In condensed matter physics, ultrafast photoexcitation has been shown to result in modification of macroscopic material properties, sometimes involving phase changes, on a subpicosecond time scale. In semiconductors, irreversible non-thermal solid-to-liquid structural transitions have been demonstrated at high laser fluences.
In the pump-probe experiments reported here, we observe a striking continuously varying low-fluence pump-induced time-dependent structural symmetry modification in intrinsic gallium arsenide (GaAs) using a probe that produces femtosecond polarization-resolved second harmonic generation (f-PRSHG) data. SHG spectroscopy is particularly suited to monitor symmetry changes since its magnitude is governed by the nonlinear optical susceptibility tensor whose elements are determined by the underlying material symmetry. Conceptually, these experiments seek to provide insight into the details of the time evolution of symmetry arising from laser induced transient states of matter in GaAs. Overall, the basic explanation of these experimental observations is that as a result of the photoinduced electronic excitation, many electrons, including bond electrons are excited to higher states. This results in subpicosecond changes in the local anharmonic potential and produces a changing nonlinear polarization response thus accounting for the nonthermal time dependent symmetry changes. Clearly, our approach may be easily extended to many different crystalline materials with different levels of defects, dopants and stresses to fully characterize the time dependent behavior of laser induced transient states in material systems.
Second harmonic generation (SHG) laser spectroscopy has been demonstrated to be a powerful, sensitive,
and non-destructive analytical technique to study crystalline phases, domain structures, and molecular dipole
orientations of ferroelectric polymeric thin films such as PVDF. While other spectroscopic techniques, such as
WXRD and FTIR, do provide valuable information on the crystalline phases, they are not sensitive enough to
provide the detailed information at molecular levels and properties at interfaces. The current study of single layered
PVDF polymer has also shown that SHG can be further developed into an in-situ, sensitive and quantitative tool to
study ferroelectric polymeric thin film structures. In combination, SHG and electric field induced SHG (EFISH)
techniques will allow us to interrogate multilayered structures layer-by-layer, the effects of physical confinement
and interfacial physics.
We review recent experiments on spin excitation and manipulation in the ferromagnetic semiconductor GaMnAs. Spin
dynamics in GaMnAs have been studied by two complementary approaches - by frequency-domain techniques, such as
Brillouin light scattering (BLS) and ferromagnetic resonance (FMR); and by optical real-time techniques, such as
ultrafast pump-probe magneto-optical spectroscopy. Using BLS and FMR, magnon frequencies (or resonance fields),
were investigated as a function of Mn concentration, temperature and direction of magnetization, leading to information
on magnetic anisotropy. Time-resolved magneto-optical Kerr effect, on the other hand, was used to study photo-induced
femtosecond magnetization rotation, ultrafast optical demagnetization, and collective magnetization precession.
Optically-induced transient changes in magnetization of GaMnAs produced by femtosecond laser pulses are analyzed
and discussed in terms of the Landau-Lifshitz-Gilbert model. Finally, for completeness, we also discuss carrier-mediated
nonthermal and thermal (lattice-heating) contributions to spin dynamics.
KEYWORDS: Absorption, Transmittance, Germanium, Laser damage threshold, Free electron lasers, Infrared radiation, FT-IR spectroscopy, High power lasers, Mid-IR, Laser energy
We have observed and characterized wavelength-dependent laser damage thresholds in crystalline germanium induced
by trains of high-power infrared picosecond laser pulses at wavelengths ranging from 2.8 μm to 5.2 μm, using the
Vanderbilt Free-Electron Laser. In this wavelength range, photon energies are well below the band-gap energy. As the
wavelength is increased, threshold fluences are observed to increase by a factor of five over the studied wavelength
range. Two- and three- photon absorption is the predominant photon energy absorption mechanism up to 4.4 μm. At
wavelengths above 4.8 μm tunnel absorption appears to be the primary absorption mechanism. Wavelength and fluence
dependent transmission and reflection measurements provide valuable insight into the nature of the damage mechanisms.
We report comprehensive temperature and photoexcitation intensity dependent studies of the photoinduced
magnetization precession in Ga1-xMnxAs (x = 0.035) by time-resolved Kerr rotation measurements. We observe coherent
oscillations of local Mn spins triggered by an ultrafast photo-induced reorientation of the easy axis due to changes in the
magnetic anisotropy. The amplitude saturation of these oscillations above certain pump intensity is indicative of
stabilization of the magnetic easy axis orientation on temperatures above ~Tc/2. We find that the observed magnetization
precession damping (Gilbert damping) is strongly dependent on pump laser intensity, but largely independent of ambient
temperature.
Femtosecond optical reflectivity measurements of La2-xSrxCuO4, La2CuO4+y, Bi2Sr2CuO6+z and Bi2Sr2CaCu2O8+δ thin films and single crystal samples indicate qualitative changes with fluence. At the lowest fluencies, there is a power law divergence in the relaxation time. The divergence has an onset temperature of 55±15K, independent of whether the sample is in the superconducting or normal states. At slightly higher fluencies, still perturbative, the additional response does not exhibit this power law divergence. At quite high fluencies- no longer perturbative- the metallic samples exhibit oscillations in the reflectivity amplitude. The period of these oscillations varies with the probe wavelength but not with the pump wavelength. The oscillations exhibit a decay time as long as 10 nsec.
We report first IR free-electron laser experiments to compare and elucidate the effects of surface-localized vibrational excitation versus bulk vibrational excitation on the ablation of polycrystalline diamond. The measured ablation yield values as a function of laser intensity indicate the existence of two separate thresholds. The lower intensity thresholds is identified as the ablation threshold, and the higher intensity threshold is associated with the formation of a plasma plume. The wavelength dependences of both thresholds indicate that eh C-H absorption occurring at surfaces and grain boundaries does not play a significant role in the ablation process. However, both thresholds are lower when the laser is resonant with the two-phonon bulk absorption band. These findings are consistent with the model that a rapid laser- induced phase transition to graphite is responsible for the low-intensity ablation of diamond at and above the first threshold.
David Schaafsma, Reza Mossadegh, Jasbinder Sanghera, Ishwar Aggarwal, M. Luce, Renato Generosi, P. Perfetti, Antonio Cricenti, Jonathan Gilligan, Norman Tolk
KEYWORDS: Near field scanning optical microscopy, Chalcogenides, Free electron lasers, Fiber lasers, Near field optics, Infrared microscopy, Infrared radiation, Optical microscopy, Absorption, Spatial resolution
We consider the denaturation process as an alteration in ordered organization of tissue structure and study the threshold and kinetics of laser-induced denaturation in cartilage and cornea undergoing irradiation from a free electron laser (FEL) in the wavelength range 2.2 - 8.5 (mu) . Light-scattering by cartilage samples was measured in real- time during FEL irradiation using a 630-nm diode laser and a diode array with time resolution of 10 ms. We found that denaturation threshold is slightly lower than that for cartilage, and both depend on laser wavelength. A strong inverse correlation between denaturation thresholds and the absorption spectrum of the tissue is observed. Only for the wavelength region near the 3 (mu) water absorption band was the denaturation threshold not inversely proportional to the absorption coefficient. We believe this was because the radiation penetration depth was very small in this high- absorption region, so tissue denaturation occurred only in a layer too thin to produce significant light scattering. ATR spectra of 2.4 mm thick cartilage samples was measured before and after irradiation at 6.0 and 2.2 (mu) . At 6.0 (mu) , where the absorption is high, the spectrum of the irradiated (front) surface showed changes, while the spectrum of the back surface was identical to that before irradiation. This difference results from dramatic denaturation (with chemical bond breaking) at the front surface due to laser heating in a small absorption depth. For 2.2 (mu) irradiation, where the absorption is small, the spectra of the front and back of the irradiated sample were unchanged from before irradiation, while light scattering alteration shown the denaturation process began, for laser fluences above the denaturation threshold. This indicates that the absorption is too small to produce deep denaturation of the tissue with dramatic alteration of structure. Thus, we have shown that light scattering is useful for measuring denaturation thresholds and kinetics for biotissues except where the initial absorptivity is very high.
Pulsed IR laser ablation on dental hard substances was studied in the wavelength range between 9.5 and 11.5 micrometers with the Free-Electron Laser (FEL) in Nieuwegein/NL and between 6.0 and 7.5 micrometers with the FEL at Vanderbilt University in Nashville/TN. Depth, diameter and volume of the ablation crater were determined with a special silicon replica method and subsequent confocal laser topometry. The irradiated surfaces and the ejected debris were examined with an SEM 9.5 - 11.5 micrometers : depth, diameter and volume of the ablation crater are greater and the ablation threshold is lower for ablation with a wavelength corresponding to the absorption max. of hydroxyapatite (9.5 micrometers ), compared to ablation at wavelengths with lower absorption (10.5 - 11.5 micrometers ). For all wavelengths, no thermal cracking can be observed after ablation in dentine, however a small amount of thermal cracking can be observed after ablation in enamel. After ablation at 9.5 micrometers , a few droplets of solidified melt were seen on the irradiated areas, whereas the debris consisted only of solidified melt. In contrast, the surface and the debris obtained from ablation using the other wavelengths showed the natural structure of dentine 6.0 - 7.5 micrometers : the depth of the ablation crater increases and the ablation threshold decreases for an increasing absorption coefficient of the target material. Different tissue components absorbed the laser radiation of different wavelengths (around 6.0 micrometers water and collagen, 6.5 micrometers collagen and water, 7.0 micrometers carbonated hydroxyapatite). Nevertheless the results have shown no major influence on the primary tissue absorber.
Carlo Coluzza, J. Almeida, E. Tuncel, Jean Staehli, P. Baudat, Giorgio Margaritondo, Jim McKinley, Akira Ueda, Alan Barnes, Royal Albridge, Norman Tolk, D. Martin, Francois Morier-Genoud, C. Dupuy, Alok Rudra, Marc Ilegems
We used optical pumping by the Vanderbilt Free Electron Laser and the technique of internal photoemission to measure with high accuracy the conduction band discontinuity of semiconductor heterojunction interfaces. The experiment is the first application of a free- electron laser to interface research.
In this paper we examine the use of a high-power, tunable free-electron laser (FEL) source to measure photoluminescence (PL) and photoluminescence excitation (PLE) spectra in two classes of disordered semiconductors, amorphous semiconductors and partially ordered III-V ternary semiconductors. The source must be tunable to follow the absorption continuously across the region of the optical energy gap, and the source must be of high power to provide enough absorbed photons in this relatively transparent spectral region so that PL processes can be measured. The usefulness of PLE spectroscopy in these semiconducting thin films lies in the fact that if the quantum efficiency (eta) for the PL process is independent of energy, then the PLE spectrum is a measure of the optical absorption. In addition, disordered semiconductors often exhibit enhanced absorption below the optical gap due to the disorder itself. PLE measurements that probe regions where the absorption coefficient (alpha) is small ((alpha) < < 103 cm-1) are most important because in these regions (alpha) is dominated by the electronic states introduced by the disorder.
Norman Tolk, Royal Albridge, Alan Barnes, Jim McKinley, H. Nielsen, Akira Ueda, J. Smith, Jeffrey Davidson, M. Languell, Carlo Coluzza, E. Tuncel, Giorgio Margaritondo
This paper describes the results of novel experiments made possible by the recently commissioned Vanderbilt Free-Electron Laser (VU-FEL_, the brightest tunable midinfrared FEL in the world. We emphasize two classes of experiments, novel semiconductor spectroscopies and wavelength-dependent laser ablation studies. Both take advantage of the high brightness and the tunability of the FEL. We have recently demonstrated the feasibility of measuring semiconductor heterojunction band discontinuities using the internal photoemission (IPE) technique and report the results for the cases of GaAs/GaAlAs and a-Ge/GaAs. The basic physical mechanism of IPE is that a photocurrent is produced by optically pumping electrons over the conduction band discontinuity (Delta) Ec. A photocurrent threshold is observed when the photon energy exceeds (Delta) Ec. Because IPE is optical in nature, (Delta) Ec can be determined with unprecedented accuracy (5 meV). By comparison, the best known direct method of measuring band discontinuities (UPS or XPS) achieves accuracies of only 100 meV.
The SUMMA International Research Institute has been established to develop advanced technology in the civilian and military sectors. An initial program of the Institute is a radiation test facility operating in conjunction with the Vanderbilt University Free Electron Laser (FEL).
The incidence of energetic photons, electrons, and heavy particles on surfaces of optical components leads to the generation of surprisingly intense radioluminescence which may interfere with sensor performance. This research focuses on the ways in which energy is deposited by incident electrons leading to fluorescence, bond-making and bond-breaking processes on surfaces and in the near-surface bulk. Knowledge of these microscopic mechanisms provides detailed clues which lead to an understanding of macroscopic processes, such as surface glow, materials modification and darkening. We describe progress in ongoing studies to determine the influence of substrate material, temperature, and cryolayer species on the intensity and the decay time of electron-induced glow, and the related phenomena leading to darkening, of optical components. Emphasis is on the identification of mechanisms responsible for both glow and darkening.
Sputtering yield measurements, which help to quantify the rate at which erosion occurs, were made for low-energy beams (50 - 200 eV) of O+, O2+, N+, and N2+ incident on Al, and Al2O3 surfaces. These materials are likely candidates for exterior portions of Space Station Freedom's power generation system. Potential differences produced by the power generation system (possibly as high as 300 volts) would accelerate the ions in the surrounding plasma to energies well above the sputtering threshold. Atomic oxygen and molecular nitrogen interactions with surfaces play a critical role in surface erosion and space glow that occur for exposed materials in a low-earth orbit. As much as 90% of the atmosphere at these altitudes is comprised of atomic oxygen which is more abundant than the molecular form since the molecular form is quickly dissociated by UV radiation. Mass-loss measurements were conducted using samples that were vacuum deposited on the surface of a quartz crystal and a novel technique was utilized to increase the sensitivity of the quartz crystal microbalance which was used to measure the mass loss.
The newly commissioned Vanderbilt Free Electron Laser Center for Biomedical and Materials Research is a multidisciplinary users facility intended as an international resource. It provides extremely intense, continuously tunable, pulsed radiation in the mid-infrared (2-10 j.tm). Projects already underway include the linear and nonlinear interaction of laser radiation with optical materials, semiconductors, and mammalian tissue, the spectroscopy of species adsorbed on surfaces, measurement of vibrational energy transfer in DNA and RNA, the dynamics of proteins in cell membranes, the biomodulation of wound healing by lasers, image-guided stereotactic neurosurgery, and the use of monochromatic X-rays in medical imaging and therapy. The purpose of this article is to introduce the machine to the user community and to describe some of the new experimental opportunities that it makes possible. Details of several research projects are presented.
Measurements of optical spectra of surfaces undergoing bombardment by N2 and N2+ jfl an ultrahigh vacuum environment provide information related to the origin of spacecraft glow and erosion. This work is complimentary to other measurements also carried out in our laboratory in which we utilize 0 and 0+ beams . These. efforts are part of a broad program whose goal is the understanding of interactions between surfaces and low-energy charged and neutral particles. 1.
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