparticles in intense femtosecond laser fields can serve as a catalysts that enable exotic molecular entities to be produced via non-traditional routes.

Electrons and •OH-radicals have been generated by using low-energy laser pulses of 6 ns duration (1064 nm wavelength) to create plasma in a suspension of plasmid DNA (pUC19) in water. Upon thermalization, these particles induce single and double strand breakages in DNA along with possible base oxidation/base degradation. The time-evolution of the ensuing structural modifications has been measured; damage to DNA is seen to occur within 30 s of laser irradiation. The time-evolution is also measured upon addition of physiologically relevant concentrations of salts containing monovalent, divalent, or trivalent alkali ions. It is shown that some alkali ions can significantly inhibit strand breakages while some do not. The inhibition is due to electrostatic shielding of DNA, but significantly, the extent of such shielding is seen to depend on how each alkali ion binds to DNA. Results of experiments on strand breakages induced by thermalized particles produced upon plasma-induced photolysis of water, and their inhibition, suggest implications beyond studies of DNA; they open new vistas for utilizing simple nanosecond lasers to explore the effect of ultralow energy radiation on living matter under physiologically relevant conditions.

Zhang and coworkers have recently reported results of experiments involving irradiation of argon clusters doped with bromofluorene chromophores by nanosecond-long pulses of 532 nm laser light. Multiply-charged ions of atomic argon (charge states, n, up to 7) and carbon (charge states up to 4) are observed which are sought to be rationalised using an evaporation model. The distinguishing facet of exploding clusters being progenitors of energetic ions and electrons constitutes the key driver for contemporary research in laser-cluster interactions; it is, therefore, important to point out inconsistencies that are intrinsic to the model of Zhang and coworkers. In light of similar reports already in the literature, we show that their model is of limited utility in describing the dynamics that govern how fast, multiply-charged atomic ions result from laser irradiation of gas-phase clusters. We posit that it is plasma behaviour that underpins cluster heating and cluster explosion dynamics.

Zhang and co-workers ( J. Phys. Chem. Lett. 2020, 11, 1100-1105) have recently reported results of experiments involving irradiation of argon clusters doped with bromofluorene chromophores by nanosecond-long pulses of 532 nm laser light. Multiply charged ions of atomic argon (Arn+, 1 ≤ n ≤ 7) and carbon (Cn+, 1 ≤ n ≤ 4) are observed, which are sought to be rationalized using an evaporation model. The distinguishing facet of exploding clusters being progenitors of energetic ions and electrons constitutes the key driver for contemporary research in laser-cluster interactions; it is, therefore, important to point out inconsistencies that are intrinsic to the model of Zhang and co-workers. In light of similar reports already in the literature, we show that their model is of limited utility in describing the dynamics that govern how fast, multiply charged atomic ions result from laser irradiation of gas-phase clusters. We posit that it is plasma behavior that underpins cluster heating and cluster explosion dynamics.

Low-power laser pulses of 6 ns duration (1064 nm wavelength) have been used to create plasma in an aqueous solution of plasmid DNA (pUC19). Thermal energy electrons and •OH radicals in the plasma induce strand breakages in DNA, including double strand breaks and possible base oxidation/base degradation. The time evolution of these modifications shows that it takes barely 30 s for damage to DNA to occur. Addition of physiologically relevant concentrations of a salt (NaCl) significantly inhibits such damage. We rationalize such inhibition using simple electrostatic considerations. The observation that DNA damage is induced by plasma-induced photolysis of water suggests implications beyond studies of DNA and opens new vistas for using simple nanosecond lasers to probe how ultralow energy radiation may affect living matter under physiological conditions.

Photon sieves, a collection of randomly positioned apertures, focus electromagnetic radiation diffractively and find applications in x-ray optics to astronomy to bio-medical imaging. Femtosecond laser direct writing is an emerging rapid, reliable, and versatile technique for creating diffraction-limited features in dielectrics and metals. Using this technique, we produce localized spots with a modified refractive index within bulk glass and thus fabricate phase photon sieves for optical wavelengths. The distribution of spots was based on numerical simulations. A comparison of the performance of the phase photon sieves and zone-plates created showed a superior performance of the former in terms of tighter focusing and reduction of secondary maxima, thus offering better spatial resolution and imaging capabilities. (C) 2019 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

Birefringence is the optical property of a material having a refractive index that depends on the polarization and propagation direction of light. Generally, this is an intrinsic optical property of a material and cannot be altered. Here, we report a novel technique—direct laser writing—that enables us to control the natural, material birefringence of sapphire over a broad range of wavelengths. The broadband form birefringence originating from self-assembled, periodic array of sub-wavelength (∼ 50–200 nm) defects created by laser writing, can enhance, suppress or maintain the material birefringence of sapphire without affecting its transparency range in visible or its surface quality.

Laser-induced crystallization is emerging as an alternative technique to crystallize biomolecules. However, its applications are limited to specific small molecules and some simple proteins, possibly because of the need to use high-intensity, pulsed lasers and relatively long laser irradiation time. Both these factors tend to denature biological molecules. If the laser-intensity and time required to crystallize biomolecules were to be reduced, laser-induced crystallization may well become of widespread utility. We report here the crystallization of nineteen natural amino acids by a laser-induced method in combination with one of three nucleants: aluminum, coconut coir, and peacock feather barbule. We have utilized a low-power, continuous wave (CW) Nd:YAG laser (λ = 1064 nm). The advantages of our method are (i) the use of very small laser powers (60 mW), and (ii) the ability to obtain diffraction quality crystals within a mere few seconds. For most amino acids our method yields several orders of magnitude reduction in crystallization time. The use of biocompatible nucleants like coir fibres and peacock feather barbules are novel; their non-toxic nature may find broad applicability in rapid crystallization of diverse biological molecules.

We report on tunnel ionization of Xe by 2-cycle, intense, infrared laser pulses and its dependence on carrier-envelope-phase (CEP). At low values of optical field ($E$), the ionization yield is maximum for cos-like pulses with the dependence becoming stronger for higher charge states. At higher $E$-values, the CEP dependence either washes out or flips. A simple phenomenological model is developed that predicts and confirms the observed results. CEP effects are seen to persist for 8-cycle pulses. Unexpectedly, electron rescattering plays an unimportant role in the observed CEP dependence. Our results provide fresh perspectives in ultrafast, strong-field ionization dynamics of multi-electron systems that lie at the core of attosecond science.

The ability to fingerprint a few molecules via surface enhanced Raman scattering (SERS) continues to be of considerable utility in diverse fields encompassing physics, chemistry, materials sciences, nanotechnology, biomedicine, and environmental engineering. However, the development of facile and low cost approaches towards the fabrication of flexible substrates with very high SERS signal enhancement remains a challenge. Compared to conventional plasmonic-based sensors, a superhydrophobic plasmonic surface provides the combined advantage of concentration enrichment of solute molecules, the fourth power dependent localized electric field enhancement as well as the enhanced light scattering on rough surface. We demonstrate here a method to fabricate flexible SERS substrates by replicating laser-written patterns created on polymethylmethacrylate (PMMA) onto a soft-elastomer, namely polydimethylsiloxane (PDMS), followed by in situ reduction of silver nanoparticles on the surface. Laser writing of structures is fluence dependent and leads to substantial enhancement of Raman signals compared to a conventional plasmonic surface. Our fabricated surfaces provide a limit of detection of eight femtomolar for Rhodamine 6G upon 532 nm resonance excitation; an enhancement factor of similar to 10(10) is achieved for methyl orange. Studies of how water droplets spread on our laser-written surfaces indicate a fluence dependent enhancement in apparent contact angle with a concomitant increase in the contact angle hysteresis (CAH). Most significantly, our replicated patterns exhibit lotus effect (superhydrophobic surface with ultra-low contact angle hysteresis), that upon reduction of silver nanoparticles, exhibit superhydrophobicity with high contact angle hysteresis (rose petal effect). Our findings offer fresh opportunities for expanding the applicability of the SERS technique via superhydrophobic flexible plasmonic nanostructures.

Eryptosisthe suicidal death of erythrocytesis characterized by membrane blebbing and cell shrinkage. Eryptosis can be triggered by various xenobiotics such as carbon monoxide, lead, and amyloid, and by stressors such as oxidative stress, osmotic shock, and rapid alteration of ambient conditions. We have used Raman tweezers spectroscopy to study eryptosis in single, live cells and have attempted to explore the underlying mechanism, specifically to identify possible Raman signatures of eryptosis. Erythrocytes (red blood cells) were exposed to free radicals, silver nanoparticles, glucose, heat, and osmotic shock to induce eryptosis, and a comparison was made of their Raman spectra, which indicated that these conditions lead to a transition of haemoglobin from the R to the T state. Consequences of eryptosis include dehydration, cell shrinkage, and pH changes, which result in deoxygenation of haemoglobin. This, in turn, can be detected by monitoring the wavenumber shifts associated with Raman marker bands of R to T transitions. In addition, the principal component analysis results indicate differentiation among red blood cells undergone eryptosis due to different conditions.

Femtosecond laser-induced damage to plasmid DNA in aqueous medium manifests itself as strand breaks arising from interactions with slow OH-radicals (and electrons) in the laser-induced plasma generated in water. Such strand breakages are found to be significantly inhibited upon addition of salts (in physiologically significant concentrations) to the aqueous medium. A simple model rationalizes our observations and suggests the feasibility of electrostatically “engineering” DNA's ion atmosphere so as to prevent damage-inducing free radicals accessing DNA strands. These findings may aid development of new strategies for cancer treatment.

Recent work is summarized that shows how microbubbles may have potential utility in biomedical situations as (i) highly localized generators of intense white light in an aqueous environment, (ii) disruptors of matter in aqueous solution, (iii) essential precursors in laser-writing structures on substrates on which biological cells can be spatially aligned, and (iv) mediators in the fabrication of hierarchical nanostructures that enhance signals in biological Raman spectroscopy. Indeed, microbubbles generated upon laser irradiation of surfaces have many more ramifications than originally thought, with implications in the laser modification of surfaces producing either hydrophilicity or hydrophobicity. Many more possibilities remain to be explored and exploited.

Surface enhanced Raman scattering (SERS) spectroscopy, a powerful contemporary tool for studying low-concentration analytes via surface plasmon induced enhancement of local electric field, is of utility in biochemistry, material science, threat detection, and environmental studies. We have developed a simple, fast, scalable, and relatively low-cost optical method of fabricating and characterizing large-area, reusable and broadband SERS substrates with long storage lifetime. We use tightly focused, intense infra-red laser pulses to write gratings on single-crystalline, Au(111) gold films on mica which act as SERS substrates. Our single-crystalline SERS substrates compare favourably, in terms of surface quality and roughness, to those fabricated in poly-crystalline Au films. Tests show that our SERS substrates have the potential of detecting urea and 1,10-phenantroline adulterants in milk and water, respectively, at 0.01 ppm (or lower) concentrations.

With an advantage in photonic integration and device miniaturization, fabrication of micron sized diffractive optical elements has gained attention due to their low volume, light weight and flexible design. We discuss the fabrication of phase zone plates in soda-lime and borosilicate glass using a femtosecond laser, and its characterization. Our technique of fabrication involves a one-step laser direct writing process in comparison to the popular photolithography based micro-structuring. In this work, the femtosecond laser oscillator system is used to successfully fabricate phase zone plate structures at low energies and high repetition rate. In addition to this, a laser induced breakdown spectroscopy (LIBS) study was done to confirm the consistency of glass obtained from different manufacturers through its composition.

A diffusion equation has been used to study migration of early humans into the South Asian subcontinent. The diffusion equation is tempered by a set of parameters that account for geographical features like proximity to water resources, altitude, and flatness of land. The ensuing diffusion of populations is followed in time-dependent computer simulations carried out over a period of 10,000 YBP. The geographical parameters are determined from readily-available satellite data. The results of our computer simulations are compared to recent genetic data so as to better correlate the migratory patterns of various populations; they suggest that the initial populations started to coalesce around 4,000 YBP before the commencement of a period of relative geographical isolation of each population group. The period during which coalescence of populations occurred appears consistent with the established timeline associated with the Harappan civilization and also, with genetic admixing that recent genetic mapping data reveal. Our results may contribute to providing a timeline for the movement of prehistoric people. Most significantly, our results appear to suggest that the Ancestral Austro-Asiatic population entered the subcontinent through an easterly direction, potentially resolving a hitherto-contentious issue.

Filamentation in gases due to high power femtosecond pulses results from the combined action of the optical Kerr effect (giving rise to self-focusing) and plasma formation (giving rise to defocusing) that confines optical energy in a small region over a distance longer than the Rayleigh range. Since the discovery of N-2 as a potential gain medium, which subsequently led to the formation of nitrogen lasers, it has held a keen interest due to its potential in achieving lasing by remote excitation. Recently, Yamanouchi and coworkers demonstrated lasing action in N-2 in the forward as well the backward directions along the femtosecond pulse propagation. In the present work, we have focused on excitation of N-2(+) (corresponding to the 391nm spectral feature) and have measured spectral narrowing. We have investigated the influence exerted by the incident pulse power and gas pressure for incident pulses of durations 40 fs and 10 fs in forward and backward detection modes. Spectral narrowing that occurs for N-2 gas at 391 nm shows a dependence on the incident pulse duration. Pressure threshold for different incident powers for lasing has been established. Increase in the signal intensity on varying the incident power is ascribed to amplified spontaneous emission (ASE). White-light-seeded lasing in N-2(+) is generated by a Ti: sapphire femtosecond laser for different focusing. The lasing lines peak over the trail of the incident broadband spectra.

We report on the use of a femtosecond fibre laser (1030 nm) to inscribe structures like waveguides and splitters inside borosilicate (BK7) glass. Inscription of two- and three-dimensional splitters (1 × 2, 1 × 4, 1 × 8) is accomplished by programing a translation stage so as to achieve smooth bends. We carry out optical characterization of these laser-written structures by measuring both spectral transmission and propagation loss. Single mode guidance with propagation loss of 0.65 dB/cm is measured at 1560 nm for straight waveguides inscribed at low incident energy of 450 nJ. The spectral transmission of our splitters in the optical communication window, 1300–1600 nm, compares very favorably with conventional optical fibre splitters. We find that the splitting ratio as a function of wavelength is significantly more constant over a wide wavelength range, 1200–1600 nm, than optical fibre splitters. We also present results on characterization for splitting ratio and insertion loss at 1550 nm.