Flat-top supercontinuum and tunable femtosecond fiber laser sources at 1.9-2.5 μm

We report the high-energy flat-top supercontinuum covering the mid-infrared wavelength range of 1.9-2.5 μm as well as electronically tunable femtosecond pulses between 1.98-2.22 μm directly from the thulium-doped fiber laser amplifier. Comparison of experimental results with numerical simulations confirms that both sources employ the same nonlinear optical mechanism - Raman soliton frequency shift occurring inside the Tm-fiber amplifier. To illustrate that, we investigate two versions of the compact diode-pumped SESAM mode-locked femtosecond thulium-doped all-silica-fiber-based laser system providing either broadband supercontinuum or tunable Raman soliton output, depending on the parameters of the system. The first system operates in the Raman soliton regime providing femtosecond pulses tunable between 1.98-2.22 μm. Wide and continuous spectral tunability over 240 nm was realized by changing only the amplifier pump diode current. The second system generates high-energy supercontinuum with the superior spectral flatness of better than 1 dB covering the wavelength range of 1.9-2.5 μm, with the total output energy as high as 0.284 μJ, the average power of 2.1 W at 7.5 MHz repetition rate. We simulate the amplifier operation in the Raman soliton self-frequency shift regime and discuss the role of induced Raman scattering in supercontinuum formation inside the fiber amplifier. We compare this system with a more traditional 1.85-2.53 μm supercontinuum source in the external highly-nonlinear commercial chalcogenide fiber using the Raman soliton MOPA as an excitation source. The reported systems1 can be readily applied to a number of industrial applications in the mid-IR, including sensing, stand-off detection, medical surgery and fine material processing.

Experimental Study of Storage Ring Free-Electron Laser with Novel Capabilities

The Duke Free-electron laser (FEL) system, driven by the Duke electron storage ring, has been at the forefront of developing new light source capabilities over the past two decades. In 1999, the Duke FEL demonstrated the first lasing of a storage ring FEL in the vacuum ultraviolet (VUV) region at $194$ nm using two planar OK-4 undulators. With two helical undulators added to the outboard sides of the planar undulators, in 2005 the highest FEL gain ($47.8\%$) of a storage ring FEL was achieved using the Duke FEL system with a four-undulator configuration. In addition, the Duke FEL has been used as the photon source to drive the High Intensity $\gamma$-ray Source (HIGS) via Compton scattering of the FEL beam and electron beam inside the FEL cavity. Taking advantage of FEL's wavelength tunability as well as the adjustability of the energy of the electron beam in the storage ring, the nearly monochromatic $\gamma$-ray beam has been produced in a wide energy range from $1$ to $100$ MeV at the HIGS. To further push the FEL short wavelength limit and enhance the FEL gain in the VUV regime for high energy $\gamma$-ray production, two additional helical undulators were installed in 2012 using an undulator switchyard system to allow switching between the two planar and two helical undulators in the middle section of the FEL system. Using different undulator configurations made possible by the switchyard, a number of novel capabilities of the storage ring FEL have been developed and exploited for a wide FEL wavelength range from infrared (IR) to VUV. These new capabilities will eventually be made available to the $\gamma$-ray operation, which will greatly enhance the $\gamma$-ray user research program, creating new opportunities for certain types of nuclear physics research.

With the wide wavelength tuning range, the FEL is an intrinsically well-suited device to produce lasing with multiple colors. Taking advantage of the availability of an undulator system with multiple undulators, we have demonstrated the first two-color lasing of a storage ring FEL. Using either a three- or four-undulator configuration with a pair of dual-band high reflectivity mirrors, we have achieved simultaneous lasing in the IR and UV spectral regions. With the low-gain feature of the storage ring FEL, the power generated at the two wavelengths can be equally built up and precisely balanced to reach FEL saturation. A systematic experimental program to characterize this two-color FEL has been carried out, including precise power control, a study of the power stability of two-color lasing, wavelength tuning, and the impact of the FEL mirror degradation. Using this two-color laser, we have started to develop a new two-color $\gamma$-ray beam for scientific research at the HIGS.

Using the undulator switchyard, four helical undulators installed in the beamline can be configured to not only enhance the FEL gain in the VUV regime, but also allow for the full polarization control of the FEL beams. For the accelerator operation, the use of helical undulators is essential to extend the FEL mirror lifetime by reducing radiation damage from harmonic undulator radiation. Using a pair of helical undulators with opposite helicities, we have realized (1) fast helicity switching between left- and right-circular polarizations, and (2) the generation of fully controllable linear polarization. In order to extend these new capabilities of polarization control to the $\gamma$-ray operation in a wide energy range at the HIGS, a set of FEL polarization diagnostic systems need to be developed to cover the entire FEL wavelength range. The preliminary development of the polarization diagnostics for the wavelength range from IR to UV has been carried out.

DEVELOPMENT OF A CONDENSED PHASE VELOCITY MAP IMAGING APPARATUS: DISSOCIATION PHOTODYNAMICS OF NITROGEN DIOXIDE AT 355 NM

The photochemistry of the polar regions of Earth, as well as the interstellar medium, is driven by the effect of ultraviolet radiation on ice surfaces and on the materials trapped within them. While the area of ice photochemistry is vast and much research has been completed, it has only recently been possible to study the dynamics of these processes on a microscopic level. One of the leading techniques for studying photoreaction dynamics is Velocity Map Imaging (VMI). This technique has been used extensively to study several types of reaction dynamics processes. Although the majority of these studies have utilized molecular beams as the main medium for reactants, new studies showed the versatility of the technique when applied to molecular dynamics of molecules adsorbed on metal surfaces. Herein the development of a velocity map imaging apparatus capable of studying the photochemistry of condensed phase materials is described. The apparatus is used to study of the photo-reactivity of NO2 condensed within argon matrices to illustrate its capabilities. A doped ice surface is formed by condensing Ar and NO2 gas onto a sapphire rod which is cooled using a helium compressor to 20 K. The matrix is irradiated using an Nd:YAG laser at 355 nm, and the resulting NO fragment is state-selectively ionized using an excimer-pumped dye laser. In all, we are able to detect transient photochemically generated species and can collect information on their quantum state and kinetic energy distribution. It is found that the REMPI spectra changes as different sections of the dissociating cloud are probed. The rotational and translational energy populations are found to be bimodal with a low temperature component roughly at the temperature of the matrix, and a second component with much higher temperature, the rotational temperature showing a possible population inversion, and the translational temperature of 100-200 K. The low temperature translational component is found to dominate at long delay times between dissociation and ionization, while at short time delays the high temperature component plays a larger role. The velocity map imaging technique allows for the detection of both the axial and radial components of the translational energy. The distribution of excess energy over the rotational, electronic and translational states of the NO photofragments provides evidence for collisional quenching of the fragments in the Ar-matrix prior to their desorption.

Photochemical dynamics of laser-irradiated semiconductor nanostructures

Thesis (Ph.D.)--University of Washington, 2016-08

Morphology and structure of particles produced by femtosecond laser ablation of fused silica

The aim of the present work was to study the morphology and structure of the nanoparticles produced by femtosecond laser ablation of fused silica. Ultrashort laser pulses of 1030 nm wavelength and 550 fs duration were tightly focused by a high numerical aperture microscope objective at the surface of fused silica samples while scanning the sample in relation to the stationary laser beam. Laser tracks were created with pulse energies in the range 5-100 mu J, resulting in ablation debris of different morphologies. The debris were examined by scanning and transmission electron microscopy for their morphology and crystal structure in relation to the incident laser pulse energy. Ejected particles with sizes ranging from a few nanometers to a few microns were found. Their morphologies can be broadly classified into three categories: very fine round nanoparticles with diameters lower than 20 nm, nanoparticles with intermediate sizes between 50 and 200 nm, and big irregular particles with typical size between 0.5 and 1.5 mu m. The fine nanoparticles of the first category are predominantly observed at higher pulse energies and tend to aggregate to form web-like and arborescent-like structures. The nanoparticles with intermediate sizes are observed for all pulse energies used and may appear isolated or aggregated in clusters. Finally, the larger irregular particles of the third category are observed for all energies and appear normally isolated.

Laser ablation-based one-step generation and bio-functionalization of gold nanoparticles conjugated with aptamers

Background: Bio-conjugated nanoparticles are important analytical tools with emerging biological and medical applications. In this context, in situ conjugation of nanoparticles with biomolecules via laser ablation in an aqueous media is a highly promising one-step method for the production of functional nanoparticles resulting in highly efficient conjugation. Increased yields are required, particularly considering the conjugation of cost-intensive biomolecules like RNA aptamers. Results: Using a DNA aptamer directed against streptavidin, in situ conjugation results in nanoparticles with diameters of approximately 9 nm exhibiting a high aptamer surface density (98 aptamers per nanoparticle) and a maximal conjugation efficiency of 40.3%. We have demonstrated the functionality of the aptamer-conjugated nanoparticles using three independent analytical methods, including an agglomeration-based colorimetric assay, and solid-phase assays proving high aptamer activity. To demonstrate the general applicability of the in situ conjugation of gold nanoparticles with aptamers, we have transferred the method to an RNA aptamer directed against prostate-specific membrane antigen (PSMA). Successful detection of PSMA in human prostate cancer tissue was achieved utilizing tissue microarrays. Conclusions: In comparison to the conventional generation of bio-conjugated gold nanoparticles using chemical synthesis and subsequent bio-functionalization, the laser-ablation-based in situ conjugation is a rapid, one-step production method. Due to high conjugation efficiency and productivity, in situ conjugation can be easily used for high throughput generation of gold nanoparticles conjugated with valuable biomolecules like aptamers.

BARIUM CONCENTRATIONS IN ROCK SALT BY LASER INDUCED BREAKDOWN SPECTROSCOPY

Time-REsolved Laser Induced Breakdown Spectroscopy (TRELIBS) was used to determine the elemental concentration of barium in Texas Dome rock salt. TRELIBS allows for an efficient and in situ concentration analysis technique that detects a wide range of elements with no sample preparation. TRELIBS measurements were made in the 545nm to 594nm wavelength range. The proximity of a strong barium emission line (553.5481 nm) to the sodium doublet (588.9950 nm and 589.5924 nm) allowed for measurement within a single frame of the spectrograph. This barium emission line was compared to the sodium doublet for relative intensity. A homemade calibration sample containing known amounts of barium and sodium was used to determine the relative concentrations. By approximating the sodium content in the rock salt as 50%, we determined the absolute concentration of barium in the salt to be (0.13±0.03)%.

Study of nanostructured targets for plasma production via laser ablation

Metal nanowires (NWs) - nanostructures 20-100 nm in diameter and up to tens of micrometers long - behave as waveguides when irradiated with light with wavelength much greater than their diameter. This is due to collective excitations of free electrons (plasmons) in the metal which couple to light and travel on the surface of the nanowire. This effect can be used to efficiently absorb laser pulses to produce dense and hot plasma on special nanostructured targets with metal nanowires vertically aligned on the surface. In this thesis work, nanostructured targets with different parameters (length, diameter, metal and fabrication process) have been irradiated with infrared laser light. X-ray flux emitted by the cooling plasma is measured during irradiation, and the depth of craters formed on the target is measured later. This data is used to choose which target parameters are best for plasma production. Different targets are compared with each other and against a control, non-nanostructured (bulk) target. As will be shown, highly significant (> 5 sigma) differences are found between targets with different nanostructures, and between nanostructured and bulk target. This differences are very difficult to explain whithout accounting for the nanostructures in the targets. Therefore, data collected and analized in this thesis work supports the hypotesys that nanostructured targets perform better than bulk targets for laser plasma production purposes, and provides useful indications for optimization of NWS' parameters.

Switchable dual-wavelength erbium-doped fibre laser utilizing two-channel fibre Bragg grating fabricated by femtosecond laser

We propose and demonstrate a switchable dual-wavelength erbium-doped fibre ring laser. Competition between the lasing wavelengths in erbium-doped fibre laser at room temperature is suppressed by incorporating a two-channel fibre Bragg grating (TC-FBG), which consists of two highly localized sub-gratings fabricated by femtosecond laser in single mode fibre. Wavelengths and polarization states of the lasing lines are selected by the TC-FBG. Laser output can be switched between single- and dual-wavelength operations by simply adjusting the polarization controller. Stable dual-wavelength output is verified at room temperature with a power fluctuation less than 0.27 dB, and wavelength fluctuation less than 0.004 nm.

Multi-kilowatt peak power nanosecond Er-doped fiber laser

We report a two-stage diode-pumped Er-doped fiber amplifier operating at the wavelength of 1550 nm at the repetition rate of 10-100 kHz with an average output power of up to 10 W. The first stage comprising Er-doped fiber was core-pumped at the wavelength of 1480 nm, whereas the second stage comprising double-clad Er/Yb-doped fiber was clad-pumped at the wavelength of 975 nm. The estimated peak power for the 0.4-nm full-width at half-maximum laser emission at the wavelength of 1550 nm exceeded 4-kW level. The initial 100-ns seed diode laser pulse was compressed to 3.5 ns as a result of the 34-dB total amplification. The observed 30-fold efficient pulse compression reveals a promising new nonlinear optical technique for the generation of high power short pulses for applications in eye-safe ranging and micromachining.