APPLICATION OF JET REMPI AND LIBS TO AIR TOXIC MONITORING

EPA Science Inventory

The paper discusses three advanced, laser-based monitoring techniques that the EPA is assisting in developing for real time measurement of toxic aerosol compounds. One of the three techniques is jet resonance enhanced multiphoton ionization (Jet REMPI) coupled with a time-of-flig...

WAVELENGTH-RESOLVED REMPI MASS SPECTROMETRY FOR THE MONITORING OF TOXIC INCINERATION TRACE GASES

EPA Science Inventory

Structure-selective measurement techniques are needed for the assessment of the toxic loading of incinerator gases. This review article shows that wavelength-resolved, resonance-enhanced, multiphoton- ionization (REMPY) mass spectrometry can be used to this end. In this case, how...

Ionic rotational branching ratios in resonant enhanced multiphoton ionization of NO via the A2Sigma(+)(3s sigma) and D2Sigma(+)(3p sigma) states

NASA Technical Reports Server (NTRS)

Rudolph, H.; Mckoy, V.; Dixit, S. N.; Huo, W. M.

1988-01-01

Results are presented for the rotationally resolved photoelectron spectra resulting from a (2 + 1) one-color resonant enhanced multiphoton ionization (REMPI) of NO via the rotationally clean S21(11.5) and mixed S11(15.5) + R21(15.5) branches of the 0-0 transition in the D-X band. The calculations were done in the fixed-nuclei frozen core approximation. The resulting photoionization spectra, convoluted with a Lorentzian detection function, agree qualitatively with experimental results of Viswanathan et al. (1986) and support their conclusion that the nonspherical nature of the molecular potential creates a substantial l-mixing in the continuum, which in turn leads to the intense Delta N = 0 peak. The rather strong photoelectron energy dependence of the rotational branching ratios of the D 2Sigma(+) S21(11.5) line was investigated and compared to the weak energy dependence of the A 2Sigma(+) R22(21.5) line.

Spatially resolved measurement of singlet delta oxygen by radar resonance-enhanced multiphoton ionization.

PubMed

Wu, Yue; Zhang, Zhili; Ombrello, Timothy M

2013-07-01

Coherent microwave Rayleigh scattering (Radar) from resonance-enhanced multiphoton ionization (REMPI) was demonstrated to directly and nonintrusively measure singlet delta oxygen, O(2)(a(1)Δ(g)), with high spatial resolution. Two different approaches, photodissociation of ozone and microwave discharge plasma in an argon and oxygen flow, were utilized for O(2)(a(1)Δ(g)) generation. The d(1)Π(g)←a(1)Δ(g) (3-0) and d(1)Π(g)←a(1)Δ(g) (1-0) bands of O(2)(a(1)Δ(g)) were detected by Radar REMPI for two different flow conditions. Quantitative absorption measurements using sensitive off-axis integrated cavity output spectroscopy (ICOS) was used simultaneously to evaluate the accuracy and sensitivity of the Radar REMPI technique. The detection limit of Radar REMPI was found to be comparable to the ICOS technique with a detection threshold of approximately 10(14) molecules/cm(3) but with a spatial resolution that was 8 orders of magnitude smaller than the ICOS technique.

Measurements of trap dynamics of cold OH molecules using resonance-enhanced multiphoton ionization

NASA Astrophysics Data System (ADS)

Gray, John M.; Bossert, Jason A.; Shyur, Yomay; Lewandowski, H. J.

2017-08-01

Trapping cold, chemically important molecules with electromagnetic fields is a useful technique to study small molecules and their interactions. Traps provide long interaction times, which are needed to precisely examine these low-density molecular samples. However, the trapping fields lead to nonuniform molecular density distributions in these systems. Therefore, it is important to be able to experimentally characterize the spatial density distribution in the trap. Ionizing molecules at different locations in the trap using resonance-enhanced multiphoton ionization (REMPI) and detecting the resulting ions can be used to probe the density distribution even at the low density present in these experiments because of the extremely high efficiency of detection. Until recently, one of the most chemically important molecules, OH, did not have a convenient REMPI scheme identified. Here, we use a newly developed 1 +1' REMPI scheme to detect trapped cold OH molecules. We use this capability to measure the trap dynamics of the central density of the cloud and the density distribution. These types of measurements can be used to optimize loading of molecules into traps, as well as to help characterize the energy distribution, which is critical knowledge for interpreting molecular collision experiments.

DEVELOPMENT OF A JET-REMPI (RESONANTLY ENHANCED MULTIPHOTON IONIZATION) CONTINUOUS MONITOR FOR ENVIRONMENTAL APPLICATIONS. (R827927)

EPA Science Inventory

The perspectives, information and conclusions conveyed in research project abstracts, progress reports, final reports, journal abstracts and journal publications convey the viewpoints of the principal investigator and may not represent the views and policies of ORD and EPA. Concl...

Monitoring of Hazardous Air Pollutant Surrogates Using Resonance Enhanced Multiphoton Ionization/Time of Flight Mass Spectrometry

EPA Science Inventory

EPA’s preferred approach for regulatory emissions compliance is based upon real-time monitoring of individual hazardous air pollutants (HAPs). Real-time, continuous monitoring not only provides the most comprehensive assurance of emissions compliance, but also can serve as...

Modeling of the initiation and evolution of a laser-ionized column in the lower atmosphere - 314.5 nm wavelength resonant multiphoton ionization of naturally occurring argon

NASA Technical Reports Server (NTRS)

Fetzer, G. J.; Stockley, J. E.

1992-01-01

A 3+1 resonant multiphoton ionization process in naturally occurring argon is studied at 314.5 nm as a candidate for providing a long ionized channel through the atmosphere. Results are presented which indicate peak electron densities up to 10 exp 8/cu cm can be created using laser intensities on the order of 10 exp 8 W/sq cm.

Photoelectron circular dichroism of bicyclic ketones from multiphoton ionization with femtosecond laser pulses.

PubMed

Lux, Christian; Wollenhaupt, Matthias; Sarpe, Cristian; Baumert, Thomas

2015-01-12

Photoelectron circular dichroism (PECD) is a CD effect up to the ten-percent regime and shows contributions from higher-order Legendre polynomials when multiphoton ionization is compared to single-photon ionization. We give a full account of our experimental methodology for measuring the multiphoton PECD and derive quantitative measures that we apply on camphor, fenchone and norcamphor. Different modulations and amplitudes of the contributing Legendre polynomials are observed despite the similarity in chemical structure. In addition, we study PECD for elliptically polarized light employing tomographic reconstruction methods. Intensity studies reveal dissociative ionization as the origin of the observed PECD effect, whereas ionization of the intermediate resonance is dominating the signal. As a perspective, we suggest to make use of our tomographic data as an experimental basis for a complete photoionization experiment and give a prospect of PECD as an analytic tool. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Field enhancement of multiphoton induced luminescence processes in ZnO nanorods

NASA Astrophysics Data System (ADS)

Hyyti, Janne; Perestjuk, Marko; Mahler, Felix; Grunwald, Rüdiger; Güell, Frank; Gray, Ciarán; McGlynn, Enda; Steinmeyer, Günter

2018-03-01

The near-ultraviolet photoluminescence of ZnO nanorods induced by multiphoton absorption of unamplified Ti:sapphire pulses is investigated. Power dependence measurements have been conducted with an adaptation of the ultrashort pulse characterization method of interferometric frequency-resolved optical gating. These measurements enable the separation of second harmonic and photoluminescence bands due to their distinct coherence properties. A detailed analysis yields fractional power dependence exponents in the range of 3-4, indicating the presence of multiple nonlinear processes. The range in measured exponents is attributed to differences in local field enhancement, which is supported by independent photoluminescence and structural measurements. Simulations based on Keldysh theory suggest contributions by three- and four-photon absorption as well as avalanche ionization in agreement with experimental findings.

Determination of polycyclic aromatic hydrocarbons and their nitro-, amino-derivatives absorbed on particulate matter 2.5 by multiphoton ionization mass spectrometry using far-, deep-, and near-ultraviolet femtosecond lasers.

PubMed

Tang, Yuanyuan; Imasaka, Tomoko; Yamamoto, Shigekazu; Imasaka, Totaro

2016-06-01

Multiphoton ionization processes of parent-polycyclic aromatic hydrocarbons (PPAHs), nitro-PAHs (NPAHs), and amino-PAHs (APAHs) were examined by gas chromatography combined with time-of-flight mass spectrometry using a femtosecond Ti:sapphire laser as the ionization source. The efficiency of multiphoton ionization was examined using lasers emitting in the far-ultraviolet (200 nm), deep-ultraviolet (267 nm), and near-ultraviolet (345 nm) regions. The largest signal intensities were obtained when the far-ultraviolet laser was employed. This favorable result can be attributed to the fact that these compounds have the largest molar absorptivities in the far-ultraviolet region. On the other hand, APAHs were ionized more efficiently than NPAHs in the near-ultraviolet region because of their low ionization energies. A sample extracted from a real particulate matter 2.5 (PM2.5) sample was measured, and numerous signal peaks arising from PAH and its analogs were observed at 200 nm. On the other hand, only a limited number of signed peaks were observed at 345 nm, some of which were signed to PPAHs, NPAHs, and APAHs. Thus, multiphoton ionization mass spectrometry has potential for the use in comprehensive analysis of toxic environmental pollutants. Copyright © 2016 Elsevier Ltd. All rights reserved.

Photoelectron circular dichroism in different ionization regimes

NASA Astrophysics Data System (ADS)

Wollenhaupt, Matthias

2016-12-01

Photoelectron circular dichroism (PECD) describes an asymmetry in the photoelectron angular distribution (PAD) from photoionization of randomly oriented enantiomers with circularly polarized light. Beaulieu et al present a comprehensive set of measured PADs from multiphoton ionization of limonene and fenchone in different ionization regimes (multiphoton and tunneling) and analyze the resulting PECD (Beaulieu et al 2016 New J. Phys. 18 102002). From their observations the authors conclude that the PECD is universal in the sense that the molecular chirality is encoded in the PAD independent of the ionization regime. The analysis is supplemented by a classical model based on electron scattering in a chiral potential. The paper presents beautiful data and is an important step towards a more complete physical picture of PECD. The results and their interpretation stimulate the ongoing vivid debate on the role of resonances in multiphoton PECD.

The 700-1500 cm{sup −1} region of the S{sub 1} (A{sup ~1}B{sub 2}) state of toluene studied with resonance-enhanced multiphoton ionization (REMPI), zero-kinetic-energy (ZEKE) spectroscopy, and time-resolved slow-electron velocity-map imaging (tr-SEVI) spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gardner, Adrian M.; Green, Alistair M.; Tamé-Reyes, Victor M.

We report (nanosecond) resonance-enhanced multiphoton ionization (REMPI), (nanosecond) zero-kinetic-energy (ZEKE) and (picosecond) time-resolved slow-electron velocity map imaging (tr-SEVI) spectra of fully hydrogenated toluene (Tol-h{sub 8}) and the deuterated-methyl group isotopologue (α{sub 3}-Tol-d{sub 3}). Vibrational assignments are made making use of the activity observed in the ZEKE and tr-SEVI spectra, together with the results from quantum chemical and previous experimental results. Here, we examine the 700–1500 cm{sup −1} region of the REMPI spectrum, extending our previous work on the region ≤700 cm{sup −1}. We provide assignments for the majority of the S{sub 1} and cation bands observed, and in particular wemore » gain insight regarding a number of regions where vibrations are coupled via Fermi resonance. We also gain insight into intramolecular vibrational redistribution in this molecule.« less

Spectroscopic study of N2(b1Πu, ν = 8) by atmospheric-pressure resonant-enhanced multiphoton ionization and fluorescence detection.

PubMed

Adams, Steven F; Williamson, James M

2013-12-19

A spectroscopic analysis of the strongly perturbed N2(b(1)Πu, ν = 8) state has been conducted, accounting for b(1)Πu(ν = 8) ← X (1)Σg(+)(ν = 0) transitions, for the first time, up to J' = 20. A novel laser spectroscopy technique, using a combination of resonant-enhanced multiphoton ionization and fluorescence detection at atmospheric pressure, avoids the severe effects of perturbation reported in past extreme vacuum ultraviolet absorption experiments that produced weak and unusable spectra for the ν = 8 level. The R, Q, and P branches of the three-photon absorption transition b(1)Πu(ν = 8) ← X(1)Σg(+)(ν = 0) were fit, allowing rotational term energy assignment up to J' = 20 and molecular constants to be determined. Evidence of the previously suspected perturbation in b(1)Πu(ν = 8) is clear in this data, with significant Λ-type doubling at higher J' along with an anomalous negative value determined for the centrifugal distortion coefficient.

Effects of the Carrier-Envelope Phase in the Multiphoton Ionization Regime

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nakajima, Takashi; Institute for Solid State Physics, University of Tokyo, 5-1-5 Kashiwanoha, Kashiwa, Chiba 277-8581; Watanabe, Shuntaro

2006-06-02

We theoretically investigate the effects of the carrier-envelope phase of few-cycle laser pulses in the multiphoton ionization regime. For atoms with low ionization potential, total ionization yield barely exhibits phase dependence, as expected. However, population of some bound states clearly shows phase dependence. This implies that the measurement of the carrier-envelope phase would be possible through the photoemission between bound states without energy-and-angle-resolved photoelectron detection. The considered scheme could be particularly useful to measure the carrier-envelope phase for a light source without an amplifier, such as a laser oscillator, which cannot provide sufficient pulse energy to induce tunneling ionization.

The generation of a tunable laser emission in the vacuum ultraviolet and its application to supersonic jet/multiphoton ionization mass spectrometry

NASA Astrophysics Data System (ADS)

Uchimura, Tomohiro; Onoda, Takayuki; Lin, Cheng-Huang; Imasaka, Totaro

1999-08-01

An optical parametric oscillator and a Ti:sapphire laser are used as a pump source for the generation of high-order vibrational stimulated Raman emission in the vacuum ultraviolet region. This tunable laser is employed as an excitation/ionization source in a supersonic jet/multiphoton ionization/time-of-flight mass spectrometric study of benzene. The merits and potential advantages of this approach are discussed in this study.

REAL-TIME EMISSION CHARACTERIZATION OF ORGANIC AIR TOXIC POLLUTANTS DURING STEADY STATE AND TRANSIENT OPERATION OF A MEDIUM DUTY DIESEL ENGINE

EPA Science Inventory

An on-line monitoring method, jet resonance-enhanced multi-photon ionization (REMPI) with time-of-flight mass spectrometry (TOFMS) was used to measure emissions of organic air toxics from a medium-duty (60 kW)diesel generator during transient and steady state operations. Emission...

A velocity-map imaging study of methyl non-resonant multiphoton ionization from the photodissociation of CH3I in the A-band

PubMed Central

Poullain, Sonia Marggi; Chicharro, David V.; Rubio-Lago, Luis; García-Vela, Alberto

2017-01-01

Chemical reaction dynamics and, particularly, photodissociation in the gas phase are generally studied using pump–probe schemes where a first laser pulse induces the process under study and a second one detects the produced fragments. Providing an efficient detection of ro-vibrationally state-selected photofragments, the resonance enhanced multiphoton ionization (REMPI) technique is, without question, the most popular approach used for the probe step, while non-resonant multiphoton ionization (NRMPI) detection of the products is scarce. The main goal of this work is to test the sensitivity of the NRMPI technique to fragment vibrational distributions arising from molecular photodissociation processes. We revisit the well-known process of methyl iodide photodissociation in the A-band at around 280 nm, using the velocity-map imaging technique in conjunction with NRMPI of the methyl fragment. The detection wavelength, carefully selected to avoid any REMPI transition, was scanned between 325 and 335 nm seeking correlations between the different observables—the product vibrational, translational and angular distributions—and the excitation wavelength of the probe laser pulse. The experimental results have been discussed on the base of quantum dynamics calculations of photofragment vibrational populations carried out on available ab initio potential-energy surfaces using a four-dimensional model. This article is part of the themed issue ‘Theoretical and computational studies of non-equilibrium and non-statistical dynamics in the gas phase, in the condensed phase and at interfaces’. PMID:28320907

Resonance Enhanced Multi-Photon Ionization and Uv-Uv Hole-Burning Spectroscopic Studies of Jet-Cooled Acetanilide Derivatives

NASA Astrophysics Data System (ADS)

Moon, Ceol Joo; Min, Ahreum; Ahn, Ahreum; Lee, Seung Jun; Choi, Myong Yong; Kim, Seong Keun

2013-06-01

Conformational investigations and photochemistry of jet-cooled methacetine (MA) and phenacetine (PA) using one color resonant two-photon ionization (REMPI), UV-UV hole-burning and IR-dip spectroscopy are presented. MA and PA are derivatives of acetanilide, substituted by methoxyl, ethoxyl group in the para position of acetanilide, respectively. Moreover, we have investigated conformational information of the acetanilide derivatives (AAP, MA and PA)-water. In this work, we will present and discuss the solvent effects of the hydroxyl group of acetanilide derivatives in the excited state.

Comparison of the Detection Characteristics of Trace Species Using Laser-Induced Breakdown Spectroscopy and Laser Breakdown Time-of-Flight Mass Spectrometry

PubMed Central

Wang, Zhenzhen; Deguchi, Yoshihiro; Yan, Junjie; Liu, Jiping

2015-01-01

The rapid and precise element measurement of trace species, such as mercury, iodine, strontium, cesium, etc. is imperative for various applications, especially for industrial needs. The elements mercury and iodine were measured by two detection methods for comparison of the corresponding detection features. A laser beam was focused to induce plasma. Emission and ion signals were detected using laser-induced breakdown spectroscopy (LIBS) and laser breakdown time-of-flight mass spectrometry (LB-TOFMS). Multi-photon ionization and electron impact ionization in the plasma generation process can be controlled by the pressure and pulse width. The effect of electron impact ionization on continuum emission, coexisting molecular and atomic emissions became weakened in low pressure condition. When the pressure was less than 1 Pa, the plasma was induced by laser dissociation and multi-photon ionization in LB-TOFMS. According to the experimental results, the detection limits of mercury and iodine in N2 were 3.5 ppb and 60 ppb using low pressure LIBS. The mercury and iodine detection limits using LB-TOFMS were 1.2 ppb and 9.0 ppb, which were enhanced due to different detection features. The detection systems of LIBS and LB-TOFMS can be selected depending on the condition of each application. PMID:25769051

UV and VUV spectroscopy and photochemistry of small molecules in a supersonic jet

NASA Technical Reports Server (NTRS)

Ruehl, E.; Vaida, V.

1990-01-01

UV and VUV absorption and emission spectroscopy is used to probe jet cooled molecules, free radicals, and clusters in the gas phase. Due to efficient cooling inhomogeneous effects on spectral line widths are eliminated. Therefore from these spectra, both structural and dynamical information is obtained. The photoproducts of these reactions are probed by resonance enhanced multiphoton ionization.

Study on the decomposition of trace benzene over V2O5-WO3/TiO2-based catalysts in simulated flue gas

EPA Science Inventory

Commercial and laboratory-prepared V2O5–WO3/TiO2-based catalysts with different compositions were tested for catalytic decomposition of chlorobenzene （ClBz） in simulated flue gas. Resonance enhanced multiphoton ionization-time of flight mass spectrometry (REMPI-TOFMS) was employe...

Development of injector/amplifier XUV lasers and initial studies of ultrashort pulse UV multiphoton ionization

NASA Astrophysics Data System (ADS)

Key, Michael H.; Blyth, W. J.; Cairns, Gerald F.; Damerell, A. R.; Dangor, A. E.; Danson, Colin N.; Evans, J. M.; Hirst, Graeme J.; Holden, M.; Hooker, Chris J.; Houliston, J. R.; Krishnan, J.; Lewis, Ciaran L. S.; Lister, J. M. D.; MacPhee, Andrew G.; Najmudin, Z.; Neely, David; Norreys, Peter A.; Offenberger, Allen A.; Osvay, Karoly; Pert, Geoffrey J.; Preston, S. G.; Ramsden, Stuart A.; Ross, Ian N.; Sibbett, Wilson; Tallents, Gregory J.; Smith, C.; Wark, Justin S.; Zhang, Jie

1994-02-01

An injector-amplifier architecture for XUV lasers has been developed and demonstrated using the Ge XXIII collisional laser. Results are described for injection into single and double plasma amplifiers. Prismatic lens-like and higher order aberrations in the amplifier are considered. Limitations on ultimate brightness are discussed and also scaling to operation at shorter wavelengths. A preliminary study has been made of UV multiphoton ionization using 300 fs pulses at high intensity.

Correlated electron and nuclear dynamics in strong field photoionization of H(2)(+).

PubMed

Silva, R E F; Catoire, F; Rivière, P; Bachau, H; Martín, F

2013-03-15

We present a theoretical study of H(2)(+) ionization under strong IR femtosecond pulses by using a method designed to extract correlated (2D) photoelectron and proton kinetic energy spectra. The results show two distinct ionization mechanisms-tunnel and multiphoton ionization-in which electrons and nuclei do not share the energy from the field in the same way. Electrons produced in multiphoton ionization share part of their energy with the nuclei, an effect that shows up in the 2D spectra in the form of energy-conservation fringes similar to those observed in weak-field ionization of diatomic molecules. In contrast, tunneling electrons lead to fringes whose position does not depend on the proton kinetic energy. At high intensity, the two processes coexist and the 2D plots show a very rich behavior, suggesting that the correlation between electron and nuclear dynamics in strong field ionization is more complex than one would have anticipated.

Observation of novel photochemistry in the multiphoton ionization of Mo(CO) sub 6 van der Waals clusters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Peifer, W.R.; Garvey, J.F.

1989-07-27

van der Waals clusters of Mo(CO){sub 6} generated in the free-jet expansion of a pulsed beam of seeded helium are subjected to multiphoton ionization and the product ions analyzed by quadrupole mass spectrometry. Oxomolybdenum and dioxomolybdenum ions are observed to be produced with high efficiency. This behavior is in striking contrast to that of metal carbonyl monomers and covalently bound cluster carbonyls, which under complete ligand loss prior to ionization. The observed photochemistry is ascribed to reactions between a photoproduced molybdenum atom and the ligands of neighboring Mo(CO){sub 6} solvent molecules within the van der Waals cluster.

Evaluating the Aging of Multiple Emulsions Using Resonance-Enhanced Multiphoton Ionization Time-of-Flight Mass Spectrometry.

PubMed

Tsuda, Yukihiro; Uchimura, Tomohiro

2016-01-01

Resonance-enhanced multiphoton ionization time-of-flight mass spectrometry was applied to measurements of multiple emulsions with no pretreatment; a method for the quantitative evaluation of aging was proposed. We prepared water-in-oil-in-water (W/O/W) multiple emulsions containing toluene and m-phenylenediamine. The samples were measured immediately following both preparation and after having been stirred for 24 h. Time profiles of the peak areas for each analyte species were obtained, and several intense spikes for toluene could be detected from each sample after stirring, which suggests that the concentration of toluene in the middle phase had increased during stirring. On the other hand, in the case of a W/O/W multiple emulsion containing phenol and m-phenylenediamine, spikes for m-phenylenediamine, rather than phenol, were detected after stirring. In the present study, the time-profile data were converted into a scatter plot in order to quantitatively evaluate the aging. As a result, the ratio of the plots where strong signal intensities of toluene were detected increased from 8.4% before stirring to 33.2% after stirring for 24 h. The present method could be a powerful tool for evaluating multiple emulsions, such as studies on the kinetics of the encapsulation and release of active ingredients.

Multi-photon ionization of atoms in intense short-wavelength radiation fields

NASA Astrophysics Data System (ADS)

Meyer, Michael

2015-05-01

The unprecedented characteristics of XUV and X-ray Free Electron Lasers (FELs) have stimulated numerous investigations focusing on the detailed understanding of fundamental photon-matter interactions in atoms and molecules. In particular, the high intensities (up to 106 W/cm2) giving rise to non-linear phenomena in the short wavelength regime. The basic phenomenology involves the production of highly charged ions via electron emission to which both sequential and direct multi-photon absorption processes contribute. The detailed investigation of the role and relative weight of these processes under different conditions (wavelength, pulse duration, intensity) is the key element for a comprehensive understanding of the ionization dynamics. Here the results of recent investigations are presented, performed at the FELs in Hamburg (FLASH) and Trieste (FERMI) on atomic systems with electronic structures of increasing complexity (Ar, Ne and Xe). Mainly, electron spectroscopy is used to obtain quantitative information about the relevance of various multi-photon ionization processes. For the case of Ar, a variety of processes including above threshold ionization (ATI) from 3p and 3s valence shells, direct 2p two-photon ionization and resonant 2p-4p two-photon excitations were observed and their role was quantitatively determined comparing the experimental ionization yields to ab-initio calculations of the cross sections for the multi-photon processes. Using Ar as a benchmark to prove the reliability of the combined experimental and theoretical approach, the more complex and intriguing case of Xe was studied. Especially, the analysis of the two-photon ATI from the Xe 4d shell reveals new insight into the character of the 4d giant resonance, which was unresolved in the linear one-photon regime. Finally, the influence of intense XUV radiation to the relaxation dynamics of the Ne 2s-3p resonance was investigated by angle-resolved electron spectroscopy, especially be observing the intensity dependent variation of the angular distribution patterns for the sequential ionization process.

Resonant- and avalanche-ionization amplification of laser-induced plasma in air

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, Yue; Zhang, Zhili, E-mail: zzhang24@utk.edu; Jiang, Naibo

2014-10-14

Amplification of laser-induced plasma in air is demonstrated utilizing resonant laser ionization and avalanche ionization. Molecular oxygen in air is ionized by a low-energy laser pulse employing (2 + 1) resonance-enhanced multi-photon ionization (REMPI) to generate seed electrons. Subsequent avalanche ionization of molecular oxygen and nitrogen significantly amplifies the laser-induced plasma. In this plasma-amplification effect, three-body attachments to molecular oxygen dominate the electron-generation and -loss processes, while either nitrogen or argon acts as the third body with low electron affinity. Contour maps of the electron density within the plasma obtained in O₂/N₂ and O₂/Ar gas mixtures are provided to showmore » relative degrees of plasma amplification with respect to gas pressure and to verify that the seed electrons generated by O₂ 2 + 1 REMPI are selectively amplified by avalanche ionization of molecular nitrogen in a relatively low-pressure condition (≤100 Torr). Such plasma amplification occurring in air could be useful in aerospace applications at high altitude.« less

Initiation of air ionization by ultrashort laser pulses: evidence for a role of metastable-state air molecules

NASA Astrophysics Data System (ADS)

Bulgakov, A. V.; Mirza, I.; Bulgakova, N. M.; Zhukov, V. P.; Machulka, R.; Haderka, O.; Campbell, E. E. B.; Mocek, T.

2018-06-01

Transmission measurements for femtosecond laser pulses focused in air with spectral analysis of emission from the focal region have been carried out for various pulse energies and air pressures. The air breakdown threshold and pulse attenuation due to plasma absorption are evaluated and compared with calculations based on the multiphoton ionization model. The plasma absorption is found to depend on the pulse repetition rate and is considerably stronger at 1 kHz than at 1–10 Hz. This suggests that accumulation of metastable states of air molecules plays an important role in initiation of air breakdown, enhancing the ionization efficiency at high repetition rates. Possible channels of metastable-state-assisted air ionization and the role of the observed accumulation effect in laser material processing are discussed.

Collective Autoionization in Multiply-Excited Systems: A novel ionization process observed in Helium Nanodroplets

PubMed Central

LaForge, A. C.; Drabbels, M.; Brauer, N. B.; Coreno, M.; Devetta, M.; Di Fraia, M.; Finetti, P.; Grazioli, C.; Katzy, R.; Lyamayev, V.; Mazza, T.; Mudrich, M.; O'Keeffe, P.; Ovcharenko, Y.; Piseri, P.; Plekan, O.; Prince, K. C.; Richter, R.; Stranges, S.; Callegari, C.; Möller, T.; Stienkemeier, F.

2014-01-01

Free electron lasers (FELs) offer the unprecedented capability to study reaction dynamics and image the structure of complex systems. When multiple photons are absorbed in complex systems, a plasma-like state is formed where many atoms are ionized on a femtosecond timescale. If multiphoton absorption is resonantly-enhanced, the system becomes electronically-excited prior to plasma formation, with subsequent decay paths which have been scarcely investigated to date. Here, we show using helium nanodroplets as an example that these systems can decay by a new type of process, named collective autoionization. In addition, we show that this process is surprisingly efficient, leading to ion abundances much greater than that of direct single-photon ionization. This novel collective ionization process is expected to be important in many other complex systems, e.g. macromolecules and nanoparticles, exposed to high intensity radiation fields. PMID:24406316

Ultrafast Electron Plasma Index: An Ionization Perspective

DTIC Science & Technology

2014-05-29

picture in mind, the derivation of the index was a combination of the principle of least action and Fermat’s principle. In the current textbook ...multiphoton ionization. Phys Rev Lett 71: 1994-1997. 27. Ivanov MY, Spanner M, Smirnova O (2005) Anatomy of strong field ionization. J. Mod.Phys 52

Detection limits of organic compounds achievable with intense, short-pulse lasers.

PubMed

Miles, Jordan; De Camillis, Simone; Alexander, Grace; Hamilton, Kathryn; Kelly, Thomas J; Costello, John T; Zepf, Matthew; Williams, Ian D; Greenwood, Jason B

2015-06-21

Many organic molecules have strong absorption bands which can be accessed by ultraviolet short pulse lasers to produce efficient ionization. This resonant multiphoton ionization scheme has already been exploited as an ionization source in time-of-flight mass spectrometers used for environmental trace analysis. In the present work we quantify the ultimate potential of this technique by measuring absolute ion yields produced from the interaction of 267 nm femtosecond laser pulses with the organic molecules indole and toluene, and gases Xe, N2 and O2. Using multiphoton ionization cross sections extracted from these results, we show that the laser pulse parameters required for real-time detection of aromatic molecules at concentrations of one part per trillion in air and a limit of detection of a few attomoles are achievable with presently available commercial laser systems. The potential applications for the analysis of human breath, blood and tissue samples are discussed.

Detection of polychlorinated biphenyls in transformer oils in Vietnam by multiphoton ionization mass spectrometry using a far-ultraviolet femtosecond laser as an ionization source.

PubMed

Duong, Vu Thi Thuy; Duong, Vu; Lien, Nghiem Thi Ha; Imasaka, Tomoko; Tang, Yuanyuan; Shibuta, Shinpei; Hamachi, Akifumi; Hoa, Do Quang; Imasaka, Totaro

2016-03-01

Polychlorinated biphenyls (PCBs) in transformer and food oils were measured using gas chromatography combined with multiphoton ionization mass spectroscopy. An ultrashort laser pulse emitting in the far-ultraviolet region was utilized for efficient ionization of the analytes. Numerous signal peaks were clearly observed for a standard sample mixture of PCBs when the third and fourth harmonic emissions (267 and 200nm) of a femtosecond Ti:sapphire laser (800nm) were employed. The signal intensities were found to be greater when measured at 200nm compared with those measured at 267nm, providing lower detection limits especially for highly chlorinated PCBs at shorter wavelengths. After simple pretreatment using disposable columns, PCB congeners were measured and found to be present in the transformer oils used in Vietnam. Copyright © 2015 Elsevier B.V. All rights reserved.

Single and double multiphoton ionization of Li and Be atoms by strong laser fields

NASA Astrophysics Data System (ADS)

Telnov, Dmitry; Heslar, John; Chu, Shih-I.

2011-05-01

The time-dependent density functional theory with self-interaction correction and proper asymptotic long-range potential is extended for nonperturbative treatment of multiphoton single and double ionization of Li and Be atoms by strong 800 nm laser fields. We make use of the time-dependent Krieger-Li-Iafrate (TDKLI) exchange-correlation potential with the integer discontinuity which improves the description of the double ionization process. However, we have found that the discontinuity of the TDKLI potential is not sufficient to reproduce the characteristic feature of double ionization. This may happen because the discontinuity of the TDKLI potential is related to the spin particle numbers only and not to the total particle number. Introducing a discontinuity with respect to the total particle number to the exchange-correlation potential, we were able to obtain the knee structure in the intensity dependence of the double ionization probability of Be. This work was partially supported by DOE and NSF and by NSC-Taiwan.

Ultrafast multiphoton ionization dynamics and control of NaK molecules

NASA Astrophysics Data System (ADS)

Davidsson, Jan; Hansson, Tony; Mukhtar, Emad

1998-12-01

The multiphoton ionization dynamics of NaK molecules is investigated experimentally using one-color pump-probe femtosecond spectroscopy at 795 nm and intermediate laser field strengths (about 10 GW/cm2). Both NaK+ and Na+ ions are detected as a function of pulse separation time, pulse intensities, and strong pulse-weak pulse order. To aid in the analysis, the potential energy curves of the two lowest electronic states of NaK+ and the electronic transition dipole moment between them are calculated by the GAUSSIAN94 UCIS method. Different ionization pathways are identified by Franck-Condon analysis, and vibrational dynamics in the A 1Σ+ and 3 1Π states, as well as in the ground state, is observed. Further, the existence of a highly excited (above the adiabatic ionization limit) neutral state of NaK is proposed. By changing the strong pulse-weak pulse order of the pulses, the ionization pathways for production of both ions can be varied and thus controlled.

Supramolecular clusters between carbohydrates and concave pyridines. Detection in the gas phase by resonance-enhanced multi-photon ionization reflectron time-of-flight mass spectrometer.

PubMed

Liebig, Timo; Lüning, Ulrich; Grotemeyer, Jürgen

2006-01-01

For the first time the formation of supramolecular clusters between concave pyridines and different carbohydrates could be observed in the gas phase. The different clusters have been investigated by means of laser desorption into a supersonic beam followed by resonant multi photon excitation yielding mass spectra with high intensity of the different cluster. These preliminary results open a way for the investigations of the hydrogen bonds in these compounds.

Analysis of plasma-mediated ablation in aqueous tissue

NASA Astrophysics Data System (ADS)

Jiao, Jian; Guo, Zhixiong

2012-06-01

Plasma-mediated ablation using ultrafast lasers in transparent media such as aqueous tissues is studied. It is postulated that a critical seed free electron density exists due to the multiphoton ionization in order to trigger the avalanche ionization which causes ablation and during the avalanche ionization process the contribution of laser-induced photon ionization is negligible. Based on this assumption, the ablation process can be treated as two separate processes - the multiphoton and avalanche ionizations - at different time stages; so that an analytical solution to the evolution of plasma formation is obtained for the first time. The analysis is applied to plasma-mediated ablation in corneal epithelium and validated via comparison with experimental data available in the literature. The critical seed free-electron density and the time to initiate the avalanche ionization for sub-picosecond laser pulses are analyzed. It is found that the critical seed free-electron density decreases as the pulse width increases, obeying a tp-5.65 rule. This model is further extended to the estimation of crater size in the ablation of tissue-mimic polydimethylsiloxane (PDMS). The results match well with the available experimental measurements.

Revisiting photon-statistics effects on multiphoton ionization

NASA Astrophysics Data System (ADS)

Mouloudakis, G.; Lambropoulos, P.

2018-05-01

We present a detailed analysis of the effects of photon statistics on multiphoton ionization. Through a detailed study of the role of intermediate states, we evaluate the conditions under which the premise of nonresonant processes is valid. The limitations of its validity are manifested in the dependence of the process on the stochastic properties of the radiation and found to be quite sensitive to the intensity. The results are quantified through detailed calculations for coherent, chaotic, and squeezed vacuum radiation. Their significance in the context of recent developments in radiation sources such as the short-wavelength free-electron laser and squeezed vacuum radiation is also discussed.

Laser-induced breakup of helium 3S 1s2s with intermediate doubly excited states

NASA Astrophysics Data System (ADS)

Simonsen, A. S.; Bachau, H.; Førre, M.

2014-02-01

Solving the time-dependent Schrödinger equation in full dimensionality for two electrons, it is found that in the XUV regime the two-photon double ionization dynamics of He(1s2s) is predominantly dictated by the process of resonance enhanced multiphoton ionization via doubly excited states (DESs). We have studied a pump-probe scenario where the full laser-driven breakup of the 3S 1s2s metastable state is dominated by intermediate quasiresonant excitation to doubly excited (autoionizing) states in the 3Po series. Clear evidence of multipath interference effects is revealed in the resulting angular distributions of the ejected electrons in cases where more than one intermediate DES is populated in the process.

Molecular symmetry group analysis of the low-wavenumber torsions and vibration-torsions in the S1 state and ground state cation of p-xylene: An investigation using resonance-enhanced multiphoton ionization (REMPI) and zero-kinetic-energy (ZEKE) spectroscopy

NASA Astrophysics Data System (ADS)

Gardner, Adrian M.; Tuttle, William D.; Groner, Peter; Wright, Timothy G.

2017-03-01

For the first time, a molecular symmetry group (MSG) analysis has been undertaken in the investigation of the electronic spectroscopy of p-xylene (p-dimethylbenzene). Torsional and vibration-torsional (vibtor) levels in the S1 state and ground state of the cation of p-xylene are investigated using resonance-enhanced multiphoton ionization (REMPI) and zero-kinetic-energy (ZEKE) spectroscopy. In the present work, we concentrate on the 0-350 cm-1 region, where there are a number of torsional and vibtor bands and we discuss the assignment of this region. In Paper II [W. D. Tuttle et al., J. Chem. Phys. 146, 124309 (2017)], we examine the 350-600 cm-1 region where vibtor levels are observed as part of a Fermi resonance. The similarity of much of the observed spectral activity to that in the related substituted benzenes, toluene and para-fluorotoluene, is striking, despite the different symmetries. The discussion necessitates a consideration of the MSG of p-xylene, which has been designated G72, but we shall also designate [{3,3}]D2h and we include the symmetry operations, character table, and direct product table for this. We also discuss the symmetries of the internal rotor (torsional) levels and the selection rules for the particular electronic transition of p-xylene investigated here.

Resonance-enhanced multiphoton ionization (REMPI) spectroscopy of bromobenzene and its perdeuterated isotopologue: Assignment of the vibrations of the S{sub 0}, S{sub 1}, and D{sub 0}{sup +} states of bromobenzene and the S{sub 0} and D{sub 0}{sup +} states of iodobenzene

DOE Office of Scientific and Technical Information (OSTI.GOV)

Andrejeva, Anna; Tuttle, William D.; Harris, Joe P.

2015-12-28

We report vibrationally resolved spectra of the S{sub 1}←S{sub 0} transition of bromobenzene using resonance-enhanced multiphoton ionization spectroscopy. We study bromobenzene-h{sub 5} as well as its perdeuterated isotopologue, bromobenzene-d{sub 5}. The form of the vibrational modes between the isotopologues and also between the S{sub 0} and S{sub 1} electronic states is discussed for each species, allowing assignment of the bands to be achieved and the activity between states and isotopologues to be established. Vibrational bands are assigned utilizing quantum chemical calculations, previous experimental results, and isotopic shifts. Previous work and assignments of the S{sub 1} spectra are discussed. Additionally, themore » vibrations in the ground state cation, D{sub 0}{sup +}, are considered, since these have also been used by previous workers in assigning the excited neutral state spectra. We also examine the vibrations of iodobenzene in the S{sub 0} and D{sub 0}{sup +} states and comment on the previous assignments of these. In summary, we have been able to assign the corresponding vibrations across the whole monohalobenzene series of molecules, in the S{sub 0}, S{sub 1}, and D{sub 0}{sup +} states, gaining insight into vibrational activity and vibrational couplings.« less

Non-volatile analysis in fruits by laser resonant ionization spectrometry: application to resveratrol (3,5,4'-trihydroxystilbene) in grapes

NASA Astrophysics Data System (ADS)

Montero, C.; Orea, J. M.; Soledad Muñoz, M.; Lobo, R. F. M.; González Ureña, A.

A laser desorption (LD) coupled with resonance-enhanced multiphoton ionisation (REMPI) and time-of-flight mass spectrometry (TOFMS) technique for non-volatile trace analysis compounds is presented. Essential features are: (a) an enhanced desorption yield due to the mixing of metal powder with the analyte in the sample preparation, (b) a high resolution, great sensitivity and low detection limit due to laser resonant ionisation and mass spectrometry detection. Application to resveratrol content in grapes demonstrated the capability of the analytical method with a sensitivity of 0.2 pg per single laser shot and a detection limit of 5 ppb.

Ion-Pair States in Triplet Molecular Hydrogen

NASA Astrophysics Data System (ADS)

Setzer, W.; Baker, B. C.; Ashman, S.; Morgan, T. J.

2016-05-01

An experimental search is underway to observe the long range triplet ionic states H+ H- of molecular hydrogen. Resonantly enhanced multi-photon ionization of the metastable c 3∏u- 2 pπ state is used access to the R(1)nd1 n = 21 Rydberg state that serves as an intermediate stepping stone state to probe the energy region above the ionization limit with a second tunable laser photon. The metastable state is prepared by electron capture of 6 keV H2+ions in potassium in a molecular beam. Formation of the H+ H- triplet configuration involves triplet excited states of the H- ion, especially the 2p23Pe state, the second bound state of H- predicted to exist with a lifetime long compared to typical auto ionization lifetimes but not yet observed experimentally. Details of the experiment and preliminary results to date will be presented at the conference.

An alternative mechanism for spin-forbidden photo-ionization of diatomic molecules and its rotation-electronic selection rules

NASA Astrophysics Data System (ADS)

Chiu, Ying-Nan; Chiu, Lue-Yung Chow

1990-02-01

The spin-forbidden photo-ionization of diatomic molecules is proposed. Spin orbit interaction is invoked, resulting in the correction and mixing of the wave functions of different multiplicities. The rotation-electronic selection rules given by Dixit and McKoy (1986) for Hund's case a based on the conventional mechanism of electric dipole transition are rederived and expressed in a different format. This new format permits the generalization of the selection rules to other photoionization transitions caused by the magnetic dipole, the electric quadrupole, and the two- and three-photon operators. These selection rules, which are for transitions from one specific rotational level of a given Kronig reflection symmetry to another, will help understand rotational branching and the dynamics of interaction in the excited state. They will also help in the selective preparation of well-defined rovibronic states in resonant-enhanced multi-photon ionization processes.

Ionization-induced solvent migration in acetanilide-methanol clusters inferred from isomer-selective infrared spectroscopy.

PubMed

Weiler, Martin; Nakamura, Takashi; Sekiya, Hiroshi; Dopfer, Otto; Miyazaki, Mitsuhiko; Fujii, Masaaki

2012-12-07

We present the resonance-enhanced multiphoton ionization, infrared-ultraviolet hole burning (IR-UV HB), and IR dip spectra of the trans-acetanilide-methanol (AA-MeOH) cluster in the S(0), S(1), and cationic ground state (D(0)) in a supersonic jet. The IR-UV HB spectra demonstrate the co-existence of two isomers in S(0,1), in which MeOH binds either to the NH or the CO site of the peptide linkage in AA, denoted as AA(NH)-MeOH and AA(CO)-MeOH. When AA(CO)-MeOH is selectively ionized, its IR spectrum in D(0) is the same as that measured for AA(+) (NH)-MeOH. Thus, photoionization of AA(CO)-MeOH induces migration of MeOH from the CO to the NH site with 100% yield. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Electron and fluorescence spectra of a water molecule irradiated by an x-ray free-electron laser pulse

NASA Astrophysics Data System (ADS)

Schäfer, Julia M.; Inhester, Ludger; Son, Sang-Kil; Fink, Reinhold F.; Santra, Robin

2018-05-01

With the highly intense x-ray light generated by x-ray free-electron lasers (XFELs), molecular samples can be ionized many times in a single pulse. Here we report on a computational study of molecular spectroscopy at the high x-ray intensity provided by XFELs. Calculated photoelectron, Auger electron, and x-ray fluorescence spectra are presented for a single water molecule that reaches many electronic hole configurations through repeated ionization steps. The rich details shown in the spectra depend on the x-ray pulse parameters in a nonintuitive way. We discuss how the observed trends can be explained by the competition of microscopic electronic transition processes. A detailed comparison between spectra calculated within the independent-atom model and within the molecular-orbital framework highlights the chemical sensitivity of the spectral lines of multiple-hole configurations. Our results demonstrate how x-ray multiphoton ionization-related effects such as charge-rearrangement-enhanced x-ray ionization of molecules and frustrated absorption manifest themselves in the electron and fluorescence spectra.

Photoionization pathways and thresholds in generation of Lyman-α radiation by resonant four-wave mixing in Kr-Ar mixture

NASA Astrophysics Data System (ADS)

Louchev, Oleg A.; Saito, Norihito; Oishi, Yu; Miyazaki, Koji; Okamura, Kotaro; Nakamura, Jumpei; Iwasaki, Masahiko; Wada, Satoshi

2016-09-01

We develop a set of analytical approximations for the estimation of the combined effect of various photoionization processes involved in the resonant four-wave mixing generation of ns pulsed Lyman-α (L-α ) radiation by using 212.556 nm and 820-845 nm laser radiation pulses in Kr-Ar mixture: (i) multi-photon ionization, (ii) step-wise (2+1)-photon ionization via the resonant 2-photon excitation of Kr followed by 1-photon ionization and (iii) laser-induced avalanche ionization produced by generated free electrons. Developed expressions validated by order of magnitude estimations and available experimental data allow us to identify the area for the operation under high input laser intensities avoiding the onset of full-scale discharge, loss of efficiency and inhibition of generated L-α radiation. Calculations made reveal an opportunity for scaling up the output energy of the experimentally generated pulsed L-α radiation without significant enhancement of photoionization.

Laser Pulse Width Dependence and Ionization Mechanism of Matrix-Assisted Laser Desorption/Ionization

NASA Astrophysics Data System (ADS)

Liang, Sheng-Ping; Lu, I.-Chung; Tsai, Shang-Ting; Chen, Jien-Lian; Lee, Yuan Tseh; Ni, Chi-Kung

2017-10-01

Ultraviolet laser pulses at 355 nm with variable pulse widths in the region from 170 ps to 1.5 ns were used to investigate the ionization mechanism of matrix-assisted laser desorption/ionization (MALDI) for matrices 2,5-dihydroxybenzoic acid (DHB), α-cyano-4-hydroxycinnamic acid (CHCA), and sinapinic acid (SA). The mass spectra of desorbed ions and the intensity and velocity distribution of desorbed neutrals were measured simultaneously for each laser shot. These quantities were found to be independent of the laser pulse width. A comparison of the experimental measurements and numerical simulations according to the multiphoton ionization, coupled photophysical and chemical dynamics (CPCD), and thermally induced proton transfer models showed that the predictions of thermally induced proton transfer model were in agreement with the experimental data, but those of the multiphoton ionization model were not. Moreover, the predictions of the CPCD model based on singlet-singlet energy pooling were inconsistent with the experimental data of CHCA and SA, but were consistent with the experimental data of DHB only when some parameters used in the model were adjusted to extreme values. [Figure not available: see fulltext.

Multiphoton ionization of many-electron atoms and highly-charged ions in intense laser fields: a relativistic time-dependent density functional theory approach

NASA Astrophysics Data System (ADS)

Tumakov, Dmitry A.; Telnov, Dmitry A.; Maltsev, Ilia A.; Plunien, Günter; Shabaev, Vladimir M.

2017-10-01

We develop an efficient numerical implementation of the relativistic time-dependent density functional theory (RTDDFT) to study multielectron highly-charged ions subject to intense linearly-polarized laser fields. The interaction with the electromagnetic field is described within the electric dipole approximation. The resulting time-dependent relativistic Kohn-Sham (RKS) equations possess an axial symmetry and are solved accurately and efficiently with the help of the time-dependent generalized pseudospectral method. As a case study, we calculate multiphoton ionization probabilities of the neutral argon atom and argon-like xenon ion. Relativistic effects are assessed by comparison of our present results with existing non-relativistic data.

Measurement of plasma decay processes in mixture of sodium and argon by coherent microwave scattering

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang Zhili; Shneider, Mikhail N.

2010-03-15

This paper presents the experimental measurement and computational model of sodium plasma decay processes in mixture of sodium and argon by using radar resonance-enhanced multiphoton ionization (REMPI), coherent microwave Rayleigh scattering of REMPI. A single laser beam resonantly ionizes the sodium atoms by means of 2+1 REMPI process. The laser beam can only generate the ionization of the sodium atoms and have negligible ionization of argon. Coherent microwave scattering in situ measures the total electron number in the laser-induced plasma. Since the sodium ions decay by recombination with electrons, microwave scattering directly measures the plasma decay processes of the sodiummore » ions. A theoretical plasma dynamic model, including REMPI of the sodium and electron avalanche ionization (EAI) of sodium and argon in the gas mixture, has been developed. It confirms that the EAI of argon is several orders of magnitude lower than the REMPI of sodium. The theoretical prediction made for the plasma decay process of sodium plasma in the mixture matches the experimental measurement.« less

Carrier-envelope-phase control of asymmetries in the multiphoton ionization of xenon atoms by ultrashort bichromatic fields

NASA Astrophysics Data System (ADS)

Kerbstadt, S.; Pengel, D.; Englert, L.; Bayer, T.; Wollenhaupt, M.

2018-06-01

We report on bichromatic multiphoton ionization of xenon atoms (Xe) to demonstrate carrier-envelope-phase (CEP) control of lateral asymmetries in the photoelectron momentum distribution. In the experiments, we employ a 4 f polarization pulse shaper to sculpture bichromatic fields with commensurable center frequencies ω1:ω2=7 :8 from an over-octave-spanning CEP-stable white light supercontinuum by spectral amplitude and phase modulation. The bichromatic fields are spectrally tailored to induce controlled interferences of 7- vs 8-photon quantum pathways in the 5 P3 /2 ionization continuum of Xe. The CEP sensitivity of the asymmetric final-state wave function arises from coherent superposition of continuum states with opposite parity. Our results demonstrate that shaper-generated bichromatic fields with tailored center frequency ratio are a suitable tool to localize CEP-sensitive asymmetries in a specific photoelectron kinetic-energy window.

Imaging photoelectron circular dichroism of chiral molecules by femtosecond multiphoton coincidence detection.

PubMed

Lehmann, C Stefan; Ram, N Bhargava; Powis, Ivan; Janssen, Maurice H M

2013-12-21

Here, we provide a detailed account of novel experiments employing electron-ion coincidence imaging to discriminate chiral molecules. The full three-dimensional angular scattering distribution of electrons is measured after photoexcitation with either left or right circular polarized light. The experiment is performed using a simplified photoelectron-photoion coincidence imaging setup employing only a single particle imaging detector. Results are reported applying this technique to enantiomers of the chiral molecule camphor after three-photon ionization by circularly polarized femtosecond laser pulses at 400 nm and 380 nm. The electron-ion coincidence imaging provides the photoelectron spectrum of mass-selected ions that are observed in the time-of-flight mass spectra. The coincident photoelectron spectra of the parent camphor ion and the various fragment ions are the same, so it can be concluded that fragmentation of camphor happens after ionization. We discuss the forward-backward asymmetry in the photoelectron angular distribution which is expressed in Legendre polynomials with moments up to order six. Furthermore, we present a method, similar to one-photon electron circular dichroism, to quantify the strength of the chiral electron asymmetry in a single parameter. The circular dichroism in the photoelectron angular distribution of camphor is measured to be 8% at 400 nm. The electron circular dichroism using femtosecond multiphoton excitation is of opposite sign and about 60% larger than the electron dichroism observed before in near-threshold one-photon ionization with synchrotron excitation. We interpret our multiphoton ionization as being resonant at the two-photon level with the 3s and 3p Rydberg states of camphor. Theoretical calculations are presented that model the photoelectron angular distribution from a prealigned camphor molecule using density functional theory and continuum multiple scattering X alpha photoelectron scattering calculations. Qualitative agreement is observed between the experimental results and the theoretical calculations of the Legendre moments representing the angular distribution for the two enantiomers. The electron-ion coincidence technique using multiphoton ionization opens new directions in table-top analytical mass-spectrometric applications of mixtures of chiral molecules.

Imaging photoelectron circular dichroism of chiral molecules by femtosecond multiphoton coincidence detection

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lehmann, C. Stefan; Ram, N. Bhargava; Janssen, Maurice H. M., E-mail: m.h.m.janssen@vu.nl

2013-12-21

Here, we provide a detailed account of novel experiments employing electron-ion coincidence imaging to discriminate chiral molecules. The full three-dimensional angular scattering distribution of electrons is measured after photoexcitation with either left or right circular polarized light. The experiment is performed using a simplified photoelectron-photoion coincidence imaging setup employing only a single particle imaging detector. Results are reported applying this technique to enantiomers of the chiral molecule camphor after three-photon ionization by circularly polarized femtosecond laser pulses at 400 nm and 380 nm. The electron-ion coincidence imaging provides the photoelectron spectrum of mass-selected ions that are observed in the time-of-flightmore » mass spectra. The coincident photoelectron spectra of the parent camphor ion and the various fragment ions are the same, so it can be concluded that fragmentation of camphor happens after ionization. We discuss the forward-backward asymmetry in the photoelectron angular distribution which is expressed in Legendre polynomials with moments up to order six. Furthermore, we present a method, similar to one-photon electron circular dichroism, to quantify the strength of the chiral electron asymmetry in a single parameter. The circular dichroism in the photoelectron angular distribution of camphor is measured to be 8% at 400 nm. The electron circular dichroism using femtosecond multiphoton excitation is of opposite sign and about 60% larger than the electron dichroism observed before in near-threshold one-photon ionization with synchrotron excitation. We interpret our multiphoton ionization as being resonant at the two-photon level with the 3s and 3p Rydberg states of camphor. Theoretical calculations are presented that model the photoelectron angular distribution from a prealigned camphor molecule using density functional theory and continuum multiple scattering X alpha photoelectron scattering calculations. Qualitative agreement is observed between the experimental results and the theoretical calculations of the Legendre moments representing the angular distribution for the two enantiomers. The electron-ion coincidence technique using multiphoton ionization opens new directions in table-top analytical mass-spectrometric applications of mixtures of chiral molecules.« less

Multiphoton Ionization Mass and Photoelectron Spectroscopy.

DTIC Science & Technology

1984-07-01

tracted information about ion vibrational energy levels. Molecules studted include benzene, toluene, aniline, paradifluorobenzene, nitric oxide ...molecules or subgroups and not to others. Ion specific electrodes play an analogous role in electro - chemistry. The prospect of selectively ionizing a... acetaldehyde and butyraldehyde have been studied at the KrF and ArF laser wavelengths. Their ionization potentials are 10.2 and 9.8 eV, respectively

Relaxation channels of multi-photon excited xenon clusters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Serdobintsev, P. Yu.; Melnikov, A. S.; Department of Physics, St. Petersburg State University, Saint Petersburg 198904

2015-09-21

The relaxation processes of the xenon clusters subjected to multi-photon excitation by laser radiation with quantum energies significantly lower than the thresholds of excitation of atoms and ionization of clusters were studied. Results obtained by means of the photoelectron spectroscopy method showed that desorption processes of excited atoms play a significant role in the decay of two-photon excited xenon clusters. A number of excited states of xenon atoms formed during this process were discovered and identified.

REMPI detection of singlet oxygen 1O2 arising from UV-photodissociation of van der Waals complex isoprene-oxygen C5H8-O2

NASA Astrophysics Data System (ADS)

Bogomolov, Alexandr S.; Dozmorov, Nikolay V.; Kochubei, Sergei A.; Baklanov, Alexey V.

2018-01-01

The one-laser two-color resonance enhanced multiphoton ionization REMPI [(1 + 1‧) + 1] and velocity map imaging have been applied to investigate formation of molecular oxygen in excited singlet O2(a1Δg) and ground O2(X3Σg-) states in the photodissociation of van der Waals complex isoprene-oxygen C5H8-O2. These molecules were found to appear in the different rotational states with translational energy varied from a value as low as ∼1 meV to a distribution with temperature of about 940 K. The observed traces of electron recoil in the images of photoions reveal participation of several ionization pathways of the resonantly excited intermediate states of O2.

Quantitative measurement of electron number in nanosecond and picosecond laser-induced air breakdown

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, Yue; Sawyer, Jordan C.; Su, Liu

2016-05-07

Here we present quantitative measurements of total electron numbers in laser-induced air breakdown at pressures ranging from atmospheric to 40 bar{sub g} by 10 ns and 100 ps laser pulses. A quantifiable definition for the laser-induced breakdown threshold is identified by a sharp increase in the measurable total electron numbers via dielectric-calibrated coherent microwave scattering. For the 10 ns laser pulse, the threshold of laser-induced breakdown in atmospheric air is defined as the total electron number of ∼10{sup 6}. This breakdown threshold decreases with an increase of pressure and laser photon energy (shorter wavelength), which is consistent with the theory of initialmore » multiphoton ionization and subsequent avalanche processes. For the 100 ps laser pulse cases, a clear threshold is not present and only marginal pressure effects can be observed, which is due to the short pulse duration leading to stronger multiphoton ionization and minimal collisional avalanche ionization.« less

Quantum description of the high-order harmonic generation in multiphoton and tunneling regimes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Perez-Hernandez, J. A.; Plaja, L.

2007-08-15

We employ a recently developed S-matrix approach [L. Plaja and J. A. Perez-Hernandez, Opt. Express 15, 3629 (2007)] to investigate the process of harmonic generation in tunnel and multiphoton ionization regimes. In contrast with most of the previous approaches, this model is developed without the stationary phase approximation and including the relevant continuum-continuum transitions. Therefore, it provides a full quantum description of the harmonic generation process in these two ionization regimes, with a good quantitative accuracy with the exact results of the time-dependent Schroedinger equation. We show how this model can be used to investigate the contribution of the electronicmore » population ionized at different times, thus giving a time-resolved description that, up to now, was reserved only to semiclassical models. In addition, we will show some aspects of harmonic generation beyond the semiclassical predictions as, for instance, the emission of radiation while the electron is leaving the parent ion and the generation of harmonics in semiclassically forbidden situations.« less

L. V. Keldysh’s “Ionization in the Field of a Strong Electromagnetic Wave” and modern physics of atomic interaction with a strong laser field

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fedorov, M. V., E-mail: fedorov@gmail.com

2016-03-15

Basic premises, approximations, and results of L.V. Keldysh’s 1964 work on multiphoton ionization of atoms are discussed, as well as its influence on the modern science of the interaction of atomic–molecular systems with a strong laser field.

Investigating multiphoton phenomena using nonlinear dynamics

NASA Astrophysics Data System (ADS)

Huang, Shu

Many seemingly simple systems can display extraordinarily complex dynamics which has been studied and uncovered through nonlinear dynamical theory. The leitmotif of this thesis is changing phase-space structures and their (linear or non-linear) stabilities by adding control functions (which act on the system as external perturbations) to the relevant Hamiltonians. These phase-space structures may be periodic orbits, invariant tori or their stable and unstable manifolds. One-electron systems and diatomic molecules are fundamental and important staging ground for new discoveries in nonlinear dynamics. In past years, increasing emphasis and effort has been put on the control or manipulation of these systems. Recent developments of nonlinear dynamical tools can provide efficient ways of doing so. In the first subtopic of the thesis, we are adding a control function to restore tori at prescribed locations in phase space. In the remainder of the thesis, a control function with parameters is used to change the linear stability of the periodic orbits which govern the processes in question. In this thesis, we report our theoretical analyses on multiphoton ionization of Rydberg atoms exposed to strong microwave fields and the dissociation of diatomic molecules exposed to bichromatic lasers using nonlinear dynamical tools. This thesis is composed of three subtopics. In the first subtopic, we employ local control theory to reduce the stochastic ionization of hydrogen atom in a strong microwave field by adding a relatively small control term to the original Hamiltonian. In the second subtopic, we perform periodic orbit analysis to investigate multiphoton ionization driven by a bichromatic microwave field. Our results show quantitative and qualitative agreement with previous studies, and hence identify the mechanism through which short periodic orbits organize the dynamics in multiphoton ionization. In addition, we achieve substantial time savings with this approach. In the third subtopic we extend our periodic orbit analysis to the dissociation of diatomic molecules driven by a bichromatic laser. In this problem, our results based on periodic orbit analysis again show good agreement with previous work, and hence promise more potential applications of this approach in molecular physics.

Multiphoton versus confocal high resolution z-sectioning of enhanced green fluorescent microtubules: increased multiphoton photobleaching within the focal plane can be compensated using a Pockels cell and dual widefield detectors.

PubMed

Drummond, D R; Carter, N; Cross, R A

2002-05-01

Multiphoton excitation was originally projected to improve live cell fluorescence imaging by minimizing photobleaching effects outside the focal plane, yet reports suggest that photobleaching within the focal plane is actually worse than with one photon excitation. We confirm that when imaging enhanced green fluorescent protein, photobleaching is indeed more acute within the multiphoton excitation volume, so that whilst fluorescence increases as predicted with the square of the excitation power, photobleaching rates increase with a higher order relationship. Crucially however, multiphoton excitation also affords unique opportunities for substantial improvements to fluorescence detection. By using a Pockels cell to minimize exposure of the specimen together with multiple nondescanned detectors we show quantitatively that for any particular bleach rate multiphoton excitation produces significantly more signal than one photon excitation confocal microscopy in high resolution Z-axis sectioning of thin samples. Both modifications are readily implemented on a commercial multiphoton microscope system.

Strong field control of the interatomic Coulombic decay process in quantum dots

NASA Astrophysics Data System (ADS)

Haller, Anika; Chiang, Ying-Chih; Menger, Maximilian; Aziz, Emad F.; Bande, Annika

2017-01-01

In recent years the laser-induced interatomic Coulombic decay (ICD) process in paired quantum dots has been predicted (Bande, 2013). In this work we target the enhancement of ICD by scanning over a range of strong-field laser intensities. The GaAs quantum dots are modeled by a one-dimensional double-well potential in which simulations are done with the space-resolved multi-configuration time-dependent Hartree method including antisymmetrization to account for the fermions. As a novelty a complementary state-resolved ansatz is developed to consolidate the interpretation of transient state populations, widths obtained for the ICD and the competing direct ionization channel, and Fano peak profiles in the photoelectron spectra. The major results are that multi-photon processes are unimportant even for the strongest fields. Further, below- π to π pulses display the highest ICD efficiency while the direct ionization becomes less dominant.

Unified Time and Frequency Picture of Ultrafast Atomic Excitation in Strong Laser Fields

NASA Astrophysics Data System (ADS)

Zimmermann, H.; Patchkovskii, S.; Ivanov, M.; Eichmann, U.

2017-01-01

Excitation and ionization in strong laser fields lies at the heart of such diverse research directions as high-harmonic generation and spectroscopy, laser-induced diffraction imaging, emission of femtosecond electron bunches from nanotips, self-guiding, filamentation and mirrorless lasing during propagation of light in atmospheres. While extensive quantum mechanical and semiclassical calculations on strong-field ionization are well backed by sophisticated experiments, the existing scattered theoretical work aiming at a full quantitative understanding of strong-field excitation lacks experimental confirmation. Here we present experiments on strong-field excitation in both the tunneling and multiphoton regimes and their rigorous interpretation by time dependent Schrödinger equation calculations, which finally consolidates the seemingly opposing strong-field regimes with their complementary pictures. Most strikingly, we observe an unprecedented enhancement of excitation yields, which opens new possibilities in ultrafast strong-field control of Rydberg wave packet excitation and laser intensity characterization.

Rotational spectroscopy with an optical centrifuge.

PubMed

Korobenko, Aleksey; Milner, Alexander A; Hepburn, John W; Milner, Valery

2014-03-07

We demonstrate a new spectroscopic method for studying electronic transitions in molecules with extremely broad range of angular momentum. We employ an optical centrifuge to create narrow rotational wave packets in the ground electronic state of (16)O2. Using the technique of resonance-enhanced multi-photon ionization, we record the spectrum of multiple ro-vibrational transitions between X(3)Σg(-) and C(3)Πg electronic manifolds of oxygen. Direct control of rotational excitation, extending to rotational quantum numbers as high as N ≳ 120, enables us to interpret the complex structure of rotational spectra of C(3)Πg beyond thermally accessible levels.

A method of extracting speed-dependent vector correlations from 2 + 1 REMPI ion images.

PubMed

Wei, Wei; Wallace, Colin J; Grubb, Michael P; North, Simon W

2017-07-07

We present analytical expressions for extracting Dixon's bipolar moments in the semi-classical limit from experimental anisotropy parameters of sliced or reconstructed non-sliced images. The current method focuses on images generated by 2 + 1 REMPI (Resonance Enhanced Multi-photon Ionization) and is a necessary extension of our previously published 1 + 1 REMPI equations. Two approaches for applying the new equations, direct inversion and forward convolution, are presented. As demonstration of the new method, bipolar moments were extracted from images of carbonyl sulfide (OCS) photodissociation at 230 nm and NO 2 photodissociation at 355 nm, and the results are consistent with previous publications.

Strong-field ionization of Li and Be: a time-dependent density functional theory with self-interaction correction

NASA Astrophysics Data System (ADS)

Telnov, Dmitry A.; Heslar, John T.; Chu, Shih-I.

2011-11-01

In the framework of the time-dependent density functional theory, we have performed 3D calculations of multiphoton ionization of Li and Be atoms by strong near-infrared laser fields. The results for the intensity-dependent probabilities of single and double ionization are presented. We make use of the time-dependent Krieger-Li-Iafrate exchange-correlation potential with self-interaction correction (TD-KLI-SIC). Such a potential possesses an integer discontinuity which improves description of the ionization process. However, we have found that the discontinuity of the TD-KLI-SIC potential is not sufficient to reproduce characteristic feature of double ionization.

SFC-APLI-(TOF)MS: Hyphenation of Supercritical Fluid Chromatography to Atmospheric Pressure Laser Ionization Mass Spectrometry.

PubMed

Klink, Dennis; Schmitz, Oliver Johannes

2016-01-05

Atmospheric-pressure laser ionization mass spectrometry (APLI-MS) is a powerful method for the analysis of polycyclic aromatic hydrocarbon (PAH) molecules, which are ionized in a selective and highly sensitive way via resonance-enhanced multiphoton ionization. APLI was presented in 2005 and has been hyphenated successfully to chromatographic separation techniques like high performance liquid chromatography (HPLC) and gas chromatography (GC). In order to expand the portfolio of chromatographic couplings to APLI, a new hyphenation setup of APLI and supercritical-fluid chromatography (SFC) was constructed and aim of this work. Here, we demonstrate the first hyphenation of SFC and APLI in a simple designed way with respect to different optimization steps to ensure a sensitive analysis. The new setup permits qualitative and quantitative determination of native and also more polar PAH molecules. As a result of the altered ambient characteristics within the source enclosure, the quantification of 1-hydroxypyrene (1-HP) in human urine is possible without prior derivatization. The limit of detection for 1-HP by SFC-APLI-TOF(MS) was found to be 0.5 μg L(-1), which is lower than the 1-HP concentrations found in exposed persons.

An Automated System for the Control of, and Data Acquisition from Multiphoton Ionization and Fluorescence Lifetime Measurements.

DTIC Science & Technology

1986-09-01

Quanta- Ray company , which also supplied the laser used for the multiphoton work. The, burner was mounted on a translator stage from Velmex, Inc...and no longer exists as a process in the system. When the user analysis program has completed, the lifetime program is again automatically re-started...KCHAR) RETURN 100 FORMAT(I3) 101 FORMAT(F7.2) END SUBROUTINE LAB4 FODA SE"oteD C This routine puts the label "INTEGRAL FROM DATA SET" on the MDP C screen

Optimized cell geometry for buffer-gas-cooled molecular-beam sources

NASA Astrophysics Data System (ADS)

Singh, Vijay; Samanta, Amit K.; Roth, Nils; Gusa, Daniel; Ossenbrüggen, Tim; Rubinsky, Igor; Horke, Daniel A.; Küpper, Jochen

2018-03-01

We have designed, constructed, and commissioned a cryogenic helium buffer-gas source for producing a cryogenically cooled molecular beam and evaluated the effect of different cell geometries on the intensity of the produced molecular beam, using ammonia as a test molecule. Planar and conical entrance and exit geometries are tested. We observe a threefold enhancement in the NH3 signal for a cell with planar entrance and conical-exit geometry, compared to that for a typically used "boxlike" geometry with planar entrance and exit. These observations are rationalized by flow field simulations for the different buffer-gas cell geometries. The full thermalization of molecules with the helium buffer gas is confirmed through rotationally resolved resonance-enhanced multiphoton ionization spectra yielding a rotational temperature of 5 K.

Wavelength dependence of nanosecond infrared laser-induced breakdown in water: Evidence for multiphoton initiation via an intermediate state

NASA Astrophysics Data System (ADS)

Linz, Norbert; Freidank, Sebastian; Liang, Xiao-Xuan; Vogelmann, Hannes; Trickl, Thomas; Vogel, Alfred

2015-04-01

Investigation of the wavelength dependence (725-1025 nm) of the threshold for nanosecond optical breakdown in water revealed steps consistent with breakdown initiation by multiphoton ionization, with an initiation energy of about 6.6 eV. This value is considerably smaller than the autoionization threshold of about 9.5 eV, which can be regarded as band gap relevant for avalanche ionization. Breakdown initiation is likely to occur via excitation of a valence band electron into a solvated state, followed by rapid excitation into the conduction band. Theoretical analysis based on these assumptions suggests that the seed electron density required for initiating avalanche ionization amounts to 2.5 ×1015c m-3 at 725 nm and drops to 1.1 ×1012c m-3 at 1025 nm. These results demand changes of future breakdown modeling for water, including the use of a larger band gap than previously employed, the introduction of an intermediate energy level for initiation, and consideration of the wavelength dependence of seed electron density.

Internal standards for use in the comprehensive analysis of polychlorinated aromatic hydrocarbons using gas chromatography combined with multiphoton ionization mass spectrometry.

PubMed

Li, Adan; Imasaka, Totaro

2016-10-28

To decrease health-risks to humans, non-toxic compounds were evaluated for use as internal standards for calibrating data obtained by gas chromatography/multiphoton ionization mass spectrometry (GC-MPI-MS) using an ultraviolet femtosecond laser as the ionization source. The retention time in the mass chromatogram was calibrated using a retention index, in which a series of n-alkanes was employed as internal standards for evaluating the retention times for polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), and polychlorinated biphenyls (PCBs). To compensate for changes in signal intensity in MPI-MS, the dependence of signal intensity on the laser pulse energy was investigated for the dioxin-like compounds, in addition to five non-toxic aromatic hydrocarbons, that were used as internal standards. Based on their similar behavior,the non-toxic PCDD/PCDF, its 13 C-isotope, and pentachlorobenzene behave similarly, we conclude that they can be used for calibrating the signal intensities in MPI-MS. Copyright © 2016 Elsevier B.V. All rights reserved.

Tabletop imaging of structural evolutions in chemical reactions demonstrated for the acetylene cation

NASA Astrophysics Data System (ADS)

Ibrahim, Heide; Wales, Benji; Beaulieu, Samuel; Schmidt, Bruno E.; Thiré, Nicolas; Fowe, Emmanuel P.; Bisson, Éric; Hebeisen, Christoph T.; Wanie, Vincent; Giguére, Mathieu; Kieffer, Jean-Claude; Spanner, Michael; Bandrauk, André D.; Sanderson, Joseph; Schuurman, Michael S.; Légaré, François

2014-07-01

The introduction of femto-chemistry has made it a primary goal to follow the nuclear and electronic evolution of a molecule in time and space as it undergoes a chemical reaction. Using Coulomb Explosion Imaging, we have shot the first high-resolution molecular movie of a to and fro isomerization process in the acetylene cation. So far, this kind of phenomenon could only be observed using vacuum ultraviolet light from a free-electron laser. Here we show that 266 nm ultrashort laser pulses are capable of initiating rich dynamics through multiphoton ionization. With our generally applicable tabletop approach that can be used for other small organic molecules, we have investigated two basic chemical reactions simultaneously: proton migration and C=C bond breaking, triggered by multiphoton ionization. The experimental results are in excellent agreement with the timescales and relaxation pathways predicted by new and quantitative ab initio trajectory simulations.

Tabletop Imaging of Structural Evolutions in Chemical Reactions

NASA Astrophysics Data System (ADS)

Ibrahim, Heide; Wales, Benji; Beaulieu, Samuel; Schmidt, Bruno E.; Thiré, Nicolas; Fowe, Emmanuel P.; Bisson, Éric; Hebeisen, Christoph T.; Wanie, Vincent; Giguére, Mathieu; Kieffer, Jean-Claude; Spanner, Michael; Bandrauk, André D.; Sanderson, Joseph; Schuurman, Michael S.; Légaré, François

The first high-resolution molecular movie of proton migration in the acetylene cation is obtained using a tabletop multiphoton pump-probe approach—an alternative to demanding free-electron-lasers and other VUV light sources when ionizing from the HOMO-1.

Production of a beam of highly vibrationally excited CO using perturbations.

PubMed

Bartels, Nils; Schäfer, Tim; Hühnert, Jens; Field, Robert W; Wodtke, Alec M

2012-06-07

An intense molecular beam of CO (X(1)Σ(+)) in high vibrational states (v = 17, 18) was produced by a new approach that we call PUMP - PUMP - PERTURB and DUMP. The basic idea is to access high vibrational states of CO e(3)Σ(-) via a two-photon doubly resonant transition that is perturbed by the A(1)Π state. DUMP -ing from this mixed (predominantly triplet) state allows access to high vibrational levels of CO (X(1)Σ(+)). The success of the approach, which avoids the use of vacuum UV radiation in any of the excitation steps, is proven by laser induced fluorescence and resonance enhanced multi-photon ionization spectroscopy.

Production of a beam of highly vibrationally excited CO using perturbations

NASA Astrophysics Data System (ADS)

Bartels, Nils; Schäfer, Tim; Hühnert, Jens; Field, Robert W.; Wodtke, Alec M.

2012-06-01

An intense molecular beam of CO (X1Σ+) in high vibrational states (v = 17, 18) was produced by a new approach that we call PUMP - PUMP - PERTURB and DUMP. The basic idea is to access high vibrational states of CO e3Σ- via a two-photon doubly resonant transition that is perturbed by the A1Π state. DUMP -ing from this mixed (predominantly triplet) state allows access to high vibrational levels of CO (X1Σ+). The success of the approach, which avoids the use of vacuum UV radiation in any of the excitation steps, is proven by laser induced fluorescence and resonance enhanced multi-photon ionization spectroscopy.

Surface Temperature Dependence of Hydrogen Ortho-Para Conversion on Amorphous Solid Water.

PubMed

Ueta, Hirokazu; Watanabe, Naoki; Hama, Tetsuya; Kouchi, Akira

2016-06-24

The surface temperature dependence of the ortho-to-para conversion of H_{2} on amorphous solid water is first reported. A combination of photostimulated desorption and resonance-enhanced multiphoton ionization techniques allowed us to sensitively probe the conversion on the surface of amorphous solid water at temperatures of 9.2-16 K. Within a narrow temperature window of 8 K, the conversion time steeply varied from ∼4.1×10^{3} to ∼6.4×10^{2}  s. The observed temperature dependence is discussed in the context of previously suggested models and the energy dissipation process. The two-phonon process most likely dominates the conversion rate at low temperatures.

Experimental observation of multiphoton Thomson scattering

NASA Astrophysics Data System (ADS)

Yan, Wenchao; Golovin, Grigory; Fruhling, Colton; Haden, Daniel; Zhang, Ping; Zhang, Jun; Zhao, Baozhen; Liu, Cheng; Chen, Shouyuan; Banerjee, Sudeep; Umstadter, Donald

2016-10-01

With the advent of high-power lasers, several multiphoton processes have been reported involving electrons in strong fields. For electrons that were initially bound to atoms, both multiphoton ionization and scattering have been reported. However, for free electrons, only low-order harmonic generation has been observed until now. This limitation stems from past difficulty in achieving the required ultra-high-field strengths in scattering experiments. Highly relativistic laser intensities are required to reach the multiphoton regime of Thomson scattering, and generate high harmonics from free electrons. The scaling parameter is the normalized vector potential (a0). Previous experiments have observed phenomena in the weakly relativistic case (a0 >> 1). In ultra-intense fields (a0 >>1), the anomalous electron trajectory is predicted to produce a spectrum characterized by the merging of multiple high-order harmonic generation into a continuum. This may be viewed as the multiphoton Thomson scattering regime analogous to the wiggler of a synchrotron. Thus, the light produced reflects the electrons behavior in an ultra-intense lase field. We discuss the first experiments in the highly relativistic case (a0 15). This material is based upon work supported by NSF No. PHY-153700; US DOE, Office of Science, BES, # DE-FG02-05ER15663; AFOSR # FA9550-11-1-0157; and DHS DNDO # HSHQDC-13-C-B0036.

Exploration of laser-driven electron-multirescattering dynamics in high-order harmonic generation

DOE PAGES

Li, Peng -Cheng; Sheu, Yae -Lin; Jooya, Hossein Z.; ...

2016-09-06

Multiple rescattering processes play an important role in high-order harmonic generation (HHG) in an intense laser field. However, the underlying multi-rescattering dynamics are still largely unexplored. Here we investigate the dynamical origin of multiple rescattering processes in HHG associated with the odd and even number of returning times of the electron to the parent ion. We perform fully ab initio quantum calculations and extend the empirical mode decomposition method to extract the individual multiple scattering contributions in HHG. We find that the tunneling ionization regime is responsible for the odd number times of rescattering and the corresponding short trajectories aremore » dominant. On the other hand, the multiphoton ionization regime is responsible for the even number times of rescattering and the corresponding long trajectories are dominant. Moreover, we discover that the multiphoton- and tunneling-ionization regimes in multiple rescattering processes occur alternatively. Our results uncover the dynamical origin of multiple rescattering processes in HHG for the first time. As a result, it also provides new insight regarding the control of the multiple rescattering processes for the optimal generation of ultrabroad band supercontinuum spectra and the production of single ultrashort attosecond laser pulse.« less

Exploration of laser-driven electron-multirescattering dynamics in high-order harmonic generation

PubMed Central

Li, Peng-Cheng; Sheu, Yae-Lin; Jooya, Hossein Z.; Zhou, Xiao-Xin; Chu, Shih-I

2016-01-01

Multiple rescattering processes play an important role in high-order harmonic generation (HHG) in an intense laser field. However, the underlying multi-rescattering dynamics are still largely unexplored. Here we investigate the dynamical origin of multiple rescattering processes in HHG associated with the odd and even number of returning times of the electron to the parent ion. We perform fully ab initio quantum calculations and extend the empirical mode decomposition method to extract the individual multiple scattering contributions in HHG. We find that the tunneling ionization regime is responsible for the odd number times of rescattering and the corresponding short trajectories are dominant. On the other hand, the multiphoton ionization regime is responsible for the even number times of rescattering and the corresponding long trajectories are dominant. Moreover, we discover that the multiphoton- and tunneling-ionization regimes in multiple rescattering processes occur alternatively. Our results uncover the dynamical origin of multiple rescattering processes in HHG for the first time. It also provides new insight regarding the control of the multiple rescattering processes for the optimal generation of ultrabroad band supercontinuum spectra and the production of single ultrashort attosecond laser pulse. PMID:27596056

Exploration of laser-driven electron-multirescattering dynamics in high-order harmonic generation.

PubMed

Li, Peng-Cheng; Sheu, Yae-Lin; Jooya, Hossein Z; Zhou, Xiao-Xin; Chu, Shih-I

2016-09-06

Multiple rescattering processes play an important role in high-order harmonic generation (HHG) in an intense laser field. However, the underlying multi-rescattering dynamics are still largely unexplored. Here we investigate the dynamical origin of multiple rescattering processes in HHG associated with the odd and even number of returning times of the electron to the parent ion. We perform fully ab initio quantum calculations and extend the empirical mode decomposition method to extract the individual multiple scattering contributions in HHG. We find that the tunneling ionization regime is responsible for the odd number times of rescattering and the corresponding short trajectories are dominant. On the other hand, the multiphoton ionization regime is responsible for the even number times of rescattering and the corresponding long trajectories are dominant. Moreover, we discover that the multiphoton- and tunneling-ionization regimes in multiple rescattering processes occur alternatively. Our results uncover the dynamical origin of multiple rescattering processes in HHG for the first time. It also provides new insight regarding the control of the multiple rescattering processes for the optimal generation of ultrabroad band supercontinuum spectra and the production of single ultrashort attosecond laser pulse.

Mechanisms of H{sub 2}O desorption from amorphous solid water by 157-nm irradiation: An experimental and theoretical study

DOE Office of Scientific and Technical Information (OSTI.GOV)

DeSimone, Alice J.; Crowell, Vernon D.; Sherrill, C. David

2013-10-28

The photodesorption of water molecules from amorphous solid water (ASW) by 157-nm irradiation has been examined using resonance-enhanced multiphoton ionization. The rotational temperature has been determined, by comparison with simulations, to be 425 ± 75 K. The time-of-flight spectrum of H{sub 2}O (v= 0) has been fit with a Maxwell-Boltzmann distribution with a translational temperature of 700 ± 200 K (0.12 ± 0.03 eV). H{sup +} and OH{sup +} fragment ions have been detected with non-resonant multiphoton ionization, indicating vibrationally excited parent water molecules with translational energies of 0.24 ± 0.08 eV. The cross section for water removal from ASWmore » by 7.9-eV photons near 100 K is (6.9 ± 1.8) × 10{sup −20} cm{sup 2} for >10 L H{sub 2}O exposure. Electronic structure computations have also probed the excited states of water and the mechanisms of desorption. Calculated electron attachment and detachment densities show that exciton delocalization leads to a dipole reversal state in the first singlet excited state of a model system of hexagonal water ice. Ab Initio Molecular Dynamics simulations show possible desorption of a photo-excited water molecule from this cluster, though the non-hydrogen bonded OH bond is stretched significantly before desorption. Potential energy curves of this OH stretch in the electronic excited state show a barrier to dissociation, lending credence to the dipole reversal mechanism.« less

New diagnostic methods for laser plasma- and microwave-enhanced combustion

PubMed Central

Miles, Richard B; Michael, James B; Limbach, Christopher M; McGuire, Sean D; Chng, Tat Loon; Edwards, Matthew R; DeLuca, Nicholas J; Shneider, Mikhail N; Dogariu, Arthur

2015-01-01

The study of pulsed laser- and microwave-induced plasma interactions with atmospheric and higher pressure combusting gases requires rapid diagnostic methods that are capable of determining the mechanisms by which these interactions are taking place. New rapid diagnostics are presented here extending the capabilities of Rayleigh and Thomson scattering and resonance-enhanced multi-photon ionization (REMPI) detection and introducing femtosecond laser-induced velocity and temperature profile imaging. Spectrally filtered Rayleigh scattering provides a method for the planar imaging of temperature fields for constant pressure interactions and line imaging of velocity, temperature and density profiles. Depolarization of Rayleigh scattering provides a measure of the dissociation fraction, and multi-wavelength line imaging enables the separation of Thomson scattering from Rayleigh scattering. Radar REMPI takes advantage of high-frequency microwave scattering from the region of laser-selected species ionization to extend REMPI to atmospheric pressures and implement it as a stand-off detection method for atomic and molecular species in combusting environments. Femtosecond laser electronic excitation tagging (FLEET) generates highly excited molecular species and dissociation through the focal zone of the laser. The prompt fluorescence from excited molecular species yields temperature profiles, and the delayed fluorescence from recombining atomic fragments yields velocity profiles. PMID:26170432

Spectroscopic Constants of the Known Electronic States of Lead Monofluoride

DOE Office of Scientific and Technical Information (OSTI.GOV)

McRaven, C.P.; Sivakumar, P.; Shafer-Ray, N.E.

2010-08-01

Based on measurements made by mass-resolved 1 + 1{prime} + 1{double_prime} resonance-enhanced multiphoton ionization spectroscopy, we have determined new molecular constants describing the rotational and fine structure levels of the B, D, E, and F states of the most abundant isotopic variant {sup 208}Pb{sup 19}F, and we summarize the spectroscopic constants for all the know electronic states of the radical. Many spectroscopic constants for the isotopologues {sup 206}Pb{sup 19}F and {sup 207}Pb{sup 19}F have also been determined. The symmetry of the D-state is found to be {sup 2}{pi}{sub 1/2}, and the F-state is found to be an {Omega} = 3/2more » state.« less

Enhancing nonlinear energy deposition into transparent solids with an elliptically polarized and mid-IR heating laser pulse under two-color femtosecond impact

NASA Astrophysics Data System (ADS)

Potemkin, F. V.; Mareev, E. I.; Bezsudnova, Yu I.; Platonenko, V. T.; Bravy, B. G.; Gordienko, V. M.

2017-06-01

We report on an enhancement of deposited energy density of up to 10 kJ cm-3 inside transparent solids (fused silica and quartz) from using two-color µJ energy level tightly focused (NA  =  0.5) co-propagating linearly polarized seeding (visible, 0.62 µm) and elliptically polarized heating (near-IR, 1.24 µm) femtosecond laser pulses. The rise in temperature under constant volume causes pressure of up to 12 GPa. It has been shown experimentally and theoretically that the production of seeding electrons through multiphoton ionization by visible laser pulse paves the way for controllability of the energy deposition and laser-induced micromodification via carrier heating by delayed infrared laser pulses inside the material. The developed theoretical approach predicts that the deposited energy density will be enhanced by up to 14 kJ cm-3 when using longer (up to 5 µm) wavelengths for heating laser pulses inside transparent solids.

Organic chemical analysis on a microscopic scale using two-step laser desorption/laser ionization mass spectrometry

NASA Technical Reports Server (NTRS)

Kovalenko, L. J.; Philippoz, J.-M.; Bucenell, J. R.; Zenobi, R.; Zare, R. N.

1991-01-01

The distribution of PAHs in the Allende meteorite has been measured using two-step laser desorption and laser multiphoton-ionization mass spectrometry. This method enables in situ analysis (with a spatial resolution of 1 mm or better) of selected organic molecules. Results show that PAH concentrations are locally high compared to the average concentration found by analysis of pulverized samples, and are found primarily in the fine-grained matrix; no PAHs were detected in the interiors of individual chondrules at the detection limit (about 0.05 ppm).

Experimental investigation of strong-field-ionization theories for laser fields from visible to midinfrared frequencies

NASA Astrophysics Data System (ADS)

Lai, Yu Hang; Xu, Junliang; Szafruga, Urszula B.; Talbert, Bradford K.; Gong, Xiaowei; Zhang, Kaikai; Fuest, Harald; Kling, Matthias F.; Blaga, Cosmin I.; Agostini, Pierre; DiMauro, Louis F.

2017-12-01

Strong-field-ionization yield versus intensity is investigated for various atomic targets (Ne, Ar, Kr, Xe, Na, K, Zn, and Mg) and light polarization from visible to mid-infrared (0.4-4 μ m ), from multiphoton to tunneling regimes. The experimental findings (normalized yield vs intensity, ratio of circular to linear polarization and saturation intensities) are compared to the theoretical models of Perelomov-Popov-Terent'ev (PPT) and Ammosov-Delone-Krainov (ADK). While PPT is generally satisfactory, ADK validity is found, as expected, to be much more limited.

Ultrafast photodissociation dynamics of 1,4-diiodobenzene

NASA Astrophysics Data System (ADS)

Stankus, Brian; Zotev, Nikola; Rogers, David M.; Gao, Yan; Odate, Asami; Kirrander, Adam; Weber, Peter M.

2018-05-01

The photodissociation dynamics of 1,4-diiodobenzene is investigated using ultrafast time-resolved photoelectron spectroscopy. Following excitation by laser pulses at 271 nm, the excited-state dynamics is probed by resonance-enhanced multiphoton ionization with 405 nm probe pulses. A progression of Rydberg states, which come into resonance sequentially, provide a fingerprint of the dissociation dynamics of the molecule. The initial excitation decays with a lifetime of 33 ± 4 fs, in good agreement with a previous study. The spectrum is interpreted by reference to ab initio calculations at the CASPT2(18,14) level, including spin-orbit coupling. We propose that both the 5B1 and 6B1 states are excited initially, and based on the calculations, we identify diabatic spin-orbit coupled states corresponding to the main dissociation pathways.

Total angular momenta of high-lying odd levels of U I at ∼ 4 eV using resonance ionization laser polarization spectroscopy

NASA Astrophysics Data System (ADS)

Rath, Asawari D.; Kundu, S.; Ray, A. K.

2018-02-01

Laser induced photoionization of atoms shows significant dependence on the choice of polarizations of lasers. In multi-step, multi-photon excitation and subsequent ionization of atoms different polarization combinations of the exciting lasers lead to distinctly different ion yields. This fact is exploited in this work to determine total angular momenta of odd-parity energy levels of U I lying at ∼ 4 eV from its ground level using resonance ionization laser polarization spectroscopy in time of flight mass spectrometer. These levels are populated by two-step resonant excitation using two pulsed dye lasers with preset polarizations of choice followed by nonresonant ionization by third laser. The dependence of ionization yield on specific polarizations of the first two lasers is studied experimentally for each level under consideration. This dependence when compared to simulations makes possible unambiguous assignment of J angular momenta to these levels.

The laser lightning rod system: thunderstorm domestication.

PubMed

Ball, L M

1974-10-01

An unusual application of the laser, namely protection of life and property from lightning, is described. The device relies on multiphoton ionization in mode-locked beams, rather than on collisional (avalanche) electron production. Feasibility is demonstrated numerically, and relevant principles explained. A method of mobile deployment is mentioned, by which economic (as opposed to scientific) feasibility might be achieved.

In situ optical measurements for characterization of flame species and remote sensing

NASA Astrophysics Data System (ADS)

Cullum, Brian Michael

1998-12-01

The following dissertation describes the use of spectroscopic techniques for both characterization of combustion intermediates and remote chemical sensing. The primary techniques that have been used for these measurements include, laser-induced fluorescence (LIF), time resolved LIF, resonance enhanced multiphoton ionization (REMPI) and Raman spectroscopy. A simple and quantitative means of measuring the efficiency of halogenated flame retardants is described, using laser-induced fluorescence (LIF). Intensity based LIF measurements of OH radical have been used to quantitatively measure the efficacy of halogenated flame retardant/polymer plaques. Temporally resolved LIF has been used to determine the extent to which the chemical kinetic theory of flame retardation applies to the effect of these compounds on combustion. We have shown that LIF of OH radicals is a very sensitive means of measuring the efficiency of these flame retardants as well as the giving information about the nature of flame retardation. In addition, we have developed a technique for the introduction of insoluble polymer plaques into a flame for fluorescence analysis. A high power pulsed Nd:YAG laser is used to ablate the sample into the flame while a second pulse from a dye laser is used to measure the LIF of OH radicals. Spectroscopic techniques are also very useful for trace remote analysis of environmental pollutants via optical fibers. A simple fiber-optic probe suitable for remote analysis using resonance enhanced multiphoton ionization (REMPI) has been developed for this purpose and is used to determine the toluene/gasoline concentration in water samples via a headspace measurement. The limit of detection for toluene in water using this probe is 0.54 ppb (wt/wt) with a sample standard deviation of 0.02 ppb (wt/wt). Another technique that has great potential for optical sensing is fluorescence lifetime imaging. A new method for measuring fluorescence lifetime images of quickly decaying species has been developed. This method employs a high powered pulsed laser that excites the fluorescent species in a dual pulse manner, and a non-gated charge coupled device (CCD) for detection of the fluorescence. Unlike other fluorescence lifetime imaging methods, this technique has the potential of monitoring fluorescent species with picosecond lifetimes.

Torsional, Vibrational and Vibration-Torsional Levels in the S_{1} and Ground Cationic D_{0}^{+} States of Para-Fluorotoluene

NASA Astrophysics Data System (ADS)

Gardner, Adrian M.; Tuttle, William Duncan; Whalley, Laura E.; Claydon, Andrew; Carter, Joseph H.; Wright, Timothy G.

2017-06-01

The S_{1} electronic state and ground state of the cation of para-fluorotoluene (pFT) have been investigated using resonance-enhanced multiphoton ionization (REMPI) spectroscopy and zero-kinetic-energy (ZEKE) spectroscopy. Here we focus on the low wavenumber region where a number of "pure" torsional, fundamental vibrational and vibration-torsional levels are expected; assignments of observed transitions are discussed, which are compared to results of published work on toluene (methylbenzene) from the Lawrance group. The similarity in the activity observed in the excitation spectrum of the two molecules is striking. A. M. Gardner, W. D. Tuttle, L. Whalley, A. Claydon, J. H. Carter and T. G. Wright, J. Chem. Phys., 145, 124307 (2016). J. R. Gascooke, E. A. Virgo, and W. D. Lawrance J. Chem. Phys., 143, 044313 (2015).

Multi-Wavelength Laser Transmitter for the Two-Step Laser Time-of-Flight Mass Spectrometer

NASA Technical Reports Server (NTRS)

Yu, Anthony W.; Li, Steven X.; Fahey, Molly E.; Grubisic, Andrej; Farcy, Benjamin J.; Uckert, Kyle; Li, Xiang; Getty, Stephanie

2017-01-01

Missions to diverse Outer Solar System bodies will require investigations that can detect a wide range of organics in complex mixtures, determine the structure of selected molecules, and provide powerful insights into their origin and evolution. Previous studies from remote spectroscopy of the Outer Solar System showed a diverse population of macromolecular species that are likely to include aromatic and conjugated hydrocarbons with varying degrees of methylation and nitrile incorporation. In situ exploration of Titan's upper atmosphere via mass and plasma spectrometry has revealed a complex mixture of organics. Similar material is expected on the Ice Giants, their moons, and other Outer Solar System bodies, where it may subsequently be deposited onto surface ices. It is evident that the detection of organics on other planetary surfaces provides insight into the chemical and geological evolution of a Solar System body of interest and can inform our understanding of its potential habitability. We have developed a prototype two-step laser desorption/ionization time-of-flight mass spectrometer (L2MS) instrument by exploiting the resonance-enhanced desorption of analyte. We have successfully demonstrated the ability of the L2MS to detect hydrocarbons in organically-doped analog minerals, including cryogenic Ocean World-relevant ices and mixtures. The L2MS instrument operates by generating a neutral plume of desorbed analyte with an IR desorption laser pulse, followed at a delay by a ultraviolet (UV) laser pulse, ionizing the plume. Desorption of the analyte, including trace organic species, may be enhanced by selecting the wavelength of the IR desorption laser to coincide with IR absorption features associated with vibration transitions of minerals or organic functional groups. In this effort, a preliminary laser developed for the instrument uses a breadboard mid-infrared (MIR) desorption laser operating at a discrete 3.475 µm wavelength, and a breadboard UV ionization laser operating at a wavelength of 266 nm. The MIR wavelength was selected to overlap the C-H stretch vibrational transition of certain aromatic hydrocarbons, and the UV wavelength provides additional selectivity to aromatic species via UV resonance-enhanced multiphoton ionization effects. The use of distinct laser wavelengths allows efficient coupling to the vibrational and electronic spectra of the analyte in independent desorption and ionization steps, mitigating excess energy that can lead to fragmentation during the ionization process and leading to selectivity that can aid in data interpretation.

Dynamics of focused femtosecond laser pulse during photodisruption of crystalline lens

NASA Astrophysics Data System (ADS)

Gupta, Pradeep Kumar; Singh, Ram Kishor; Sharma, R. P.

2018-04-01

Propagation of laser pulses of femtosecond time duration (focused through a focusing lens inside the crystalline lens) has been investigated in this paper. Transverse beam diffraction, group velocity dispersion, graded refractive index structure of the crystalline lens, self-focusing, and photodisruption in which plasma is formed due to the high intensity of laser pulses through multiphoton ionization have been taken into account. The model equations are the modified nonlinear Schrödinger equation along with a rate equation that takes care of plasma generation. A close analysis of model equations suggests that the femtosecond laser pulse duration is critical to the breakdown in the lens. Our numerical simulations reveal that the combined effect of self-focusing and multiphoton ionization provides the breakdown threshold. During the focusing of femtosecond laser pulses, additional spatial pulse splitting arises along with temporal splitting. This splitting of laser pulses arises on account of self-focusing, laser induced breakdown, and group velocity distribution, which modifies the shape of laser pulses. The importance of the present study in cavitation bubble generation to improve the elasticity of the eye lens has also been discussed in this paper.

Oleic acid-enhanced transdermal delivery pathways of fluorescent nanoparticles

NASA Astrophysics Data System (ADS)

Lo, Wen; Ghazaryan, Ara; Tso, Chien-Hsin; Hu, Po-Sheng; Chen, Wei-Liang; Kuo, Tsung-Rong; Lin, Sung-Jan; Chen, Shean-Jen; Chen, Chia-Chun; Dong, Chen-Yuan

2012-05-01

Transdermal delivery of nanocarriers provides an alternative pathway to transport therapeutic agents, alleviating pain, improving compliance of patients, and increasing overall effectiveness of delivery. In this work, enhancement of transdermal delivery of fluorescent nanoparticles and sulforhodamine B with assistance of oleic acid was visualized utilizing multiphoton microscopy (MPM) and analyzed quantitatively using multi-photon excitation-induced fluorescent signals. Results of MPM imaging and MPM intensity-based spatial depth-dependent analysis showed that oleic acid is effective in facilitating transdermal delivery of nanoparticles.

O({sup 3}P{sub J}) formation and desorption by 157-nm photoirradiation of amorphous solid water

DOE Office of Scientific and Technical Information (OSTI.GOV)

DeSimone, Alice J.; Orlando, Thomas M., E-mail: thomas.orlando@chemistry.gatech.edu; School of Physics, Georgia Institute of Technology, Atlanta, Georgia 30332–0400

2014-03-07

Photodissociation of amorphous solid water (ASW) deposited on a thinly oxidized copper substrate at 82 K was studied by measuring O({sup 3}P{sub J=2,1,0}) photoproducts detected with resonance-enhanced multiphoton ionization. For each spin-orbit state, the oxygen atom time-of-flight spectrum was measured as a function of H{sub 2}O exposure, which is related to ice thickness, and 157-nm irradiation time. Four Maxwell-Boltzmann distributions with translational temperatures of 10 000 K, 1800 K, 400 K, and 82 K were found to fit the data. The most likely formation mechanisms are molecular elimination following ionization of water and ion-electron recombination, secondary recombination of hydroxyl radicals, andmore » photodissociation of adsorbed hydroxyl radicals. Evidence for O-atom diffusion through bulk ASW was found for H{sub 2}O exposures of at least 5 Langmuir (1 L = 10{sup −6} Torr s). The cross sections for O({sup 3}P{sub 2}) depletion were 1.3 × 10{sup −19} and 6.5 × 10{sup −20} cm{sup 2} for 1 and 5 L, respectively.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Barc, B.; Ryszka, M.; Spurrell, J.

Multi-photon ionization (MPI) of the RNA base uracil has been studied in the wavelength range 220–270 nm, coinciding with excitation to the S{sub 2}(ππ*) state. A fragment ion at m/z = 84 was produced by 2-photon absorption at wavelengths ≤232 nm and assigned to C{sub 3}H{sub 4}N{sub 2}O{sup +} following CO abstraction. This ion has not been observed in alternative dissociative ionization processes (notably electron impact) and its threshold is close to recent calculations of the minimum activation energy for a ring opening conical intersection to a σ(n-π)π* closed shell state. Moreover, the predicted ring opening transition leaves a COmore » group at one end of the isomer, apparently vulnerable to abstraction. An MPI mass spectrum of uracil-water clusters is presented for the first time and compared with an equivalent dry measurement. Hydration enhances certain fragment ion pathways (particularly C{sub 3}H{sub 3}NO{sup +}) but represses C{sub 3}H{sub 4}N{sub 2}O{sup +} production. This indicates that hydrogen bonding to water stabilizes uracil with respect to neutral excited-state ring opening.« less

Spatial Characterization of Polycyclic Aromatic Hydrocarbons in 2008 TC3 Samples

NASA Astrophysics Data System (ADS)

Sabbah, Hassan; Morrow, A.; Zare, R. N.; Jenniskens, P.

2009-09-01

Hassan Sabbah1, Amy L. Morrow1, Richard N. Zare1 and Petrus Jenniskens2 1Stanford University, Stanford, California 94305, 2 SETI Institute, Carl Sagan Center, 515 North Whisman Road, Mountain View, California 94043, USA. In October 2006 a small asteroid (2-3 meters) was observed in outer space. On October 7, 2008, it entered the Earth's atmosphere creating a fireball over Northern Sudan. Some 280 meteorites were collected by the University of Khartoum. In order to explore the existence of organic materials, specifically polycyclic aromatic hydrocarbons (PAHs), we applied two-step laser desorption laser ionization mass spectrometry (L2MS) to some selected fragments. This technique consists of desorbing with a pulsed infrared laser beam the solid materials into a gaseous phase with no fragmentation followed by resonance enhanced multiphoton ionization to analyze the PAH content. L2MS was already applied to an array of extraterrestrial objects including interplanetary dust particles IDPs, carbonaceous chondrites and comet coma particles. Moreover, spatial resolution of PAHs in 2008 TC3 samples was achieved to explore the heterogeneity within individual fragments. The results of these studies and their contribution to understanding the formation of this asteroid will be discussed.

Wavelength Dependence of Nanosecond IR Laser-Induced Breakdown in Water: Evidence for Multiphoton Initiation via an Intermediate State

DTIC Science & Technology

2015-04-29

bubble generation and shock wave emission in water for femtosecond to nanosecond laser pulses . ...breakdown threshold in water for nanosecond (ns) IR laser pulses . Avalanche ionization (AI) is the most powerful mechanism driving IR ns laser-induced...acknowledged that femtosecond (fs) and picosecond (ps) IR breakdown is initiated by photoionization because ultrashort pulses are sufficiently

Analysis of Parent/Nitrated Polycyclic Aromatic Hydrocarbons in Particulate Matter 2.5 Based on Femtosecond Ionization Mass Spectrometry.

PubMed

Itouyama, Noboru; Matsui, Taiki; Yamamoto, Shigekazu; Imasaka, Tomoko; Imasaka, Totaro

2016-02-01

Particulate matter 2.5 (PM2.5), collected from ambient air in Fukuoka City, was analyzed by gas chromatography combined with multiphoton ionization mass spectrometry using an ultraviolet femtosecond laser (267 nm) as the ionization source. Numerous parent polycyclic aromatic hydrocarbons (PPAHs) were observed in a sample extracted from PM2.5, and their concentrations were determined to be in the range from 30 to 190 pg/m(3) for heavy PPAHs. Standard samples of nitrated polycyclic aromatic hydrocarbons (NPAHs) were examined, and the limits of detection were determined to be in the picogram range. The concentration of NPAH adsorbed on PM2.5 in the air was less than 900-1300 pg/m(3). Graphical Abstract ᅟ.

Impact of Coulomb potential on peak structures arising in momentum and low-energy photoelectron spectra produced in strong-field ionization of laser-irradiated atoms

NASA Astrophysics Data System (ADS)

Pyak, P. E.; Usachenko, V. I.

2018-03-01

The phenomenon of pronounced peak structure(s) of longitudinal momentum distributions as well as a spike-like structure of low-energy spectra of photoelectrons emitted from laser-irradiated Ar and Ne atoms in a single ionization process is theoretically studied in the tunneling and multiphoton regimes of ionization. The problem is addressed assuming only the direct above-threshold ionization (ATI) as a physical mechanism underlying the phenomenon under consideration (viz. solely contributing to observed photoelectron momentum distributions (PMD)) and using the Coulomb-Volkov (CV) ansatz within the frame of conventional strong-field approximation (SFA) applied in the length-gauge formulation. The developed CV-SFA approach also incorporates the density functional theory essentially exploited for numerical composition of initial (laser-free) atomic state(s) constructed from atomic orbitals of Gaussian type. Our presented CV-SFA based (and laser focal-volume averaged) calculation results proved to be well reproducing both the pronounced double-peak and/or ATI-like multi-peak structure(s) experimentally observed in longitudinal PMD under conditions of tunneling and/or multiphoton regime, respectively. In addition, our CV-SFA results presented for tunneling regime also suggest and remarkably reproduce a pronounced structure observed in relevant experiments as a ‘spike-like’ enhanced maximum arising in low-energy region (around the value of about 1 eV) of photoelectron spectra. The latter consistency allows to identify and interpret these results as the so-called low-energy structure (LES) since the phenomenon proved to appear as the most prominent if the influence of Coulomb potential on photoelectron continuum states is maximally taken into account under calculations (viz. if the parameter Z in CV’s functions is put equal to 1). Moreover, the calculated LES proved to correspond (viz., established as closely related) to the mentioned double-peak structure arising in the low-momentum region ({p}| | ≤slant | 0.2| a.u.) of longitudinal PMDs calculated under condition of the tunneling regime. Thus, the phenomena under consideration can be well understood and adequately interpreted beyond the terms and/or concepts of various different alternative strong-field approaches and models (such as e.g., extensively invoked and exploited nowadays though, more sophisticated SFA-based ‘rescattering’ mechanism) compared to which, the currently applied CV-SFA model (through the same underlying physical mechanism of solely direct ATI suggested) is additionally able to provide and reveal an intimate and transparent interrelation between the phenomena of LES and double-peak structure arising in PMDs observed in the tunneling regime.

A multiphoton objective design with incorporated beam splitter for enhanced fluorescence collection

PubMed Central

McMullen, Jesse D.; Zipfel, Warren R.

2010-01-01

We present a de novo design of an objective for use in multi-photon (MPM) and second harmonic generation (SHG) microscopy. This objective was designed to have a large field of view (FOV), while maintaining a moderate numerical aperture (NA) and relative straight forward construction. A dichroic beam splitter was incorporated within the objective itself allowing for an increase in the front aperture of the objective and corresponding enhancement of the solid angle of collected emission by an order of magnitude over existing designs. PMID:20389554

A multiphoton objective design with incorporated beam splitter for enhanced fluorescence collection.

PubMed

McMullen, Jesse D; Zipfel, Warren R

2010-03-15

We present a de novo design of an objective for use in multi-photon (MPM) and second harmonic generation (SHG) microscopy. This objective was designed to have a large field of view (FOV), while maintaining a moderate numerical aperture (NA) and relative straight forward construction. A dichroic beam splitter was incorporated within the objective itself allowing for an increase in the front aperture of the objective and corresponding enhancement of the solid angle of collected emission by an order of magnitude over existing designs.

Detection of gaseous compounds by needle trap sampling and direct thermal-desorption photoionization mass spectrometry: concept and demonstrative application to breath gas analysis.

PubMed

Kleeblatt, Juliane; Schubert, Jochen K; Zimmermann, Ralf

2015-02-03

A fast detection method to analyze gaseous organic compounds in complex gas mixtures was developed, using a needle trap device (NTD) in conjunction with thermal-desorption photoionization time-of-flight mass spectrometry (TD-PI-TOFMS). The mass spectrometer was coupled via a deactivated fused silica capillary to an injector of a gas chromatograph. In the hot injector, the analytes collected on the NTD were thermally desorbed and directly transferred to the PI-TOFMS ion source. The molecules are softly ionized either by single photon ionization (SPI, 118 nm) or by resonance enhanced multiphoton ionization (REMPI, 266 nm), and the molecular ion signals are detected in the TOF mass analyzer. Analyte desorption and the subsequent PI-TOFMS detection step only lasts ten seconds. The specific selectivity of REMPI (i.e., aromatic compounds) and universal ionization characteristics render PI-MS as a promising detection system. As a first demonstrative application, the alveolar phase breath gas of healthy, nonsmoking subjects was sampled on NTDs. While smaller organic compounds such as acetone, acetaldehyde, isoprene, or cysteamine can be detected in the breath gas with SPI, REMPI depicts the aromatic substances phenol and indole at 266 nm. In the breath gas of a healthy, smoking male subject, several xenobiotic substances such as benzene, toluene, styrene, and ethylbenzene can be found as well. Furthermore, the NTD-REMPI-TOFMS setup was tested for breath gas taken from a mechanically ventilated pig under continuous intravenous propofol (2,6-diisopropylphenol, narcotic drug) infusion.

Measurements of the Activation Energies for Atomic Hydrogen Diffusion on Pure Solid CO

NASA Astrophysics Data System (ADS)

Kimura, Y.; Tsuge, M.; Pirronello, V.; Kouchi, A.; Watanabe, N.

2018-05-01

The diffusion of hydrogen atoms on dust grains is a key process in the formation of interstellar H2 and some hydrogenated molecules such as formaldehyde and methanol. We investigate the adsorption and diffusion of H atoms on pure solid CO as an analog of dust surfaces observed toward some cold interstellar regions. Using a combination of photostimulated desorption and resonance-enhanced multiphoton ionization methods to detect H atoms directly, the relative adsorption probabilities and diffusion coefficients of the H atoms are measured on pure solid CO at 8, 12, and 15 K. There is little difference between the diffusion coefficients of the hydrogen and deuterium atoms, indicating that the diffusion is limited by thermal hopping. The activation energies controlling the H-atom diffusion depend on the surface temperature, and values of 22, 30, and ∼37 meV were obtained for 8, 12, and 15 K, respectively.

Spectroscopic study on deuterated benzenes. II. High-resolution laser spectroscopy and rotational structure in the S{sub 1} state

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kunishige, Sachi; Katori, Toshiharu; Baba, Masaaki, E-mail: baba@kuchem.kyoto-u.ac.jp

High-resolution spectra of the S{sub 1}←S{sub 0} transition in jet-cooled deuterated benzenes were observed using pulse dye amplification of single-mode laser light and mass-selective resonance enhanced multiphoton ionization (REMPI) detection. The vibrational and rotational structures were accurately analyzed for the vibronic levels in the S{sub 1} state. The degenerate 6{sup 1} levels of C{sub 6}H{sub 6} or C{sub 6}D{sub 6} are split into 6a{sup 1} and 6b{sup 1} in many of deuterated benzenes. The rigid-rotor rotational constants were assessed and found to be slightly different between 6a and 6b because of different mean molecular structures. Their rotational levels are significantlymore » shifted by Coriolis interactions. It was found that the Coriolis parameter proportionally changed with the number of substituted D atoms.« less

Torsional, Vibrational and Vibration-Torsional Levels in the S_{1} and Ground Cationic D_{0}^{+} States of Para-Xylene

NASA Astrophysics Data System (ADS)

Gardner, Adrian M.; Tuttle, William Duncan; Groner, Peter; Wright, Timothy G.

2017-06-01

Insight gained from examining the "pure" torsional, vibrational and vibration-torsional (vibtor) levels of the single rotor molecules: toluene (methylbenzene) and para-fluorotoluene (pFT), is applied to the double rotor para-xylene (p-dimethylbenzene) molecule . Resonance-enhanced multiphoton ionization (REMPI) spectroscopy and zero-kinetic-energy (ZEKE) spectroscopy are employed in order to investigate the S_{1} and ground cationic states of para-xylene. Observed transitions are assigned in the full molecular symmetry group (G_{72}) for the first time. J. R. Gascooke, E. A. Virgo, and W. D. Lawrance, J. Chem. Phys., 143, 044313 (2015). A. M. Gardner, W. D. Tuttle, L. Whalley, A. Claydon, J. H. Carter and T. G. Wright, J. Chem. Phys., 145, 124307 (2016). A. M. Gardner, W. D. Tuttle, P. Groner and T. G. Wright, J. Chem. Phys., (2017, in press).

Mass-Selective Chiral Analysis

NASA Astrophysics Data System (ADS)

Boesl, Ulrich; Kartouzian, Aras

2016-06-01

Three ways of realizing mass-selective chiral analysis are reviewed. The first is based on the formation of diastereomers that are of homo- and hetero- type with respect to the enantiomers of involved chiral molecules. This way is quite well-established with numerous applications. The other two ways are more recent developments, both based on circular dichroism (CD). In one, conventional or nonlinear electronic CD is linked to mass spectrometry (MS) by resonance-enhanced multiphoton ionization. The other is based on CD in the angular distribution of photoelectrons, which is measured in combination with MS via photoion photoelectron coincidence. Among the many important applications of mass-selective chiral analysis, this review focuses on its use as an analytical tool for the development of heterogeneous enantioselective chemical catalysis. There exist other approaches to combine chiral analysis and mass-selective detection, such as chiral chromatography MS, which are not discussed here.

Detailed Observation of Multiphoton Emission Enhancement from a Single Colloidal Quantum Dot Using a Silver-Coated AFM Tip.

PubMed

Takata, Hiroki; Naiki, Hiroyuki; Wang, Li; Fujiwara, Hideki; Sasaki, Keiji; Tamai, Naoto; Masuo, Sadahiro

2016-09-14

The enhancement of multiphoton emission from a single colloidal nanocrystal quantum dot (NQD) interacting with a plasmonic nanostructure was investigated using a silver-coated atomic force microscopy tip (AgTip) as the plasmonic nanostructure. Using the AgTip, which exhibited a well-defined localized surface plasmon (LSP) resonance band, we controlled the spectral overlap and the distance between the single NQD and the AgTip. The emission behavior of the single NQD when approaching the AgTip at the nanometer scale was measured using off-resonance (405 nm) and resonance (465 nm) excitation of the LSP. We directly observed the conversion of the single-photon emission from a single NQD to multiphoton emission with reduction of the emission lifetime at both excitation wavelengths as the NQD-AgTip distance decreased, whereas a decrease and increase in the emission intensity were observed at 405 and 465 nm excitation, respectively. By combining theoretical analysis and the numerical simulation of the AgTip, we deduced that the enhancement of the multiphoton emission was caused by the quenching of the single-exciton state due to the energy transfer from the NQD to the AgTip and that the emission intensity was increased by enhancement of the excitation rate due to the electric field of the LSP on the AgTip. These results provide evidence that the photon statistics and the photon flux from the single NQD can be manipulated by the plasmonic nanostructure through control of the spectral overlap and the distance.

Platinum Acetylide Two-Photon Chromophores (Preprint)

DTIC Science & Technology

2007-04-01

nonlinear photonics,6-s microfabrication,9,10 fluorescence imaging, II and photodynamic therapy.12Instantaneous absorption of two lower energy photons...results in initiation of the same photophysical processes as one-photon absorption (lP A) of one high- energy photon. This is advantageous for two...reasons. The first is that because of the use of a lower energy photon a material will be guarded from ionization effects from multiphoton absorption in

Optimal control of multiphoton ionization dynamics of small alkali aggregates

NASA Astrophysics Data System (ADS)

Lindinger, A.; Bartelt, A.; Lupulescu, C.; Vajda, S.; Woste, Ludger

2003-11-01

We have performed transient multi-photon ionization experiments on small alkali clusters of different size in order to probe their wave packet dynamics, structural reorientations, charge transfers and dissociative events in different vibrationally excited electronic states including their ground state. The observed processes were highly dependent on the irradiated pulse parameters like wavelength range or its phase and amplitude; an emphasis to employ a feedback control system for generating the optimum pulse shapes. Their spectral and temporal behavior reflects interesting properties about the investigated system and the irradiated photo-chemical process. First, we present the vibrational dynamics of bound electronically excited states of alkali dimers and trimers. The scheme for observing the wave packet dynamics in the electronic ground state using stimulated Raman-pumping is shown. Since the employed pulse parameters significantly influence the efficiency of the irradiated dynamic pathways photo-induced ioniziation experiments were carried out. The controllability of 3-photon ionization pathways is investigated on the model-like systems NaK and K2. A closed learning loop for adaptive feedback control is used to find the optimal fs pulse shape. Sinusoidal parameterizations of the spectral phase modulation are investigated in regard to the obtained optimal field. By reducing the number of parameters and thereby the complexity of the phase moduation, optimal pulse shapes can be generated that carry fingerprints of the molecule's dynamical properties. This enables to find "understandable" optimal pulse forms and offers the possiblity to gain insight into the photo-induced control process. Characteristic motions of the involved wave packets are proposed to explain the optimized dynamic dissociation pathways.

Which role does multiphoton interference play in small phase estimation in quantum Fourier transform interferometers?

NASA Astrophysics Data System (ADS)

Zimmermann, Olaf; Tamma, Vincenzo

Recently, quantum Fourier transform interferometers have been demonstrated to allow a quantum metrological enhancement in phase sensitivity for a small number n of identical input single photons [J. P. Olson, K. R. Motes, P. M. Birchall, N. M. Studer, M. LaBorde, T. Moulder, P. P. Rohde and J. P. Dowling, Phys. Rev. A 96 (2017) 013810; K. R. Motes, J. P. Olson, E. J. Rabeaux, J. P. Dowling, S. J. Olson and P. P. Rohde, Phys. Rev. Lett. 114 (2015) 170802; O. Zimmermann, Bachelor Thesis (Ulm University, 2015) arXiv: 1710.03805.]. However, multiphoton distinguishability at the detectors can play an important role from an experimental point of view [V. Tamma and S. Laibacher, Phys. Rev. Lett. 114 (2015) 243601.]. This raises a fundamental question: How is the phase sensitivity affected when the photons are completely distinguishable at the detectors and therefore do not interfere? In other words, which role does multiphoton interference play in these schemes? Here, we show that for small phase values, the phase sensitivity achievable in the proposed schemes with indistinguishable photons is enhanced only by a constant factor with respect to the case of completely distinguishable photons at the detectors. Interestingly, this enhancement arises from the interference of only a polynomial number (in n) of the total n! multiphoton path amplitudes in the n-port interferometer. These results are independent of the number n of single photons and of the phase weight factors employed at each interferometer channel.

Interatomic Coulombic decay cascades in multiply excited neon clusters

PubMed Central

Nagaya, K.; Iablonskyi, D.; Golubev, N. V.; Matsunami, K.; Fukuzawa, H.; Motomura, K.; Nishiyama, T.; Sakai, T.; Tachibana, T.; Mondal, S.; Wada, S.; Prince, K. C.; Callegari, C.; Miron, C.; Saito, N.; Yabashi, M.; Demekhin, Ph. V.; Cederbaum, L. S.; Kuleff, A. I.; Yao, M.; Ueda, K.

2016-01-01

In high-intensity laser light, matter can be ionized by direct multiphoton absorption even at photon energies below the ionization threshold. However on tuning the laser to the lowest resonant transition, the system becomes multiply excited, and more efficient, indirect ionization pathways become operative. These mechanisms are known as interatomic Coulombic decay (ICD), where one of the species de-excites to its ground state, transferring its energy to ionize another excited species. Here we show that on tuning to a higher resonant transition, a previously unknown type of interatomic Coulombic decay, intra-Rydberg ICD occurs. In it, de-excitation of an atom to a close-lying Rydberg state leads to electron emission from another neighbouring Rydberg atom. Moreover, systems multiply excited to higher Rydberg states will decay by a cascade of such processes, producing even more ions. The intra-Rydberg ICD and cascades are expected to be ubiquitous in weakly-bound systems exposed to high-intensity resonant radiation. PMID:27917867

Real-time detection of hazardous materials in air

NASA Astrophysics Data System (ADS)

Schechter, Israel; Schroeder, Hartmut; Kompa, Karl L.

1994-03-01

A new detection system has been developed for real-time analysis of organic compounds in ambient air. It is based on multiphoton ionization by an unfocused laser beam in a single parallel-plate device. Thus, the ionization volume can be relatively large. The amount of laser created ions is determined quantitatively from the induced total voltage drop between the biased plates (Q equals (Delta) V(DOT)C). Mass information is obtained from computer analysis of the time-dependent signal. When a KrF laser (5 ev) is used, most of the organic compounds can be ionized in a two-photon process, but none of the standard components of atmospheric air are ionized by this process. Therefore, this instrument may be developed as a `sniffer' for organic materials. The method has been applied for benzene analysis in air. The detection limit is about 10 ppb. With a simple preconcentration technique the detection limit can be decreased to the sub-ppb range. Simple binary mixtures are also resolved.

Multiphoton microscopy and image guided light activated therapy using nanomaterials (Conference Presentation)

NASA Astrophysics Data System (ADS)

Prasad, Paras N.

2017-02-01

This talk will focus on design and applications of nanomaterials exhibiting strong multiphoton upconversion for multiphoton microscopy as well as for image-guided and light activated therapy .1-3 Such processes can occur by truly nonlinear optical interactions proceeding through virtual intermediate states or by stepwise coupled linear excitations through real intermediate states. Multiphoton processes in biocompatible multifunctional nanoparticles allow for 3D deep tissue imaging. In addition, they can produce in-situ photon conversion of deep tissue penetrating near IR light into a needed shorter wavelength light for photo-activated therapy at a targeted site, thus overcoming the limited penetration of UV or visible light into biological media. We are using near IR emitters such as silicon quantum dots which also exhibit strong multiphoton excitation for multiphoton microscopy. Another approach involves nonlinear nanocrystals such as ZnO which can produce four wave mixing, sum frequency generation as well as second harmonic generation to convert a deep tissue penetrating Near IR light at the targeted biological site to a desired shorter wavelength light suitable for bio imaging or activation of a therapy. We have utilized this approach to activate a photosensitizer for photodynamic therapy. Yet another type of upconversion materials is rare-earth ion doped optical nanotransformers which transform a Near IR (NIR) light from an external source by sequential single photon absorption, in situ and on demand, to a needed wavelength. Applications of these nanotransformers in multiphoton photoacoustic imaging will also be presented. An exciting direction pursued by us using these multiphoton nanoparticles, is functional imaging of brain. Simultaneously, they can effect optogenetics for regioselective stimulation of neurons for providing an effective intervention/augmentation strategy to enhance the cognitive state and lead to a foundation for futuristic vision of super human capabilities. Challenges and opportunities will be discussed.

Reaction dynamics of Al + O₂ → AlO + O studied by a crossed-beam velocity map imaging technique: vib-rotational state selected angular-kinetic energy distribution.

PubMed

Honma, Kenji; Miyashita, Kazuki; Matsumoto, Yoshiteru

2014-06-07

Oxidation reaction of a gas-phase aluminum atom by a molecular oxygen was studied by a crossed-beam condition at 12.4 kJ/mol of collision energy. A (1+1) resonance-enhanced multiphoton ionization (REMPI) via the D(2)Σ(+)-X(2)Σ(+) transition of AlO was applied to ionize the product. The REMPI spectrum was analyzed to determine rotational state distributions for v = 0-2 of AlO. For several vib-rotational states of AlO, state selected angular and kinetic energy distributions were determined by a time-sliced ion imaging technique for the first time. Kinetic energy distributions were well represented by that taken into account initial energy spreads of collision energy and the population of the spin-orbit levels of the counter product O((3)P(J)) determined previously. All angular distributions showed forward and backward peaks, and the forward peaks were more pronounced than the backward one for the states of low internal energy. The backward peak intensity became comparable to the forward one for the states of high internal energy. These results and the rotational state distributions suggested that the reaction proceeds via an intermediate which has a lifetime comparable to or shorter than its rotational period.

Laser Ionization Studies of Hydrocarbon Flames.

NASA Astrophysics Data System (ADS)

Bernstein, Jeffrey Scott

Resonance-enhanced multiphoton ionization (REMPI) and laser induced fluorescence (LIF) are applied as laser based flame diagnostics for studies of hydrocarbon combustion chemistry. rm CH_4/O_2, C _2H_4/O_2, and rm C_2H_6/O_2 low pressure ( ~20 Torr), stoichiometric burner stabilized flat flames are studied. Density profiles of intermediate flame species, existing at ppm concentrations, are mapped out as a function of distance from the burner head. Profiles resulting from REMPI and LIF detection are obtained for HCO, CH_3, H, O, OH, CH, and CO flame radicals. The above flame systems are computer modeled against currently accepted combustion mechanisms using the Chemkin and Premix flame codes developed at Sandia National Laboratories. The modeled profile densities show good agreement with the experimental results of the CH_4/O_2 flame system, thus confirming the current C1 kinetic flame mechanism. Discrepancies between experimental and modeled results are found with the C2 flames. These discrepancies are partially amended by modifying the rate constant of the rm C_2H_3+rm O_2 to H_2CO + HCO reaction. The modeled results computed with the modified rate constant strongly suggest that the kinetics of several or possibly many reactions in the C2 mechanism need refinement.

Photoelectron spectroscopy of aqueous solutions: Streaming potentials of NaX (X = Cl, Br, and I) solutions and electron binding energies of liquid water and X{sup −}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kurahashi, Naoya; Horio, Takuya; Suzuki, Toshinori, E-mail: suzuki@kuchem.kyoto-u.ac.jp

2014-05-07

The streaming potentials of liquid beams of aqueous NaCl, NaBr, and NaI solutions are measured using soft X-ray, He(I), and laser multiphoton ionization photoelectron spectroscopy. Gaseous molecules are ionized in the vicinity of liquid beams and the photoelectron energy shifts are measured as a function of the distance between the ionization point and the liquid beam. The streaming potentials change their polarity with concentration of electrolytes, from which the singular points of concentration eliminating the streaming potentials are determined. The streaming currents measured in air also vanish at these concentrations. The electron binding energies of liquid water and I{sup −},more » Br{sup −}, and Cl{sup −} anions are revisited and determined more accurately than in previous studies.« less

Chemical analyses of provided samples

NASA Technical Reports Server (NTRS)

Becker, Christopher H.

1993-01-01

Two batches of samples were received and chemical analysis was performed of the surface and near surface regions of the samples by the surface analysis by laser ionization (SALI) method. The samples included four one-inch optics and several paint samples. The analyses emphasized surface contamination or modification. In these studies, pulsed sputtering by 7 keV Ar+ and primarily single-photon ionization (SPI) by coherent 118 nm radiation (at approximately 5 x 10(exp 5) W/cm(sup 2) were used. For two of the samples, also multiphoton ionization (MPI) at 266 nm (approximately 5 x 10(exp 11) W/cm(sup 2) was used. Most notable among the results was the silicone contamination on Mg2 mirror 28-92, and that the Long Duration Exposure Facility (LDEF) paint sample had been enriched in K and Na and depleted in Zn, Si, B, and organic compounds relative to the control paint.

Far-Infrared Magneto-Optical Studies in Germanium and Indium-Antimonide at High Intensities

NASA Astrophysics Data System (ADS)

Leung, Michael

Observations of nonlinear magneto-optical phenomena occurring in p-type Germanium and n-type Indium Antimonide are reported. These include multi-photon ionization of impurity states, and a new observation, the magneto-photon ionization of impurity states, and a new observation, the magneto-photon drag effect. A novel source of far-infrared radiation has been used. This source uses a pulsed CO(,2) LASER to optically pump a super-radiant cell, generating light with intensities up to 100 KW/cm('2) and wavelengths from 66 (mu)m to 496 (mu)m in a pulse of 150 nanoseconds duration. The Germanium samples were doped with Gallium, which is a shallow acceptor with an ionization potential of 11 meV. At liquid Helium temperature virtually all charge carriers are bound to acceptor sites. However, the high intensity radiation unexpectedly ionizes the acceptors. This is demonstrated through measurements of photoconductivity, transmission and the photo-Hall Effect. This observation is unexpected because the photon energy is one-fourth the ionization potential. Rate equations describing sequential multiphoton excitations are in agreement with the experimental results. The intermediate states are postulated to be acceptor exciton band states. Studies of the photoexcited mobility at 496 (mu)m suggest that at non-saturating levels of photoexcitation, the primary scattering mechanism of hot holes in Germanium is by neutral impurities. A new magneto-optical effect, the magneto-photon drag effect, has been studied in both Germanium and Indium Antimonide. This is simply the absorption of momentum by free carriers, from an incident photon field. It has been found that the mechanism for this effect is different in the two materials. In Germanium, the effect occurs when carriers make optical transitions from the heavy hole band to the light hole band. Thus, the magneto-optical behavior depends heavily upon the band structure. On the other hand, a modified Drude model (independent electron) has been found to be reasonably successful in describing the effect in InSb. The inclusion of non-parabolicity and hot electron effects gives a consistent description of the experimental observations.

Fundamental mechanisms of laser damage of dielectric crystals by ultrashort pulse: ionization dynamics for the Keldysh model

NASA Astrophysics Data System (ADS)

Gruzdev, Vitaly

2014-12-01

Laser-induced ionization is a major process that initiates and drives the initial stages of laser-induced damage (LID) of high-quality transparent solids. The ionization and its contribution to LID are characterized in terms of the time-dependent ionization rate and conduction-band electron density. Considering femtosecond pulses of various durations (from 35 to 706 fs) and variable peak irradiances (from 0.01 to 60 TW/cm2), we use a single-rate equation to simulate time variations of conduction-band electron density and rates of the photoionization and impact ionization. The photoionization rate is evaluated with the Keldysh equation. At low irradiance, the electron density and total ionization rate demonstrate power scaling characteristic of multiphoton ionization. With the increase of irradiance, there is observed a saturation of the photoionization rate due to photoionization suppression by the Keldysh-type singularity during the increase in the number of simultaneously absorbed photons by 1. A striking result is that the saturation is followed by a stepwise transition from the ionization regime which is completely dominated by the photoionization to a regime totally dominated by the impact ionization. The transition results in the increase of the electron density by a few orders of magnitude induced by a variation of peak laser irradiance by about 15% to 20%. The physical effects that are involved are discussed.

Modification of emission photon statistics from single quantum dots using metal/SiO2 core/shell nanostructures.

PubMed

Naiki, Hiroyuki; Oikawa, Hidetoshi; Masuo, Sadahiro

2017-04-12

Emission photon statistics, i.e., single-photon and multi-photon emissions, of isolated QDs is required for tailoring optoelectronic applications. In this article, we demonstrate that the emission photon statistics can be modified by the control of the spectral overlap of the QDs with the localized surface plasmon resonance (LSPR) of the metal nanoparticle (metal NP) and by the distance between the QD and the metal NP. Moreover, the contribution to the modification of the emission photon statistics, which is the excitation and emission enhancements and the quenching generated by the spectral overlap and the distance, is elucidated. By fabricating well-defined SiO 2 -coated AgNPs and AuNPs (metal/SiO 2 ), the spectral overlap originated from the metal species of Ag and Au and the distance constituted by the thickness of the SiO 2 shell are controlled. The probability of single-photon emission of single QD was increased by the enhancement of the excitation rate via adjusting the distance using Ag/SiO 2 while the single-photon emission was converted to multi-photon emission by the effect of exciton quenching at a short distance and a small spectral overlap. By contrast, the probability of multi-photon emission was increased by enhancement of the multi-photon emission rate and the quenching via the spectral overlap using Au/SiO 2 . These results indicated the fundamental finding to control emission photon statistics in single QDs by controlling the spectral overlap and the distance, and understand the interaction of plasmonic nanostructures and single QD systems.

Differentiation and Distributions of DNA/Cisplatin Crosslinks by Liquid Chromatography-Electrospray Ionization-Infrared Multiphoton Dissociation Mass Spectrometry

PubMed Central

Xu, Zhe; Brodbelt, Jennifer S.

2013-01-01

Liquid chromatography-electrospray ionization-infrared multiphoton dissociation (IRMPD) mass spectrometry was developed to investigate the distributions of intrastrand crosslinks formed between cisplatin and two oligodeoxynucleotides (ODNs), d(A1T2G3G4G5T6A7C8C9C10A11T12) (G3-D) and its analog d(A1T2G3G4G5T6T7C8C9C10A11T12) (G3-H), that have been reported to adopt different secondary structures in solution. Based on the formation of site-specific fragment ions upon IRMPD, two isobaric crosslink products were differentiated for each ODN. The preferential formation of G3G4 and G4G5 crosslinks was determined as a function of reaction conditions, including incubation temperature and presence of metal ions. G3-D consistently exhibited a greater preference for formation of the G4G5 crosslink compared to the G3-H ODN. The ratio of G3G4:G4G5 crosslinks increased for both G3-D and G3-H at higher incubation temperatures or when metal salts were added. Comparison of the IRMPD fragmentation patterns of the unmodified ODNs and the intramolecular platinated crosslinks indicated that backbone cleavage was significantly suppressed near the crosslink. PMID:24135806

Correlated electron-nuclear dynamics in above-threshold multiphoton ionization of asymmetric molecule.

PubMed

Wang, Zhuo; Li, Min; Zhou, Yueming; Lan, Pengfei; Lu, Peixiang

2017-02-20

The partition of the photon energy into the subsystems of molecules determines many photon-induced chemical and physical dynamics in laser-molecule interactions. The electron-nuclear energy sharing from multiphoton ionization of molecules has been used to uncover the correlated dynamics of the electron and fragments. However, most previous studies focus on symmetric molecules. Here we study the electron-nuclear energy sharing in strong-field photoionization of HeH 2+ by solving the one-dimensional time-dependent Schrödinger equation (TDSE). Compared with symmetric molecules, the joint electron-nuclear energy spectrum (JES) of HeH 2+ reveals an anomalous energy shift at certain nuclear energies, while it disappears at higher and lower nuclear energies. Through tracing the time evolution of the wavepacket of bound states, we identify that this energy shift originates from the joint effect of the Stark shift, associated with the permanent dipole, and the Autler-Townes effect due to the coupling of the 2pσ and 2sσ states in strong fields. The energy shift in the JES appears at certain nuclear distances only when both Stark effect and Autler-Townes effect play important roles. We further demonstrate that the electron-nuclei energy sharing can be controlled by varying laser intensity for asymmetric molecules, providing alternative approaches to manipulate photochemical reactions for more complex molecules.

Factorization of laser-pulse ionization probabilities in the multiphotonic regime

NASA Astrophysics Data System (ADS)

Della Picca, R.; Fiol, J.; Fainstein, P. D.

2013-09-01

We present a detailed study of the ionization probability of H and H_{2}^{+} induced by a short intense laser pulse. Starting from a Coulomb-Volkov description of the process we derive a multipole-like expansion where each term is factored into two contributions: one that accounts for the effect of the electromagnetic field on the free-electron final state and a second factor that depends only on the target structure. Such a separation may be valuable to solve complex atomic or molecular systems as well as to interpret the dynamics of the process in simpler terms. We show that the series expansion converges rapidly, and thus the inclusion of the first few terms is sufficient to produce accurate results.

Jet-resolved vibronic structure in the higher excited states of N2O - Ultraviolet three-photon absorption spectroscopy from 80,000 to 90,000/cm

NASA Technical Reports Server (NTRS)

Patsilinakou, E.; Wiedmann, R. T.; Fotakis, C.; Grant, E. R.

1989-01-01

Ionization-detected UV multiphoton absorption spectroscopy of the excited states of N2O is presented, showing Rydberg structure within 20,000/cm of the first ionization threshold. Despite evidence for strong Rydberg-continuum coupling in the form of broadened bands and Fano line-shapes, the Rydberg structure persists, with atomic-like quantum defects and vibration structure well-matched with that of the ion. In the most clearly resolved spectrum, corresponding to the 3p(delta)1Pi state, Renner-Teller and Herzberg-Teller coupling of electronic and vibrational angular momentum are revealed. It is suggested that these mixings are properties of the N2O(+)Pi ion core.

Photochemical and Spectroscopic Effects Resulting from Excimer Laser Excitation.

NASA Astrophysics Data System (ADS)

Wang, Xuan Xiao

I. Photochemical production of ozone from pure oxygen using excimer lasers. Production of ozone was observed from experiments when oxygen was under a broadband pulsed KrF laser radiation. The production process was found to be autocatalytic. Mechanisms for the ozone formation were proposed. Experimental results over a range of oxygen pressure and laser pulse energy (irradiance) provided evidences in favor of the proposed mechanisms. Experiments were also numerically modeled. Good agreement between the experimental and the numerical results were observed, which provided further evidence to support the proposed mechanisms. Cross sections for some photochemical processes in the mechanisms were estimated. Production of ozone from pure oxygen under a ArF excimer laser radiation (193 nm) was also studied and numerically modeled. Effects of ambient water vapor on ozone production were investigated. Experimental results showed a fast ozone destruction when water vapor was present in the cell. However, numerical results obtained from the well-known OH and HO _2 chain ozone destruction mechanism predicted a slower ozone destruction. Possible reasons for the discrepancy are discussed. II. Resonance-enhanced multiphoton ionization of N_2 at 193 and 248 nm detected by N_sp{2}{+} fluorescence. Using a broadband excimer laser operating at 193 and 248 nm multiphoton ionization at high pressures in air and pure nitrogen has been detected by fluorescence from N_sp{2}{+} in the B-X firstnegative system. Measurements of the fluorescence intensity as a function of beam irradiance indicate resonance in N_2 at the energy of two 193 nm photons (2 + 1 REMPI) and three 248 nm photons (3 + 1 REMPI). Possible intermediate states are discussed. III. Excimer laser-induced fluorescence from some organic solvents. Fluorescence was observed from vapor phase benzene, toluene, p-xylene, benzyl chloride, methyl benzoate, acetic anhydride, ether, methanol, ethyl acetone, acetone, and 2-butanone using a broadband excimer laser operating at 248 nm and 308 nm as the source of excitation. Absolute fluorescence quantum yields for the substances under study were measured at 248 nm using toluene as the fluorescence standard. Fluorescence spectra from species produced from nonlinear photochemical processes were also studied.

Femtosecond response of polyatomic molecules to ultra-intense hard X-rays.

PubMed

Rudenko, A; Inhester, L; Hanasaki, K; Li, X; Robatjazi, S J; Erk, B; Boll, R; Toyota, K; Hao, Y; Vendrell, O; Bomme, C; Savelyev, E; Rudek, B; Foucar, L; Southworth, S H; Lehmann, C S; Kraessig, B; Marchenko, T; Simon, M; Ueda, K; Ferguson, K R; Bucher, M; Gorkhover, T; Carron, S; Alonso-Mori, R; Koglin, J E; Correa, J; Williams, G J; Boutet, S; Young, L; Bostedt, C; Son, S-K; Santra, R; Rolles, D

2017-06-01

X-ray free-electron lasers enable the investigation of the structure and dynamics of diverse systems, including atoms, molecules, nanocrystals and single bioparticles, under extreme conditions. Many imaging applications that target biological systems and complex materials use hard X-ray pulses with extremely high peak intensities (exceeding 10 20 watts per square centimetre). However, fundamental investigations have focused mainly on the individual response of atoms and small molecules using soft X-rays with much lower intensities. Studies with intense X-ray pulses have shown that irradiated atoms reach a very high degree of ionization, owing to multiphoton absorption, which in a heteronuclear molecular system occurs predominantly locally on a heavy atom (provided that the absorption cross-section of the heavy atom is considerably larger than those of its neighbours) and is followed by efficient redistribution of the induced charge. In serial femtosecond crystallography of biological objects-an application of X-ray free-electron lasers that greatly enhances our ability to determine protein structure-the ionization of heavy atoms increases the local radiation damage that is seen in the diffraction patterns of these objects and has been suggested as a way of phasing the diffraction data. On the basis of experiments using either soft or less-intense hard X-rays, it is thought that the induced charge and associated radiation damage of atoms in polyatomic molecules can be inferred from the charge that is induced in an isolated atom under otherwise comparable irradiation conditions. Here we show that the femtosecond response of small polyatomic molecules that contain one heavy atom to ultra-intense (with intensities approaching 10 20 watts per square centimetre), hard (with photon energies of 8.3 kiloelectronvolts) X-ray pulses is qualitatively different: our experimental and modelling results establish that, under these conditions, the ionization of a molecule is considerably enhanced compared to that of an individual heavy atom with the same absorption cross-section. This enhancement is driven by ultrafast charge transfer within the molecule, which refills the core holes that are created in the heavy atom, providing further targets for inner-shell ionization and resulting in the emission of more than 50 electrons during the X-ray pulse. Our results demonstrate that efficient modelling of X-ray-driven processes in complex systems at ultrahigh intensities is feasible.

Femtosecond response of polyatomic molecules to ultra-intense hard X-rays

DOE PAGES

Rudenko, A.; Inhester, L.; Hanasaki, K.; ...

2017-05-31

We report x-ray free-electron lasers enable the investigation of the structure and dynamics of diverse systems, including atoms, molecules, nanocrystals and single bioparticles, under extreme conditions. Many imaging applications that target biological systems and complex materials use hard X-ray pulses with extremely high peak intensities (exceeding 10 20 watts per square centimetre). However, fundamental investigations have focused mainly on the individual response of atoms and small molecules using soft X-rays with much lower intensities. Studies with intense X-ray pulses have shown that irradiated atoms reach a very high degree of ionization, owing to multiphoton absorption, which in a heteronuclear molecularmore » system occurs predominantly locally on a heavy atom (provided that the absorption cross-section of the heavy atom is considerably larger than those of its neighbours) and is followed by efficient redistribution of the induced charge. In serial femtosecond crystallography of biological objects—an application of X-ray free-electron lasers that greatly enhances our ability to determine protein structure—the ionization of heavy atoms increases the local radiation damage that is seen in the diffraction patterns of these objects and has been suggested as a way of phasing the diffraction data. On the basis of experiments using either soft or less-intense hard X-rays, it is thought that the induced charge and associated radiation damage of atoms in polyatomic molecules can be inferred from the charge that is induced in an isolated atom under otherwise comparable irradiation conditions. Here we show that the femtosecond response of small polyatomic molecules that contain one heavy atom to ultra-intense (with intensities approaching 10 20 watts per square centimetre), hard (with photon energies of 8.3 kiloelectronvolts) X-ray pulses is qualitatively different: our experimental and modelling results establish that, under these conditions, the ionization of a molecule is considerably enhanced compared to that of an individual heavy atom with the same absorption cross-section. This enhancement is driven by ultrafast charge transfer within the molecule, which refills the core holes that are created in the heavy atom, providing further targets for inner-shell ionization and resulting in the emission of more than 50 electrons during the X-ray pulse. Fnally, our results demonstrate that efficient modelling of X-ray-driven processes in complex systems at ultrahigh intensities is feasible.« less

Femtosecond response of polyatomic molecules to ultra-intense hard X-rays

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rudenko, A.; Inhester, L.; Hanasaki, K.

We report x-ray free-electron lasers enable the investigation of the structure and dynamics of diverse systems, including atoms, molecules, nanocrystals and single bioparticles, under extreme conditions. Many imaging applications that target biological systems and complex materials use hard X-ray pulses with extremely high peak intensities (exceeding 10 20 watts per square centimetre). However, fundamental investigations have focused mainly on the individual response of atoms and small molecules using soft X-rays with much lower intensities. Studies with intense X-ray pulses have shown that irradiated atoms reach a very high degree of ionization, owing to multiphoton absorption, which in a heteronuclear molecularmore » system occurs predominantly locally on a heavy atom (provided that the absorption cross-section of the heavy atom is considerably larger than those of its neighbours) and is followed by efficient redistribution of the induced charge. In serial femtosecond crystallography of biological objects—an application of X-ray free-electron lasers that greatly enhances our ability to determine protein structure—the ionization of heavy atoms increases the local radiation damage that is seen in the diffraction patterns of these objects and has been suggested as a way of phasing the diffraction data. On the basis of experiments using either soft or less-intense hard X-rays, it is thought that the induced charge and associated radiation damage of atoms in polyatomic molecules can be inferred from the charge that is induced in an isolated atom under otherwise comparable irradiation conditions. Here we show that the femtosecond response of small polyatomic molecules that contain one heavy atom to ultra-intense (with intensities approaching 10 20 watts per square centimetre), hard (with photon energies of 8.3 kiloelectronvolts) X-ray pulses is qualitatively different: our experimental and modelling results establish that, under these conditions, the ionization of a molecule is considerably enhanced compared to that of an individual heavy atom with the same absorption cross-section. This enhancement is driven by ultrafast charge transfer within the molecule, which refills the core holes that are created in the heavy atom, providing further targets for inner-shell ionization and resulting in the emission of more than 50 electrons during the X-ray pulse. Fnally, our results demonstrate that efficient modelling of X-ray-driven processes in complex systems at ultrahigh intensities is feasible.« less

Application of Laser Mass Spectrometry to Art and Archaeology

NASA Technical Reports Server (NTRS)

Gulian, Lase Lisa E.; Callahan, Michael P.; Muliadi, Sarah; Owens, Shawn; McGovern, Patrick E.; Schmidt, Catherine M.; Trentelman, Karen A.; deVries, Mattanjah S.

2011-01-01

REMPI laser mass spectrometry is a combination of resonance enhanced multiphoton ionization spectroscopy and time of flight mass spectrometry, This technique enables the collection of mass specific optical spectra as well as of optically selected mass spectra. Analytes are jet-cooled by entrainment in a molecular beam, and this low temperature gas phase analysis has the benefit of excellent vibronic resolution. Utilizing this method, mass spectrometric analysis of historically relevant samples can be simplified and improved; Optical selection of targets eliminates the need for chromatography while knowledge of a target's gas phase spectroscopy allows for facile differentiation of molecules that are in the aqueous phase considered spectroscopically indistinguishable. These two factors allow smaller sample sizes than commercial MS instruments, which in turn will require less damage to objects of antiquity. We have explored methods to optimize REMPI laser mass spectrometry as an analytical tool to archaeology using theobromine and caffeine as molecular markers in Mesoamerican pottery, and are expanding this approach to the field of art to examine laccaic acid in shellacs.

Dramatic enhancement of supercontinuum generation in elliptically-polarized laser filaments

PubMed Central

Rostami, Shermineh; Chini, Michael; Lim, Khan; Palastro, John P.; Durand, Magali; Diels, Jean-Claude; Arissian, Ladan; Baudelet, Matthieu; Richardson, Martin

2016-01-01

Broadband laser sources based on supercontinuum generation in femtosecond laser filamentation have enabled applications from stand-off sensing and spectroscopy to the generation and self-compression of high-energy few-cycle pulses. Filamentation relies on the dynamic balance between self-focusing and plasma defocusing – mediated by the Kerr nonlinearity and multiphoton or tunnel ionization, respectively. The filament properties, including the supercontinuum generation, are therefore highly sensitive to the properties of both the laser source and the propagation medium. Here, we report the anomalous spectral broadening of the supercontinuum for filamentation in molecular gases, which is observed for specific elliptical polarization states of the input laser pulse. The resulting spectrum is accompanied by a modification of the supercontinuum polarization state and a lengthening of the filament plasma column. Our experimental results and accompanying simulations suggest that rotational dynamics of diatomic molecules play an essential role in filamentation-induced supercontinuum generation, which can be controlled with polarization ellipticity. PMID:26847427

High-precision laser spectroscopy of the CO A(1)Π - X(1)Σ(+) (2,0), (3,0), and (4,0) bands.

PubMed

Niu, M L; Ramirez, F; Salumbides, E J; Ubachs, W

2015-01-28

High-precision two-photon Doppler-free frequency measurements have been performed on the CO A(1)Π - X(1)Σ(+) fourth-positive system (2,0), (3,0), and (4,0) bands. Absolute frequencies of forty-three transitions, for rotational quantum numbers up to J = 5, have been determined at an accuracy of 1.6 × 10(-3) cm(-1), using advanced techniques of two-color 2  +  1' resonance-enhanced multi-photon ionization, Sagnac interferometry, frequency-chirp analysis on the laser pulses, and correction for AC-Stark shifts. The accurate transition frequencies of the CO A(1)Π - X(1)Σ(+) system are of relevance for comparison with astronomical data in the search for possible drifts of fundamental constants in the early universe. The present accuracies in laboratory wavelengths of Δλ/λ = 2 × 10(-8) may be considered exact for the purpose of such comparisons.

Conformational analysis of quinine and its pseudo enantiomer quinidine: a combined jet-cooled spectroscopy and vibrational circular dichroism study.

PubMed

Sen, Ananya; Bouchet, Aude; Lepère, Valeria; Le Barbu-Debus, Katia; Scuderi, D; Piuzzi, F; Zehnacker-Rentien, A

2012-08-16

Laser-desorbed quinine and quinidine have been studied in the gas phase by combining supersonic expansion with laser spectroscopy, namely, laser-induced fluorescence (LIF), resonance-enhanced multiphoton ionization (REMPI), and IR-UV double resonance experiments. Density funtional theory (DFT) calculations have been done in conjunction with the experimental work. The first electronic transition of quinine and quinidine is of π-π* nature, and the studied molecules weakly fluoresce in the gas phase, in contrast to what was observed in solution (Qin, W. W.; et al. J. Phys. Chem. C2009, 113, 11790). The two pseudo enantiomers quinine and quinidine show limited differences in the gas phase; their main conformation is of open type as it is in solution. However, vibrational circular dichroism (VCD) experiments in solution show that additional conformers exist in condensed phase for quinidine, which are not observed for quinine. This difference in behavior between the two pseudo enantiomers is discussed.

Mass Spectroscopy of Neutral Metal Oxide Clusters Using a Desk-Top Soft X-Ray Laser

NASA Astrophysics Data System (ADS)

Dong, F.; Heinbuch, S.; Bernstein, E. R.; Rocca, J. J.

We report the use of a compact 46.9 nm capillary discharge soft x-ray laser in the study of metal-oxide nanoclusters using mass spectroscopy. Transition metal oxides are widely used as heterogeneous catalysts and catalytic supports in industrial processes. There are numerous applications for transition metal oxide catalysts, and although they are widely used, there is a lack of fundamental understanding of the complicated processes that occur on the metal oxide surface during catalysis. Conventional nanocluster spectroscopy techniques have used 193 nm radiation from an ArF excimer laser corresponding to a photon energy of 6.4 eV in order to photoionize a sample. Typical metal oxide nanocluster ionization energies fall into the range of 7-12 eV while some have even higher energies. Therefore a single 6.4 eV photon can not ionize the cluster making multiphoton processes the dominant ionization method. A major problem associated with mass spectroscopy can become evident during the multiphoton ionization of clusters. Specifically, the clusters may fragment during the ionization process and the identification of the neutral parent cluster can become difficult. In the present experiment neutral vanadium, niobium and tantalum oxide clusters are studied by single photon ionization with the 26.5 eV photons produced by a capillary discharge soft x-ray laser.1 During ionization, the metal oxide clusters are observed to be almost free of serious fragmentation. The most stable neutral cluster of vanadium, niobium, and tantalum oxide growth in a saturated oxygen condition are identified as MO2, M2O4/M2O5, M3O7, M4O10, M5O12, M6O15, M7O17, M8O20, and M9O22, which can be represented as a form (MO2)0,1(M2O5)y. M2O5 is identified as a basic unit to build-up the three kinds of metal oxide clusters. In the case of niobium and tantalum oxide clusters, the oxygen-deficient clusters with a structure of (MO2)2(M2O5)y are detected for groups that contain an even number of metal atoms. For vanadium oxide clusters, the oxygen-deficient clusters are detected for every family, indicating a stable structure of (VO2)x(V2O5)y. The stoichiometry of oxygen-rich clusters can be expressed as (MO2)0,1(M2O5)yO1-3 and their structures are consistent with chemically bonded species.

Disentangling Intracycle Interferences in Photoelectron Momentum Distributions Using Orthogonal Two-Color Laser Fields

NASA Astrophysics Data System (ADS)

Xie, Xinhua; Wang, Tian; Yu, ShaoGang; Lai, XuanYang; Roither, Stefan; Kartashov, Daniil; Baltuška, Andrius; Liu, XiaoJun; Staudte, André; Kitzler, Markus

2017-12-01

We use orthogonally polarized two-color (OTC) laser pulses to separate quantum paths in the multiphoton ionization of Ar atoms. Our OTC pulses consist of 400 and 800 nm light at a relative intensity ratio of 10 ∶1 . We find a hitherto unobserved interference in the photoelectron momentum distribution, which exhibits a strong dependence on the relative phase of the OTC pulse. Analysis of model calculations reveals that the interference is caused by quantum pathways from nonadjacent quarter cycles.

Carrier-envelope phase-dependent atomic coherence and quantum beats

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu Ying; State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences, Wuhan 430071; Yang Xiaoxue

2007-07-15

It is shown that the carrier-envelope phase (CEP) of few-cycle laser pulses has profound effects on the bound-state atomic coherence even in the weak-field regime where both tunneling and multiphoton ionization hardly take place. The atomic coherence thus produced is shown to be able to be mapped onto the CEP-dependent signal of quantum beats (and other quantum-interference phenomena) and hence might be used to extract information about and ultimately to measure the carrier-envelope phase.

Charge transfer and charge localization in extended radical cations: Investigation of model molecules for peptides

NASA Astrophysics Data System (ADS)

Weinkauf, Rainer; Lehrer, Florian

1998-12-01

Molecules consisting of a flexible tail and an aromatic chromophore are used as model systems to understand the situation of a single chromophore in a small peptide. Their S0-S1 resonant multiphoton ionization (REMPI) spectra show, that in neutral molecules the tail-chromophore interaction is weak and electronic excitation is localized at the chromophore. For molecules, where the ionization energy of the tail is considerable higher than that of the chromophore, by high resolution REMPI photoelectron spectroscopy we find the charge to be localized on the aromatic chromophore. This scheme also in suitable peptides allows local ionization at the aromatic chromophore. An estimate for various charge positions in peptide chains, however, shows, that for most of the amino acids electron hole positions in the nitrogen and oxygen "lone pair" orbitals of the peptide bond are nearly degenerate. REMPI photoelectron spectra of phenylethylamine, which as a model system contains such two degenerate charge positions, show small energetic shift of the ionization energy but strong geometry changes upon electron removal. This result is interpreted as direct ionization into a mixed charge delocalized state. Consequences for the charge transfer mechanism in peptides are discussed.

A least squares approach to estimating the probability distribution of unobserved data in multiphoton microscopy

NASA Astrophysics Data System (ADS)

Salama, Paul

2008-02-01

Multi-photon microscopy has provided biologists with unprecedented opportunities for high resolution imaging deep into tissues. Unfortunately deep tissue multi-photon microscopy images are in general noisy since they are acquired at low photon counts. To aid in the analysis and segmentation of such images it is sometimes necessary to initially enhance the acquired images. One way to enhance an image is to find the maximum a posteriori (MAP) estimate of each pixel comprising an image, which is achieved by finding a constrained least squares estimate of the unknown distribution. In arriving at the distribution it is assumed that the noise is Poisson distributed, the true but unknown pixel values assume a probability mass function over a finite set of non-negative values, and since the observed data also assumes finite values because of low photon counts, the sum of the probabilities of the observed pixel values (obtained from the histogram of the acquired pixel values) is less than one. Experimental results demonstrate that it is possible to closely estimate the unknown probability mass function with these assumptions.

Quasistatic limit of the strong-field approximation describing atoms in intense laser fields: Circular polarization

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bauer, Jaroslaw H.

2011-03-15

In the recent work of Vanne and Saenz [Phys. Rev. A 75, 063403 (2007)] the quasistatic limit of the velocity gauge strong-field approximation describing the ionization rate of atomic or molecular systems exposed to linearly polarized laser fields was derived. It was shown that in the low-frequency limit the ionization rate is proportional to the laser frequency {omega} (for a constant intensity of the laser field). In the present work I show that for circularly polarized laser fields the ionization rate is proportional to {omega}{sup 4} for H(1s) and H(2s) atoms, to {omega}{sup 6} for H(2p{sub x}) and H(2p{sub y})more » atoms, and to {omega}{sup 8} for H(2p{sub z}) atoms. The analytical expressions for asymptotic ionization rates (which become nearly accurate in the limit {omega}{yields}0) contain no summations over multiphoton contributions. For very low laser frequencies (optical or infrared) these expressions usually remain with an order-of-magnitude agreement with the velocity gauge strong-field approximation.« less

High-order above-threshold dissociation of molecules

NASA Astrophysics Data System (ADS)

Lu, Peifen; Wang, Junping; Li, Hui; Lin, Kang; Gong, Xiaochun; Song, Qiying; Ji, Qinying; Zhang, Wenbin; Ma, Junyang; Li, Hanxiao; Zeng, Heping; He, Feng; Wu, Jian

2018-03-01

Electrons bound to atoms or molecules can simultaneously absorb multiple photons via the above-threshold ionization featured with discrete peaks in the photoelectron spectrum on account of the quantized nature of the light energy. Analogously, the above-threshold dissociation of molecules has been proposed to address the multiple-photon energy deposition in the nuclei of molecules. In this case, nuclear energy spectra consisting of photon-energy spaced peaks exceeding the binding energy of the molecular bond are predicted. Although the observation of such phenomena is difficult, this scenario is nevertheless logical and is based on the fundamental laws. Here, we report conclusive experimental observation of high-order above-threshold dissociation of H2 in strong laser fields where the tunneling-ionized electron transfers the absorbed multiphoton energy, which is above the ionization threshold to the nuclei via the field-driven inelastic rescattering. Our results provide an unambiguous evidence that the electron and nuclei of a molecule as a whole absorb multiple photons, and thus above-threshold ionization and above-threshold dissociation must appear simultaneously, which is the cornerstone of the nowadays strong-field molecular physics.

Multiphoton Rydberg and valence dynamics of CH3Br probed by mass spectrometry and slice imaging.

PubMed

Hafliðason, Arnar; Glodic, Pavle; Koumarianou, Greta; Samartzis, Peter C; Kvaran, Ágúst

2018-06-18

The multiphoton dynamics of CH3Br were probed by Mass Resolved MultiPhoton Ionization (MR-MPI), Slice Imaging and Photoelectron Imaging in the two-photon excitation region of 66 000 to 80 000 cm-1. Slice images of the CH3+ and Br+ photoproducts of ten two-photon resonant transitions to np and nd Rydberg states of the parent molecule were recorded. CH3+ ions dominate the mass spectra. Kinetic energy release spectra (KERs) were derived from slice and photoelectron images and anisotropy parameters were extracted from the angular distributions of the ions to identify the processes and the dynamics involved. At all wavelengths we observe three-photon excitations, via the two-photon resonant transitions to molecular Rydberg states, forming metastable, superexcited (CH3Br#) states which dissociate to form CH3 Rydberg states (CH3**) along with Br/Br*. A correlation between the parent Rydberg states excited and CH3** formed is evident. For the three highest excitation energies used, the CH3Br# metastable states also generate high kinetic energy fragments of CH3(X) and Br/Br*. In addition for two out of these three wavelengths we also measure one-photon photolysis of CH3Br in the A band forming CH3(X) in various vibrational modes and bromine atoms in the ground (Br) and spin-orbit excited (Br*) states.

Comparison of the resonance-enhanced multiphoton ionization spectra of pyrrole and 2,5-dimethylpyrrole: Building toward an understanding of the electronic structure and photochemistry of porphyrins

DOE Office of Scientific and Technical Information (OSTI.GOV)

Beames, Joseph M.; Nix, Michael G. D.; Hudson, Andrew J.

The photophysical properties of porphyrins have relevance for their use as light-activated drugs in cancer treatment and sensitizers in solid-state solar cells. However, the appearance of their UV-visible spectra is usually explained inadequately by qualitative molecular-orbital theories. We intend to gain a better insight into the intense absorption bands, and excited-state dynamics, that make porphyrins appropriate for both of these applications by gradually building toward an understanding of the macrocyclic structure, starting with studies of smaller pyrrolic subunits. We have recorded the (1+1) and (2+1) resonance-enhanced multiphoton ionization (REMPI) spectra of pyrrole and 2,5-dimethylpyrrole between 25 600 cm{sup -1} (390more » nm) and 48 500 cm{sup -1} (206 nm). We did not observe a (1+1) REMPI signal through the optically bright {sup 1}B{sub 2} ({pi}{pi}*) and {sup 1}A{sub 1} ({pi}{pi}*) states in pyrrole due to ultrafast deactivation via conical intersections with the dissociative {sup 1}A{sub 2} ({pi}{sigma}*) and {sup 1}B{sub 1} ({pi}{sigma}{sup *}) states. However, we did observe (2+1) REMPI through Rydberg states with a dominant feature at 27 432 cm{sup -1} (two-photon energy, 54 864 cm{sup -1}) assigned to a 3d(leftarrow){pi} transition. In contrast, 2,5-dimethylpyrrole has a broad and structured (1+1) REMPI spectrum between 36 000 and 42 500 cm{sup -1} as a result of vibronic transitions to the {sup 1}B{sub 2} ({pi}{pi}*) state, and it does not show the 3d(leftarrow){pi} Rydberg transition via (2+1) REMPI. We have complemented the experimental studies by a theoretical treatment of the excited states of both molecules using time-dependent density functional theory (TD-DFT) and accounted for the contrasting features in the spectra. TD-DFT modeled the photochemical activity of both the optically dark {sup 1}{pi}{sigma}* states (dissociative) and optically bright {sup 1}{pi}{pi}* states well, predicting the barrierless deactivation of the {sup 1}B{sub 2} ({pi}{pi}*) state of pyrrole and the bound minimum of the {sup 1}B{sub 2} ({pi}{pi}*) state in 2,5-dimethylpyrrole. However, the quantitative agreement between vibronic transition energies and the excited-state frequencies calculated by TD-DFT was hampered by inaccurate modeling of Rydberg orbital mixing with the valence states, caused by the lack of an asymptotic correction to the exchange-correlation functionals used.« less

Circular dichroism in photoelectron images from aligned nitric oxide molecules

DOE PAGES

Sen, Ananya; Pratt, S. T.; Reid, K. L.

2017-05-03

We have used velocity map photoelectron imaging to study circular dichroism of the photoelectron angular distributions (PADs) of nitric oxide following two-color resonanceenhanced two-photon ionization via selected rotational levels of the A 2Σ +, v' = 0 state. By using a circularly polarized pump beam and a counter-propagating, circularly polarized probe beam, cylindrical symmetry is preserved in the ionization process, and the images can be reconstructed using standard algorithms. The VMI set up enables individual ion rotational states to be resolved with excellent collection efficiency, rendering the measurements considerably simpler to perform than previous measurements conducted with a conventional photoelectronmore » spectrometer. The results demonstrate that circular dichroism is observed even when cylindrical symmetry is maintained, and serve as a reminder that dichroism is a general feature of the multiphoton ionization of atoms and molecules. Furthermore, the observed PADs are in good agreement with calculations based on parameters extracted from previous experimental results obtained by using a time-offlight electron spectrometer.« less

Circular dichroism in photoelectron images from aligned nitric oxide molecules

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sen, Ananya; Pratt, S. T.; Reid, K. L.

We have used velocity map photoelectron imaging to study circular dichroism of the photoelectron angular distributions (PADs) of nitric oxide following two-color resonanceenhanced two-photon ionization via selected rotational levels of the A 2Σ +, v' = 0 state. By using a circularly polarized pump beam and a counter-propagating, circularly polarized probe beam, cylindrical symmetry is preserved in the ionization process, and the images can be reconstructed using standard algorithms. The VMI set up enables individual ion rotational states to be resolved with excellent collection efficiency, rendering the measurements considerably simpler to perform than previous measurements conducted with a conventional photoelectronmore » spectrometer. The results demonstrate that circular dichroism is observed even when cylindrical symmetry is maintained, and serve as a reminder that dichroism is a general feature of the multiphoton ionization of atoms and molecules. Furthermore, the observed PADs are in good agreement with calculations based on parameters extracted from previous experimental results obtained by using a time-offlight electron spectrometer.« less

Five-Photon Absorption and Selective Enhancement of Multiphoton Absorption Processes

PubMed Central

2015-01-01

We study one-, two-, three-, four-, and five-photon absorption of three centrosymmetric molecules using density functional theory. These calculations are the first ab initio calculations of five-photon absorption. Even- and odd-order absorption processes show different trends in the absorption cross sections. The behavior of all even- and odd-photon absorption properties shows a semiquantitative similarity, which can be explained using few-state models. This analysis shows that odd-photon absorption processes are largely determined by the one-photon absorption strength, whereas all even-photon absorption strengths are largely dominated by the two-photon absorption strength, in both cases modulated by powers of the polarizability of the final excited state. We demonstrate how to selectively enhance a specific multiphoton absorption process. PMID:26120588

Five-Photon Absorption and Selective Enhancement of Multiphoton Absorption Processes.

PubMed

Friese, Daniel H; Bast, Radovan; Ruud, Kenneth

2015-05-20

We study one-, two-, three-, four-, and five-photon absorption of three centrosymmetric molecules using density functional theory. These calculations are the first ab initio calculations of five-photon absorption. Even- and odd-order absorption processes show different trends in the absorption cross sections. The behavior of all even- and odd-photon absorption properties shows a semiquantitative similarity, which can be explained using few-state models. This analysis shows that odd-photon absorption processes are largely determined by the one-photon absorption strength, whereas all even-photon absorption strengths are largely dominated by the two-photon absorption strength, in both cases modulated by powers of the polarizability of the final excited state. We demonstrate how to selectively enhance a specific multiphoton absorption process.

Photon-number-resolving SSPDs with system detection efficiency over 50% at telecom range

NASA Astrophysics Data System (ADS)

Zolotov, P.; Divochiy, A.; Vakhtomin, Yu.; Moshkova, M.; Morozov, P.; Seleznev, V.; Smirnov, K.

2018-02-01

We used technology of making high-efficiency superconducting single-photon detectors as a basis for improvement of photon-number-resolving devices. By adding optical cavity and using an improved NbN superconducting film, we enhanced previously reported system detection efficiency at telecom range for such detectors. Our results show that implementation of optical cavity helps to develop four-section device with quantum efficiency over 50% at 1.55 µm. Performed experimental studies of detecting multi-photon optical pulses showed irregularities over defining multi-photon through single-photon quantum efficiency.

Laser-induced radiation microbeam technology and simultaneous real-time fluorescence imaging in live cells.

PubMed

Botchway, Stanley W; Reynolds, Pamela; Parker, Anthony W; O'Neill, Peter

2012-01-01

The use of nano- and microbeam techniques to induce and identify subcellular localized energy deposition within a region of a living cell provides a means to investigate the effects of low radiation doses. Particularly within the nucleus where the propagation and processing of deoxyribonucleic acid (DNA) damage (and repair) in both targeted and nontargeted cells, the latter being able to study cell-cell (bystander) effects. We have pioneered a near infrared (NIR) femtosecond laser microbeam to mimic ionizing radiation through multiphoton absorption within a 3D femtoliter volume of a highly focused Gaussian laser beam. The novel optical microbeam mimics both complex ionizing and UV-radiation-type cell damage including double strand breaks (DSBs). Using the microbeam technology, we have been able to investigate the formation of DNA DSB and subsequent recruitment of repair proteins to the submicrometer size site of damage introduced in viable cells. The use of a phosphorylated H2AX (γ-H2AX a marker for DSBs, visualized by immunofluorescent staining) and real-time imaging of fluorescently labeling proteins, the dynamics of recruitment of repair proteins in viable mammalian cells can be observed. Here we show the recruitment of ATM, p53 binding protein 1 (53BP1), and RAD51, an integral protein of the homologous recombination process in the DNA repair pathway and Ku-80-GFP involved in the nonhomologous end joining (NHEJ) pathway as exemplar repair process to show differences in the repair kinetics of DNA DSBs. The laser NIR multiphoton microbeam technology shows persistent DSBs at later times post laser irradiation which are indicative of DSBs arising at replication presumably from UV photoproducts or clustered damage containing single strand breaks (SSBs) that are also observed. Effects of the cell cycle may also be investigated in real time. Postirradiation and fixed cells studies show that in G1 cells a fraction of multiphoton laser-induced DSBs is persistent for >6h in addition to those induced at replication demonstrating the broad range of timescales taken to repair DNA damage. Copyright © 2012 Elsevier Inc. All rights reserved.

OSA (Optical Society of America) Proceedings on Short Wavelength Coherent Radiation: Generation and Applications Held in North Falmouth, Massachusetts on 26-29 September 1988. Volume 2

DTIC Science & Technology

1988-09-01

obtained using CVI 6d-2p line 142 Axial as a reference line[5]. The maximum en- hancement factor of 4.2 and corresponding cv1 gain length product of...C. Solem, and C. K. Rhodes ..... .............. 220 Multiphoton Ionization for the Production of X-Ray Laser Plasmas by P. B. Corkum and N. H...Diffraction Using Synchrotron Radiation by Rudolf Ruffer ......... ............................... 400 The Production of Long Coherence-Length Hard X

Free Radical-Surface Interactions Using Multiphoton Ionization of Free Radicals

DTIC Science & Technology

1989-01-01

Atoms, Rgf4PI 9 t Free Radl!cals)aj" i Atoms, Cross Section -’r RE)* I of Free Radicals arid Atonn. 𔄃 43S’RACT (Conti n reverse if necessary Ind identi...these surfaces. The basic philosophy of our CF 3I -+- nhv-CF, - t - I . program consists of generating a particular neutral species at A low pressures...constant for the escape of radicals out of the " reactor is shown in Eq. (6): .= k =, 4 .4,., I /V, (6) L !J 7 where t ,,, is the thermal molecular

Single-shot measurements of laser-induced avalanche breakdown demonstrating spatial and temporal control by an external source

NASA Astrophysics Data System (ADS)

Woodbury, Daniel; Wahlstrand, Jared; Goers, Andy; Feder, Linus; Miao, Bo; Hine, George; Salehi, Fatholah; Milchberg, Howard

2016-10-01

We report on the use of single-shot supercontinuum spectral interferometry (SSSI) to make temporally and spatially resolved measurements of laser-induced avalanche breakdown in ambient air by a 200 ps pulse. By seeding the breakdown using an external 100 fs pulse, we demonstrate control over the timing and spatial characteristics of the avalanche. In addition, we calculate the collisional ionization rates at various laser intensities and demonstrate seeding of the avalanche breakdown both by multiphoton ionization and by photodetaching ions produced from a radioactive source. These observations provide proof-of-concept support for recent proposals to remotely measure radioactivity using laser-induced avalanche breakdown. This work supported by a DTRA, C-WMD Basic Research Program, and by the DOE NNSA Stewardship Science Graduate Fellowship, provided under Grant Number DE-NA0002135.

High-order above-threshold dissociation of molecules.

PubMed

Lu, Peifen; Wang, Junping; Li, Hui; Lin, Kang; Gong, Xiaochun; Song, Qiying; Ji, Qinying; Zhang, Wenbin; Ma, Junyang; Li, Hanxiao; Zeng, Heping; He, Feng; Wu, Jian

2018-02-27

Electrons bound to atoms or molecules can simultaneously absorb multiple photons via the above-threshold ionization featured with discrete peaks in the photoelectron spectrum on account of the quantized nature of the light energy. Analogously, the above-threshold dissociation of molecules has been proposed to address the multiple-photon energy deposition in the nuclei of molecules. In this case, nuclear energy spectra consisting of photon-energy spaced peaks exceeding the binding energy of the molecular bond are predicted. Although the observation of such phenomena is difficult, this scenario is nevertheless logical and is based on the fundamental laws. Here, we report conclusive experimental observation of high-order above-threshold dissociation of H 2 in strong laser fields where the tunneling-ionized electron transfers the absorbed multiphoton energy, which is above the ionization threshold to the nuclei via the field-driven inelastic rescattering. Our results provide an unambiguous evidence that the electron and nuclei of a molecule as a whole absorb multiple photons, and thus above-threshold ionization and above-threshold dissociation must appear simultaneously, which is the cornerstone of the nowadays strong-field molecular physics. Copyright © 2018 the Author(s). Published by PNAS.

How the laser-induced ionization of transparent solids can be suppressed

NASA Astrophysics Data System (ADS)

Gruzdev, Vitaly

2013-12-01

A capability to suppress laser-induced ionization of dielectric crystals in controlled and predictable way can potentially result in substantial improvement of laser damage threshold of optical materials. The traditional models that employ the Keldysh formula do not predict any suppression of the ionization because of the oversimplified description of electronic energy bands underlying the Keldysh formula. To fix this gap, we performed numerical simulations of time evolution of conduction-band electron density for a realistic cosine model of electronic bands characteristic of wide-band-gap cubic crystals. The simulations include contributions from the photo-ionization (evaluated by the Keldysh formula and by the formula for the cosine band of volume-centered cubic crystals) and from the avalanche ionization (evaluated by the Drude model). Maximum conduction-band electron density is evaluated from a single rate equation as a function of peak intensity of femtosecond laser pulses for alkali halide crystals. Results obtained for high-intensity femtosecond laser pulses demonstrate that the ionization can be suppressed by proper choice of laser parameters. In case of the Keldysh formula, the peak electron density exhibits saturation followed by gradual increase. For the cosine band, the electron density increases with irradiance within the low-intensity multiphoton regime and switches to decrease with intensity approaching threshold of the strong singularity of the ionization rate characteristic of the cosine band. Those trends are explained with specific modifications of band structure by electric field of laser pulses.

Dissociation of heme from gaseous myoglobin ions studied by infrared multiphoton dissociation spectroscopy and Fourier-transform ion cyclotron resonance mass spectrometry

NASA Astrophysics Data System (ADS)

Wang, Yi-Sheng; Sabu, Sahadevan; Wei, Shih-Chia; Josh Kao, C.-M.; Kong, Xianglei; Liau, Shing-Chih; Han, Chau-Chung; Chang, Huan-Cheng; Tu, Shih-Yu; Kung, A. H.; Zhang, John Z. H.

2006-10-01

Detachment of heme prosthetic groups from gaseous myoglobin ions has been studied by collision-induced dissociation and infrared multiphoton dissociation in combination with Fourier-transform ion cyclotron resonance mass spectrometry. Multiply charged holomyoglobin ions (hMbn +) were generated by electrospray ionization and transferred to an ion cyclotron resonance cell, where the ions of interest were isolated and fragmented by either collision with Ar atoms or irradiation with 3μm photons, producing apomyoglobin ions (aMbn +). Both charged heme loss (with [Fe(III)-heme]+ and aMb(n-1)+ as the products) and neutral heme loss (with [Fe(II)-heme] and aMbn + as the products) were detected concurrently for hMbn + produced from a myoglobin solution pretreated with reducing reagents. By reference to Ea=0.9eV determined by blackbody infrared radiative dissociation for charged heme loss of ferric hMbn +, an activation energy of 1.1eV was deduced for neutral heme loss of ferrous hMbn + with n =9 and 10.

The dynamics of the Cl+C2H6→HCl(v',j')+C2H5 reaction at 0.24 eV: Is ethyl a spectator?

NASA Astrophysics Data System (ADS)

Bass, M. J.; Brouard, M.; Vallance, C.; Kitsopoulos, T. N.; Samartzis, P. C.; Toomes, R. L.

2003-10-01

The hydrogen atom abstraction reaction between Cl(2P3/2) and ethane has been studied at a mean collision energy of 0.24 eV. The experiments were performed in a coexpansion of molecular chlorine and ethane, with the atomic Cl reactants generated by laser photodissociation of Cl2 at 355 nm. HCl(v',j') products were detected quantum state selectively using (2+1) resonantly enhanced multiphoton ionization, coupled with velocity-map ion imaging. The ion images were used to determine center-of-mass angular and kinetic energy release distributions. Several analysis methods were employed and have been carefully assessed. It is shown that the single beam experiments can be used with confidence to determine both center-of-mass angular and energy release distributions. For the title reaction the angular distribution is found to be forward peaking, with on average 22% of the available energy channeled into internal excitation of the ethyl coproducts. Possible sources of this internal excitation are discussed.

Combined experimental and theoretical study of the benzocaine/Ar van der Waals system in supersonic expansions.

PubMed

León, Iker; Aguado, Edurne; Lesarri, Alberto; Fernández, José A; Castaño, Fernando

2009-02-12

The electronic spectra of Benzocaine x Ar(n), n = 0-4 were obtained using two-color resonance enhanced multiphoton ionization; the 1:1 and 1:2 clusters were investigated by ultraviolet/ultraviolet hole burning, stimulated emission pumping, and other laser spectroscopies. A single isomer was found for the 1:1 cluster, while two isomers of the 1:2 cluster were found: one with the two Ar atoms on the same side of the chromophore, and the other with the two Ar atoms sitting on opposite sides of the chromophore. The observed shifts point to the existence of a single isomer for the 1:3 and 1:4 species. Dissociation energies for the neutral ground and first excited electronic state and the ion ground electronic state of the complexes have been determined by the fragmentation threshold method and by ab initio calculations conducted at the MP2 level with 6-31++g(2d, p), 6-311++g(2d, p) and AUG-cc-pVTZ basis sets. The results are compared with those obtained for other similar systems.

Dynamics of the reactions of O(1D) with HCl, DCl, and Cl2

NASA Astrophysics Data System (ADS)

Matsumi, Yutaka; Tonokura, Kenichi; Kawasaki, Masahiro; Tsuji, Kazuhide; Obi, Kinichi

1993-05-01

The reactions O(1D)+HCl→OH+Cl (1a) and OCl+H (1b), O(1D)+DCl→OD+Cl (2a) and OCl+D (2b), and O(1D)+Cl2→OCl+Cl (3) are studied at an average collision energy of 7.6, 7.7, and 8.8 kcal/mol for (1), (2), and (3), respectively. H, D, and Cl atoms are detected by the resonance-enhanced multiphoton ionization technique. The average kinetic energies released to the products are estimated from Doppler profile measurements of the product atoms. The relative yields [OCl+H]/[OH+Cl] and [OCl+D]/[OD+Cl] are directly measured, and a strong isotope effect (H/D) on the relative yields is found. The fine-structure branding ratios [Cl(2P1/2]/[Cl(2P3/2)] of the reaction products are also measured. The results suggest that nonadiabatic couplings take place at the exit channels of the reactions (1a) and (2a), while the reaction (3) is totally adiabatic.

Collisional quenching of atoms and molecules on spacecraft thermal protection surfaces

NASA Technical Reports Server (NTRS)

Marinelli, W. J.; Green, B. D.

1988-01-01

Preliminary results of a research program to determine energy partitioning in spacecraft thermal protection materials due to atom recombination at the gas-surface interface are presented. The primary focus of the research is to understand the catalytic processes which determine heat loading on Shuttle, Aeroassisted OTV, and NASP thermal protection surfaces in nonequilibrium flight regimes. Highly sensitive laser diagnostics based on laser-induced fluorescence and resonantly-enhanced multiphoton ionization spectroscopy are used to detect atoms and metastable molecules. At low temperatures, a discharge flow reactor is employed to measure deactivation/recombination coefficients for O-atoms, N-atoms, and O2. Detection methods are presented for measuring O-atoms, O2 and N2, and results for deactivation of O2 and O-atoms on reaction-cured glass and Ni surfaces. Both atom recombination and metastable product formation are examined. Radio-frequency discharges are used to produce highly dissociated beams of atomic species at energies characteristic of the surface temperature. Auger electron spectroscopy is employed as a diagnostic of surface composition in order to accurately define and control measurement conditions.

On the properties of microsolvated molecules in the ground (S0) and excited (S1) states: The anisole-ammonia 1:1 complex

NASA Astrophysics Data System (ADS)

Biczysko, Malgorzata; Piani, Giovanni; Pasquini, Massimiliano; Schiccheri, Nicola; Pietraperzia, Giangaetano; Becucci, Maurizio; Pavone, Michele; Barone, Vincenzo

2007-10-01

State-of-the-art spectroscopic and theoretical methods have been exploited in a joint effort to elucidate the subtle features of the structure and the energetics of the anisole-ammonia 1:1 complex, a prototype of microsolvation processes. Resonance enhanced multiphoton ionization and laser-induced fluorescence spectra are discussed and compared to high-level first-principles theoretical models, based on density functional, many body second order perturbation, and coupled cluster theories. In the most stable nonplanar structure of the complex, the ammonia interacts with the delocalized π electron density of the anisole ring: hydrogen bonding and dispersive forces provide a comparable stabilization energy in the ground state, whereas in the excited state the dispersion term is negligible because of electron density transfer from the oxygen to the aromatic ring. Ground and excited state geometrical parameters deduced from experimental data and computed by quantum mechanical methods are in very good agreement and allow us to unambiguously determine the molecular structure of the anisole-ammonia complex.

Controlled energy deposition and void-like modification inside transparent solids by two-color tightly focused femtosecond laser pulses

NASA Astrophysics Data System (ADS)

Potemkin, Fedor; Mareev, Evgeniy; Bezsudnova, Yulia; Platonenko, Victor; Bravy, Boris; Gordienko, Vyacheslav

2017-04-01

We report a bulk void-like micromodification of fused silica using two-color μJ-energy level tightly focused (NA = 0.5) co-propagating seeding (visible, 0.62 μm) and heating (near-IR, 1.24 μm) femtosecond laser pulses with online third harmonic diagnostics of created microplasmas as well as subsequent laser-induced void-like defects. It has been shown experimentally and theoretically that production of seeding electrons through multiphoton ionization by visible laser pulses paves the way for controllability of the energy deposition and laser-induced micromodification via carrier heating by delayed infrared laser pulses inside the material. Experimental results demonstrate wide possibilities to increase the density of energy deposited up to 6 kJ cm-3 inside the dielectric by tight focusing of two color fs-laser pulses and elliptical polarization for infrared heating fs-laser pulses. The developed theoretical approach predicts the enhancement of deposited energy density up to 9 kJ cm-3 using longer (mid-IR) wavelengths for heating laser pulses.

Imaging spectroscopy of the missing REMPI bands of methyl radicals: Final touches on all vibrational frequencies of the 3p Rydberg states

NASA Astrophysics Data System (ADS)

Pan, Huilin; Liu, Kopin

2018-01-01

(2 + 1) resonance-enhanced multiphoton ionization (REMPI) detection of methyl radicals, in particular that via the intermediate 3p Rydberg states, has shown to be a powerful method and thus enjoyed a wide range of applications. Methyl has six vibrational modes. Among them—including partially and fully deuterated isotopologs—four out of twenty vibrational frequencies in the intermediate 3p states have so far eluded direct spectroscopic determination. Here, by exploiting the imaging spectroscopy approach to a few judiciously selected chemical reactions, the four long-sought REMPI bands—CHD2(611), CH2D(311), CH2D(511), and CH2D(611)—are discovered, which complete the REMPI identification for probing any vibrational mode of excitation of methyl radical and its isotopologs. These results, in conjunction with those previously reported yet scattered in the literature, are summarized here for ready reference, which should provide all necessary information for further spectral assignments and future studies of chemical dynamics using this versatile REMPI scheme.

Experiments and PIC simulations on liquid crystal plasma mirrors for pulse contrast enhancement

NASA Astrophysics Data System (ADS)

Cochran, G. E.; Poole, P. L.; Krygier, A.; Foster, P. S.; Scott, G. G.; Wilson, L. A.; Bailey, J.; Bourgeois, N.; Hernandez-Gomez, C.; Heery, R.; Purcell, J.; Neely, D.; Rajeev, P. P.; Freeman, R. R.; Schumacher, D. W.

2016-10-01

High pulse contrast is crucial for performing many experiments on high intensity lasers in order to minimize modification of the target surface by pre-pulse. This is often achieved through the use of solid dielectric plasma mirrors which can limit laser shot rates. Liquid crystal films, originally developed as variable thickness ion acceleration targets, have been demonstrated as effective plasma mirrors for pulse cleaning, reaching peak reflectivities over 70%. These films were used as plasma mirrors in an ion acceleration experiment on the Scarlet laser and the resultant increase in peak proton energy and change in acceleration direction will be discussed. Also presented here are novel 2D3V, LSP particle-in-cell simulations of dielectric plasma mirror operation. By including multiphoton ionization and dimensionality corrections, an excellent match to experiment is obtained over 4 decades in intensity. Analysis of pulse shortening and plasma critical surface behavior in these simulations will be discussed. Formation of thin films at 1.5 Hz will also be presented. Performed with support from the DARPA PULSE program through AMRDEC, from NNSA, and from OSC.

Nonlinear structured-illumination enhanced temporal focusing multiphoton excitation microscopy with a digital micromirror device.

PubMed

Cheng, Li-Chung; Lien, Chi-Hsiang; Da Sie, Yong; Hu, Yvonne Yuling; Lin, Chun-Yu; Chien, Fan-Ching; Xu, Chris; Dong, Chen Yuan; Chen, Shean-Jen

2014-08-01

In this study, the light diffraction of temporal focusing multiphoton excitation microscopy (TFMPEM) and the excitation patterning of nonlinear structured-illumination microscopy (NSIM) can be simultaneously and accurately implemented via a single high-resolution digital micromirror device. The lateral and axial spatial resolutions of the TFMPEM are remarkably improved through the second-order NSIM and projected structured light, respectively. The experimental results demonstrate that the lateral and axial resolutions are enhanced from 397 nm to 168 nm (2.4-fold) and from 2.33 μm to 1.22 μm (1.9-fold), respectively, in full width at the half maximum. Furthermore, a three-dimensionally rendered image of a cytoskeleton cell featuring ~25 nm microtubules is improved, with other microtubules at a distance near the lateral resolution of 168 nm also able to be distinguished.

Investigation of the 6 p 2(3 P 0) n p Rydberg series of bismuth by multiphoton excitation

NASA Astrophysics Data System (ADS)

Bühler, B.; Cremer, C.; Gerber, G.

1985-03-01

Rydberg states of the odd-parity series 6 p 2(3 p 0) n p of BiI are excited by a three-photon process. A two-photon dissociation of Bi2 into excited atomic states followed by a one-photon absorption leads to highly excited atomic Rydberg states up to n = 32. States of the even-parity Rydberg series 6 p 2(3 p 0) nsJ=1/2, ndJ=3/2 and ndJ=5/2 are also observed. In order to avoid the background caused by ionization of the bismuth molecules we performed a two-color excitation with pulsed dye lasers. With this experiment the 6 p 2(3 p 0) npJ=3/2 Rydberg series could be resolved up to n=75. The increasing quantum defect of this series is due to a perturbing state close to the first ionization limit. By a MQDT analysis we obtain the energy of the perturbing state and a value of 58,761.68±0.1 cm-1 for the first ionization limit of atomic bismuth.

Revisiting the relaxation dynamics of isolated pyrrole

DOE Office of Scientific and Technical Information (OSTI.GOV)

Montero, Raúl; Ovejas, Virginia; Fernández-Fernández, Marta

Herein, the interpretation of the femtosecond-scale temporal evolution of the pyrrole ion signal, after excitation in the 267–217 nm interval, recently published by our group [R. Montero, A. Peralta Conde, V. Ovejas, M. Fernández-Fernández, F. Castaño, J. R. Vázquez de Aldana, and A. Longarte, J. Chem. Phys.137, 064317 (2012)] is re-visited. The observation of a shift in the pyrrole{sup +} transient respect to zero delay reference, initially attributed to ultrafast dynamics on the πσ{sup *} type state (3s a{sub 1} ← π 1a{sub 2}), is demonstrated to be caused by the existence of pump + probe populated states, along themore » ionization process. The influence of these resonances in pump-prone ionization experiments, when multi-photon probes are used, and the significance of a proper zero-time reference, is discussed. The possibility of preparing the πσ{sup *} state by direct excitation is investigated by collecting 1 + 1 photoelectron spectra, at excitation wavelengths ranging from 255 to 219 nm. No conclusive evidences of ionization through this state are found.« less

Engineering Photon-Photon Interactions within Rubidium-Filled Waveguides

NASA Astrophysics Data System (ADS)

Perrella, C.; Light, P. S.; Vahid, S. Afshar; Benabid, F.; Luiten, A. N.

2018-04-01

Strong photon-photon interactions are a required ingredient for deterministic two-photon optical quantum logic gates. Multiphoton transitions in dense atomic vapors have been shown to be a promising avenue for producing such interactions. The strength of a multiphoton interaction can be enhanced by conducting the interaction in highly confined geometries such as small-cross-section optical waveguides. We demonstrate, both experimentally and theoretically, that the strength of such interactions scale only with the optical mode diameter, d , not d2 as might be initially expected. This weakening of the interaction arises from atomic motion inside the waveguides. We create an interaction between two optical signals, at 780 and 776 nm, using the 5 S1 /2→5 D5 /2 two-photon transition in rubidium vapor within a range of hollow-core fibers with different core sizes. The interaction strength is characterized by observing the absorption and phase shift induced on the 780-nm beam, which is in close agreement with theoretical modeling that accounts for the atomic motion inside the fibers. These observations demonstrate that transit-time effects upon multiphoton transitions are of key importance when engineering photon-photon interactions within small-cross-section waveguides that might otherwise be thought to lead to enhanced optical nonlinearity through increased intensities.

Multiphoton laser ionization for energy conversion in barium vapor

NASA Astrophysics Data System (ADS)

Makdisi, Y.; Kokaj, J.; Afrousheh, K.; Mathew, J.; Nair, R.; Pichler, G.

2013-03-01

We have studied the ion detection of barium atoms in special heated ovens with a tungsten rod in the middle of the stainless steel tube. The tungsten rod was heated indirectly by the oven body heaters. A bias voltage between the cell body and the tungsten rod of 9 V was used to collect electrons, after the barium ions had been created. However, we could collect the electrons even without the bias voltage, although with ten times less efficiency. We studied the conditions for the successful bias-less thermionic signal detection using excimer/dye laser two-photon excitation of Rydberg states below and above the first ionization limit (two-photon wavelength at 475.79 nm). We employed a hot-pipe oven and heat-pipe oven (with inserted mesh) in order to generate different barium vapor distributions inside the oven. The thermionic signal increased by a factor of two under heat-pipe oven conditions.

Second generation measurement of the electric dipole moment of the electron using trapped ThF+ ions

NASA Astrophysics Data System (ADS)

Ng, Kia Boon; Zhou, Yan; Gresh, Daniel; Cairncross, William; Grau, Matthew; Ni, Yiqi; Ye, Jun; Cornell, Eric

2016-05-01

ThF+ has been chosen as the candidate for a second generation measurement of the electric dipole moment of the electron (eEDM). Compared to the current HfF+ eEDM experiment, ThF+ has several advantages: (i) the eEDM-sensitive state (3Δ1) is the ground state, which facilitates a long coherence time; (ii) its effective electric field (38 GV/cm) is 50% larger than that of HfF+, which promises a direct increase of the eEDM sensitivity; and (iii) the ionization energy of neutral ThF is lower than its dissociation energy, which introduces greater flexibility in rotational state-selective photoionization via core-nonpenetrating Rydberg states. Here, we present progress of our experimental setup, preliminary spectroscopic data of multi-photon ionization, and discussions of new features in ion trapping, state preparation and population readout.

Resonantly enhanced multiple exciton generation through below-band-gap multi-photon absorption in perovskite nanocrystals.

PubMed

Manzi, Aurora; Tong, Yu; Feucht, Julius; Yao, En-Ping; Polavarapu, Lakshminarayana; Urban, Alexander S; Feldmann, Jochen

2018-04-17

Multi-photon absorption and multiple exciton generation represent two separate strategies for enhancing the conversion efficiency of light into usable electric power. Targeting below-band-gap and above-band-gap energies, respectively, to date these processes have only been demonstrated independently. Here we report the combined interaction of both nonlinear processes in CsPbBr 3 perovskite nanocrystals. We demonstrate nonlinear absorption over a wide range of below-band-gap excitation energies (0.5-0.8 E g ). Interestingly, we discover high-order absorption processes, deviating from the typical two-photon absorption, at specific energetic positions. These energies are associated with a strong enhancement of the photoluminescence intensity by up to 10 5 . The analysis of the corresponding energy levels reveals that the observed phenomena can be ascribed to the resonant creation of multiple excitons via the absorption of multiple below-band-gap photons. This effect may open new pathways for the efficient conversion of optical energy, potentially also in other semiconducting materials.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ghosh Deb, S.; Sinha, C.; Chattopadhyay, A.

The modification in the dynamics of the electron-impact ionization process of a Li{sup +} ion due to an intense linearly polarized monochromatic laser field (n{gamma}e,2e) is studied theoretically using coplanar geometry. Significant laser modifications are noted due to multiphoton effects both in the shape and magnitude of the triple-differential cross sections (TDCSs) with respect to the field-free (FF) situation. The net effect of the laser field is to suppress the FF cross sections in the zeroth-order approximation [Coulomb-Volkov (CV)] of the ejected electron wave function, while in the first order [modified Coulomb-Volkov (MCV)], the TDCSs are found to be enhancedmore » or suppressed depending on the kinematics of the process. The strong FF recoil dominance for the (e,2e) process of an ionic target at low incident energy is destroyed in the presence of the laser field. The FF binary-to-recoil ratio changes remarkably in the presence of the laser field, particularly at low incident energies. The difference between the multiphoton CV and the FF results indicates that for the ionic target, the Kroll-Watson sum rule does not hold well at the present energy range in contrast to the neutral atom (He) case. The TDCSs are found to be quite sensitive with respect to the initial phase of the laser field, particularly at higher incident energies. A significant qualitative difference is noted in the multiphoton ejected energy distribution (double-differential cross sections) between the CV and the MCV models. Variation of the TDCSs with respect to the laser phase is also studied.« less

Tuning the photon statistics of a strongly coupled nanophotonic system

NASA Astrophysics Data System (ADS)

Dory, Constantin; Fischer, Kevin A.; Müller, Kai; Lagoudakis, Konstantinos G.; Sarmiento, Tomas; Rundquist, Armand; Zhang, Jingyuan L.; Kelaita, Yousif; Sapra, Neil V.; Vučković, Jelena

2017-02-01

We investigate the dynamics of single- and multiphoton emission from detuned strongly coupled systems based on the quantum-dot-photonic-crystal resonator platform. Transmitting light through such systems can generate a range of nonclassical states of light with tunable photon counting statistics due to the nonlinear ladder of hybridized light-matter states. By controlling the detuning between emitter and resonator, the transmission can be tuned to strongly enhance either single- or two-photon emission processes. Despite the strongly dissipative nature of these systems, we find that by utilizing a self-homodyne interference technique combined with frequency filtering we are able to find a strong two-photon component of the emission in the multiphoton regime. In order to explain our correlation measurements, we propose rate equation models that capture the dominant processes of emission in both the single- and multiphoton regimes. These models are then supported by quantum-optical simulations that fully capture the frequency filtering of emission from our solid-state system.

Enhanced Axial Resolution of Wide-Field Two-Photon Excitation Microscopy by Line Scanning Using a Digital Micromirror Device.

PubMed

Park, Jong Kang; Rowlands, Christopher J; So, Peter T C

2017-01-01

Temporal focusing multiphoton microscopy is a technique for performing highly parallelized multiphoton microscopy while still maintaining depth discrimination. While the conventional wide-field configuration for temporal focusing suffers from sub-optimal axial resolution, line scanning temporal focusing, implemented here using a digital micromirror device (DMD), can provide substantial improvement. The DMD-based line scanning temporal focusing technique dynamically trades off the degree of parallelization, and hence imaging speed, for axial resolution, allowing performance parameters to be adapted to the experimental requirements. We demonstrate this new instrument in calibration specimens and in biological specimens, including a mouse kidney slice.

Enhanced Axial Resolution of Wide-Field Two-Photon Excitation Microscopy by Line Scanning Using a Digital Micromirror Device

PubMed Central

Park, Jong Kang; Rowlands, Christopher J.; So, Peter T. C.

2017-01-01

Temporal focusing multiphoton microscopy is a technique for performing highly parallelized multiphoton microscopy while still maintaining depth discrimination. While the conventional wide-field configuration for temporal focusing suffers from sub-optimal axial resolution, line scanning temporal focusing, implemented here using a digital micromirror device (DMD), can provide substantial improvement. The DMD-based line scanning temporal focusing technique dynamically trades off the degree of parallelization, and hence imaging speed, for axial resolution, allowing performance parameters to be adapted to the experimental requirements. We demonstrate this new instrument in calibration specimens and in biological specimens, including a mouse kidney slice. PMID:29387484

Numerical calculation of nonlinear ultrashort laser pulse propagation in transparent Kerr media

NASA Astrophysics Data System (ADS)

Arnold, Cord L.; Heisterkamp, Alexander; Ertmer, Wolfgang; Lubatschowski, Holger

2005-03-01

In the focal region of tightly focused ultrashort laser pulses, sufficient high intensities to initialize nonlinear ionization processes are easily achieved. Due to these nonlinear ionization processes, mainly multiphoton ionization and cascade ionization, free electrons are generated in the focus resulting in optical breakdown. A model including both nonlinear pulse propagation and plasma generation is used to calculate numerically the interaction of ultrashort pulses with their self-induced plasma in the vicinity of the focus. The model is based on a (3+1)-dimensional nonlinear Schroedinger equation describing the pulse propagation coupled to a system of rate equations covering the generation of free electrons. It is applicable to any transparent Kerr medium, whose linear and nonlinear optical parameters are known. Numerical calculations based on this model are used to understand nonlinear side effects, such as streak formation, occurring in addition to optical breakdown during short pulse refractive eye surgeries like fs-LASIK. Since the optical parameters of water are a good first-order approximation to those of corneal tissue, water is used as model substance. The free electron density distribution induced by focused ultrashort pulses as well as the pulses spatio-temporal behavior are studied in the low-power regime around the critical power for self-focusing.

Nonlinear structured-illumination enhanced temporal focusing multiphoton excitation microscopy with a digital micromirror device

PubMed Central

Cheng, Li-Chung; Lien, Chi-Hsiang; Da Sie, Yong; Hu, Yvonne Yuling; Lin, Chun-Yu; Chien, Fan-Ching; Xu, Chris; Dong, Chen Yuan; Chen, Shean-Jen

2014-01-01

In this study, the light diffraction of temporal focusing multiphoton excitation microscopy (TFMPEM) and the excitation patterning of nonlinear structured-illumination microscopy (NSIM) can be simultaneously and accurately implemented via a single high-resolution digital micromirror device. The lateral and axial spatial resolutions of the TFMPEM are remarkably improved through the second-order NSIM and projected structured light, respectively. The experimental results demonstrate that the lateral and axial resolutions are enhanced from 397 nm to 168 nm (2.4-fold) and from 2.33 μm to 1.22 μm (1.9-fold), respectively, in full width at the half maximum. Furthermore, a three-dimensionally rendered image of a cytoskeleton cell featuring ~25 nm microtubules is improved, with other microtubules at a distance near the lateral resolution of 168 nm also able to be distinguished. PMID:25136483

Fast monitoring of motor exhaust components by resonant multi-photon ionisation and time-of-flight mass spectrometry

NASA Astrophysics Data System (ADS)

Franzen, Jochen; Frey, Rüdiger; Nagel, Holger

1995-03-01

A new analytical procedure is provided by the combination of two types of spectroscopy. Resonant ionization of selected compounds by multiphoton ionization is based on results of absorption spectroscopy for the compound molecules of interest and time-of-flight mass spectrometry serves for the unambigious detection of these compounds. An interesting application of this method is the fast exhaust gas analysis. In the development of future combustion engines, the management of dynamic motor processes becomes predominant because by more than 90 % of all the dangerous exhaust pollutions are produced in instationary motor phases such as fast speed or load changes. The investigation of dynamic processes however, requires fast analytical procedures with millisecond time resolution together with the capability to measure individual components in a very complex gas mixture The objectives for a development project of such an instrument were set by the Research Association for Combustion Engines (Forschungsvereinigung Verbrennungskraftmaschinen, FVV, Germany): Up to ten substances should be monitored synchroneously with a time resolution of about 10 milliseconds, with concentration limits of 1 part per million and with a precision better than 10 % relative standard deviation. Such a laser mass spectrometer for fast multi-component automotive exhaust analyses has been developed in a joint research project by Bruker-Franzen Analytik GmbH, Dornier GmbH and the Technical University of Munich. The system has been applied at a motor test facility to investigate the emissions of the aromatic hydrocarbons benzene, toluene and xylene, of nitric oxide and acetaldehyde in stationary and dynamic engine operation. These measurements demonstrate that strong emission of these pollutants takes place at instationary engine operation and in particular that these compounds are emitted at different times, giving new information about the processes in the combustion chamber and in the exhaust pipe.

Structural characterization of arginine-vasopressin and lysine-vasopressin by Fourier- transform ion cyclotron resonance mass spectrometry and infrared multiphoton dissociation.

PubMed

Bianco, Giuliana; Battista, Fabio; Buchicchio, Alessandro; Amarena, Concetta G; Schmitt-Kopplin, Philippe; Guerrieri, Antonio

2015-01-01

Arginine-vasopressin (AVP) and lysine-vasopressin (LVP) were analyzed by reversed-phase liquid chromatography/mass spectrometry (LC-MS) using Fourier-transform ion cyclotron resonance (FT-ICR) mass spectrometry (MS) electrospray ionization (ESI) in the positive ion mode. LVP and AVP exhibited the protonated adduct [M+H](+) as the predominant ion at m/z 1056.43965 and at m/z 1084.44561, respectively. Infrared multiphoton dissociation (IRMPD), using a CO(2) laser source at a wavelength of 10.6 μm, was applied to protonated vasopressin molecules. The IRMPD mass spectra presented abundant mass fragments essential for a complete structural information. Several fragment ions, shared between two target molecules, are discussed in detail. Some previously unpublished fragments were identified unambiguously utilizing the high resolution and accurate mass information provided by the FT-ICR mass spectrometer. The opening of the disulfide loop and the cleavage of the peptide bonds within the ring were observed even under low-energy fragmentation conditions. Coupling the high-performance FT-ICR mass spectrometer with IRMPD as a contemporary fragmentation technique proved to be very promising for the structural characterization of vasopressin.

Tunable Spectrum Selectivity for Multiphoton Absorption with Enhanced Visible Light Trapping in ZnO Nanorods.

PubMed

Tan, Kok Hong; Lim, Fang Sheng; Toh, Alfred Zhen Yang; Zheng, Xia-Xi; Dee, Chang Fu; Majlis, Burhanuddin Yeop; Chai, Siang-Piao; Chang, Wei Sea

2018-04-17

Observation of visible light trapping in zinc oxide (ZnO) nanorods (NRs) correlated to the optical and photoelectrochemical properties is reported. In this study, ZnO NR diameter and c-axis length respond primarily at two different regions, UV and visible light, respectively. ZnO NR diameter exhibits UV absorption where large ZnO NR diameter area increases light absorption ability leading to high efficient electron-hole pair separation. On the other hand, ZnO NR c-axis length has a dominant effect in visible light resulting from a multiphoton absorption mechanism due to light reflection and trapping behavior in the free space between adjacent ZnO NRs. Furthermore, oxygen vacancies and defects in ZnO NRs are associated with the broad visible emission band of different energy levels also highlighting the possibility of the multiphoton absorption mechanism. It is demonstrated that the minimum average of ZnO NR c-axis length must satisfy the linear regression model of Z p,min = 6.31d to initiate the multiphoton absorption mechanism under visible light. This work indicates the broadening of absorption spectrum from UV to visible light region by incorporating a controllable diameter and c-axis length on vertically aligned ZnO NRs, which is important in optimizing the design and functionality of electronic devices based on light absorption mechanism. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Spectroscopic study on deuterated benzenes. III. Vibronic structure and dynamics in the S1 state

NASA Astrophysics Data System (ADS)

Kunishige, Sachi; Katori, Toshiharu; Kawabata, Megumi; Yamanaka, Takaya; Baba, Masaaki

2015-12-01

We observed the fluorescence excitation spectra and mass-selected resonance enhanced multiphoton ionization (REMPI) excitation spectra for the 6 01 , 6 01 10 1 , and 6 01 10 2 bands of the S1←S0 transition of jet-cooled deuterated benzene and assigned the vibronic bands of C6D6 and C6HD5. The 60 1 10 n (n = 0, 1, 2) and 00 0 transition energies were found to be dependent only on the number of D atoms (ND), which was reflected by the zero-point energy of each H/D isotopomer. In some isotopomers some bands, such as those of out-of-plane vibrations mixed with 611n, make the spectra complex. These included the 611021n level or combination bands with ν12 which are allowed because of reduced molecular symmetry. From the lifetime measurements of each vibronic band, some enhancement of the nonradiative intramolecular vibrational redistribution (IVR) process was observed. It was also found that the threshold excess energy of "channel three" was higher than the 6112 levels, which were similar for all the H/D isotopomers. We suggest that the channel three nonradiative process could be caused mainly by in-plane processes such as IVR and internal conversion at the high vibrational levels in the S1 state of benzene, although the out-of-plane vibrations might contribute to some degree.

Fast detection of narcotics by single photon ionization mass spectrometry and laser ion mobility spectrometry

NASA Astrophysics Data System (ADS)

Laudien, Robert; Schultze, Rainer; Wieser, Jochen

2010-10-01

In this contribution two analytical devices for the fast detection of security-relevant substances like narcotics and explosives are presented. One system is based on an ion trap mass spectrometer (ITMS) with single photon ionization (SPI). This soft ionization technique, unlike electron impact ionization (EI), reduces unwanted fragment ions in the mass spectra allowing the clear determination of characteristic (usually molecular) ions. Their enrichment in the ion trap and identification by tandem MS investigations (MS/MS) enables the detection of the target substances in complex matrices at low concentrations without time-consuming sample preparation. For SPI an electron beam pumped excimer light source of own fabrication (E-Lux) is used. The SPI-ITMS system was characterized by the analytical study of different drugs like cannabis, heroin, cocaine, amphetamines, and some precursors. Additionally, it was successfully tested on-site in a closed illegal drug laboratory, where low quantities of MDMA could be directly detected in samples from floors, walls and lab equipments. The second analytical system is based on an ion mobility (IM) spectrometer with resonant multiphoton ionization (REMPI). With the frequency quadrupled Nd:YAG laser (266 nm), used for ionization, a selective and sensitive detection of aromatic compounds is possible. By application of suited aromatic dopants, in addition, also non-aromatic polar compounds are accessible by ion molecule reactions like proton transfer or complex formation. Selected drug precursors could be successfully detected with this device as well, qualifying it to a lower-priced alternative or useful supplement of the SPI-ITMS system for security analysis.

Disentangling formation of multiple-core holes in aminophenol molecules exposed to bright X-FEL radiation

NASA Astrophysics Data System (ADS)

Zhaunerchyk, V.; Kamińska, M.; Mucke, M.; Squibb, R. J.; Eland, J. H. D.; Piancastelli, M. N.; Frasinski, L. J.; Grilj, J.; Koch, M.; McFarland, B. K.; Sistrunk, E.; Gühr, M.; Coffee, R. N.; Bostedt, C.; Bozek, J. D.; Salén, P.; Meulen, P. v. d.; Linusson, P.; Thomas, R. D.; Larsson, M.; Foucar, L.; Ullrich, J.; Motomura, K.; Mondal, S.; Ueda, K.; Richter, R.; Prince, K. C.; Takahashi, O.; Osipov, T.; Fang, L.; Murphy, B. F.; Berrah, N.; Feifel, R.

2015-12-01

Competing multi-photon ionization processes, some leading to the formation of double core hole states, have been examined in 4-aminophenol. The experiments used the linac coherent light source (LCLS) x-ray free electron laser, in combination with a time-of-flight magnetic bottle electron spectrometer and the correlation analysis method of covariance mapping. The results imply that 4-aminophenol molecules exposed to the focused x-ray pulses of the LCLS sequentially absorb more than two x-ray photons, resulting in the formation of multiple core holes as well as in the sequential removal of photoelectrons and Auger electrons (so-called PAPA sequences).

Disentangling formation of multiple-core holes in aminophenol molecules exposed to bright X-FEL radiation

DOE PAGES

Zhaunerchyk, V.; Kaminska, M.; Mucke, M.; ...

2015-10-28

Competing multi-photon ionization processes, some leading to the formation of double core hole states, have been examined in 4-aminophenol. The experiments used the linac coherent light source (LCLS) x-ray free electron laser, in combination with a time-of-flight magnetic bottle electron spectrometer and the correlation analysis method of covariance mapping. Furthermore, the results imply that 4-aminophenol molecules exposed to the focused x-ray pulses of the LCLS sequentially absorb more than two x-ray photons, resulting in the formation of multiple core holes as well as in the sequential removal of photoelectrons and Auger electrons (so-called PAPA sequences).

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fu, H.B.; Hu, Y.J.; Bernstein, E.R.

Small methanol clusters are formed by expanding a mixture of methanol vapor seeded in helium and are detected using vacuum UV (vuv) (118 nm) single-photon ionization/linear time-of-flight mass spectrometer (TOFMS). Protonated cluster ions, (CH{sub 3}OH){sub n-1}H{sup +} (n=2-8), formed through intracluster ion-molecule reactions following ionization, essentially correlate to the neutral clusters, (CH{sub 3}OH){sub n}, in the present study using 118 nm light as the ionization source. Both experimental and Born-Haber calculational results clarify that not enough excess energy is released into protonated cluster ions to initiate further fragmentation in the time scale appropriate for linear TOFMS. Size-specific spectra for (CH{submore » 3}OH){sub n} (n=4 to 8) clusters in the OH stretch fundamental region are recorded by IR+vuv (118 nm) nonresonant ion-dip spectroscopy through the detection chain of IR multiphoton predissociation and subsequent vuv single-photon ionization. The general structures and gross features of these cluster spectra are consistent with previous theoretical calculations. The lowest-energy peak contributed to each cluster spectrum is redshifted with increasing cluster size from n=4 to 8, and limits near {approx}3220 cm{sup -1} in the heptamer and octamer. Moreover, IR+vuv nonresonant ionization detected spectroscopy is employed to study the OH stretch first overtone of the methanol monomer. The rotational temperature of the clusters is estimated to be at least 50 K based on the simulation of the monomer rotational envelope under clustering conditions.« less

Femtosecond laser three-dimensional micro- and nanofabrication

NASA Astrophysics Data System (ADS)

Sugioka, Koji; Cheng, Ya

2014-12-01

The rapid development of the femtosecond laser has revolutionized materials processing due to its unique characteristics of ultrashort pulse width and extremely high peak intensity. The short pulse width suppresses the formation of a heat-affected zone, which is vital for ultrahigh precision fabrication, whereas the high peak intensity allows nonlinear interactions such as multiphoton absorption and tunneling ionization to be induced in transparent materials, which provides versatility in terms of the materials that can be processed. More interestingly, irradiation with tightly focused femtosecond laser pulses inside transparent materials makes three-dimensional (3D) micro- and nanofabrication available due to efficient confinement of the nonlinear interactions within the focal volume. Additive manufacturing (stereolithography) based on multiphoton absorption (two-photon polymerization) enables the fabrication of 3D polymer micro- and nanostructures for photonic devices, micro- and nanomachines, and microfluidic devices, and has applications for biomedical and tissue engineering. Subtractive manufacturing based on internal modification and fabrication can realize the direct fabrication of 3D microfluidics, micromechanics, microelectronics, and photonic microcomponents in glass. These microcomponents can be easily integrated in a single glass microchip by a simple procedure using a femtosecond laser to realize more functional microdevices, such as optofluidics and integrated photonic microdevices. The highly localized multiphoton absorption of a tightly focused femtosecond laser in glass can also induce strong absorption only at the interface of two closely stacked glass substrates. Consequently, glass bonding can be performed based on fusion welding with femtosecond laser irradiation, which provides the potential for applications in electronics, optics, microelectromechanical systems, medical devices, microfluidic devices, and small satellites. This review paper describes the concepts and principles of femtosecond laser 3D micro- and nanofabrication and presents a comprehensive review on the state-of-the-art, applications, and the future prospects of this technology.

Femtosecond laser three-dimensional micro- and nanofabrication

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sugioka, Koji, E-mail: ksugioka@riken.jp; Cheng, Ya, E-mail: ya.cheng@siom.ac.cn

2014-12-15

The rapid development of the femtosecond laser has revolutionized materials processing due to its unique characteristics of ultrashort pulse width and extremely high peak intensity. The short pulse width suppresses the formation of a heat-affected zone, which is vital for ultrahigh precision fabrication, whereas the high peak intensity allows nonlinear interactions such as multiphoton absorption and tunneling ionization to be induced in transparent materials, which provides versatility in terms of the materials that can be processed. More interestingly, irradiation with tightly focused femtosecond laser pulses inside transparent materials makes three-dimensional (3D) micro- and nanofabrication available due to efficient confinement ofmore » the nonlinear interactions within the focal volume. Additive manufacturing (stereolithography) based on multiphoton absorption (two-photon polymerization) enables the fabrication of 3D polymer micro- and nanostructures for photonic devices, micro- and nanomachines, and microfluidic devices, and has applications for biomedical and tissue engineering. Subtractive manufacturing based on internal modification and fabrication can realize the direct fabrication of 3D microfluidics, micromechanics, microelectronics, and photonic microcomponents in glass. These microcomponents can be easily integrated in a single glass microchip by a simple procedure using a femtosecond laser to realize more functional microdevices, such as optofluidics and integrated photonic microdevices. The highly localized multiphoton absorption of a tightly focused femtosecond laser in glass can also induce strong absorption only at the interface of two closely stacked glass substrates. Consequently, glass bonding can be performed based on fusion welding with femtosecond laser irradiation, which provides the potential for applications in electronics, optics, microelectromechanical systems, medical devices, microfluidic devices, and small satellites. This review paper describes the concepts and principles of femtosecond laser 3D micro- and nanofabrication and presents a comprehensive review on the state-of-the-art, applications, and the future prospects of this technology.« less

An investigation on 800 nm femtosecond laser ablation of K9 glass in air and vacuum

NASA Astrophysics Data System (ADS)

Xu, Shi-zhen; Yao, Cai-zhen; Dou, Hong-qiang; Liao, Wei; Li, Xiao-yang; Ding, Ren-jie; Zhang, Li-juan; Liu, Hao; Yuan, Xiao-dong; Zu, Xiao-tao

2017-06-01

Ablation rates of K9 glass were studied as a function of femtosecond laser fluences. The central wavelength was 800 nm, and pulse durations of 35 fs and 500 fs in air and vacuum were employed. Ablation thresholds of 0.42 J/cm2 and 2.1 J/cm2 were obtained at 35 fs and 500 fs, respectively, which were independent with the ambient conditions and depend on the incident pulse numbers due to incubation effects. The ablation rate of 35 fs pulse laser increased with the increasing of laser fluence in vacuum, while in air condition, it slowly increased to a plateau at high fluence. The ablation rate of 500 fs pulse laser showed an increase at low fluence and a slow drop of ablation rate was observed at high fluence in air and vacuum, which may due to the strong defocusing effects associated with the non-equilibrium ionization of air, and/or the shielding effects of conduction band electrons (CBEs) produced by multi-photon ionization and impact ionization in K9 glass surface. The typical ablation morphologies, e.g. smooth zone and laser-induced periodic surface structures (LIPSS) were also presented and illustrated.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sturm, F. P.; Tong, X. M.; Palacios, A.

Here, we used ultrashort femtosecond vacuum ultraviolet (VUV) and infrared (IR) pulses in a pump-probe scheme to map the dynamics and nonequilibrium dissociation channels of excited neutral H 2 molecules. A nuclear wave packet is created in the B 1Σmore » $$+\\atop{u}$$ state of the neutral H 2 molecule by absorption of the ninth harmonic of the driving infrared laser field. Due to the large stretching amplitude of the molecule excited in the B 1Σ$$+\\atop{u}$$ electronic state, the effective H 2 + ionization potential changes significantly as the nuclear wave packet vibrates in the bound, highly electronically and vibrationally excited B potential-energy curve. We probed such dynamics by ionizing the excited neutral molecule using time-delayed VUV-or-IR radiation. We identified the nonequilibrium dissociation channels by utilizing three-dimensional momentum imaging of the ion fragments. We also found that different dissociation channels can be controlled, to some extent, by changing the IR laser intensity and by choosing the wavelength of the probe laser light. Furthermore, we concluded that even in a benchmark molecular system such as H 2*, the interpretation of the nonequilibrium multiphoton and multicolor ionization processes is still a challenging task, requiring intricate theoretical analysis.« less

Zero kinetic energy photoelectron spectroscopy of triphenylene.

PubMed

Harthcock, Colin; Zhang, Jie; Kong, Wei

2014-06-28

We report vibrational information of both the first electronically excited state and the ground cationic state of jet-cooled triphenylene via the techniques of resonantly enhanced multiphoton ionization (REMPI) and zero kinetic energy (ZEKE) photoelectron spectroscopy. The first excited electronic state S1 of the neutral molecule is of A1' symmetry and is therefore electric dipole forbidden in the D3h group. Consequently, there are no observable Franck-Condon allowed totally symmetric a1' vibrational bands in the REMPI spectrum. All observed vibrational transitions are due to Herzberg-Teller vibronic coupling to the E' third electronically excited state S3. The assignment of all vibrational bands as e' symmetry is based on comparisons with calculations using the time dependent density functional theory and spectroscopic simulations. When an electron is eliminated, the molecular frame undergoes Jahn-Teller distortion, lowering the point group to C2v and resulting in two nearly degenerate electronic states of A2 and B1 symmetry. Here we follow a crude treatment by assuming that all e' vibrational modes resolve into b2 and a1 modes in the C2v molecular frame. Some observed ZEKE transitions are tentatively assigned, and the adiabatic ionization threshold is determined to be 63 365 ± 7 cm(-1). The observed ZEKE spectra contain a consistent pattern, with a cluster of transitions centered near the same vibrational level of the cation as that of the intermediate state, roughly consistent with the propensity rule. However, complete assignment of the detailed vibrational structure due to Jahn-Teller coupling requires much more extensive calculations, which will be performed in the future.

Multiple product pathways in photodissociation of nitromethane at 213 nm

NASA Astrophysics Data System (ADS)

Sumida, Masataka; Kohge, Yasunori; Yamasaki, Katsuyoshi; Kohguchi, Hiroshi

2016-02-01

In this paper, we present a photodissociation dynamics study of nitromethane at 213 nm in the π → π* transition. Resonantly enhanced multiphoton ionization spectroscopy and ion-imaging were applied to measure the internal state distributions and state-resolved scattering distributions of the CH3, NO(X 2Π, A 2Σ+), and O(3PJ) photofragments. The rotationally state-resolved scattering distribution of the CH3 fragment showed two velocity components, of which the slower one decreased the relative intensity as the rotational and vibrational excitations. The translational energy distribution of the faster CH3 fragment indicated the production of the NO2 counter-product in the electronic excited state, wherein 1 2B2 was the most probable. The NO(v = 0) fragment exhibited a bimodal translational energy distribution, whereas the NO(v = 1 and 2) fragment exhibited a single translational energy component with a relatively larger internal energy. The translational energy of a portion of the O(3PJ) photofragment was found to be higher than the one-photon dissociation threshold, indicating the two-photon process involved. The NO(A 2Σ+) fragment, which was detected by ionization spectroscopy via the Rydberg ←A 2Σ+ transition, also required two-photon energy. These experimental data corroborate the existence of competing photodissociation product pathways, CH3 + NO2,CH3 + NO + O,CH3O + NO, and CH3NO + O, following the π → π* transition. The origins of the observed photofragments are discussed in this report along with recent theoretical studies and previous dynamics experiments performed at 193 nm.

Multiple product pathways in photodissociation of nitromethane at 213 nm.

PubMed

Sumida, Masataka; Kohge, Yasunori; Yamasaki, Katsuyoshi; Kohguchi, Hiroshi

2016-02-14

In this paper, we present a photodissociation dynamics study of nitromethane at 213 nm in the π → π(*) transition. Resonantly enhanced multiphoton ionization spectroscopy and ion-imaging were applied to measure the internal state distributions and state-resolved scattering distributions of the CH3, NO(X (2)Π, A (2)Σ(+)), and O((3)PJ) photofragments. The rotationally state-resolved scattering distribution of the CH3 fragment showed two velocity components, of which the slower one decreased the relative intensity as the rotational and vibrational excitations. The translational energy distribution of the faster CH3 fragment indicated the production of the NO2 counter-product in the electronic excited state, wherein 1 (2)B2 was the most probable. The NO(v = 0) fragment exhibited a bimodal translational energy distribution, whereas the NO(v = 1 and 2) fragment exhibited a single translational energy component with a relatively larger internal energy. The translational energy of a portion of the O((3)PJ) photofragment was found to be higher than the one-photon dissociation threshold, indicating the two-photon process involved. The NO(A (2)Σ(+)) fragment, which was detected by ionization spectroscopy via the Rydberg ← A (2)Σ(+) transition, also required two-photon energy. These experimental data corroborate the existence of competing photodissociation product pathways, CH3 + NO2,CH3 + NO + O,CH3O + NO, and CH3NO + O, following the π → π(*) transition. The origins of the observed photofragments are discussed in this report along with recent theoretical studies and previous dynamics experiments performed at 193 nm.

Setup and use of a two-laser multiphoton microscope for multichannel intravital fluorescence imaging

PubMed Central

Entenberg, David; Wyckoff, Jeffrey; Gligorijevic, Bojana; Roussos, Evanthia T; Verkhusha, Vladislav V; Pollard, Jeffrey W; Condeelis, John

2014-01-01

Characterizing biological mechanisms dependent upon the interaction of many cell types in vivo requires both multiphoton microscope systems capable of expanding the number and types of fluorophores that can be imaged simultaneously while removing the wavelength and tunability restrictions of existing systems, and enhanced software for extracting critical cellular parameters from voluminous 4D data sets. We present a procedure for constructing a two-laser multiphoton microscope that extends the wavelength range of excitation light, expands the number of simultaneously usable fluorophores and markedly increases signal to noise via ‘over-clocking’ of detection. We also utilize a custom-written software plug-in that simplifies the quantitative tracking and analysis of 4D intravital image data. We begin by describing the optics, hardware, electronics and software required, and finally the use of the plug-in for analysis. We demonstrate the use of the setup and plug-in by presenting data collected via intravital imaging of a mouse model of breast cancer. The procedure may be completed in ~24 h. PMID:21959234

Photofragment slice imaging studies of pyrrole and the Xe{center_dot}{center_dot}{center_dot}pyrrole cluster

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rubio-Lago, L.; Zaouris, D.; Sakellariou, Y.

The photolysis of pyrrole has been studied in a molecular beam at wavelengths of 250, 240, and 193.3 nm, using two different carrier gases, He and Xe. A broad bimodal distribution of H-atom fragment velocities has been observed at all wavelengths. Near threshold at both 240 and 250 nm, sharp features have been observed in the fast part of the H-atom distribution. Under appropriate molecular beam conditions, the entire H-atom loss signal from the photolysis of pyrrole at both 240 and 250 nm (including the sharp features) disappear when using Xe as opposed to He as the carrier gas. Wemore » attribute this phenomenon to cluster formation between Xe and pyrrole, and this assumption is supported by the observation of resonance enhanced multiphoton ionization spectra for the (Xe{center_dot}{center_dot}{center_dot}pyrrole) cluster followed by photofragmentation of the nascent cation cluster. Ab initio calculations are presented for the ground states of the neutral and cationic (Xe{center_dot}{center_dot}{center_dot}pyrrole) clusters as a means of understanding their structural and energetic properties.« less

Angular distributions for the inelastic scattering of NO(X2Π ) with O2(X3Σg-)

NASA Astrophysics Data System (ADS)

Brouard, M.; Gordon, S. D. S.; Nichols, B.; Squires, E.; Walpole, V.; Aoiz, F. J.; Stolte, S.

2017-05-01

The inelastic scattering of NO(X2Π ) by O2(X3Σg-) was studied at a mean collision energy of 550 cm-1 using velocity-map ion imaging. The initial quantum state of the NO(X2Π , v = 0, j = 0.5, Ω =0.5 , 𝜖 = -1 , f) molecule was selected using a hexapole electric field, and specific Λ-doublet levels of scattered NO were probed using (1 +1' ) resonantly enhanced multiphoton ionization. A modified "onion-peeling" algorithm was employed to extract angular scattering information from the series of "pancaked," nested Newton spheres arising as a consequence of the rotational excitation of the molecular oxygen collision partner. The extracted differential cross sections for NO(X) f →f and f →e Λ-doublet resolved, spin-orbit conserving transitions, partially resolved in the oxygen co-product rotational quantum state, are reported, along with O2 fragment pair-correlated rotational state population. The inelastic scattering of NO with O2 is shown to share many similarities with the scattering of NO(X) with the rare gases. However, subtle differences in the angular distributions between the two collision partners are observed.

Design, fabrication and characterization of rugged, high-performance quantum dot photocathodes

NASA Astrophysics Data System (ADS)

Pietryga, Jeffrey; Robel, Istvan; Makarov, Nikolay; Lim, Jaehoon; Lin, Qianglu; Lewellen, John; Moody, Nathan

Semiconductor nanocrystal quantum dots (QDs) are bright, tunable fluorophores used as, e.g., biolabels and downcoverting phosphors. Such applications make use of over three decades in advances in techniques for overcoming the natural tendency of these materials toward losing photoexcited carriers to surface defect states or to ionization. Ironically, QDs first gained attention as a material class for use in photocatalysis, which uses QD photoionization to drive redox reactions. Here, we explore the use of QDs in an alternative application that also exploits photoionization, namely within photocathodes for the electron guns that will enable next-generation light sources. We evaluate the efficiency of electron photoemission of conductive, solution-cast QD films of a variety of compositions in a typical electron gun configuration. By quantifying photocurrent as a function of excitation photon energy, excitation intensity and pulse duration, we demonstrate efficiencies superior to standard copper cathodes in films that are more robust against oxidation. Finally, we establish the dominant mechanism responsible for electron emission in the multi-photon excitation regime, which suggests numerous pathways for further enhancements. We gratefully acknowledge the support of the Los Alamos National Laboratory Directed Research and Development (LDRD) program.

REAL-TIME MONITORING OF DIOXINS AND OTHER ...

EPA Pesticide Factsheets

This project is part of EPA's EMPACT program which was begun in 1998 and is jointly administered by EPA's Office of Research and Development, the National Center for Environmental Research and Quality Assurance (NCERQA), and the National Center for Environmental Assessment. The program was developed to provide understandable environmental information on various research initiatives to the public in a timely manner on various issues of importance. This particular project involves development of the application of an on-line, real time, trace organic air toxic monitor, with special emphasis on dioxin-related compounds. Research efforts demonstrate the utility and usefulness of the Resonance Enhanced Multi-Photon Ionization (REMPI) analytical method for trace organics control, monitoring, and compliance assurance. Project objectives will be to develop the REMPI instrumental method into a tool that will be used for assessment of potential dioxin sources, control and prevention of dioxin formation in known sources, and communication of facility performance. This will be accomplished through instrument development, laboratory verification, thermokinetic modelling, equilibrium modelling, statistical determinations, field validation, program publication and presentation, regulatory office support, and development of data communication/presentation procedures. For additional information on this EMPACT project, visit the website at http://www.epa.gov/appcdwww/crb/empa

SALI chemical analysis of provided samples

NASA Technical Reports Server (NTRS)

Becker, Christopher H.

1993-01-01

SRI has completed the chemical analysis of all the samples supplied by NASA. The final batch of four samples consisted of: one inch diameter MgF2 mirror, control 1200-ID-FL3; one inch diameter neat resin, PMR-15, AO171-IV-55, half exposed and half unexposed; one inch diameter chromic acid anodized, EOIM-3 120-47 aluminum disc; and AO-exposed and unexposed samples of fullerene extract material in powdered form, pressed into In foil for analysis. Chemical analyses of the surfaces were performed by the surface analysis by laser ionization (SALI) method. The analyses emphasize surface contamination or general organic composition. SALI uses nonselective photoionization of sputtered or desorbed atoms and molecules above but close (approximately one mm) to the surface, followed by time-of-flight (TOF) mass spectrometry. In these studies, we used laser-induced desorption by 5-ns pulse-width 355-nm light (10-100 mJ/sq cm) and single-photon ionization (SPI) by coherent 118-nm radiation (at approximately 5 x 10(exp 5) W/sq cm). SPI was chosen primarily for its ability to obtain molecular information, whereas multiphoton ionization (not used in the present studies) is intended primarily for elemental and small molecule information. In addition to these four samples, the Au mirror (EOIM-3 200-11, sample four) was depth profiled again. Argon ion sputtering was used together with photoionization with intense 355-nm radiation (35-ps pulsewidths). Depth profiles are similar to those reported earlier, showing reproducibility. No chromium was found in the sample above noise level; its presence could at most be at the trace level. Somewhat more Ni appears to be present in the Au layer in the unexposed side, indicating thermal diffusion without chemical enhancement. The result of the presence of oxygen is apparently to tie-up/draw out the Ni as an oxide at the surface. The exposed region has a brownish tint appearance to the naked eye.

Transition-matrix theory for two-photon ionization of rare-gas atoms and isoelectronic ions with application to argon

NASA Astrophysics Data System (ADS)

Starace, Anthony F.; Jiang, Tsin-Fu

1987-08-01

A transition-matrix theory for two-photon ionization processes in rare-gas atoms or isoelectronic ions is presented. Uncoupled ordinary differential equations are obtained for the radial functions needed to calculate the two-photon transition amplitude. The implications of these equations are discussed in detail. In particular, the role of correlations involving virtually excited electron pairs, which are known to be essential to the description of single-photon processes, is examined for multiphoton ionization processes. Additionally, electron scattering interactions between two electron-hole pairs are introduced into our transition amplitude in the boson approximation since these have been found important in two-photon ionization of xenon by L'Huillier and Wendin [J. Phys. B 20, L37 (1987)]. Application of our theory is made to two-photon ionization of the 3p subshell of argon below the one-photon ionization threshold. Our results are compared to previous calculations of McGuire [Phys. Rev. A 24, 835 (1981)], of Moccia, Rahman, and Rizzo [J. Phys. B 16, 2737 (1983)], and of Pindzola and Kelly [Phys. Rev. A 11, 1543 (1975)]. Results are presented for both circularly and linearly polarized photons. Among our findings are, firstly, that the electron scattering interactions, which have not been included in previous calculations for argon, produce a substantial reduction in the two-photon single-ionization cross section below the one-photon ionization threshold, which is in agreement with findings of L'Huillier and Wendin for xenon. Secondly, we find that de-excitation of virtually excited electron pairs by absorption of a photon is important for describing the interaction of the atom with the photon field, as in the case of single-photon ionization processes, but that further excitation of virtually excited electron pairs by the photon field has completely negligible effects, indicating a major simplification of the theory for higher-order absorption processes.

Far-UV photochemical bond cleavage of n-amyl nitrite: bypassing a repulsive surface.

PubMed

Minitti, Michael P; Zhang, Yao; Rosenberg, Martin; Brogaard, Rasmus Y; Deb, Sanghamitra; Sølling, Theis I; Weber, Peter M

2012-01-19

We have investigated the deep-UV photoinduced, homolytic bond cleavage of amyl nitrite to form NO and pentoxy radicals. One-color multiphoton ionization with ultrashort laser pulses through the S(2) state resonance gives rise to photoelectron spectra that reflect ionization from the S(1) state. Time-resolved pump-probe photoionization measurements show that upon excitation at 207 nm, the generation of NO in the v = 2 state is delayed, with a rise time of 283 (16) fs. The time-resolved mass spectrum shows the NO to be expelled with a kinetic energy of 1.0 eV, which is consistent with dissociation on the S(1) state potential energy surface. Combined, these observations show that the first step of the dissociation reaction involves an internal conversion from the S(2) to the S(1) state, which is followed by the ejection of the NO radical on the predissociative S(1) state potential energy surface.

Alignment, orientation, and Coulomb explosion of difluoroiodobenzene studied with the pixel imaging mass spectrometry (PImMS) camera.

PubMed

Amini, Kasra; Boll, Rebecca; Lauer, Alexandra; Burt, Michael; Lee, Jason W L; Christensen, Lauge; Brauβe, Felix; Mullins, Terence; Savelyev, Evgeny; Ablikim, Utuq; Berrah, Nora; Bomme, Cédric; Düsterer, Stefan; Erk, Benjamin; Höppner, Hauke; Johnsson, Per; Kierspel, Thomas; Krecinic, Faruk; Küpper, Jochen; Müller, Maria; Müller, Erland; Redlin, Harald; Rouzée, Arnaud; Schirmel, Nora; Thøgersen, Jan; Techert, Simone; Toleikis, Sven; Treusch, Rolf; Trippel, Sebastian; Ulmer, Anatoli; Wiese, Joss; Vallance, Claire; Rudenko, Artem; Stapelfeldt, Henrik; Brouard, Mark; Rolles, Daniel

2017-07-07

Laser-induced adiabatic alignment and mixed-field orientation of 2,6-difluoroiodobenzene (C 6 H 3 F 2 I) molecules are probed by Coulomb explosion imaging following either near-infrared strong-field ionization or extreme-ultraviolet multi-photon inner-shell ionization using free-electron laser pulses. The resulting photoelectrons and fragment ions are captured by a double-sided velocity map imaging spectrometer and projected onto two position-sensitive detectors. The ion side of the spectrometer is equipped with a pixel imaging mass spectrometry camera, a time-stamping pixelated detector that can record the hit positions and arrival times of up to four ions per pixel per acquisition cycle. Thus, the time-of-flight trace and ion momentum distributions for all fragments can be recorded simultaneously. We show that we can obtain a high degree of one-and three-dimensional alignment and mixed-field orientation and compare the Coulomb explosion process induced at both wavelengths.

Facile time-of-flight methods for characterizing pulsed superfluid helium droplet beams

DOE Office of Scientific and Technical Information (OSTI.GOV)

He, Yunteng; Zhang, Jie; Li, Yang

2015-08-15

We present two facile time-of-flight (TOF) methods of detecting superfluid helium droplets and droplets with neutral dopants. Without an electron gun and with only a heated filament and pulsed electrodes, the electron impact ionization TOF mass spectrometer can resolve ionized helium clusters such as He{sub 2}{sup +} and He{sub 4}{sup +}, which are signatures of superfluid helium droplets. Without ionizing any helium atoms, multiphoton non-resonant laser ionization of CCl{sub 4} doped in superfluid helium droplets at 266 nm generates complex cluster ions of dopant fragments with helium atoms, including (He){sub n}C{sup +}, (He){sub n}Cl{sup +}, and (He){sub n}CCl{sup +}. Usingmore » both methods, we have characterized our cryogenic pulsed valve—the Even-Lavie valve. We have observed a primary pulse with larger helium droplets traveling at a slower speed and a rebound pulse with smaller droplets at a faster speed. In addition, the pickup efficiency of dopant is higher for the primary pulse when the nozzle temperature is higher than 13 K, and the total time duration of the doped droplet pulse is only on the order of 20 μs. These results stress the importance of fast and easy characterization of the droplet beam for sensitive measurements such as electron diffraction of doped droplets.« less

COMPACT NON-CONTACT TOTAL EMISSION DETECTION FOR IN-VIVO MULTI-PHOTON EXCITATION MICROSCOPY

PubMed Central

Glancy, Brian; Karamzadeh, Nader S.; Gandjbakhche, Amir H.; Redford, Glen; Kilborn, Karl; Knutson, Jay R.; Balaban, Robert S.

2014-01-01

Summary We describe a compact, non-contact design for a Total Emission Detection (c-TED) system for intra-vital multi-photon imaging. To conform to a standard upright two-photon microscope design, this system uses a parabolic mirror surrounding a standard microscope objective in concert with an optical path that does not interfere with normal microscope operation. The non-contact design of this device allows for maximal light collection without disrupting the physiology of the specimen being examined. Tests were conducted on exposed tissues in live animals to examine the emission collection enhancement of the c-TED device compared to heavily optimized objective-based emission collection. The best light collection enhancement was seen from murine fat (5×-2× gains as a function of depth), while murine skeletal muscle and rat kidney showed gains of over two and just under two-fold near the surface, respectively. Gains decreased with imaging depth (particularly in the kidney). Zebrafish imaging on a reflective substrate showed close to a two-fold gain throughout the entire volume of an intact embryo (approximately 150 μm deep). Direct measurement of bleaching rates confirmed that the lower laser powers (enabled by greater light collection efficiency) yielded reduced photobleaching in vivo. The potential benefits of increased light collection in terms of speed of imaging and reduced photo-damage, as well as the applicability of this device to other multi-photon imaging methods is discussed. PMID:24251437

Temporal focusing-based multiphoton excitation microscopy via digital micromirror device.

PubMed

Yih, Jenq-Nan; Hu, Yvonne Yuling; Sie, Yong Da; Cheng, Li-Chung; Lien, Chi-Hsiang; Chen, Shean-Jen

2014-06-01

This Letter presents an enhanced temporal focusing-based multiphoton excitation (MPE) microscope in which the conventional diffraction grating is replaced by a digital micromirror device (DMD). Experimental results from imaging a thin fluorescence film show that the 4.0 μm axial resolution of the microscope is comparable with that of a setup incorporating a 600  lines/mm grating; hence, the optical sectioning ability of the proposed setup is demonstrated. Similar to a grating, the DMD diffracts illuminating light frequencies for temporal focusing; additionally, it generates arbitrary patterns. Since the DMD is placed on the image-conjugate plane of the objective lens' focal plane, the MPE pattern can be projected on the focal plane precisely.

Propagation of intense short laser pulses in the atmosphere.

PubMed

Sprangle, P; Peñano, J R; Hafizi, B

2002-10-01

The propagation of short, intense laser pulses in the atmosphere is investigated theoretically and numerically. A set of three-dimensional (3D), nonlinear propagation equations is derived, which includes the effects of dispersion, nonlinear self-focusing, stimulated molecular Raman scattering, multiphoton and tunneling ionization, energy depletion due to ionization, relativistic focusing, and ponderomotively excited plasma wakefields. The instantaneous frequency spread along a laser pulse in air, which develops due to various nonlinear effects, is analyzed and discussed. Coupled equations for the power, spot size, and electron density are derived for an intense ionizing laser pulse. From these equations we obtain an equilibrium for a single optical-plasma filament, which involves a balancing between diffraction, nonlinear self-focusing, and plasma defocusing. The equilibrium is shown to require a specific distribution of power along the filament. It is found that in the presence of ionization a self-guided optical filament is not realizable. A method for generating a remote spark in the atmosphere is proposed, which utilizes the dispersive and nonlinear properties of air to cause a low-intensity chirped laser pulse to compress both longitudinally and transversely. For optimally chosen parameters, we find that the transverse and longitudinal focal lengths can be made to coincide, resulting in rapid intensity increase, ionization, and white light generation in a localized region far from the source. Coupled equations for the laser spot size and pulse duration are derived, which can describe the focusing and compression process in the low-intensity regime. More general examples involving beam focusing, compression, ionization, and white light generation near the focal region are studied by numerically solving the full set of 3D, nonlinear propagation equations.

A High Pressure Pulsed Expansion Valve for Gases, Liquids, and Supercritical Fluids

NASA Astrophysics Data System (ADS)

Köster, C.; Grotemeyer, J.; Schlag, E. W.

1990-12-01

A novel design of a pulsed valve for coupling chromatographic techniques with gaseous and liquid mobile phases to a time-of-flight mass spectrometer with multiphoton ionization (MUPI) is presented. The valve can be operated in low pressure regions ( <10 bar) up to temperatures of 350 °C and at higher pressures (300 bar) up to temperatures of 200 °C. Pulse widths lower than 100 μs could be measured. First results demonstrate the ability of interfacing of liquid chromatography to MUPI-mass spectrometry. Additional coupling of CO2-laser desorption to the valve allows the interface to be used for mass spectrometric measurements of nonvolatile biomolecules.

Spatially resolved organic analysis of the Allende meteorite

NASA Technical Reports Server (NTRS)

Zenobi, Renato; Philippoz, Jean-Michel; Zare, Richard N.; Buseck, Peter R.

1989-01-01

The distribution of polycyclic aromatic hydrocarbons (PAHs) in the Allende meteorite has been probed with two-step laser desorption/laser multiphoton ionization mass spectrometry. This method allows direct in situ analysis with a spatial resolution of 1 sq mm or better of selected organic molecules. Spectra from freshly fractured interior surfaces of the meteorite show that PAH concentrations are locally high compared to the average concentrations found by wet chemical analysis of pulverized samples. The data suggest that the PAHs are primarily associated with the fine-grained matrix, where the organic polymer occurs. In addition, highly substituted PAH skeletons were observed. Interiors of individual chondrules were devoid of PAHs at the detection limit (about 0.05 ppm).

Measurement of absorption spectrum of deuterium oxide (D{sub 2}O) and its application to signal enhancement in multiphoton microscopy at the 1700-nm window

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Yuxin; Wen, Wenhui; Wang, Kai

2016-01-11

1700-nm window has been demonstrated to be a promising excitation window for deep-tissue multiphoton microscopy (MPM). Long working-distance water immersion objective lenses are typically used for deep-tissue imaging. However, absorption due to immersion water at 1700 nm is still high and leads to dramatic decrease in signals. In this paper, we demonstrate measurement of absorption spectrum of deuterium oxide (D{sub 2}O) from 1200 nm to 2600 nm, covering the three low water-absorption windows potentially applicable for deep-tissue imaging (1300 nm, 1700 nm, and 2200 nm). We apply this measured result to signal enhancement in MPM at the 1700-nm window. Compared with water immersion, D{sub 2}O immersionmore » enhances signal levels in second-harmonic generation imaging, 3-photon fluorescence imaging, and third-harmonic generation imaging by 8.1, 24.8, and 24.7 times with 1662-nm excitation, in good agreement with theoretical calculation based on our absorption measurement. This suggests D{sub 2}O a promising immersion medium for deep-tissue imaging.« less

A giant enhancement of multiphoton absorption in single-layer molybdenum disulfide

NASA Astrophysics Data System (ADS)

Zhou, Feng; Ji, Wei

Identifying light absorption mechanisms in nanoscale materials, which are more efficient than those observed in bulk semiconductors, are of paramount importance to next-generation, infrared photo-detection. Here, we report considerable enhancement of degenerate two-photon absorption (2PA) and three-photon absorption (3PA) through two-dimensional (2D) excitonic effects in single-layer molybdenum disulfide (1L-MoS2) . We theoretically predict that both degenerate 2PA and 3PA coefficients of 1L-MoS2 are enhanced by 10-1000 times in the near-infrared (NIR), as compared with those of bulk semiconductors. Our theoretical prediction is validated by measuring photocurrents induced by 2PA or 3PA in a 1L-MoS2 photo-detector at room temperature where excitons in the immediate vicinity of the bandgap are transferred to the conduction band by a very small amount of thermal energy and dissociated under an external electric field. Our finding lays theoretical foundation and provides experimental evidence for developing sensitive infrared multiphoton detectors for nano-photonics. This work was supported by National University of Singapore through a research Grant: R144-000-327-112.

USE OF REMPI-TOFMS FOR REAL-TIME MEASUREMENT OF TRACE AROMATICS DURING OPERATION OF AIRCRAFT GROUND EQUIPMENT

EPA Science Inventory

Emissions of aromatic air toxics from aircraft ground equipment were measured with a resonance enhanced multiphoton ionization—time of flight mass spectrometry (REMPI-TOFMS) system consisting of a pulsed solid state laser for photoionization and a TOFMS for mass discrimination. T...

Mapping and controlling ultrafast dynamics of highly excited H 2 molecules by VUV-IR pump-probe schemes

DOE PAGES

Sturm, F. P.; Tong, X. M.; Palacios, A.; ...

2017-01-09

Here, we used ultrashort femtosecond vacuum ultraviolet (VUV) and infrared (IR) pulses in a pump-probe scheme to map the dynamics and nonequilibrium dissociation channels of excited neutral H 2 molecules. A nuclear wave packet is created in the B 1Σmore » $$+\\atop{u}$$ state of the neutral H 2 molecule by absorption of the ninth harmonic of the driving infrared laser field. Due to the large stretching amplitude of the molecule excited in the B 1Σ$$+\\atop{u}$$ electronic state, the effective H 2 + ionization potential changes significantly as the nuclear wave packet vibrates in the bound, highly electronically and vibrationally excited B potential-energy curve. We probed such dynamics by ionizing the excited neutral molecule using time-delayed VUV-or-IR radiation. We identified the nonequilibrium dissociation channels by utilizing three-dimensional momentum imaging of the ion fragments. We also found that different dissociation channels can be controlled, to some extent, by changing the IR laser intensity and by choosing the wavelength of the probe laser light. Furthermore, we concluded that even in a benchmark molecular system such as H 2*, the interpretation of the nonequilibrium multiphoton and multicolor ionization processes is still a challenging task, requiring intricate theoretical analysis.« less

Modeling of ablation threshold dependence on pulse duration for dielectrics with ultrashort pulsed laser

NASA Astrophysics Data System (ADS)

Sun, Mingying; Zhu, Jianqiang; Lin, Zunqi

2017-01-01

We present a numerical model of plasma formation in ultrafast laser ablation on the dielectrics surface. Ablation threshold dependence on pulse duration is predicted with the model and the numerical results for water agrees well with the experimental data for pulse duration from 140 fs to 10 ps. Influences of parameters and approximations of photo- and avalanche-ionization on the ablation threshold prediction are analyzed in detail for various pulse lengths. The calculated ablation threshold is strongly dependent on electron collision time for all the pulse durations. The complete photoionization model is preferred for pulses shorter than 1 ps rather than the multiphoton ionization approximations. The transition time of inverse bremsstrahlung absorption needs to be considered when pulses are shorter than 5 ps and it can also ensure the avalanche ionization (AI) coefficient consistent with that in multiple rate equations (MREs) for pulses shorter than 300 fs. The threshold electron density for AI is only crucial for longer pulses. It is reasonable to ignore the recombination loss for pulses shorter than 100 fs. In addition to thermal transport and hydrodynamics, neglecting the threshold density for AI and recombination could also contribute to the disagreements between the numerical and the experimental results for longer pulses.

Ophthalmic imaging using multiphoton microscopy

NASA Astrophysics Data System (ADS)

Teng, Shu-Wen; Peng, Ju-Li; Lin, Huei-Hsing; Wu, Hai-Yin; Lo, Wen; Sun, Yen; Lin, Wei-Chou; Lin, Sung-Jan; Jee, Shiou-Hwa; Tan, Hsin-Yuan; Dong, Chen-Yuan

2005-04-01

This purpose of this study is to demonstrate the feasibility of using multiphoton microscopy in ophthalmologic imaging. Without the introduction of extrinsic fluorescence molecules, multiphoton induced autofluorescence and second harmonic generation signals can be used to obtain useful structural information of normal and diseased corneas. Our work can potentially lead to the in vivo application of multiphoton microscopy in investigating corneal physiology and pathologies.

Multiple product pathways in photodissociation of nitromethane at 213 nm

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sumida, Masataka; Kohge, Yasunori; Yamasaki, Katsuyoshi

2016-02-14

In this paper, we present a photodissociation dynamics study of nitromethane at 213 nm in the π → π{sup *} transition. Resonantly enhanced multiphoton ionization spectroscopy and ion-imaging were applied to measure the internal state distributions and state-resolved scattering distributions of the CH{sub 3}, NO(X {sup 2}Π, A {sup 2}Σ{sup +}), and O({sup 3}P{sub J}) photofragments. The rotationally state-resolved scattering distribution of the CH{sub 3} fragment showed two velocity components, of which the slower one decreased the relative intensity as the rotational and vibrational excitations. The translational energy distribution of the faster CH{sub 3} fragment indicated the production of themore » NO{sub 2} counter-product in the electronic excited state, wherein 1 {sup 2}B{sub 2} was the most probable. The NO(v = 0) fragment exhibited a bimodal translational energy distribution, whereas the NO(v = 1 and 2) fragment exhibited a single translational energy component with a relatively larger internal energy. The translational energy of a portion of the O({sup 3}P{sub J}) photofragment was found to be higher than the one-photon dissociation threshold, indicating the two-photon process involved. The NO(A {sup 2}Σ{sup +}) fragment, which was detected by ionization spectroscopy via the Rydberg ←A {sup 2}Σ{sup +} transition, also required two-photon energy. These experimental data corroborate the existence of competing photodissociation product pathways, CH{sub 3} + NO{sub 2},CH{sub 3} + NO + O,CH{sub 3}O + NO, and CH{sub 3}NO + O, following the π → π{sup *} transition. The origins of the observed photofragments are discussed in this report along with recent theoretical studies and previous dynamics experiments performed at 193 nm.« less

Probing Long-Range Configurations of Molecular Hydrogen

NASA Astrophysics Data System (ADS)

McCormack, Elizabeth

2011-05-01

Very long-range molecular configurations are of interest in a variety of contexts, for example, in the astro-chemistry of cold molecular clouds and in planetary atmospheres, including our own. Such states can be more than 10 times the size of the ground state and often possess energies above multiple ionization potentials and dissociation limits resulting in diverse and complex decay dynamics. Many of these configurations possess a double-well character arising from the interaction of molecular Rydberg states, repulsive doubly-excited states, and ionic states. The ion pair in hydrogen, an unusual molecular configuration consisting of one proton shrouded in a cloud of two electrons separated very far from the other proton, is notoriously difficult to create and study. We report results from on our investigation of such states using resonantly enhanced multi-photon ionization via the E,F v = 6, J = 0, 1, and 2 states to probe the H(n = 1) + H(n = 3) dissociation threshold energy region. Both molecular and atomic ion production were detected as a function of wavelength by using a time-of-flight mass spectrometer. Below threshold a series of highly excited vibrational levels of several long range states are observed. Above threshold broad resonances are observed with energies that agree well with the predictions of a mass-scaled Rydberg formula for bound states of the H+ H- ion pair. Measured linewidths, quantum defects, and rotational dependences are reported for ion pair principal quantum numbers in the range of n = 130 to 206. Our new results can be compared to recent experimental work using a different excitation scheme, which was the first spectroscopic observation of heavy Rydberg states in hydrogen, and new ab initio theoretical work. Supported by the National Science Foundation.

Multiphoton gradient index endoscopy for evaluation of diseased human prostatic tissue ex vivo

NASA Astrophysics Data System (ADS)

Huland, David M.; Jain, Manu; Ouzounov, Dimitre G.; Robinson, Brian D.; Harya, Diana S.; Shevchuk, Maria M.; Singhal, Paras; Xu, Chris; Tewari, Ashutosh K.

2014-11-01

Multiphoton microscopy can instantly visualize cellular details in unstained tissues. Multiphoton probes with clinical potential have been developed. This study evaluates the suitability of multiphoton gradient index (GRIN) endoscopy as a diagnostic tool for prostatic tissue. A portable and compact multiphoton endoscope based on a 1-mm diameter, 8-cm length GRIN lens system probe was used. Fresh ex vivo samples were obtained from 14 radical prostatectomy patients and benign and malignant areas were imaged and correlated with subsequent H&E sections. Multiphoton GRIN endoscopy images of unfixed and unprocessed prostate tissue at a subcellular resolution are presented. We note several differences and identifying features of benign versus low-grade versus high-grade tumors and are able to identify periprostatic tissues such as adipocytes, periprostatic nerves, and blood vessels. Multiphoton GRIN endoscopy can be used to identify both benign and malignant lesions in ex vivo human prostate tissue and may be a valuable diagnostic tool for real-time visualization of suspicious areas of the prostate.

In vivo multiphoton tomography and fluorescence lifetime imaging of human brain tumor tissue.

PubMed

Kantelhardt, Sven R; Kalasauskas, Darius; König, Karsten; Kim, Ella; Weinigel, Martin; Uchugonova, Aisada; Giese, Alf

2016-05-01

High resolution multiphoton tomography and fluorescence lifetime imaging differentiates glioma from adjacent brain in native tissue samples ex vivo. Presently, multiphoton tomography is applied in clinical dermatology and experimentally. We here present the first application of multiphoton and fluorescence lifetime imaging for in vivo imaging on humans during a neurosurgical procedure. We used a MPTflex™ Multiphoton Laser Tomograph (JenLab, Germany). We examined cultured glioma cells in an orthotopic mouse tumor model and native human tissue samples. Finally the multiphoton tomograph was applied to provide optical biopsies during resection of a clinical case of glioblastoma. All tissues imaged by multiphoton tomography were sampled and processed for conventional histopathology. The multiphoton tomograph allowed fluorescence intensity- and fluorescence lifetime imaging with submicron spatial resolution and 200 picosecond temporal resolution. Morphological fluorescence intensity imaging and fluorescence lifetime imaging of tumor-bearing mouse brains and native human tissue samples clearly differentiated tumor and adjacent brain tissue. Intraoperative imaging was found to be technically feasible. Intraoperative image quality was comparable to ex vivo examinations. To our knowledge we here present the first intraoperative application of high resolution multiphoton tomography and fluorescence lifetime imaging of human brain tumors in situ. It allowed in vivo identification and determination of cell density of tumor tissue on a cellular and subcellular level within seconds. The technology shows the potential of rapid intraoperative identification of native glioma tissue without need for tissue processing or staining.

Enhanced eumelanin emission by stepwise three-photon excitation

NASA Astrophysics Data System (ADS)

Kerimo, Josef; Rajadhyaksha, Milind; DiMarzio, Charles A.

2011-03-01

Eumelanin fluorescence from Sepia officinalis and black human hair was activated with near-infrared radiation and multiphoton excitation. A third order multiphoton absorption by a step-wise process appears to be the underlying mechanism. The activation was caused by a photochemical process since it could not be reproduced by simple heating. Both fluorescence and brightfield imaging indicate the near-infrared irradiation caused photodamage to the eumelanin and the activated emission originated from the photodamaged region. At least two different components with about thousand-fold enhanced fluorescence were activated and could be distinguished by their excitation properties. One component was excited with wavelengths in the visible region and exhibited linear absorption dependence. The second component could be excited with near-infrared wavelengths and had a third order dependence on the laser power. The third order dependence is explained by a step-wise excited state absorption (ESA) process since it could be observed equally with the CW and femtosecond lasers. The new method for photoactivating the eumelanin fluorescence was used to map the melanin content in human hair.

Investigation of the RbCa molecule: Experiment and theory.

PubMed

Pototschnig, Johann V; Krois, Günter; Lackner, Florian; Ernst, Wolfgang E

2015-04-01

We present a thorough theoretical and experimental study of the electronic structure of RbCa. The mixed alkali-alkaline earth molecule RbCa was formed on superfluid helium nanodroplets. Excited states of the molecule in the range of 13 000-23 000 cm -1 were recorded by resonance enhanced multi-photon ionization time-of-flight spectroscopy. The experiment is accompanied by high level ab initio calculations of ground and excited state properties, utilizing a multireference configuration interaction method based on multiconfigurational self consistent field calculations. With this approach the potential energy curves and permanent electric dipole moments of 24 electronic states were calculated. In addition we computed the transition dipole moments for transitions from the ground into excited states. The combination of experiment and theory allowed the assignment of features in the recorded spectrum to the excited [Formula: see text], [Formula: see text], [Formula: see text], [Formula: see text], [Formula: see text], [Formula: see text], [Formula: see text], and [Formula: see text] states, where the experiment allowed to benchmark the calculation. This is the first experimental work giving insight into the previously unknown RbCa molecule, which offers great prospects in ultracold molecular physics due to its magnetic and electronic dipole moment in the [Formula: see text] ground state.

Velocity-tunable slow beams of cold O2 in a single spin-rovibronic state with full angular-momentum orientation by multistage Zeeman deceleration

NASA Astrophysics Data System (ADS)

Wiederkehr, A. W.; Schmutz, H.; Motsch, M.; Merkt, F.

2012-08-01

Cold samples of oxygen molecules in supersonic beams have been decelerated from initial velocities of 390 and 450 m s-1 to final velocities in the range between 150 and 280 m s-1 using a 90-stage Zeeman decelerator. (2 + 1) resonance-enhanced-multiphoton-ionization (REMPI) spectra of the 3sσ g 3Π g (C) ? two-photon transition of O2 have been recorded to characterize the state selectivity of the deceleration process. The decelerated molecular sample was found to consist exclusively of molecules in the J ‧‧ = 2 spin-rotational component of the X ? ground state of O2. Measurements of the REMPI spectra using linearly polarized laser radiation with polarization vector parallel to the decelerator axis, and thus to the magnetic-field vector of the deceleration solenoids, further showed that only the ? magnetic sublevel of the N‧‧ = 1, J ‧‧ = 2 spin-rotational level is populated in the decelerated sample, which therefore is characterized by a fully oriented total-angular-momentum vector. By maintaining a weak quantization magnetic field beyond the decelerator, the polarization of the sample could be maintained over the 5 cm distance separating the last deceleration solenoid and the detection region.

Real-time monitoring of BTEX in air via ambient-pressure MPI

NASA Astrophysics Data System (ADS)

Swenson, Orven F.; Carriere, Josef P.; Isensee, Harlan; Gillispie, Gregory D.; Cooper, William F.; Dvorak, Michael A.

1998-05-01

We have developed and begun to field test a very sensitive method for real-time measurements of single-ring aromatic hydrocarbons in ambient air. In this study, we focus on the efficient 1 + 1 resonance enhanced multiphoton ionization (REMPI) of the BTEX species in the narrow region between 266 and 267 nm. We particularly emphasize 266.7 nm, a wavelength at which both benzene and toluene exhibit a sharp absorbance feature and benzene and its alkylated derivatives all absorb. An optical parametric oscillator system generating 266.7 nm, a REMPI cell, and digital oscilloscope detector are mounted on a breadboard attached to a small cart. In the first field test, the cart was wheeled through the various rooms of a chemistry research complex. Leakage of fuel through the gas caps of cars and light trucks in a parking lot was the subject of the second field test. The same apparatus was also used for a study in which the performance of the REMPI detector and a conventional photoionization detector were compared as a BTEX mixture was eluted by gas chromatography. Among the potential applications of the methodology are on-site analysis of combustion and manufacturing processes, soil gas and water headspace monitoring, space cabin and building air quality, and fuel leak detection.

Three-dimensional femtosecond laser processing for lab-on-a-chip applications

NASA Astrophysics Data System (ADS)

Sima, Felix; Sugioka, Koji; Vázquez, Rebeca Martínez; Osellame, Roberto; Kelemen, Lóránd; Ormos, Pal

2018-02-01

The extremely high peak intensity associated with ultrashort pulse width of femtosecond laser allows us to induce nonlinear interaction such as multiphoton absorption and tunneling ionization with materials that are transparent to the laser wavelength. More importantly, focusing the femtosecond laser beam inside the transparent materials confines the nonlinear interaction only within the focal volume, enabling three-dimensional (3D) micro- and nanofabrication. This 3D capability offers three different schemes, which involve undeformative, subtractive, and additive processing. The undeformative processing preforms internal refractive index modification to construct optical microcomponents including optical waveguides. Subtractive processing can realize the direct fabrication of 3D microfluidics, micromechanics, microelectronics, and photonic microcomponents in glass. Additive processing represented by two-photon polymerization enables the fabrication of 3D polymer micro- and nanostructures for photonic and microfluidic devices. These different schemes can be integrated to realize more functional microdevices including lab-on-a-chip devices, which are miniaturized laboratories that can perform reaction, detection, analysis, separation, and synthesis of biochemical materials with high efficiency, high speed, high sensitivity, low reagent consumption, and low waste production. This review paper describes the principles and applications of femtosecond laser 3D micro- and nanofabrication for lab-on-a-chip applications. A hybrid technique that promises to enhance functionality of lab-on-a-chip devices is also introduced.

Gas-phase spectroscopy of synephrine by laser desorption supersonic jet technique.

PubMed

Ishiuchi, Shun-ichi; Asakawa, Toshiro; Mitsuda, Haruhiko; Miyazaki, Mitsuhiko; Chakraborty, Shamik; Fujii, Masaaki

2011-09-22

In our previous work, we found that synephrine has six conformers in the gas phase, while adrenaline, which is a catecholamine and has the same side chain as synephrine, has been reported to have only two conformers. To determine the conformational geometries of synephrine, we measured resonance enhanced multiphoton ionization, ultraviolet-ultraviolet hole burning, and infrared dip spectra by utilizing the laser desorption supersonic jet technique. By comparing the observed infrared spectra with theoretical ones, we assigned geometries except for the orientations of the phenolic OH group. Comparison between the determined structures of synephrine and those of 2-methylaminno-1-phenylethanol, which has the same side chain as synephrine but no phenol OH group, leads to the conclusion that the phenolic OH group in synephrine does not affect the conformational flexibility of the side chain. In the case of adrenaline, which is expected to have 12 conformers if there are no interactions between the catecholic OH groups and the side chain, some interactions possibly exist between them because only two conformations are observed. By estimation of the dipole-dipole interaction energy between partial dipole moments of the catecholic OH groups and the side chain, it was concluded that the dipole-dipole interaction stabilizes specific conformers which are actually observed. © 2011 American Chemical Society

Electron Capture Dissociation of Divalent Metal-adducted Sulfated N-Glycans Released from Bovine Thyroid Stimulating Hormone

NASA Astrophysics Data System (ADS)

Zhou, Wen; Håkansson, Kristina

2013-11-01

Sulfated N-glycans released from bovine thyroid stimulating hormone (bTSH) were ionized with the divalent metal cations Ca2+, Mg2+, and Co by electrospray ionization (ESI). These metal-adducted species were subjected to infrared multiphoton dissociation (IRMPD) and electron capture dissociation (ECD) and the corresponding fragmentation patterns were compared. IRMPD generated extensive glycosidic and cross-ring cleavages, but most product ions suffered from sulfonate loss. Internal fragments were also observed, which complicated the spectra. ECD provided complementary structural information compared with IRMPD, and all observed product ions retained the sulfonate group, allowing sulfonate localization. To our knowledge, this work represents the first application of ECD towards metal-adducted sulfated N-glycans released from a glycoprotein. Due to the ability of IRMPD and ECD to provide complementary structural information, the combination of the two strategies is a promising and valuable tool for glycan structural characterization. The influence of different metal ions was also examined. Calcium adducts appeared to be the most promising species because of high sensitivity and ability to provide extensive structural information.

Investigation of depilatory mechanism by use of multiphoton fluorescent microscopy

NASA Astrophysics Data System (ADS)

Lin, Chiao-Ying; Lee, Gie-ne; Jee, Shiou-Hwa; Dong, Chen-Yuan; Lin, Sung-Jan

2007-07-01

Transdermal drug delivery provides a non-invasive route of drug administration, and can be a alternative method to oral delivery and injection. The stratum corneum (SC) of skin acts as the main barrier to transdermal drug delivery. Studies suggest that depilatory enhances permeability of drug through the epidermis. However, transdermal delivery pathway and mechanism are not completely understood. Previous studies have found that depilatory changes the keratinocytes of epidermis, and cause the protein in combination with lipid extraction of SC to become disordered. Nevertheless, those studies did not provide images of those processes. The aim of this study is to characterize the penetration enhancing effect of depilatory agent and the associated structural alterations of stratum corneum. Fresh human foreskin is treated by a depilatory agent for 10 minutes and then subjected to the treatment of fluorescent model drugs of hydrophilic rhodamine and hydrophobic rhodamine-RE. The penetration of model drugs is imaged and quantified by multiphoton microscopy. Our results showed that the penetration of both hydrophilic and hydrophobic agents can be enhanced and multifocal detachment of surface corneocytes is revealed. Nile red staining revealed, instead of a regular motar distribution of lipid around the brick of corneocytes, a disorganized and homogenized pattern of lipid distribution. We concluded that depilatory agents enhance drug penetration by disrupting both the cellular integrity of corneocytes and the regular packing of intercellular lipid of stratum corneum.

Photon-momentum transfer in molecular photoionization

NASA Astrophysics Data System (ADS)

Chelkowski, Szczepan; Bandrauk, André D.

2018-05-01

In most models and theoretical calculations describing multiphoton ionization by infrared light, the dipole approximation is used. This is equivalent to setting the very small photon momentum to zero. Using numerical solutions of the (nondipole) three-dimensional time-dependent Schrödinger equation for one electron in a H2+ molecular ion we investigate the effect the photon-momentum transfer to the photoelectron in an H2+ ion in various regimes. We find that the photon-momentum transfer in a molecule is very different from the transfer in atoms due to two-center interference effects. The photon-momentum transfer is very sensitive to the symmetry of the initial electronic state and is strongly dependent on the internuclear distance and on the ellipticity of the laser.

An ultracold potassium Rydberg source for experiments in quantum optics and many-body physics

NASA Astrophysics Data System (ADS)

Conover, Charles; Dupre, Pamela; Tong, Ai Phuong; Sanon, Carlvin; Clarke, Kevin; Doolittle, Brian; Louria, Stephen; Adamson, Philip

2017-04-01

We report on the development of an apparatus for the study of quantum dynamics of Rydberg atoms of potassium. Samples of Rydberg atoms at 1 mK and varying density are excited in a magneto-optical trap of 107 K-39 atoms. The atoms are excited to Rydberg states in a steps from 4s to 5p and from 5p to ns and nd states using stabilized external-cavity diode lasers at 405 nm and 980 nm. Selective field ionization and detection with microchannel plates provides a platform for spectroscopic measurements in potassium, exploration of multiphoton processes, and experiments on cold atom collisions. This research was supported by the National Science Foundation under Grant PHY-1126599.

Bond-selective photodissociation of partially deuterated ammonia molecules: Photodissociations of vibrationally excited NHD2 in the 5νNH state and NH2D in the 5νND state

NASA Astrophysics Data System (ADS)

Akagi, Hiroshi; Yokoyama, Keiichi; Yokoyama, Atsushi

2004-03-01

Ultraviolet photodissociation of NHD2 excited to the fourth overtone state of the NH stretching mode (5νNH) and NH2D excited to that of the ND stretching mode (5νND) has been investigated by using a crossed laser and molecular beams method. Branching ratio between the NH and ND bond dissociations has been determined by utilizing a (2+1) resonance enhanced multiphoton ionization scheme of H and D atoms. For the photolysis of NHD2 in the 5νNH state, the NH dissociation cross section is 5.1±1.4 times as large as the ND dissociation cross section per bond. On the other hand, for the photolysis of NH2D in the 5νND state, the ratio of the NH dissociation cross section per bond to the ND dissociation cross section decreases to 0.68±0.16. In comparison with the branching ratios for the photolysis of vibrationally unexcited NH2D and NHD2 [Koda and Back, Can. J. Chem. 55, 1380 (1977)], the present results indicate that the excitation of the NH stretching mode enhances the NH dissociation with ca. two times larger NH/ND branching ratio, whereas the excitation of the ND stretching mode results in the preferential ND dissociation with ca. 3-4 times larger ND/NH branching ratio than that for the vibrational ground states. The mechanism of the bond-selective enhancement has been discussed in terms of the energetics and dynamics of wave packet.

Multiphoton dynamics of qutrits in the ultrastrong coupling regime with a quantized photonic field

DOE Office of Scientific and Technical Information (OSTI.GOV)

Avetissian, H. K., E-mail: avetissian@ysu.am; Avetissian, A. K.; Mkrtchian, G. F.

2015-12-15

Multiphoton resonant excitation of a three-state quantum system (a qutrit) with a single-mode photonic field is considered in the ultrastrong coupling regime, when the qutrit–photonic field coupling rate is comparable to appreciable fractions of the photon frequency. For ultrastrong couplings, the obtained solutions of the Schrödinger equation that reveal multiphoton Rabi oscillations in qutrits with the interference effects leading to the collapse and revival of atomic excitation probabilities at the direct multiphoton resonant transitions.

High-resolution multimodal clinical multiphoton tomography of skin

NASA Astrophysics Data System (ADS)

König, Karsten

2011-03-01

This review focuses on multimodal multiphoton tomography based on near infrared femtosecond lasers. Clinical multiphoton tomographs for 3D high-resolution in vivo imaging have been placed into the market several years ago. The second generation of this Prism-Award winning High-Tech skin imaging tool (MPTflex) was introduced in 2010. The same year, the world's first clinical CARS studies have been performed with a hybrid multimodal multiphoton tomograph. In particular, non-fluorescent lipids and water as well as mitochondrial fluorescent NAD(P)H, fluorescent elastin, keratin, and melanin as well as SHG-active collagen has been imaged with submicron resolution in patients suffering from psoriasis. Further multimodal approaches include the combination of multiphoton tomographs with low-resolution wide-field systems such as ultrasound, optoacoustical, OCT, and dermoscopy systems. Multiphoton tomographs are currently employed in Australia, Japan, the US, and in several European countries for early diagnosis of skin cancer, optimization of treatment strategies, and cosmetic research including long-term testing of sunscreen nanoparticles as well as anti-aging products.

Application of Negative Curvature Hollow-Core Fiber in an Optical Fiber Sensor Setup for Multiphoton Spectroscopy

PubMed Central

Stawska, Hanna Izabela; Mazur, Leszek Mateusz; Kosolapov, Alexey; Kolyadin, Anton; Bereś-Pawlik, Elżbieta

2017-01-01

In this paper, an application of negative curvature hollow core fiber (NCHCF) in an all-fiber, multiphoton fluorescence sensor setup is presented. The dispersion parameter (D) of this fiber does not exceed the value of 5 ps/nm × km across the optical spectrum of (680–750) nm, making it well suited for the purpose of multiphoton excitation of biological fluorophores. Employing 1.5 m of this fiber in a simple, all-fiber sensor setup allows us to perform multiphoton experiments without any dispersion compensation methods. Multiphoton excitation of nicotinamide adenine dinucleotide (NADH) and flavin adenine dinucleotide (FAD) with this fiber shows a 6- and 9-fold increase, respectively, in the total fluorescence signal collected when compared with the commercial solution in the form of a hollow-core photonic band gap fiber (HCPBF). To the author’s best knowledge, this is the first time an NCHCF was used in an optical-fiber sensor setup for multiphoton fluorescence experiments. PMID:28984838

Application of Negative Curvature Hollow-Core Fiber in an Optical Fiber Sensor Setup for Multiphoton Spectroscopy.

PubMed

Popenda, Maciej Andrzej; Stawska, Hanna Izabela; Mazur, Leszek Mateusz; Jakubowski, Konrad; Kosolapov, Alexey; Kolyadin, Anton; Bereś-Pawlik, Elżbieta

2017-10-06

In this paper, an application of negative curvature hollow core fiber (NCHCF) in an all-fiber, multiphoton fluorescence sensor setup is presented. The dispersion parameter (D) of this fiber does not exceed the value of 5 ps/nm × km across the optical spectrum of (680-750) nm, making it well suited for the purpose of multiphoton excitation of biological fluorophores. Employing 1.5 m of this fiber in a simple, all-fiber sensor setup allows us to perform multiphoton experiments without any dispersion compensation methods. Multiphoton excitation of nicotinamide adenine dinucleotide (NADH) and flavin adenine dinucleotide (FAD) with this fiber shows a 6- and 9-fold increase, respectively, in the total fluorescence signal collected when compared with the commercial solution in the form of a hollow-core photonic band gap fiber (HCPBF). To the author's best knowledge, this is the first time an NCHCF was used in an optical-fiber sensor setup for multiphoton fluorescence experiments.

Strong-Field Control of Laser Filamentation Mechanisms

NASA Astrophysics Data System (ADS)

Levis, Robert; Romanov, Dmitri; Filin, Aleskey; Compton, Ryan

2008-05-01

The propagation of short strong-file laser pulses in gas and solution phases often result in formation of filaments. This phenomenon involves many nonlinear processes including Kerr lensing, group velocity dispersion, multi-photon ionization, plasma defocusing, intensity clamping, and self-steepening. Of these, formation and dynamics of pencil-shape plasma areas plays a crucial role. The fundamental understanding of these laser-induced plasmas requires additional effort, because the process is highly nonlinear and complex. We studied the ultrafast laser-generated plasma dynamics both experimentally and theoretically. Ultrafast plasma dynamics was probed using Coherent Anti-Stokes Raman Scattering. The measurements were made in a room temperature gas maintained at 1 atm in a flowing cell. The time dependent scattering was measured by delaying the CARS probe with respect to the intense laser excitation pulse. A general trend is observed between the spacing of the ground state and the first allowed excited state with the rise time for the noble gas series and the molecular gases. This trend is consistent with our theoretical model, which considers the ultrafast dynamics of the strong field generated plasma as a three-step process; (i) strong-field ionization followed by the electron gaining considerable kinetic energy during the pulse; (ii) immediate post-pulse dynamics: fast thermalization, impact-ionization-driven electron multiplication and cooling; (iii) ensuing relaxation: evolution to electron-ion equilibrium and eventual recombination.

Toward Rotational State-Selective Photoionization of ThF+ Ions

NASA Astrophysics Data System (ADS)

Zhou, Yan; Ng, Kia Boon; Gresh, Dan; Cairncross, William; Grau, Matt; Ni, Yiqi; Cornell, Eric; Ye, Jun

2016-06-01

ThF+ has been chosen to replace HfF+ for a second-generation measurement of the electric dipole moment of the electron (eEDM). Compared to the currently running HfF+ eEDM experiment, ThF+ has several advantages: (i) the eEDM-sensitive state (3Δ1) is the ground state, which facilitates a long coherence time [1]; (ii) its effective electric field (35 GV/cm) is 50% larger than that of HfF+, which promises a direct increase of the eEDM sensitivity [2]; and (iii) the ionization energy of neutral ThF is lower than its dissociation energy, which introduces greater flexibility in rotational state-selective photoionization via core-nonpenetrating Rydberg states [3]. In this talk, we first present our strategy of preparing and utilizing core-nonpenetrating Rydberg states for rotational state-selective ionization. Then, we report spectroscopic data of laser-induced fluorescence of neutral ThF, which provides critical information for multi-photon ionization spectroscopy. [1] D. N. Gresh, K. C. Cossel, Y. Zhou, J. Ye, E. A. Cornell, Journal of Molecular Spectroscopy, 319 (2016), 1-9 [2] M. Denis, M. S. Nørby, H. J. A. Jensen, A. S. P. Gomes, M. K. Nayak, S. Knecht, T. Fleig, New Journal of Physics, 17 (2015) 043005. [3] Z. J. Jakubek, R. W. Field, Journal of Molecular Spectroscopy 205 (2001) 197-220.

Compton spectra of atoms at high x-ray intensity

NASA Astrophysics Data System (ADS)

Son, Sang-Kil; Geffert, Otfried; Santra, Robin

2017-03-01

Compton scattering is the nonresonant inelastic scattering of an x-ray photon by an electron and has been used to probe the electron momentum distribution in gas-phase and condensed-matter samples. In the low x-ray intensity regime, Compton scattering from atoms dominantly comes from bound electrons in neutral atoms, neglecting contributions from bound electrons in ions and free (ionized) electrons. In contrast, in the high x-ray intensity regime, the sample experiences severe ionization via x-ray multiphoton multiple ionization dynamics. Thus, it becomes necessary to take into account all the contributions to the Compton scattering signal when atoms are exposed to high-intensity x-ray pulses provided by x-ray free-electron lasers (XFELs). In this paper, we investigate the Compton spectra of atoms at high x-ray intensity, using an extension of the integrated x-ray atomic physics toolkit, xatom. As the x-ray fluence increases, there is a significant contribution from ionized electrons to the Compton spectra, which gives rise to strong deviations from the Compton spectra of neutral atoms. The present study provides not only understanding of the fundamental XFEL-matter interaction but also crucial information for single-particle imaging experiments, where Compton scattering is no longer negligible. , which features invited work from the best early-career researchers working within the scope of J. Phys. B. This project is part of the Journal of Physics series’ 50th anniversary celebrations in 2017. Sang-Kil Son was selected by the Editorial Board of J. Phys. B as an Emerging Leader.

Application of modern online instrumentation for chemical analysis of gas and particulate phases of exhaust at the European Commission heavy-duty vehicle emission laboratory.

PubMed

Adam, T W; Chirico, R; Clairotte, M; Elsasser, M; Manfredi, U; Martini, G; Sklorz, M; Streibel, T; Heringa, M F; Decarlo, P F; Baltensperger, U; De Santi, G; Krasenbrink, A; Zimmermann, R; Prevot, A S H; Astorga, C

2011-01-01

The European Commission recently established a novel test facility for heavy-duty vehicles to enhance more sustainable transport. The facility enables the study of energy efficiency of various fuels/scenarios as well as the chemical composition of evolved exhaust emissions. Sophisticated instrumentation for real-time analysis of the gas and particulate phases of exhaust has been implemented. Thereby, gas-phase characterization was carried out by a Fourier transform infrared spectrometer (FT-IR; carbonyls, nitrogen-containing species, small hydrocarbons) and a resonance-enhanced multiphoton ionization time-of-flight mass spectrometer (REMPI-TOFMS; monocyclic and polycyclic aromatic hydrocarbons). For analysis of the particulate phase, a high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS; organic matter, chloride, nitrate), a condensation particle counter (CPC; particle number), and a multiangle absorption photometer (MAAP; black carbon) were applied. In this paper, the first application of the new facility in combination with the described instruments is presented, whereby a medium-size truck was investigated by applying different driving cycles. The goal was simultaneous chemical characterization of a great variety of gaseous compounds and particulate matter in exhaust on a real-time basis. The time-resolved data allowed new approaches to view the results; for example, emission factors were normalized to time-resolved consumption of fuel and were related to emission factors evolved during high speeds. Compounds could be identified that followed the fuel consumption, others showed very different behavior. In particular, engine cold start, engine ignition (unburned fuel), and high-speed events resulted in unique emission patterns.

Study on the decomposition of trace benzene over V2O5-WO3 ...

EPA Pesticide Factsheets

Commercial and laboratory-prepared V2O5–WO3/TiO2-based catalysts with different compositions were tested for catalytic decomposition of chlorobenzene （ClBz） in simulated flue gas. Resonance enhanced multiphoton ionization-time of flight mass spectrometry (REMPI-TOFMS) was employed to measure real-time, trace concentrations of ClBz contained in the flue gas before and after the catalyst. The effects of various parameters, including vanadium content of the catalyst, the catalyst support, as well as the reaction temperature on decomposition of ClBz were investigated. The results showed that the ClBz decomposition efficiency was significantly enhanced when nano-TiO2 instead of conventional TiO2 was used as the catalyst support. No promotion effects were found in the ClBz decomposition process when the catalysts were wet-impregnated with CuO and CeO2. Tests with different concentrations (1,000, 500, and 100 ppb) of ClBz showed that ClBz-decomposition efficiency decreased with increasing concentration, unless active sites were plentiful. A comparison between ClBz and benzene decomposition on the V2O5–WO3/TiO2-based catalyst and the relative kinetics analysis showed that two different active sites were likely involved in the decomposition mechanism and the V=O and V-O-Ti groups may only work for the degradation of the phenyl group and the benzene ring rather than the C-Cl bond. V2O5-WO3/TiO2 based catalysts, that have been used for destruction of a wide variet

QED theory of multiphoton transitions in atoms and ions

NASA Astrophysics Data System (ADS)

Zalialiutdinov, Timur A.; Solovyev, Dmitry A.; Labzowsky, Leonti N.; Plunien, Günter

2018-03-01

This review surveys the quantum theory of electromagnetic radiation for atomic systems. In particular, a review of current theoretical studies of multiphoton processes in one and two-electron atoms and highly charged ions is provided. Grounded on the quantum electrodynamics description the multiphoton transitions in presence of cascades, spin-statistic behaviour of equivalent photons and influence of external electric fields on multiphoton in atoms and anti-atoms are discussed. Finally, the nonresonant corrections which define the validity of the concept of the excited state energy levels are introduced.

Wavefront sensorless adaptive optics temporal focusing-based multiphoton microscopy

PubMed Central

Chang, Chia-Yuan; Cheng, Li-Chung; Su, Hung-Wei; Hu, Yvonne Yuling; Cho, Keng-Chi; Yen, Wei-Chung; Xu, Chris; Dong, Chen Yuan; Chen, Shean-Jen

2014-01-01

Temporal profile distortions reduce excitation efficiency and image quality in temporal focusing-based multiphoton microscopy. In order to compensate the distortions, a wavefront sensorless adaptive optics system (AOS) was integrated into the microscope. The feedback control signal of the AOS was acquired from local image intensity maximization via a hill-climbing algorithm. The control signal was then utilized to drive a deformable mirror in such a way as to eliminate the distortions. With the AOS correction, not only is the axial excitation symmetrically refocused, but the axial resolution with full two-photon excited fluorescence (TPEF) intensity is also maintained. Hence, the contrast of the TPEF image of a R6G-doped PMMA thin film is enhanced along with a 3.7-fold increase in intensity. Furthermore, the TPEF image quality of 1μm fluorescent beads sealed in agarose gel at different depths is improved. PMID:24940539

Improvement of axial excitation confinement in temporal focusing-based multiphoton microscopy via spatially modulated illumination

NASA Astrophysics Data System (ADS)

Chang, Chia-Yuan; Chen, Shean-Jen

2017-02-01

Conventional temporal focusing-based multiphoton excitation microscopy (TFMPEM) can offer widefield optical sectioning with an axial excitation confinement (AEC) of a few microns. Herein, a developed TFMPEM with a digital micromirror device (DMD), acting as the blazed grating for light spatial dispersion and simultaneous patterned illumination, has been extended to implement spatially modulated illumination at structured frequency and orientation. By implementing the spatially modulated illumination, the beam coverage at the back-focal aperture of the objective lens can be increased. As a result, the AEC can be condensed from 3.0 μm to 1.5 μm in full width at half maximum for a 2-fold enhancement. Furthermore, by using HiLo microscopy with two structured illuminations at the same spatial frequency but different orientation, biotissue images according to the structured illumination with condensed AEC is obviously superior in contrast and scattering suppression.

Multiphoton microscopy guides neurotrophin modification with poly(ethylene glycol) to enhance interstitial diffusion

NASA Astrophysics Data System (ADS)

Stroh, Mark; Zipfel, Warren R.; Williams, Rebecca M.; Ma, Shu Chin; Webb, Watt W.; Saltzman, W. Mark

2004-07-01

Brain-derived neurotrophic factor (BDNF) is a promising therapeutic agent for the treatment of neurodegenerative diseases. However, the limited distribution of this molecule after administration into the brain tissue considerably hampers its efficacy. Here, we show how multiphoton microscopy of fluorescently tagged BDNF in brain-tissue slices provides a useful and rapid screening method for examining the diffusion of large molecules in tissues, and for studying the effects of chemical modifications-for example, conjugating with polyethylene glycol (PEG)-on the diffusion constant. This single variable, obtained by monitoring short-term diffusion in real time, can be effectively used for rational drug design. In this study on fluorescently tagged BDNF and BDNF-PEG, we identify slow diffusion as a major contributing factor to the limited penetration of BDNF, and demonstrate how chemical modification can be used to overcome this barrier.

Coherent control of photoelectron wavepacket angular interferograms

NASA Astrophysics Data System (ADS)

Hockett, P.; Wollenhaupt, M.; Baumert, T.

2015-11-01

Coherent control over photoelectron wavepackets, via the use of polarization-shaped laser pulses, can be understood as a time and polarization-multiplexed process, where the final (time-integrated) observable coherently samples all instantaneous states of the light-matter interaction. In this work, we investigate this multiplexing via computation of the observable photoelectron angular interferograms resulting from multi-photon atomic ionization with polarization-shaped laser pulses. We consider the polarization sensitivity of both the instantaneous and cumulative continuum wavefunction; the nature of the coherent control over the resultant photoelectron interferogram is thus explored in detail. Based on this understanding, the use of coherent control with polarization-shaped pulses as a methodology for a highly multiplexed coherent quantum metrology is also investigated, and defined in terms of the information content of the observable.

Self-channeling of high-power laser pulses through strong atmospheric turbulence

NASA Astrophysics Data System (ADS)

Peñano, J.; Palastro, J. P.; Hafizi, B.; Helle, M. H.; DiComo, G. P.

2017-07-01

We present an unusual example of truly long-range propagation of high-power laser pulses through strong atmospheric turbulence. A form of nonlinear self-channeling is achieved when the laser power is close to the self-focusing power of air and the transverse dimensions of the pulse are smaller than the coherence diameter of turbulence. In this mode, nonlinear self-focusing counteracts diffraction, and turbulence-induced spreading is greatly reduced. Furthermore, the laser intensity is below the ionization threshold so that multiphoton absorption and plasma defocusing are avoided. Simulations show that the pulse can propagate many Rayleigh lengths (several kilometers) while maintaining a high intensity. In the presence of aerosols, or other extinction mechanisms that deplete laser energy, the pulse can be chirped to maintain the channeling.

Current developments in clinical multiphoton tomography

NASA Astrophysics Data System (ADS)

König, Karsten; Weinigel, Martin; Breunig, Hans Georg; Gregory, Axel; Fischer, Peter; Kellner-Höfer, Marcel; Bückle, Rainer

2010-02-01

Two-photon microscopy has been introduced in 1990 [1]. 13 years later, CE-marked clinical multiphoton systems for 3D imaging of human skin with subcellular resolution have been launched by the JenLab company with the tomograph DermaInspectTM. In 2010, the second generation of clinical multiphoton tomographs was introduced. The novel mobile multiphoton tomograph MPTflexTM, equipped with a flexible articulated optical arm, provides an increased flexibility and accessibility especially for clinical and cosmetical examinations. The multiphoton excitation of fluorescent biomolecules like NAD(P)H, flavins, porphyrins, elastin, and melanin as well as the second harmonic generation of collagen is induced by picojoule femtosecond laser pulses from an tunable turn-key near infrared laser system. The ability for rapid highquality image acquisition, the user-friendly operation of the system, and the compact and flexible design qualifies this system to be used for melanoma detection, diagnostics of dermatological disorders, cosmetic research, and skin aging measurements as well as in situ drug monitoring and animal research. So far, more than 1,000 patients and volunteers have been investigated with the multiphoton tomographs in Europe, Asia, and Australia.

Amplitudes for multiphoton quantum processes in linear optics

NASA Astrophysics Data System (ADS)

Urías, Jesús

2011-07-01

The prominent role that linear optical networks have acquired in the engineering of photon states calls for physically intuitive and automatic methods to compute the probability amplitudes for the multiphoton quantum processes occurring in linear optics. A version of Wick's theorem for the expectation value, on any vector state, of products of linear operators, in general, is proved. We use it to extract the combinatorics of any multiphoton quantum processes in linear optics. The result is presented as a concise rule to write down directly explicit formulae for the probability amplitude of any multiphoton process in linear optics. The rule achieves a considerable simplification and provides an intuitive physical insight about quantum multiphoton processes. The methodology is applied to the generation of high-photon-number entangled states by interferometrically mixing coherent light with spontaneously down-converted light.

Invited Review Article: Imaging techniques for harmonic and multiphoton absorption fluorescence microscopy

PubMed Central

Carriles, Ramón; Schafer, Dawn N.; Sheetz, Kraig E.; Field, Jeffrey J.; Cisek, Richard; Barzda, Virginijus; Sylvester, Anne W.; Squier, Jeffrey A.

2009-01-01

We review the current state of multiphoton microscopy. In particular, the requirements and limitations associated with high-speed multiphoton imaging are considered. A description of the different scanning technologies such as line scan, multifoci approaches, multidepth microscopy, and novel detection techniques is given. The main nonlinear optical contrast mechanisms employed in microscopy are reviewed, namely, multiphoton excitation fluorescence, second harmonic generation, and third harmonic generation. Techniques for optimizing these nonlinear mechanisms through a careful measurement of the spatial and temporal characteristics of the focal volume are discussed, and a brief summary of photobleaching effects is provided. Finally, we consider three new applications of multiphoton microscopy: nonlinear imaging in microfluidics as applied to chemical analysis and the use of two-photon absorption and self-phase modulation as contrast mechanisms applied to imaging problems in the medical sciences. PMID:19725639

Multi-photon EIT

NASA Astrophysics Data System (ADS)

Laarits, Toomas; O'Gorman, Bryan; Crescimanno, Michael

2008-03-01

We describe and solve a quantum optics models for multiphoton interrogation of an electromagnetically induced transparency (EIT) resonance. Multiphoton EIT, like its well studied Lambda-system EIT progenitor, is a generalization of the N-resonance process recently studied for atomic time keeping. The solution of these models allows a preliminary determination of this processes utility as the basis of a frequency standard.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Avetissian, H. K.; Avchyan, B. R.; Mkrtchian, G. F.

The multiphoton resonant excitation of three-level atoms by the two laser fields of different frequencies is investigated. The time evolution of the system and analytical solutions expressing Rabi oscillations of the probability amplitudes at the two-color multiphoton resonant excitation are found using a nonperturbative resonant approach. The specific examples for experimental implementation of two-color multiphoton resonant excitation of hydrogen atoms are considered.

Laser machining of explosives

DOEpatents

Perry, Michael D.; Stuart, Brent C.; Banks, Paul S.; Myers, Booth R.; Sefcik, Joseph A.

2000-01-01

The invention consists of a method for machining (cutting, drilling, sculpting) of explosives (e.g., TNT, TATB, PETN, RDX, etc.). By using pulses of a duration in the range of 5 femtoseconds to 50 picoseconds, extremely precise and rapid machining can be achieved with essentially no heat or shock affected zone. In this method, material is removed by a nonthermal mechanism. A combination of multiphoton and collisional ionization creates a critical density plasma in a time scale much shorter than electron kinetic energy is transferred to the lattice. The resulting plasma is far from thermal equilibrium. The material is in essence converted from its initial solid-state directly into a fully ionized plasma on a time scale too short for thermal equilibrium to be established with the lattice. As a result, there is negligible heat conduction beyond the region removed resulting in negligible thermal stress or shock to the material beyond a few microns from the laser machined surface. Hydrodynamic expansion of the plasma eliminates the need for any ancillary techniques to remove material and produces extremely high quality machined surfaces. There is no detonation or deflagration of the explosive in the process and the material which is removed is rendered inert.

Overcritical plasma ignition and diagnostics from oncoming interaction of two color low energy tightly focused femtosecond laser pulses inside fused silica

NASA Astrophysics Data System (ADS)

Potemkin, F. V.; Bravy, B. G.; Bezsudnova, Yu I.; Mareev, E. I.; Starostin, V. M.; Platonenko, V. T.; Gordienko, V. M.

2016-04-01

We report overcritical (3.3  ×  1021 cm-3) microplasma produced by low energy colliding IR (infrared) (1.24 μm) and visible (0.62 μm) femtosecond pulses tightly focused (NA  =  0.5) into the bulk of fused silica with on-line monitoring based on third harmonic generated by the IR beam. It was established that the absorbed energy density is the key parameter that determines the micromodification formation threshold and in our experimental conditions it is close to 4.5 kJ cm-3. Non-monotonic behavior of the third harmonic signal as a function of time delay between visible (0.62 μm) and IR (1.24 μm) femtosecond pulses demonstrates the qualitative differences about the two phenomena: one is the seed electrons generation by the visible pulse via multiphoton ionization and second is the avalanche ionization by the IR pulse. We predict that the tandem two-color excitation of wide-bandgap dielectric in comparison with single-color pulse interaction regime allows providing a much higher absorbed energy density and overcritical plasma.

Production of cold beams of ND{sub 3} with variable rotational state distributions by electrostatic extraction of He and Ne buffer-gas-cooled beams

DOE Office of Scientific and Technical Information (OSTI.GOV)

Twyman, Kathryn S.; Bell, Martin T.; Heazlewood, Brianna R.

2014-07-14

The measurement of the rotational state distribution of a velocity-selected, buffer-gas-cooled beam of ND{sub 3} is described. In an apparatus recently constructed to study cold ion-molecule collisions, the ND{sub 3} beam is extracted from a cryogenically cooled buffer-gas cell using a 2.15 m long electrostatic quadrupole guide with three 90° bends. (2+1) resonance enhanced multiphoton ionization spectra of molecules exiting the guide show that beams of ND{sub 3} can be produced with rotational state populations corresponding to approximately T{sub rot} = 9–18 K, achieved through manipulation of the temperature of the buffer-gas cell (operated at 6 K or 17 K),more » the identity of the buffer gas (He or Ne), or the relative densities of the buffer gas and ND{sub 3}. The translational temperature of the guided ND{sub 3} is found to be similar in a 6 K helium and 17 K neon buffer-gas cell (peak kinetic energies of 6.92(0.13) K and 5.90(0.01) K, respectively). The characterization of this cold-molecule source provides an opportunity for the first experimental investigations into the rotational dependence of reaction cross sections in low temperature collisions.« less

Spectroscopy of Cold LiCa Molecules Formed on Helium Nanodroplets

PubMed Central

2013-01-01

We report on the formation of mixed alkali–alkaline earth molecules (LiCa) on helium nanodroplets and present a comprehensive experimental and theoretical study of the ground and excited states of LiCa. Resonance enhanced multiphoton ionization time-of-flight (REMPI-TOF) spectroscopy and laser induced fluorescence (LIF) spectroscopy were used for the experimental investigation of LiCa from 15000 to 25500 cm–1. The 42Σ+ and 32Π states show a vibrational structure accompanied by distinct phonon wings, which allows us to determine molecular parameters as well as to study the interaction of the molecule with the helium droplet. Higher excited states (42Π, 52Σ+, 52Π, and 62Σ+) are not vibrationally resolved and vibronic transitions start to overlap. The experimental spectrum is well reproduced by high-level ab initio calculations. By using a multireference configuration interaction (MRCI) approach, we calculated the 19 lowest lying potential energy curves (PECs) of the LiCa molecule. On the basis of these calculations, we could identify previously unobserved transitions. Our results demonstrate that the helium droplet isolation approach is a powerful method for the characterization of tailor-made alkali–alkaline earth molecules. In this way, important contributions can be made to the search for optimal pathways toward the creation of ultracold alkali–alkaline earth ground state molecules from the corresponding atomic species. Furthermore, a test for PECs calculated by ab initio methods is provided. PMID:24028555

Advanced Laser Architecture for Two-Step Laser Tandem Mass Spectrometer

NASA Technical Reports Server (NTRS)

Fahey, Molly E.; Li, Steven X.; Yu, Anthony W.; Getty, Stephanie A.

2016-01-01

Future astrobiology missions will focus on planets with significant astrochemical or potential astrobiological features, such as small, primitive bodies and the icy moons of the outer planets that may host diverse organic compounds. These missions require advanced instrument techniques to fully and unambiguously characterize the composition of surface and dust materials. Laser desorptionionization mass spectrometry (LDMS) is an emerging instrument technology for in situ mass analysis of non-volatile sample composition. A recent Goddard LDMS advancement is the two-step laser tandem mass spectrometer (L2MS) instrument to address the need for future flight instrumentation to deconvolve complex organic signatures. The L2MS prototype uses a resonance enhanced multi-photon laser ionization mechanism to selectively detect aromatic species from a more complex sample. By neglecting the aliphatic and inorganic mineral signatures in the two-step mass spectrum, the L2MS approach can provide both mass assignments and clues to structural information for an in situ investigation of non-volatile sample composition. In this paper we will describe our development effort on a new laser architecture that is based on the previously flown Lunar Orbiter Laser Altimeter (LOLA) laser transmitter for the L2MS instrument. The laser provides two discrete midinfrared wavelengths (2.8 m and 3.4 m) using monolithic optical parametric oscillators and ultraviolet (UV) wavelength (266 nm) on a single laser bench with a straightforward development path toward flight readiness.

Near-real-time combustion monitoring for PCDD/PCDF indicators by GC-REMPI-TOFMS.

PubMed

Gullett, Brian K; Oudejans, Lukas; Tabor, Dennis; Touati, Abderrahmane; Ryan, Shawn

2012-01-17

The boiler exit flue gas of a municipal waste combustor was sampled to evaluate an online monitoring system for chlorobenzene congeners as indicators of polychlorinated dibenzodioxin and dibenzofuran (PCDD/PCDF) concentrations. Continuous measurements of chlorobenzene congeners using gas chromatography coupled to a resonance-enhanced multiphoton ionization - time-of-flight mass spectrometry (GC-REMPI-TOFMS) system were compared over 5-min periods with conventional sampling methods for PCDD/PCDF. Three pairs of values were taken every hour over a period of three days to characterize the combustor's response to transient operating conditions (shutdowns and startups). Isolation of specific chlorobenzene congeners from other same-mass compounds was accomplished by using a GC column separator ahead of the REMPI-TOFMS. The 50-fold variation of PCDD/PCDF concentration was paralleled by similar changes in monitored compounds of 1,4-dichlorobenzene, 1,2,4-trichlorobenzene, 1,2,3-trichlorobenzene, and 1,2,4,5-tetrachlorobenzene. A correlation of R = 0.85 and 0.89 was established between 40 pairs of simultaneous 5-min GC-REMPI-TOFMS measurements of 1,2,4-trichlorobenzene and 5 min conventional sampling and analysis for the TEQ and Total measures of PCDD/PCDF, respectively. The GC-REMPI-TOFMS system can be used to provide frequent measures of correlative PCDD/PCDF concentration thereby allowing for an understanding of measures to minimize PCDD/PCDF formation and develop operational feedback to limit emissions.

Consistent Assignment of the Vibrations of Monohalosubstituted Benzenes

NASA Astrophysics Data System (ADS)

Harris, Joe; Andrejeva, Anna; Tuttle, William Duncan; Pugliesi, Igor; Schriever, Christian; Wright, Tim

2014-06-01

When substituted benzenes become a focus of a spectroscopic study there are various well known vibrational labelling schemes present, however it was shown in recent works the description of monohalobenzene vibrations in terms of benzene modes (ie. Wilson notation) is questionable in some cases. A new scheme is presented which uses the motions of monofluorobenzene vibrations as a basis for labelling vibrational assignments of monosubstituted benzenes.d The scheme has been successfully applied to the ground and excited states of toluene and its deuterated-methyl group isotopologue. Here we present the application of the scheme to fluorobenzene and its fully deuterated analogue. One-colour resonance-enhanced multiphoton ionization (REMPI) spectroscopy was employed in order to characterise the fluorobenzene and fluorobenzene-d5 excited state. E. B. Wilson Jr., Phys. Rev., 45, 706 (1934) G .Varsanyi, Assignments of the Vibrational Spectra of Seven Hundred Benzene Derivatives,Wiley, New York, 1974, Vol. I and II I. Pugliesi, N. C. Tonge and M. C. R. Cockett, J. Chem. Phys., 129, 104303 (2008) A. M. Gardner and T. G. Wright, J. Chem. Phys., 135,114305 (2011) A. M. Gardner, A. M. Green, V. M. Tame-Reyes, V. H. K. Wilton and T. G. Wright, 138, 134303 (2013) A. M. Gardner, A. M. Green, V. M. Tame-Reyes, K. L. Reid, J. A. Davies, V. H. K. Wilton and T. G. Wright, manuscript accepted

Photodissociation dynamics of propanal and isobutanal: The Norrish Type I pathway

NASA Astrophysics Data System (ADS)

Harrison, Aaron W.; Kable, Scott H.

2018-04-01

The Norrish Type I photodissociation of two aliphatic aldehydes, propanal and isobutanal, has been investigated using velocity-map imaging. The HCO photoproduct of this reaction was probed using a 1+1 resonance-enhanced multiphoton ionization scheme via the 3p2Π Rydberg state. The velocity map images of HCO+ were collected across a range of photolysis energies for both species from 30 500 to 33 000 cm-1 (λ = 312-327 nm). The corresponding translational energy distributions show that the majority of the available energy goes into the translational motion of the products (55%-68%) with this fraction increasing as the T1 barrier is approached. Analysis of the translational energy distributions was also used to determine the aldehyde α C-C bond dissociation energies which were found to be 339.8 ± 2.5 and 331.2 ± 2.5 kJ/mol for propanal and isobutanal, respectively. These values were also found to be in good agreement with the computed dissociation energies using G4 and CCSD(T)/aug-cc-pVTZ//M062X/aug-cc-pVTZ levels of theory. Furthermore, these dissociation energies, combined with the known ΔfH (0 K) of the reaction products, provided the ΔfH (0 K) of propanal and isobutanal which were calculated to be -167.3 ± 2.5 and -184.0 ± 2.5 kJ/mol, respectively.

Multiphoton excitation and high-harmonics generation in topological insulator.

PubMed

Avetissian, H K; Avetissian, A K; Avchyan, B R; Mkrtchian, G F

2018-05-10

Multiphoton interaction of coherent electromagnetic radiation with 2D metallic carriers confined on the surface of the 3D topological insulator is considered. A microscopic theory describing the nonlinear interaction of a strong wave and metallic carriers with many-body Coulomb interaction is developed. The set of integrodifferential equations for the interband polarization and carrier occupation distribution is solved numerically. Multiphoton excitation of Fermi-Dirac sea of 2D massless carriers is considered for a THz pump wave. It is shown that in the moderately strong pump wave field along with multiphoton interband/intraband transitions the intense radiation of high harmonics takes place.

Multiphoton excitation and high-harmonics generation in topological insulator

NASA Astrophysics Data System (ADS)

Avetissian, H. K.; Avetissian, A. K.; Avchyan, B. R.; Mkrtchian, G. F.

2018-05-01

Multiphoton interaction of coherent electromagnetic radiation with 2D metallic carriers confined on the surface of the 3D topological insulator is considered. A microscopic theory describing the nonlinear interaction of a strong wave and metallic carriers with many-body Coulomb interaction is developed. The set of integrodifferential equations for the interband polarization and carrier occupation distribution is solved numerically. Multiphoton excitation of Fermi–Dirac sea of 2D massless carriers is considered for a THz pump wave. It is shown that in the moderately strong pump wave field along with multiphoton interband/intraband transitions the intense radiation of high harmonics takes place.

Computational code in atomic and nuclear quantum optics: Advanced computing multiphoton resonance parameters for atoms in a strong laser field

NASA Astrophysics Data System (ADS)

Glushkov, A. V.; Gurskaya, M. Yu; Ignatenko, A. V.; Smirnov, A. V.; Serga, I. N.; Svinarenko, A. A.; Ternovsky, E. V.

2017-10-01

The consistent relativistic energy approach to the finite Fermi-systems (atoms and nuclei) in a strong realistic laser field is presented and applied to computing the multiphoton resonances parameters in some atoms and nuclei. The approach is based on the Gell-Mann and Low S-matrix formalism, multiphoton resonance lines moments technique and advanced Ivanov-Ivanova algorithm of calculating the Green’s function of the Dirac equation. The data for multiphoton resonance width and shift for the Cs atom and the 57Fe nucleus in dependence upon the laser intensity are listed.

In vivo multiphoton imaging of human skin: assessment of topical corticosteroid-induced epidermis atrophy and depigmentation

NASA Astrophysics Data System (ADS)

Ait El Madani, Hassan; Tancrède-Bohin, Emmanuelle; Bensussan, Armand; Colonna, Anne; Dupuy, Alain; Bagot, Martine; Pena, Ana-Maria

2012-02-01

Multiphoton microscopy has emerged in the past decade as a promising tool for noninvasive skin imaging. Our aim was to evaluate the potential of multiphoton microscopy to detect topical corticosteroids side effects within the epidermis and to provide new insights into their dynamics. Healthy volunteers were topically treated with clobetasol propionate on a small region of their forearms under overnight occlusion for three weeks. The treated region of each patient was investigated at D0, D7, D15, D22 (end of the treatment), and D60. Our study shows that multiphoton microscopy allows for the detection of corticoid-induced epidermis modifications: thinning of stratum corneum compactum and epidermis, decrease of keratinocytes size, and changes in their morphology from D7 to D22. We also show that multiphoton microscopy enables in vivo three-dimensional (3-D) quantitative assessment of melanin content. We observe that melanin density decreases during treatment and almost completely disappears at D22. Moreover, these alterations are reversible as they are no longer present at D60. Our study demonstrates that multiphoton microscopy is a convenient and powerful tool for noninvasive 3-D dynamical studies of skin integrity and pigmentation.

New developments in multimodal clinical multiphoton tomography

NASA Astrophysics Data System (ADS)

König, Karsten

2011-03-01

80 years ago, the PhD student Maria Goeppert predicted in her thesis in Goettingen, Germany, two-photon effects. It took 30 years to prove her theory, and another three decades to realize the first two-photon microscope. With the beginning of this millennium, first clinical multiphoton tomographs started operation in research institutions, hospitals, and in the cosmetic industry. The multiphoton tomograph MPTflexTM with its miniaturized flexible scan head became the Prism-Award 2010 winner in the category Life Sciences. Multiphoton tomographs with its superior submicron spatial resolution can be upgraded to 5D imaging tools by adding spectral time-correlated single photon counting units. Furthermore, multimodal hybrid tomographs provide chemical fingerprinting and fast wide-field imaging. The world's first clinical CARS studies have been performed with a hybrid multimodal multiphoton tomograph in spring 2010. In particular, nonfluorescent lipids and water as well as mitochondrial fluorescent NAD(P)H, fluorescent elastin, keratin, and melanin as well as SHG-active collagen have been imaged in patients with dermatological disorders. Further multimodal approaches include the combination of multiphoton tomographs with low-resolution imaging tools such as ultrasound, optoacoustic, OCT, and dermoscopy systems. Multiphoton tomographs are currently employed in Australia, Japan, the US, and in several European countries for early diagnosis of skin cancer (malignant melanoma), optimization of treatment strategies (wound healing, dermatitis), and cosmetic research including long-term biosafety tests of ZnO sunscreen nanoparticles and the measurement of the stimulated biosynthesis of collagen by anti-ageing products.

Multiphoton entanglement concentration and quantum cryptography.

PubMed

Durkin, Gabriel A; Simon, Christoph; Bouwmeester, Dik

2002-05-06

Multiphoton states from parametric down-conversion can be entangled both in polarization and photon number. Maximal high-dimensional entanglement can be concentrated postselectively from these states via photon counting. This makes them natural candidates for quantum key distribution, where the presence of more than one photon per detection interval has up to now been considered undesirable. We propose a simple multiphoton cryptography protocol for the case of low losses.

Visualizing Angiogenesis by Multiphoton Microscopy In Vivo in Genetically Modified 3D-PLGA/nHAp Scaffold for Calvarial Critical Bone Defect Repair.

PubMed

Li, Jian; Jahr, Holger; Zheng, Wei; Ren, Pei-Gen

2017-09-07

The reconstruction of critically sized bone defects remains a serious clinical problem because of poor angiogenesis within tissue-engineered scaffolds during repair, which gives rise to a lack of sufficient blood supply and causes necrosis of the new tissues. Rapid vascularization is a vital prerequisite for new tissue survival and integration with existing host tissue. The de novo generation of vasculature in scaffolds is one of the most important steps in making bone regeneration more efficient, allowing repairing tissue to grow into a scaffold. To tackle this problem, the genetic modification of a biomaterial scaffold is used to accelerate angiogenesis and osteogenesis. However, visualizing and tracking in vivo blood vessel formation in real-time and in three-dimensional (3D) scaffolds or new bone tissue is still an obstacle for bone tissue engineering. Multiphoton microscopy (MPM) is a novel bio-imaging modality that can acquire volumetric data from biological structures in a high-resolution and minimally-invasive manner. The objective of this study was to visualize angiogenesis with multiphoton microscopy in vivo in a genetically modified 3D-PLGA/nHAp scaffold for calvarial critical bone defect repair. PLGA/nHAp scaffolds were functionalized for the sustained delivery of a growth factor pdgf-b gene carrying lentiviral vectors (LV-pdgfb) in order to facilitate angiogenesis and to enhance bone regeneration. In a scaffold-implanted calvarial critical bone defect mouse model, the blood vessel areas (BVAs) in PHp scaffolds were significantly higher than in PH scaffolds. Additionally, the expression of pdgf-b and angiogenesis-related genes, vWF and VEGFR2, increased correspondingly. MicroCT analysis indicated that the new bone formation in the PHp group dramatically improved compared to the other groups. To our knowledge, this is the first time multiphoton microscopy was used in bone tissue-engineering to investigate angiogenesis in a 3D bio-degradable scaffold in vivo and in real-time.

Ionization enhancement in atmospheric pressure chemical ionization and suppression in electrospray ionization between target drugs and stable-isotope-labeled internal standards in quantitative liquid chromatography/tandem mass spectrometry.

PubMed

Liang, H R; Foltz, R L; Meng, M; Bennett, P

2003-01-01

The phenomena of ionization suppression in electrospray ionization (ESI) and enhancement in atmospheric pressure chemical ionization (APCI) were investigated in selected-ion monitoring and selected-reaction monitoring modes for nine drugs and their corresponding stable-isotope-labeled internal standards (IS). The results showed that all investigated target drugs and their co-eluting isotope-labeled IS suppress each other's ionization responses in ESI. The factors affecting the extent of suppression in ESI were investigated, including structures and concentrations of drugs, matrix effects, and flow rate. In contrast to the ESI results, APCI caused seven of the nine investigated target drugs and their co-eluting isotope-labeled IS to enhance each other's ionization responses. The mutual ionization suppression or enhancement between drugs and their isotope-labeled IS could possibly influence assay sensitivity, reproducibility, accuracy and linearity in quantitative liquid chromatography/mass spectrometry (LC/MS) and liquid chromatography/tandem mass spectrometry (LC/MS/MS). However, calibration curves were linear if an appropriate IS concentration was selected for a desired calibration range to keep the response factors constant. Copyright 2003 John Wiley & Sons, Ltd.

A new high intensity and short-pulse molecular beam valve

NASA Astrophysics Data System (ADS)

Yan, B.; Claus, P. F. H.; van Oorschot, B. G. M.; Gerritsen, L.; Eppink, A. T. J. B.; van de Meerakker, S. Y. T.; Parker, D. H.

2013-02-01

In this paper, we report on the design and performance of a new home-built pulsed gas valve, which we refer to as the Nijmegen Pulsed Valve (NPV). The main output characteristics include a short pulse width (as short as 20 μs) combined with operating rates up to 30 Hz. The operation principle of the NPV is based on the Lorentz force created by a pulsed current passing through an aluminum strip located within a magnetic field, which opens the nozzle periodically. The amplitude of displacement of the opening mechanism is sufficient to allow the use of nozzles with up to 1.0 mm diameter. To investigate the performance of the valve, several characterizations were performed with different experimental methods. First, a fast ionization gauge was used to measure the beam intensity of the free jet emanating from the NPV. We compare free jets from the NPV with those from several other pulsed valves in current use in our laboratory. Results showed that a high intensity and short pulse-length beam could be generated by the new valve. Second, the NPV was tested in combination with a skimmer, where resonance enhanced multiphoton ionization combined with velocity map imaging was used to show that the NPV was able to produce a pulsed molecular beam with short pulse duration (˜20 μs using 0.1% NO/He at 6 bars) and low rotational temperature (˜1 K using 0.5% NO/Ar at 6 bars). Third, a novel two-point pump-probe method was employed which we label double delay scan. This method allows a full kinematic characterization of the molecular beam, including accurate speed ratios at different temporal positions. It was found that the speed ratio was maximum (S = 50 using 0.1% NO/He at 3 bars) at the peak position of the molecular beam and decreased when it was on the leading or falling edge.

Distinguishing human normal or cancerous esophagus tissue ex vivo using multiphoton microscopy

NASA Astrophysics Data System (ADS)

Liu, N. R.; Chen, G. N.; Wu, S. S.; Chen, R.

2014-02-01

Application of multiphoton microscopy (MPM) to clinical cancer research has greatly developed over the last few years. In this paper, we mainly focus on two-photon excitation fluorescence (TPEF) and second harmonic generation (SHG) for investigating esophageal cancer. We chiefly discuss the SHG/TPEF image and spectral characteristics of normal and cancerous esophagus submucosa with the combined multi-channel imaging mode and Lambda mode of a multiphoton microscope (LSM 510 META). Great differences can be detected, such as collagen content and morphology, glandular-shaped cancer cells, TPEF/SHG intensity ratio, and so on, which demonstrate that the multiphoton imaging technique has the potential ability for minimally-invasive early cancer diagnosis.

Photodissociation of Non-Covalent Peptide-Crown Ether Complexes

PubMed Central

Wilson, Jeffrey J.; Kirkovits, Gregory J.; Sessler, Jonathan L.; Brodbelt, Jennifer S.

2008-01-01

Highly chromogenic 18-crown-6-dipyrrolylquinoxaline coordinates primary amines of peptides, forming non-covalent complexes that can be transferred to the gas phase by electrospray ionization. The appended chromogenic crown ether facilitates efficient energy transfer to the peptide upon ultraviolet irradiation in the gas phase, resulting in diagnostic peptide fragmentation. Collisional activated dissociation (CAD) and infrared multiphoton dissociation (IRMPD) of these non-covalent complexes results only in their disassembly with the charge retained on either the peptide or crown ether, yielding no sequence ions. Upon UV photon absorption the intermolecular energy transfer is facilitated by the fast activation time scale of UVPD (< 10 ns) and by the collectively strong hydrogen bonding between the crown ether and peptide, thus allowing effective transfer of energy to the peptide moiety prior to disruption of the intermolecular hydrogen bonds. PMID:18077179

Fingerprints of Both Watson-Crick and Hoogsteen Isomers of the Isolated (Cytosine-Guanine)H+ Pair.

PubMed

Cruz-Ortiz, Andrés F; Rossa, Maximiliano; Berthias, Francis; Berdakin, Matías; Maitre, Philippe; Pino, Gustavo A

2017-11-16

 Gas phase protonated guanine-cytosine (CGH + ) pair was generated using an electrospray ionization source from solutions at two different pH (5.8 and 3.2). Consistent evidence from MS/MS fragmentation patterns and differential ion mobility spectra (DIMS) point toward the presence of two isomers of the CGH + pair, whose relative populations depend strongly on the pH of the solution. Gas phase infrared multiphoton dissociation (IRMPD) spectroscopy in the 900-1900 cm -1 spectral range further confirms that the Watson-Crick isomer is preferentially produced (91%) at pH = 5.8, while the Hoogsteen isomer predominates (66%) at pH = 3.2). These fingerprint signatures are expected to be useful for the development of new analytical methodologies and to trigger isomer selective photochemical studies of protonated DNA base pairs.

Strong Field Theories beyond Dipole Approximations in Nonrelativistic Regimes

NASA Astrophysics Data System (ADS)

He, Pei-Lun; Lao, Di; He, Feng

2017-04-01

The exact nondipole Volkov solutions to the Schrödinger equation and Pauli equation are found, based on which a strong field theory beyond the dipole approximation is built for describing the nondipole effects in nonrelativistic laser driven electron dynamics. This theory is applied to investigate momentum partition laws for multiphoton and tunneling ionization and explicitly shows that the complex interplay of a laser field and Coulomb action may reverse the expected photoelectron momentum along the laser propagation direction. The magnetic-spin coupling does not bring observable effects on the photoelectron momentum distribution and can be neglected. Compared to the strong field approximation within the dipole approximation, this theory works in a much wider range of laser parameters and lays a solid foundation for describing nonrelativistic electron dynamics in both short wavelength and midinfrared regimes where nondipole effects are unavoidable.

Photoelectron spectrometer for liquid and gas-phase attosecond spectroscopy with field-free and magnetic bottle operation modes

NASA Astrophysics Data System (ADS)

Jordan, Inga; Jain, Arohi; Gaumnitz, Thomas; Ma, Jun; Wörner, Hans Jakob

2018-05-01

A compact time-of-flight spectrometer for applications in attosecond spectroscopy in the liquid and gas phases is presented. It allows for altering the collection efficiency by transitioning between field-free and magnetic-bottle operation modes. High energy resolution (ΔE/E = 0.03 for kinetic energies >20 eV) is achieved despite the short flight-tube length through a homogeneous deceleration potential at the beginning of the flight tube. A closing mechanism allows isolating the vacuum system of the flight tube from the interaction region in order to efficiently perform liquid-microjet experiments. The capabilities of the instrument are demonstrated through photoelectron spectra from multiphoton ionization of argon and xenon, as well as photoelectron spectra of liquid and gaseous water generated by an attosecond pulse train.

Self-referenced axial chromatic dispersion measurement in multiphoton microscopy through 2-color THG imaging.

PubMed

Du, Yu; Zhuang, Ziwei; He, Jiexing; Liu, Hongji; Qiu, Ping; Wang, Ke

2018-05-16

With tunable excitation light, multiphoton microscopy (MPM) is widely used for imaging biological structures at subcellular resolution. Axial chromatic dispersion, present in virtually every transmissive optical system including the multiphoton microscope, leads to focal (and the resultant image) plane separation. Here we demonstrate experimentally a technique to measure the axial chromatic dispersion in a multiphoton microscope, using simultaneous 2-color third-harmonic generation (THG) imaging excited by a 2-color soliton source with tunable wavelength separation. Our technique is self-referenced, eliminating potential measurement error when 1-color tunable excitation light is used which necessitates reciprocating motion of the mechanical translation stage. Using this technique, we demonstrate measured axial chromatic dispersion with 2 different objective lenses in a multiphoton microscope. Further measurement in a biological sample also indicates that this axial chromatic dispersion, in combination with 2-color imaging, may open up opportunity for simultaneous imaging of two different axial planes. This article is protected by copyright. All rights reserved. This article is protected by copyright. All rights reserved.

Spatiotemporal focusing-based widefield multiphoton microscopy for fast optical sectioning of thick tissues

NASA Astrophysics Data System (ADS)

Cheng, Li-Chung; Chang, Chia-Yuan; Yen, Wei-Chung; Chen, Shean-Jen

2012-10-01

Conventional multiphoton microscopy employs beam scanning; however, in this study a microscope based on spatiotemporal focusing offering widefield multiphoton excitation has been developed to provide fast optical sectioning images. The microscope integrates a 10 kHz repetition rate ultrafast amplifier featuring strong instantaneous peak power (maximum 400 μJ/pulse at 90 fs pulse width) with a TE-cooled, ultra-sensitive photon detecting, electron multiplying charge-coupled device camera. This configuration can produce multiphoton excited images with an excitation area larger than 200 × 100 μm2 at a frame rate greater than 100 Hz. Brownian motions of fluorescent microbeads as small as 0.5 μm have been instantaneously observed with a lateral spatial resolution of less than 0.5 μm and an axial resolution of approximately 3.5 μm. Moreover, we combine the widefield multiphoton microscopy with structure illuminated technique named HiLo to reject the background scattering noise to get better quality for bioimaging.

Nanoparticle-assisted-multiphoton microscopy for in vivo brain imaging of mice

NASA Astrophysics Data System (ADS)

Qian, Jun

2015-03-01

Neuro/brain study has attracted much attention during past few years, and many optical methods have been utilized in order to obtain accurate and complete neural information inside the brain. Relying on simultaneous absorption of two or more near-infrared photons by a fluorophore, multiphoton microscopy can achieve deep tissue penetration and efficient light detection noninvasively, which makes it very suitable for thick-tissue and in vivo bioimaging. Nanoparticles possess many unique optical and chemical properties, such as anti-photobleaching, large multiphoton absorption cross-section, and high stability in biological environment, which facilitates their applications in long-term multiphoton microscopy as contrast agents. In this paper, we will introduce several typical nanoparticles (e.g. organic dye doped polymer nanoparticles and gold nanorods) with high multiphoton fluorescence efficiency. We further applied them in two- and three-photon in vivo functional brain imaging of mice, such as brain-microglia imaging, 3D architecture reconstruction of brain blood vessel, and blood velocity measurement.

Imaging of cardiovascular structures using near-infrared femtosecond multiphoton laser scanning microscopy.

PubMed

Schenke-Layland, Katja; Riemann, Iris; Stock, Ulrich A; König, Karsten

2005-01-01

Multiphoton imaging represents a novel and very promising medical diagnostic technology for the high-resolution analysis of living biological tissues. We performed multiphoton imaging to analyzed structural features of extracellular matrix (ECM) components, e.g., collagen and elastin, of vital pulmonary and aortic heart valves. High-resolution autofluorescence images of collagenous and elastic fibers were demonstrated using multifluorophore, multiphoton excitation at two different wavelengths and optical sectioning, without the requirement of embedding, fixation, or staining. Collagenous structures were selectively imaged by detection of second harmonic generation (SHG). Additionally, routine histology and electron microscopy were integrated to verify the observed results. In comparison with pulmonary tissues, aortic heart valve specimens show very similar matrix formations. The quality of the resulting three-dimensional (3-D) images enabled the differentiation between collagenous and elastic fibers. These experimental results indicate that multiphoton imaging with near-infrared (NIR) femtosecond laser pulses may prove to be a useful tool for the nondestructive monitoring and characterization of cardiovascular structures. Copyright 2005 Society of Photo-Optical Instrumentation Engineers.

Application of Multiphoton Microscopy in Dermatological Studies: a Mini-Review

PubMed Central

Yew, Elijah; Rowlands, Christopher

2014-01-01

This review summarizes the historical and more recent developments of multiphoton microscopy, as applied to dermatology. Multiphoton microscopy offers several advantages over competing microscopy techniques: there is an inherent axial sectioning, penetration depths that compete well with confocal microscopy on account of the use of near-infrared light, and many two-photon contrast mechanisms, such as second-harmonic generation, have no analogue in one-photon microscopy. While the penetration depths of photons into tissue are typically limited on the order of hundreds of microns, this is of less concern in dermatology, as the skin is thin and readily accessible. As a result, multiphoton microscopy in dermatology has generated a great deal of interest, much of which is summarized here. The review covers the interaction of light and tissue, as well as the various considerations that must be made when designing an instrument. The state of multiphoton microscopy in imaging skin cancer and various other diseases is also discussed, along with the investigation of aging and regeneration phenomena, and finally, the use of multiphoton microscopy to analyze the transdermal transport of drugs, cosmetics and other agents is summarized. The review concludes with a look at potential future research directions, especially those that are necessary to push these techniques into widespread clinical acceptance. PMID:25075226

Structure of multiphoton quantum optics. I. Canonical formalism and homodyne squeezed states

NASA Astrophysics Data System (ADS)

dell'Anno, Fabio; de Siena, Silvio; Illuminati, Fabrizio

2004-03-01

We introduce a formalism of nonlinear canonical transformations for general systems of multiphoton quantum optics. For single-mode systems the transformations depend on a tunable free parameter, the homodyne local-oscillator angle; for n -mode systems they depend on n heterodyne mixing angles. The canonical formalism realizes nontrivial mixing of pairs of conjugate quadratures of the electromagnetic field in terms of homodyne variables for single-mode systems, and in terms of heterodyne variables for multimode systems. In the first instance the transformations yield nonquadratic model Hamiltonians of degenerate multiphoton processes and define a class of non-Gaussian, nonclassical multiphoton states that exhibit properties of coherence and squeezing. We show that such homodyne multiphoton squeezed states are generated by unitary operators with a nonlinear time evolution that realizes the homodyne mixing of a pair of conjugate quadratures. Tuning of the local-oscillator angle allows us to vary at will the statistical properties of such states. We discuss the relevance of the formalism for the study of degenerate (up-)down-conversion processes. In a companion paper [

Structure of multiphoton quantum optics. I. Canonical formalism and homodyne squeezed states

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dell'Anno, Fabio; De Siena, Silvio; Illuminati, Fabrizio

2004-03-01

We introduce a formalism of nonlinear canonical transformations for general systems of multiphoton quantum optics. For single-mode systems the transformations depend on a tunable free parameter, the homodyne local-oscillator angle; for n-mode systems they depend on n heterodyne mixing angles. The canonical formalism realizes nontrivial mixing of pairs of conjugate quadratures of the electromagnetic field in terms of homodyne variables for single-mode systems, and in terms of heterodyne variables for multimode systems. In the first instance the transformations yield nonquadratic model Hamiltonians of degenerate multiphoton processes and define a class of non-Gaussian, nonclassical multiphoton states that exhibit properties of coherencemore » and squeezing. We show that such homodyne multiphoton squeezed states are generated by unitary operators with a nonlinear time evolution that realizes the homodyne mixing of a pair of conjugate quadratures. Tuning of the local-oscillator angle allows us to vary at will the statistical properties of such states. We discuss the relevance of the formalism for the study of degenerate (up-)down-conversion processes. In a companion paper [F. Dell'Anno, S. De Siena, and F. Illuminati, 69, 033813 (2004)], we provide the extension of the nonlinear canonical formalism to multimode systems, we introduce the associated heterodyne multiphoton squeezed states, and we discuss their possible experimental realization.« less

Femtosecond laser pulse optimization for multiphoton cytometry and control of fluorescence

NASA Astrophysics Data System (ADS)

Tkaczyk, Eric Robert

This body of work encompasses optimization of near infrared femtosecond laser pulses both for enhancement of flow cytometry as well as adaptive pulse shaping to control fluorescence. A two-photon system for in vivo flow cytometry is demonstrated, which allows noninvasive quantification of circulating cell populations in a single live mouse. We monitor fluorescently-labeled red blood cells for more than two weeks, and are also able to noninvasively measure circulation times of two distinct populations of breast cancer cells simultaneously in a single mouse. We build a custom laser excitation source in the form of an extended cavity mode-locked oscillator, which enables superior detection in whole blood or saline of cell lines expressing fluorescent proteins including the green fluorescent protein (GFP), tdTomato and mPlum. A mathematical model explains unique features of the signals. The ability to distinguish different fluorescent species is central to simultaneous measurement of multiple molecular targets in high throughput applications including the multiphoton flow cytometer. We demonstrate that two dyes which are not distinguishable to one-photon measurements can be differentiated and in fact quantified in mixture via phase-shaped two-photon excitation pulses found by a genetic algorithm. We also selectively enhance or suppress two-photon fluorescence of numerous common dyes with tailored pulse shapes. Using a multiplicative (rather than ratiometric) fitness parameter, we are able to control the fluorescence while maintaining a strong signal. With this method, we control the two-photon fluorescence of the blue fluorescent protein (BFP), which is of particular interest in investigations of protein-protein interactions, and has frustrated previous attempts of control. Implementing an acousto-optic interferometer, we use the same experimental setup to measure two-photon excitation cross-sections of dyes and prove that photon-photon interferences are the predominant mechanism of control. This research establishes the basis for molecularly tailored pulse shaping in multiphoton flow cytometry, which will advance our ability to probe the biology of circulating cells during disease progression and response to therapy.

Advanced Multi-Photon Chromophores for Broad-Band Ultra-Fast Optical Limiting

DTIC Science & Technology

2014-11-04

for this collection of information is estimated to average 1 hour per response, including the time for reviewing instructions, searching existing data ...sources, gathering and maintaining the data needed, and completing and reviewing this collection of information. Send comments regarding this...with expanded -system. This data provides crucial insight into the push-pull 2PA-enhancement mechanism. Following systems were studied in detail: i

Multiphoton microscopy as a diagnostic imaging modality for pancreatic neoplasms without hematoxylin and eosin stains

NASA Astrophysics Data System (ADS)

Chen, Youting; Chen, Jing; Chen, Hong; Hong, Zhipeng; Zhu, Xiaoqin; Zhuo, Shuangmu; Chen, Yanling; Chen, Jianxin

2014-09-01

Hematoxylin and eosin (H&E) staining of tissue samples is the standard approach in histopathology for imaging and diagnosing cancer. Recent reports have shown that multiphoton microscopy (MPM) provides better sample interface with single-cell resolution, which enhances traditional H&E staining and offers a powerful diagnostic tool with potential applications in oncology. The purpose of this study was to further expand the versatility of MPM by establishing the optical parameters required for imaging unstained histological sections of pancreatic neoplasms, thereby providing an efficient and environmentally sustainable alternative to H&E staining while improving the accuracy of pancreatic cancer diagnoses. We found that the high-resolution MPM images clearly distinguish between the structure of normal pancreatic tissues compared with pancreatic neoplasms in unstained histological sections, and discernable differences in tissue architecture and cell morphology between normal versus tumorigenic cells led to enhanced optical diagnosis of cancerous tissue. Moreover, quantitative assessment of the cytomorphological features visualized from MPM images showed significant differences in the nuclear-cytoplasmic ratios of pancreatic neoplasms compared with normal pancreas, as well as further distinguished pancreatic malignant tumors from benign tumors. These results indicate that the MPM could potentially serve as an optical tool for the diagnosis of pancreatic neoplasms in unstained histological sections.

Real-time analysis of aromatics in combustion engine exhaust by resonance-enhanced multiphoton ionisation time-of-flight mass spectrometry (REMPI-TOF-MS): a robust tool for chassis dynamometer testing.

PubMed

Adam, T W; Clairotte, M; Streibel, T; Elsasser, M; Pommeres, A; Manfredi, U; Carriero, M; Martini, G; Sklorz, M; Krasenbrink, A; Astorga, C; Zimmermann, R

2012-07-01

Resonance-enhanced multiphoton ionisation time-of-flight mass spectrometry (REMPI-TOF-MS) is a robust method for real-time analysis of monocyclic and polycyclic aromatic hydrocarbons in complex emissions. A mobile system has been developed which enables direct analysis on site. In this paper, we utilize a multicomponent calibration scheme based on the analytes' photo-ionisation cross-sections relative to a calibrated species. This allows semi-quantification of a great number of components by only calibrating one compound of choice, here toluene. The cross-sections were determined by injecting nebulised solutions of aromatic compounds into the TOF-MS ion source with the help of a HPLC pump. Then, REMPI-TOF-MS was implemented at various chassis dynamometers and test cells and the exhaust of the following vehicles and engines investigated: a compression ignition light-duty (LD) passenger car, a compression ignition LD van, two spark ignition LD passenger cars, 2 two-stroke mopeds, and a two-stroke engine of a string gas trimmer. The quantitative time profiles of benzene are shown. The results indicate that two-stroke engines are a significant source for toxic and cancerogenic compounds. Air pollution and health effects caused by gardening equipment might still be underestimated.

Active temporal multiplexing of indistinguishable heralded single photons

PubMed Central

Xiong, C.; Zhang, X.; Liu, Z.; Collins, M. J.; Mahendra, A.; Helt, L. G.; Steel, M. J.; Choi, D. -Y.; Chae, C. J.; Leong, P. H. W.; Eggleton, B. J.

2016-01-01

It is a fundamental challenge in quantum optics to deterministically generate indistinguishable single photons through non-deterministic nonlinear optical processes, due to the intrinsic coupling of single- and multi-photon-generation probabilities in these processes. Actively multiplexing photons generated in many temporal modes can decouple these probabilities, but key issues are to minimize resource requirements to allow scalability, and to ensure indistinguishability of the generated photons. Here we demonstrate the multiplexing of photons from four temporal modes solely using fibre-integrated optics and off-the-shelf electronic components. We show a 100% enhancement to the single-photon output probability without introducing additional multi-photon noise. Photon indistinguishability is confirmed by a fourfold Hong–Ou–Mandel quantum interference with a 91±16% visibility after subtracting multi-photon noise due to high pump power. Our demonstration paves the way for scalable multiplexing of many non-deterministic photon sources to a single near-deterministic source, which will be of benefit to future quantum photonic technologies. PMID:26996317

Electron detachment dissociation of fluorescently labeled sialylated oligosaccharides.

PubMed

Zhou, Wen; Håkansson, Kristina

2011-12-01

We explored the application of electron detachment dissociation (EDD) and infrared multiphoton dissociation (IRMPD) tandem mass spectrometry to fluorescently labeled sialylated oligosaccharides. Standard sialylated oligosaccharides and a sialylated N-linked glycan released from human transferrin were investigated. EDD yielded extensive glycosidic cleavages and cross-ring cleavages in all cases studied, consistently providing complementary structural information compared with infrared multiphoton dissociation. Neutral losses and satellite ions such as C-2H ions were also observed following EDD. In addition, we examined the influence of different fluorescent labels. The acidic label 2-aminobenzoic acid (2-AA) enhanced signal abundance in negative-ion mode. However, few cross-ring fragments were observed for 2-AA-labeled oligosaccharides. The neutral label 2-aminobenzamide (2-AB) resulted in more cross-ring cleavages compared with 2-AA-labeled species, but not as extensive fragmentation as for native oligosaccharides, likely resulting from altered negative charge locations from introduction of the fluorescent tag. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

A pragmatic guide to multiphoton microscope design

PubMed Central

Young, Michael D.; Field, Jeffrey J.; Sheetz, Kraig E.; Bartels, Randy A.; Squier, Jeff

2016-01-01

Multiphoton microscopy has emerged as a ubiquitous tool for studying microscopic structure and function across a broad range of disciplines. As such, the intent of this paper is to present a comprehensive resource for the construction and performance evaluation of a multiphoton microscope that will be understandable to the broad range of scientific fields that presently exploit, or wish to begin exploiting, this powerful technology. With this in mind, we have developed a guide to aid in the design of a multiphoton microscope. We discuss source selection, optical management of dispersion, image-relay systems with scan optics, objective-lens selection, single-element light-collection theory, photon-counting detection, image rendering, and finally, an illustrated guide for building an example microscope. PMID:27182429

Generation of single- and two-mode multiphoton states in waveguide QED

NASA Astrophysics Data System (ADS)

Paulisch, V.; Kimble, H. J.; Cirac, J. I.; González-Tudela, A.

2018-05-01

Single- and two-mode multiphoton states are the cornerstone of many quantum technologies, e.g., metrology. In the optical regime, these states are generally obtained combining heralded single photons with linear optics tools and post-selection, leading to inherent low success probabilities. In a recent paper [A. González-Tudela et al., Phys. Rev. Lett. 118, 213601 (2017), 10.1103/PhysRevLett.118.213601], we design several protocols that harness the long-range atomic interactions induced in waveguide QED to improve fidelities and protocols of single-mode multiphoton emission. Here, we give full details of these protocols, revisit them to simplify some of their requirements, and also extend them to generate two-mode multiphoton states, such as Yurke or NOON states.

Ex-vivo multiphoton analysis of rabbit corneal wound healing following photorefractive keratectomy

NASA Astrophysics Data System (ADS)

Wang, Tsung-Jen; Lo, Wen; Dong, Chen-Yuan; Hu, Fung-Rong

2008-02-01

The aim of this study is to assess the application of multiphoton autofluorescence and second harmonic generation (SHG) microscopy for investigating corneal wound healing after high myopic (-10.0D) photorefractive keratectomy (PRK) procedures on the rabbit eyes. The effect of PRK on the morphology and distribution of keratocytes were investigated using multiphoton excited autofluorescence imaging, while the effect of PRK on the arrangement of collagen fibers was monitored by second-harmonic generation imaging. Without histological processing, multiphoton microscopy is able to characterize corneal damage and wound healing from PRK. Our results show that this technique has potential application in the clinical evaluation of corneal damage due to refractive surgery, and may be used to study the unwanted side effects of these procedures.

Deep Tissue Fluorescent Imaging in Scattering Specimens Using Confocal Microscopy

PubMed Central

Clendenon, Sherry G.; Young, Pamela A.; Ferkowicz, Michael; Phillips, Carrie; Dunn, Kenneth W.

2015-01-01

In scattering specimens, multiphoton excitation and nondescanned detection improve imaging depth by a factor of 2 or more over confocal microscopy; however, imaging depth is still limited by scattering. We applied the concept of clearing to deep tissue imaging of highly scattering specimens. Clearing is a remarkably effective approach to improving image quality at depth using either confocal or multiphoton microscopy. Tissue clearing appears to eliminate the need for multiphoton excitation for deep tissue imaging. PMID:21729357

In vivo 3D measurement of moxifloxacin and gatifloxacin distributions in the mouse cornea using multiphoton microscopy

NASA Astrophysics Data System (ADS)

Lee, Seunghun; Lee, Jun Ho; Park, Jin Hyoung; Yoon, Yeoreum; Chung, Wan Kyun; Tchah, Hungwon; Kim, Myoung Joon; Kim, Ki Hean

2016-05-01

Moxifloxacin and gatifloxacin are fourth-generation fluoroquinolone antibiotics used in the clinic to prevent or treat ocular infections. Their pharmacokinetics in the cornea is usually measured from extracted ocular fluids or tissues, and in vivo direct measurement is difficult. In this study multiphoton microscopy (MPM), which is a 3D optical microscopic technique based on multiphoton fluorescence, was applied to the measurement of moxifloxacin and gatifloxacin distribution in the cornea. Intrinsic multiphoton fluorescence properties of moxifloxacin and gatifloxacin were characterized, and their distributions in mouse cornea in vivo were measured by 3D MPM imaging. Both moxifloxacin and gatifloxacin had similar multiphoton spectra, while moxifloxacin had stronger fluorescence than gatifloxacin. MPM imaging of mouse cornea in vivo showed (1) moxifloxacin had good penetration through the superficial corneal epithelium, while gatifloxacin had relatively poor penetration, (2) both ophthalmic solutions had high intracellular distribution. In vivo MPM results were consistent with previous studies. This study demonstrates the feasibility of MPM as a method for in vivo direct measurement of moxifloxacin and gatifloxacin in the cornea.

In vivo 3D measurement of moxifloxacin and gatifloxacin distributions in the mouse cornea using multiphoton microscopy

PubMed Central

Lee, Seunghun; Lee, Jun Ho; Park, Jin Hyoung; Yoon, Yeoreum; Chung, Wan Kyun; Tchah, Hungwon; Kim, Myoung Joon; Kim, Ki Hean

2016-01-01

Moxifloxacin and gatifloxacin are fourth-generation fluoroquinolone antibiotics used in the clinic to prevent or treat ocular infections. Their pharmacokinetics in the cornea is usually measured from extracted ocular fluids or tissues, and in vivo direct measurement is difficult. In this study multiphoton microscopy (MPM), which is a 3D optical microscopic technique based on multiphoton fluorescence, was applied to the measurement of moxifloxacin and gatifloxacin distribution in the cornea. Intrinsic multiphoton fluorescence properties of moxifloxacin and gatifloxacin were characterized, and their distributions in mouse cornea in vivo were measured by 3D MPM imaging. Both moxifloxacin and gatifloxacin had similar multiphoton spectra, while moxifloxacin had stronger fluorescence than gatifloxacin. MPM imaging of mouse cornea in vivo showed (1) moxifloxacin had good penetration through the superficial corneal epithelium, while gatifloxacin had relatively poor penetration, (2) both ophthalmic solutions had high intracellular distribution. In vivo MPM results were consistent with previous studies. This study demonstrates the feasibility of MPM as a method for in vivo direct measurement of moxifloxacin and gatifloxacin in the cornea. PMID:27138688

Multiphoton imaging microscopy at deeper layers with adaptive optics control of spherical aberration.

PubMed

Bueno, Juan M; Skorsetz, Martin; Palacios, Raquel; Gualda, Emilio J; Artal, Pablo

2014-01-01

Despite the inherent confocality and optical sectioning capabilities of multiphoton microscopy, three-dimensional (3-D) imaging of thick samples is limited by the specimen-induced aberrations. The combination of immersion objectives and sensorless adaptive optics (AO) techniques has been suggested to overcome this difficulty. However, a complex plane-by-plane correction of aberrations is required, and its performance depends on a set of image-based merit functions. We propose here an alternative approach to increase penetration depth in 3-D multiphoton microscopy imaging. It is based on the manipulation of the spherical aberration (SA) of the incident beam with an AO device while performing fast tomographic multiphoton imaging. When inducing SA, the image quality at best focus is reduced; however, better quality images are obtained from deeper planes within the sample. This is a compromise that enables registration of improved 3-D multiphoton images using nonimmersion objectives. Examples on ocular tissues and nonbiological samples providing different types of nonlinear signal are presented. The implementation of this technique in a future clinical instrument might provide a better visualization of corneal structures in living eyes.

Characterizing lamina propria of human gastric mucosa by multiphoton microscopy

NASA Astrophysics Data System (ADS)

Liu, Y. C.; Yang, H. Q.; Chen, G.; Zhuo, S. M.; Chen, J. X.; Yan, J.

2011-01-01

Lamina propria (LP) of gastric mucosa plays an important role in progression of gastric cancer because of the site at where inflammatory reactions occur. Multiphoton imaging has been recently employed for microscopic examination of intact tissue. In this paper, using multiphoton microscopy (MPM) based on two-photon excited fluorescence (TPEF) and second harmonic generation (SHG), high resolution multiphoton microscopic images of lamina propria (LP) are obtained in normal human gastric mucosa at excitation wavelength λex = 800 nm. The main source of tissue TPEF originated from the cells of gastric glands, and loose connective tissue, collagen, produced SHG signals. Our results demonstrated that MPM can be effective for characterizing the microstructure of LP in human gastric mucosa. The findings will be helpful for diagnosing and staging early gastric cancer in the clinics.

In vivo microscopy of the mouse brain using multiphoton laser scanning techniques

NASA Astrophysics Data System (ADS)

Yoder, Elizabeth J.

2002-06-01

The use of multiphoton microscopy for imaging mouse brain in vivo offers several advantages and poses several challenges. This tutorial begins by briefly comparing multiphoton microscopy with other imaging modalities used to visualize the brain and its activity. Next, an overview of the techniques for introducing fluorescence into whole animals to generate contrast for in vivo microscopy using two-photon excitation is presented. Two different schemes of surgically preparing mice for brain imaging with multiphoton microscopy are reviewed. Then, several issues and problems with in vivo microscopy - including motion artifact, respiratory and cardiac rhythms, maintenance of animal health, anesthesia, and the use of fiducial markers - are discussed. Finally, examples of how these techniques have been applied to visualize the cerebral vasculature and its response to hypercapnic stimulation are provided.

A review of biomedical multiphoton microscopy and its laser sources

NASA Astrophysics Data System (ADS)

Lefort, Claire

2017-10-01

Multiphoton microscopy (MPM) has been the subject of major development efforts for about 25 years for imaging biological specimens at micron scale and presented as an elegant alternative to classical fluorescence methods such as confocal microscopy. In this topical review, the main interests and technical requirements of MPM are addressed with a focus on the crucial role of excitation source for optimization of multiphoton processes. Then, an overview of the different sources successfully demonstrated in literature for MPM is presented, and their physical parameters are inventoried. A classification of these sources in function with their ability to optimize multiphoton processes is proposed, following a protocol found in literature. Starting from these considerations, a suggestion of a possible identikit of the ideal laser source for MPM concludes this topical review. Dedicated to Martin.

Effects of ultrashort laser pulses on angular distributions of photoionization spectra.

PubMed

Ooi, C H Raymond; Ho, W L; Bandrauk, A D

2017-07-27

We study the photoelectron spectra by intense laser pulses with arbitrary time dependence and phase within the Keldysh framework. An efficient semianalytical approach using analytical transition matrix elements for hydrogenic atoms in any initial state enables efficient and accurate computation of the photoionization probability at any observation point without saddle point approximation, providing comprehensive three dimensional photoelectron angular distribution for linear and elliptical polarizations, that reveal the intricate features and provide insights on the photoionization characteristics such as angular dispersions, shift and splitting of photoelectron peaks from the tunneling or above threshold ionization(ATI) regime to non-adiabatic(intermediate) and multiphoton ionization(MPI) regimes. This facilitates the study of the effects of various laser pulse parameters on the photoelectron spectra and their angular distributions. The photoelectron peaks occur at multiples of 2ħω for linear polarization while  odd-ordered peaks are suppressed in the direction perpendicular to the electric field. Short pulses create splitting and angular dispersion where the peaks are strongly correlated to the angles. For MPI and elliptical polarization with shorter pulses the peaks split into doublets and the first peak vanishes. The carrier envelope phase(CEP) significantly affects the ATI spectra while the Stark effect shifts the spectra of intermediate regime to higher energies due to interference.

Laser spectroscopy on organic molecules.

PubMed

Imasaka, T

1996-06-01

Various laser spectrometric methods have been developed until now. Especially, laser fluorometry is most sensitive and is frequently combined with a separation technique such as capillary electrophoresis. For non-fluorescent compounds, photothermal spectrometry may be used instead. A diode laser is potentially useful for practical trace analysis, because of its low cost and long-term trouble-free operation. On the other hand, monochromaticity of the laser is essential in high-resolution spectrometry, e.g. in low temperature spectrometry providing a very sharp spectral feature. Closely-related compounds such as isomers can easily be differentiated, and information for assignment is obtained from the spectrum. Multiphoton ionization mass spectrometry is useful for soft ionization, providing additional information concerned with molecular weight and chemical structure. A short laser pulse with a sufficient energy is suitable for rapid heating of the solid surface. A matrix-assisted laser desorption/ion-ization technique is recently employed for introduction of a large biological molecule into a vacuum for mass analysis. In the future, laser spectrometry will be developed by a combination with state-of-the-art laser technology. In the 21st century, new laser spectrometry will be developed, which may be based on revolutionary ideas or unexpected discoveries. Such studies will open new frontiers in analytical laser spectroscopy.

In vivo multiphoton microscopy of deep tissue with gradient index lenses

NASA Astrophysics Data System (ADS)

Levene, Michael J.; Dombeck, Daniel A.; Williams, Rebecca M.; Skoch, Jesse; Hickey, Gregory A.; Kasischke, Karl A.; Molloy, Raymond P.; Ingelsson, Martin; Stern, Edward A.; Klucken, Jochen; Bacskai, Brian J.; Zipfel, Warren R.; Hyman, Bradley T.; Webb, Watt W.

2004-06-01

Gradient index lenses enable multiphoton microscopy of deep tissues in the intact animal. In order to assess their applicability to clinical research, we present in vivo multiphoton microscopy with gradient index lenses in brain regions associated with Alzheimer's disease and Parkinson's disease in both transgenic and wild-type mice. We also demonstrate microscopy of ovary in wild type mouse using only intrinsic fluorescence and second harmonic generation, signal sources which may prove useful for both the study and diagnosis of cancer.

In vivo multiphoton microscopy beyond 1 mm in the brain

NASA Astrophysics Data System (ADS)

Miller, David R.; Medina, Flor A.; Hassan, Ahmed; Perillo, Evan P.; Hagan, Kristen; Kazmi, S. M. Shams; Zemelman, Boris V.; Dunn, Andrew K.

2017-02-01

We perform high-resolution, non-invasive, in vivo deep-tissue imaging of the mouse neocortex using multiphoton microscopy with a high repetition rate optical parametric amplifier laser source tunable between λ=1,100 and 1,400 nm. We demonstrate an imaging depth of 1,200 μm in vasculature and 1,160 μm in neurons. We also demonstrate deep-tissue imaging using Indocyanine Green (ICG), which is FDA approved and a promising route to translate multiphoton microscopy to human applications.

Spectroscopy of Isolated Prebiotic Nucleobases

NASA Technical Reports Server (NTRS)

Svadlenak, Nathan; Callahan, Michael P.; Ligare, Marshall; Gulian, Lisa; Gengeliczki, Zsolt; Nachtigallova, Dana; Hobza, Pavel; deVries, Mattanjah

2011-01-01

We use multiphoton ionization and double resonance spectroscopy to study the excited state dynamics of biologically relevant molecules as well as prebiotic nucleobases, isolated in the gas phase. Molecules that are biologically relevant to life today tend to exhibit short excited state lifetimes compared to similar but non-biologically relevant analogs. The mechanism is internal conversion, which may help protect the biologically active molecules from UV damage. This process is governed by conical intersections that depend very strongly on molecular structure. Therefore we have studied purines and pyrimidines with systematic variations of structure, including substitutions, tautomeric forms, and cluster structures that represent different base pair binding motifs. These structural variations also include possible alternate base pairs that may shed light on prebiotic chemistry. With this in mind we have begun to probe the ultrafast dynamics of molecules that exhibit very short excited states and search for evidence of internal conversions.

Ultrafast dynamics of electrons in ammonia.

PubMed

Vöhringer, Peter

2015-04-01

Solvated electrons were first discovered in solutions of metals in liquid ammonia. The physical and chemical properties of these species have been studied extensively for many decades using an arsenal of electrochemical, spectroscopic, and theoretical techniques. Yet, in contrast to their hydrated counterpart, the ultrafast dynamics of ammoniated electrons remained completely unexplored until quite recently. Femtosecond pump-probe spectroscopy on metal-ammonia solutions and femtosecond multiphoton ionization spectroscopy on the neat ammonia solvent have provided new insights into the optical properties and the reactivities of this fascinating species. This article reviews the nature of the optical transition, which gives the metal-ammonia solutions their characteristic blue appearance, in terms of ultrafast relaxation processes involving bound and continuum excited states. The recombination processes following the injection of an electron via photoionization of the solvent are discussed in the context of the electronic structure of the liquid and the anionic defect associated with the solvated electron.

Polycyclic aromatic hydrocarbons in the atmospheres of Titan and Jupiter

NASA Technical Reports Server (NTRS)

Sagan, Carl; Khare, B. N.; Thompson, W. R.; Mcdonald, G. D.; Wing, Michael R.; Bada, Jeffrey L.; Vo-Dinh, Tuan; Arakawa, E. T.

1993-01-01

PAHs are important components of the interstellar medium and carbonaceous chondrites, but have never been identified in the reducing atmospheres of the outer solar system. Incompletely characterized complex organic solids (tholins) produced by irradiating simulated Titan atmospheres reproduce well the observed UV/visible/IR optical constants of the Titan stratospheric haze. Titan tholin and a tholin generated in a crude simulation of the atmosphere of Jupiter are examined by two-step laser desorption/multiphoton ionization mass spectrometry. A range of two- to four-ring PAHs, some with one to four alkylation sites, are identified, with a net abundance of about 0.0001 g/g (grams per gram) of tholins produced. Synchronous fluorescence techniques confirm this detection. Titan tholins have proportionately more one- and two-ring PAHs than do Jupiter tholins, which in turn have more four-ring and larger PAHs. The four-ringed PAH chrysene, prominent in some discussions of interstellar grains, is found in Jupiter tholins.

Strong Field Optical and Quantum Control

NASA Astrophysics Data System (ADS)

Schumacher, Douglass William

1995-01-01

This work presents the results of an effort to use unique forms of optical radiation to better probe and control matter. Results are presented of a study of intense field photo-ionization of krypton and xenon in a two-color field. The use of a two-color field provides a valuable probe, the relative optical phase, into the dynamics of the ionization process. It is found that phase dependent tunneling character is preserved even though the photoelectron spectra indicate that the experiments performed were well into the multi-photon regime of ionization. Evidence for core scattering of the departing electrons is seen in the changes to the phase dependent spectra as the polarization of the exciting light is varied from linear to slightly elliptical. To further control the optical field, a pulse shaper was constructed using liquid crystal modulators that allowed either spectral phase or spectral amplitude shaping of a short pulse. The results were characterized using cross-correlations. The shaped light was then subsequently amplified in a chirped pulse amplifier. This light was characterized using Frequency Resolved Optical Gating, a newly developed technique for the complete determination of the optical field in a short pulse. The shaped pulses were then used to tailor atomic radial wavepackets in cesium. The evolution of the wavepackets was monitored by measuring atomic auto-interferograms for the case of amplitude shaping, which was used to control the atomic states excited. Cross -interferograms were used for phase shaping, which was used to select the initial phase of the atomic states. The cross-interferograms required the simultaneous amplification of a shaped and an unshaped pulse in our amplifier.

Simulation of deleterious processes in a static-cell diode pumped alkali laser

NASA Astrophysics Data System (ADS)

Oliker, Benjamin Q.; Haiducek, John D.; Hostutler, David A.; Pitz, Greg A.; Rudolph, Wolfgang; Madden, Timothy J.

2014-02-01

The complex interactions in a diode pumped alkali laser (DPAL) gain cell provide opportunities for multiple deleterious processes to occur. Effects that may be attributable to deleterious processes have been observed experimentally in a cesium static-cell DPAL at the United States Air Force Academy [B.V. Zhdanov, J. Sell, R.J. Knize, "Multiple laser diode array pumped Cs laser with 48 W output power," Electronics Letters, 44, 9 (2008)]. The power output in the experiment was seen to go through a "roll-over"; the maximum power output was obtained with about 70 W of pump power, then power output decreased as the pump power was increased beyond this point. Research to determine the deleterious processes that caused this result has been done at the Air Force Research Laboratory utilizing physically detailed simulation. The simulations utilized coupled computational fluid dynamics (CFD) and optics solvers, which were three-dimensional and time-dependent. The CFD code used a cell-centered, conservative, finite-volume discretization of the integral form of the Navier-Stokes equations. It included thermal energy transport and mass conservation, which accounted for chemical reactions and state kinetics. Optical models included pumping, lasing, and fluorescence. The deleterious effects investigated were: alkali number density decrease in high temperature regions, convective flow, pressure broadening and shifting of the absorption lineshape including hyperfine structure, radiative decay, quenching, energy pooling, off-resonant absorption, Penning ionization, photoionization, radiative recombination, three-body recombination due to free electron and buffer gas collisions, ambipolar diffusion, thermal aberration, dissociative recombination, multi-photon ionization, alkali-hydrocarbon reactions, and electron impact ionization.

Observations of the high vibrational levels of the B ' ' B ¯ 1 Σu + state of H2

NASA Astrophysics Data System (ADS)

Chartrand, A. M.; Duan, W.; Ekey, R. C.; McCormack, E. F.

2016-01-01

Double-resonance laser spectroscopy via the E F 1 Σg + , v ' = 6 , J ' = 0 -2 state was used to probe the high vibrational levels of the B ' ' B ¯ 1 Σu + state of molecular hydrogen. Resonantly enhanced multiphoton ionization spectra were recorded by detecting ion production as a function of energy using a time of flight mass spectrometer. New measurements of energies for the v = 51-66 levels for the B ' ' B ¯ state of H2 are reported, which, taken with previous results, span the v = 46-69 vibrational levels. Results for energy levels are compared to theoretical close-coupled calculations [L. Wolniewicz, T. Orlikowski, and G. Staszewska, J. Mol. Spectrosc. 238, 118-126 (2006)]. The average difference between the 84 measured energies and calculated energies is -3.8 cm-1 with a standard deviation of 5.3 cm-1. This level of agreement showcases the success of the theoretical calculations in accounting for the strong rovibronic mixing of the 1 Σu + and 1 Πu + states. Due to the ion-pair character of the outer well, the observed energies of the vibrational levels below the third dissociation limit smoothly connect with previously observed energies of ion-pair states above this limit. The results provide an opportunity for testing a heavy Rydberg multi-channel quantum defect analysis of the high vibrational states below the third dissociation limit.

Ultraviolet photodissociation dynamics of the benzyl radical.

PubMed

Song, Yu; Zheng, Xianfeng; Lucas, Michael; Zhang, Jingsong

2011-05-14

Ultraviolet (UV) photodissociation dynamics of jet-cooled benzyl radical via the 4(2)B(2) electronically excited state is studied in the photolysis wavelength region of 228 to 270 nm using high-n Rydberg atom time-of-flight (HRTOF) and resonance enhanced multiphoton ionization (REMPI) techniques. In this wavelength region, H-atom photofragment yield (PFY) spectra are obtained using ethylbenzene and benzyl chloride as the precursors of benzyl radical, and they have a broad peak centered around 254 nm and are in a good agreement with the previous UV absorption spectra of benzyl. The H + C(7)H(6) product translational energy distributions, P(E(T))s, are derived from the H-atom TOF spectra. The P(E(T)) distributions peak near 5.5 kcal mol(-1), and the fraction of average translational energy in the total excess energy, , is ∼0.3. The P(E(T))s indicate the production of fulvenallene + H, which was suggested by recent theoretical studies. The H-atom product angular distribution is isotropic, with the anisotropy parameter β ≈ 0. The H/D product ratios from isotope labeling studies using C(6)H(5)CD(2) and C(6)D(5)CH(2) are reasonably close to the statistical H/D ratios, suggesting that the H/D atoms are scrambled in the photodissociation of benzyl. The dissociation mechanism is consistent with internal conversion of the electronically excited benzyl followed by unimolecular decomposition of the hot benzyl radical on the ground state.

Use of REMPI-TOFMS for real-time measurement of trace aromatics during operation of aircraft ground equipment

NASA Astrophysics Data System (ADS)

Gullett, Brian; Touati, Abderrahmane; Oudejans, Lukas

Emissions of aromatic air toxics from aircraft ground equipment (AGE) were measured with a resonance enhanced multiphoton ionization-time of flight mass spectrometry (REMPI-TOFMS) system consisting of a pulsed solid state laser for photoionization and a TOFMS for mass discrimination. This instrument was capable of characterizing turbine emissions and the effect of varying load operations on pollutant production. REMPI-TOFMS is capable of high selectivity and low detection limits (part per trillion to part per billion) in real time (1 s resolution). Hazardous air pollutants and criteria pollutants were measured during startups and idle and full load operations. Measurements of compounds such as benzene, toluene, ethylbenzene, xylenes, styrene, and polycyclic aromatic hydrocarbons compared well with standard methods. Startup emissions from the AGE data showed persistent concentrations of pollutants, unlike those from a diesel generator, where a sharp spike in emissions rapidly declined to steady state levels. The time-resolved responses of air toxics concentrations varied significantly by source, complicating efforts to minimize these emissions with common operating prescriptions. The time-resolved measurements showed that pollutant concentrations decline (up to 5×) in a species-specific manner over the course of multiple hours of operation, complicating determination of accurate and precise emission factors via standard extractive sampling. Correlations of air toxic concentrations with more commonly measured pollutants such as CO or PM were poor due to the relatively greater changes in the measured toxics' concentrations.

Photodissociation dynamics of bromoiodomethane from the first and second absorption bands. A combined velocity map and slice imaging study.

PubMed

Marggi Poullain, Sonia; Chicharro, David V; Navarro, Eduardo; Rubio-Lago, Luis; González-Vázquez, Jesús; Bañares, Luis

2018-01-31

The photodissociation dynamics of bromoiodomethane (CH 2 BrI) have been investigated at the maximum of the first A and second A' absorption bands, at 266 and 210 nm excitation wavelengths, respectively, using velocity map and slice imaging techniques in combination with a probe detection of both iodine and bromine fragments, I( 2 P 3/2 ), I*( 2 P 1/2 ), Br( 2 P 3/2 ) and Br*( 2 P 1/2 ) via (2 + 1) resonance enhanced multiphoton ionization. Experimental results, i.e. translational energy and angular distributions, are reported and discussed in conjunction with high level ab initio calculations of potential energy curves and absorption spectra. The results indicate that in the A-band, direct dissociation through the 5A' excited state leads to the I( 2 P 3/2 ) channel while I*( 2 P 1/2 ) atoms are produced via the 5A' → 4A'/4A'' nonadiabatic crossing. The presence of Br and Br* fragments upon excitation to the A-band is attributed to indirect dissociation via a curve crossing between the 5A' with upper excited states such as the 9A'. The A'-band is characterized by a strong photoselectivity leading exclusively to the Br( 2 P 3/2 ) and Br*( 2 P 1/2 ) channels, which are likely produced by dissociation through the 9A' excited state. Avoided crossings between several excited states from both the A and A' bands entangle however the possible reaction pathways.

The visible spectrum of zirconium dioxide, ZrO2

NASA Astrophysics Data System (ADS)

Le, Anh; Steimle, Timothy C.; Gupta, Varun; Rice, Corey A.; Maier, John P.; Lin, Sheng H.; Lin, Chih-Kai

2011-09-01

The electronic spectrum of a cold molecular beam of zirconium dioxide, ZrO2, has been investigated using laser induced fluorescence (LIF) in the region from 17 000 cm-1 to 18 800 cm-1 and by mass-resolved resonance enhanced multi-photon ionization (REMPI) spectroscopy from 17 000 cm-1-21 000 cm-1. The LIF and REMPI spectra are assigned to progressions in the tilde A{^1}B_2(ν1, ν2, ν3) ← tilde X{^1}A_1(0, 0, 0) transitions. Dispersed fluorescence from 13 bands was recorded and analyzed to produce harmonic vibrational parameters for the tilde X{^1}A_1 state of ω1 = 898(1) cm-1, ω2 = 287(2) cm-1, and ω3 = 808(3) cm-1. The observed transition frequencies of 45 bands in the LIF and REMPI spectra produce origin and harmonic vibrational parameters for the tilde A{^1}B_2 state of Te = 16 307(8) cm-1, ω1 = 819(3) cm-1, ω2 = 149(3) cm-1, and ω3 = 518(4) cm-1. The spectra were modeled using a normal coordinate analysis and Franck-Condon factor predictions. The structures, harmonic vibrational frequencies, and the potential energies as a function of bending angle for the tilde A{^1}B_2 and tilde X{^1}A_1 states are predicted using time-dependent density functional theory, complete active space self-consistent field, and related first-principle calculations. A comparison with isovalent TiO2 is made.

Single-field slice-imaging with a movable repeller: photodissociation of N₂O from a hot nozzle.

PubMed

Harding, Dan J; Neugebohren, J; Grütter, M; Schmidt-May, A F; Auerbach, D J; Kitsopoulos, T N; Wodtke, A M

2014-08-07

We present a new photo-fragment imaging spectrometer, which employs a movable repeller in a single field imaging geometry. This innovation offers two principal advantages. First, the optimal fields for velocity mapping can easily be achieved even using a large molecular beam diameter (5 mm); the velocity resolution (better than 1%) is sufficient to easily resolve photo-electron recoil in (2 + 1) resonant enhanced multiphoton ionization of N2 photoproducts from N2O or from molecular beam cooled N2. Second, rapid changes between spatial imaging, velocity mapping, and slice imaging are straightforward. We demonstrate this technique's utility in a re-investigation of the photodissociation of N2O. Using a hot nozzle, we observe slice images that strongly depend on nozzle temperature. Our data indicate that in our hot nozzle expansion, only pure bending vibrations--(0, v2, 0)--are populated, as vibrational excitation in pure stretching or bend-stretch combination modes are quenched via collisional near-resonant V-V energy transfer to the nearly degenerate bending states. We derive vibrationally state resolved absolute absorption cross-sections for (0, v2 ≤ 7, 0). These results agree well with previous work at lower values of v2, both experimental and theoretical. The dissociation energy of N2O with respect to the O((1)D) + N2¹Σ(g)⁺ asymptote was determined to be 3.65 ± 0.02 eV.

Fast volumetric imaging with patterned illumination via digital micro-mirror device-based temporal focusing multiphoton microscopy.

PubMed

Chang, Chia-Yuan; Hu, Yvonne Yuling; Lin, Chun-Yu; Lin, Cheng-Han; Chang, Hsin-Yu; Tsai, Sheng-Feng; Lin, Tzu-Wei; Chen, Shean-Jen

2016-05-01

Temporal focusing multiphoton microscopy (TFMPM) has the advantage of area excitation in an axial confinement of only a few microns; hence, it can offer fast three-dimensional (3D) multiphoton imaging. Herein, fast volumetric imaging via a developed digital micromirror device (DMD)-based TFMPM has been realized through the synchronization of an electron multiplying charge-coupled device (EMCCD) with a dynamic piezoelectric stage for axial scanning. The volumetric imaging rate can achieve 30 volumes per second according to the EMCCD frame rate of more than 400 frames per second, which allows for the 3D Brownian motion of one-micron fluorescent beads to be spatially observed. Furthermore, it is demonstrated that the dynamic HiLo structural multiphoton microscope can reject background noise by way of the fast volumetric imaging with high-speed DMD patterned illumination.

Imaging rat esophagus using combination of reflectance confocal and multiphoton microscopy

NASA Astrophysics Data System (ADS)

Zhuo, S. M.; Chen, J. X.; Jiang, X. S.; Lu, K. C.; Xie, S. S.

2008-08-01

We combine reflectance confocal microscopy (RCM) with multiphoton microscopy (MPM) to image rat esophagus. The two imaging modalities allow detection of layered-resolved complementary information from esophagus. In the keratinizing layer, the keratinocytes boundaries can be characterized by RCM, while the keratinocytes cytoplasm (keratin) can be further imaged by multiphoton autofluorescence signal. In the epithelium, the epithelial cellular boundaries and nucleus can be detected by RCM, and MPM can be used for imaging epithelial cell cytoplasm and monitoring metabolic state of epithelium. In the stroma, multiphoton autofluorescence signal is used to image elastin and second harmonic generation signal is utilized to detect collagen, while RCM is used to determine the optical property of stroma. Overall, these results suggest that the combination of RCM and MPM has potential to provide more important and comprehensive information for early diagnosis of esophageal cancer.

EDITORIAL: Theory of Quantum Gases and Quantum Coherence: The Cortona BEC Workshop, 29 October-2 November 2005

NASA Astrophysics Data System (ADS)

Capuzzi, Pablo; Chitra, R.; Menotti, Chiara; Minguzz, Anna; Vignolo, Patrizia

2006-05-01

Nonlinear, or multiphoton, interaction of intense laser radiation with matter has been a key research subject for about four decades. Every three years, the International Conference on Multiphoton Processes (ICOMP) covers the latest advances in the field. Intense-field physics has seen phenomenal progress over the last decade. What looked like dreams in the mid-nineties have become routine today. Major theoretical, experimental and technological advances in fundamental science and applications of multiphoton processes cover such diverse areas as precision measurements, femtosecond and now attosecond metrology, quantum control of atomic and molecular dynamics, laser machining of solid state materials, laser acceleration of electrons and protons, and medical applications. This special issue of Journal of Physics B: Atomic, Molecular and Optical Physics (J. Phys. B) contains a collection of articles originating from the Tenth International Conference on Multiphoton Processes (ICOMP 2005) held on 9-14 October 2005 in Orford, Quebec, Canada (general chair Lou DiMauro, Ohio State University, program co-chairs Paul Corkum and Misha Ivanov, National Research Council of Canada). The conference focused on atoms and molecules in strong fields, femtosecond and attosecond processes, propagation of intense pulses, and of course multiphoton processes which lie at the foundation of all these subjects. Articles presented in this issue cover several key areas of intense-field physics. These include strong field ionization of atoms, molecules and inside transparent dielectric materials, methods of generation and characterization of attosecond XUV pulses and pulse trains, and new approaches to using intense laser fields and/or attosecond pulses for studying entangled systems and imaging electronic and nuclear dynamics with sub-Ångstrom spatial and sub-femtosecond temporal resolution. We have tried to group the papers according to these general areas. We would like to use this opportunity to thank all the participants of ICOMP-X, and in particular the contributors to this issue, for the high quality of science presented at the conference and in this journal. The success of the conference would not have been possible without the program committee which included D Charalambidis, L Cocke, R Freeman, Y Fujimura, S Goreslavsky, A L'Huillier, F Krausz, R Levis, S H Lin, A Maquet, J Marangos, K Midorikawa, G Mourou, P Salieres, W Sandner, K Schafer, A Scrinzi, A M Sergeev, H Stapelfeldt, A Starace, J Ullrich, M Vrakking, and K Yamanouchi. A particularly lively atmosphere in the discussions was ensured by many students who were able to participate in the conference, in part due to generous support of the Canadian Institute for Photonic Innovations (CIPI) to the Canadian, and of the US Department of Energy Office of Basic Energy Sciences to the American students. Additional support to the conference was provided by the Natural Sciences and Engineering Research Council (NSERC), the National Research Council of Canada (NRC), Pfeiffer Vacuum, Femtolasers Produktions GmbH, Roentdek Handels GmbH, Coherent Laser Products, and Amplitude Technologies. Last but not least, the guest editors of this special issue would like to acknowledge the tremendous amount of work done by the staff of J. Phys. B in handling all aspects of the publication process. In particular, we would like to thank Isabelle Auffret-Babak, Alice Malhador and Joanna Dingley from the editorial team, Katie Gerrard in production and the Editor-in-Chief, Professor J-M Rost.

Resolution enhancement of 2-photon microscopy using high-refractive index microspheres

NASA Astrophysics Data System (ADS)

Tehrani, Kayvan Forouhesh; Darafsheh, Arash; Phang, Sendy; Mortensen, Luke J.

2018-02-01

Intravital microscopy using multiphoton processes is the standard tool for deep tissue imaging inside of biological specimens. Usually, near-infrared and infrared light is used to excite the sample, which enables imaging several mean free path inside a scattering tissues. Using longer wavelengths, however, increases the width of the effective multiphoton Point Spread Function (PSF). Many features inside of cells and tissues are smaller than the diffraction limit, and therefore not possible to distinguish using a large PSF. Microscopy using high refractive index microspheres has shown promise to increase the numerical aperture of an imaging system and enhance the resolution. It has been shown that microspheres can image features λ/7 using single photon process fluorescence. In this work, we investigate resolution enhancement for Second Harmonic Generation (SHG) and 2-photon fluorescence microscopy. We used Barium Titanate glass microspheres with diameters ˜20-30 μm and refractive index ˜1.9-2.1. We show microsphere-assisted SHG imaging in bone collagen fibers. Since bone is a very dense tissue constructed of bundles of collagen fibers, it is nontrivial to image individual fibers. We placed microspheres on a dense area of the mouse cranial bone, and achieved imaging of individual fibers. We found that microsphere assisted SHG imaging resolves features of the bone fibers that are not readily visible in conventional SHG imaging. We extended this work to 2-photon microscopy of mitochondria in mouse soleus muscle, and with the help of microsphere resolving power, we were able to trace individual mitochondrion from their ensemble.

Transverse correlations in multiphoton entanglement

NASA Astrophysics Data System (ADS)

Wen, Jianming; Rubin, Morton H.; Shih, Yanhua

2007-10-01

We have analyzed the transverse correlation in multiphoton entanglement. The generalization of quantum ghost imaging is extended to the N -photon state. The Klyshko’s two-photon advanced-wave picture is generalized to the N -photon case.

Quantum cryptography with perfect multiphoton entanglement.

PubMed

Luo, Yuhui; Chan, Kam Tai

2005-05-01

Multiphoton entanglement in the same polarization has been shown theoretically to be obtainable by type-I spontaneous parametric downconversion (SPDC), which can generate bright pulses more easily than type-II SPDC. A new quantum cryptographic protocol utilizing polarization pairs with the detected type-I entangled multiphotons is proposed as quantum key distribution. We calculate the information capacity versus photon number corresponding to polarization after considering the transmission loss inside the optical fiber, the detector efficiency, and intercept-resend attacks at the level of channel error. The result compares favorably with all other schemes employing entanglement.

Remote focusing for programmable multi-layer differential multiphoton microscopy

PubMed Central

Hoover, Erich E.; Young, Michael D.; Chandler, Eric V.; Luo, Anding; Field, Jeffrey J.; Sheetz, Kraig E.; Sylvester, Anne W.; Squier, Jeff A.

2010-01-01

We present the application of remote focusing to multiphoton laser scanning microscopy and utilize this technology to demonstrate simultaneous, programmable multi-layer imaging. Remote focusing is used to independently control the axial location of multiple focal planes that can be simultaneously imaged with single element detection. This facilitates volumetric multiphoton imaging in scattering specimens and can be practically scaled to a large number of focal planes. Further, it is demonstrated that the remote focusing control can be synchronized with the lateral scan directions, enabling imaging in orthogonal scan planes. PMID:21326641

Hybrid reflecting objectives for functional multiphoton microscopy in turbid media

PubMed Central

Vučinić, Dejan; Bartol, Thomas M.; Sejnowski, Terrence J.

2010-01-01

Most multiphoton imaging of biological specimens is performed using microscope objectives optimized for high image quality under wide-field illumination. We present a class of objectives designed de novo without regard for these traditional constraints, driven exclusively by the needs of fast multiphoton imaging in turbid media: the delivery of femtosecond pulses without dispersion and the efficient collection of fluorescence. We model the performance of one such design optimized for a typical brain-imaging setup and show that it can greatly outperform objectives commonly used for this task. PMID:16880851

Systematic investigation of ion suppression and enhancement effects of fourteen stable-isotope-labeled internal standards by their native analogues using atmospheric-pressure chemical ionization and electrospray ionization and the relevance for multi-analyte liquid chromatographic/mass spectrometric procedures.

PubMed

Remane, Daniela; Wissenbach, Dirk K; Meyer, Markus R; Maurer, Hans H

2010-04-15

In clinical and forensic toxicology, multi-analyte procedures are very useful to quantify drugs and poisons of different classes in one run. For liquid chromatographic/tandem mass spectrometric (LC/MS/MS) multi-analyte procedures, often only a limited number of stable-isotope-labeled internal standards (SIL-ISs) are available. If an SIL-IS is used for quantification of other analytes, it must be excluded that the co-eluting native analyte influences its ionization. Therefore, the effect of ion suppression and enhancement of fourteen SIL-ISs caused by their native analogues has been studied. It could be shown that the native analyte concentration influenced the extent of ion suppression and enhancement effects leading to more suppression with increasing analyte concentration especially when electrospray ionization (ESI) was used. Using atmospheric-pressure chemical ionization (APCI), methanolic solution showed mainly enhancement effects, whereas no ion suppression and enhancement effect, with one exception, occurred when plasma extracts were used under these conditions. Such differences were not observed using ESI. With ESI, eleven SIL-ISs showed relevant suppression effects, but only one analyte showed suppression effects when APCI was used. The presented study showed that ion suppression and enhancement tests using matrix-based samples of different sources are essential for the selection of ISs, particularly if used for several analytes to avoid incorrect quantification. In conclusion, only SIL-ISs should be selected for which no suppression and enhancement effects can be observed. If not enough ISs are free of ionization interferences, a different ionization technique should be considered. 2010 John Wiley & Sons, Ltd.

Multi-photon UV photolysis of gaseous polycyclic aromatic hydrocarbons: Extinction spectra and dynamics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Walsh, A. J.; Gash, E. W.; Mansfield, M. W. D.

The extinction spectra of static naphthalene and static biphenylene vapor, each buffered with a noble gas at room temperature, were measured as a function of time in the region between 390 and 850 nm after UV multi-photon laser photolysis at 308 nm. Employing incoherent broadband cavity enhanced absorption spectroscopy (IBBCEAS), the spectra were found to be unstructured with a general lack of isolated features suggesting that the extinction was not solely based on absorption but was in fact dominated by scattering from particles formed in the photolysis of the respective polycyclic aromatic hydrocarbon. Following UV multi-photon photolysis, the extinction dynamicsmore » of the static (unstirred) closed gas-phase system exhibits extraordinary quasi-periodic and complex oscillations with periods ranging from seconds to many minutes, persisting for up to several hours. Depending on buffer gas type and pressure, several types of dynamical responses could be generated (classified as types I, II, and III). They were studied as a function of temperature and chamber volume for different experimental conditions and possible explanations for the oscillations are discussed. A conclusive model for the observed phenomena has not been established. However, a number of key hypotheses have made based on the measurements in this publication: (a) Following the multi-photon UV photolysis of naphthalene (or biphenylene), particles are formed on a timescale not observable using IBBCEAS. (b) The observed temporal behavior cannot be described on basis of a chemical reaction scheme alone. (c) The pressure dependence of the system's responses is due to transport phenomena of particles in the chamber. (d) The size distribution and the refractive indices of particles are time dependent and evolve on a timescale of minutes to hours. The rate of particle coagulation, involving coalescent growth and particle agglomeration, affects the observed oscillations. (e) The walls of the chamber act as a sink. The wall conditions (which could not be quantitatively characterized) have a profound influence on the dynamics of the system and on its slow return to an equilibrium state.« less

Coherent beam control through inhomogeneous media in multi-photon microscopy

NASA Astrophysics Data System (ADS)

Paudel, Hari Prasad

Multi-photon fluorescence microscopy has become a primary tool for high-resolution deep tissue imaging because of its sensitivity to ballistic excitation photons in comparison to scattered excitation photons. The imaging depth of multi-photon microscopes in tissue imaging is limited primarily by background fluorescence that is generated by scattered light due to the random fluctuations in refractive index inside the media, and by reduced intensity in the ballistic focal volume due to aberrations within the tissue and at its interface. We built two multi-photon adaptive optics (AO) correction systems, one for combating scattering and aberration problems, and another for compensating interface aberrations. For scattering correction a MEMS segmented deformable mirror (SDM) was inserted at a plane conjugate to the objective back-pupil plane. The SDM can pre-compensate for light scattering by coherent combination of the scattered light to make an apparent focus even at a depths where negligible ballistic light remains (i.e. ballistic limit). This problem was approached by investigating the spatial and temporal focusing characteristics of a broad-band light source through strongly scattering media. A new model was developed for coherent focus enhancement through or inside the strongly media based on the initial speckle contrast. A layer of fluorescent beads under a mouse skull was imaged using an iterative coherent beam control method in the prototype two-photon microscope to demonstrate the technique. We also adapted an AO correction system to an existing in three-photon microscope in a collaborator lab at Cornell University. In the second AO correction approach a continuous deformable mirror (CDM) is placed at a plane conjugate to the plane of an interface aberration. We demonstrated that this "Conjugate AO" technique yields a large field-of-view (FOV) advantage in comparison to Pupil AO. Further, we showed that the extended FOV in conjugate AO is maintained over a relatively large axial misalignment of the conjugate planes of the CDM and the aberrating interface. This dissertation advances the field of microscopy by providing new models and techniques for imaging deeply within strongly scattering tissue, and by describing new adaptive optics approaches to extending imaging FOV due to sample aberrations.

Multi-photon UV photolysis of gaseous polycyclic aromatic hydrocarbons: Extinction spectra and dynamics

NASA Astrophysics Data System (ADS)

Walsh, A. J.; Ruth, A. A.; Gash, E. W.; Mansfield, M. W. D.

2013-08-01

The extinction spectra of static naphthalene and static biphenylene vapor, each buffered with a noble gas at room temperature, were measured as a function of time in the region between 390 and 850 nm after UV multi-photon laser photolysis at 308 nm. Employing incoherent broadband cavity enhanced absorption spectroscopy (IBBCEAS), the spectra were found to be unstructured with a general lack of isolated features suggesting that the extinction was not solely based on absorption but was in fact dominated by scattering from particles formed in the photolysis of the respective polycyclic aromatic hydrocarbon. Following UV multi-photon photolysis, the extinction dynamics of the static (unstirred) closed gas-phase system exhibits extraordinary quasi-periodic and complex oscillations with periods ranging from seconds to many minutes, persisting for up to several hours. Depending on buffer gas type and pressure, several types of dynamical responses could be generated (classified as types I, II, and III). They were studied as a function of temperature and chamber volume for different experimental conditions and possible explanations for the oscillations are discussed. A conclusive model for the observed phenomena has not been established. However, a number of key hypotheses have made based on the measurements in this publication: (a) Following the multi-photon UV photolysis of naphthalene (or biphenylene), particles are formed on a timescale not observable using IBBCEAS. (b) The observed temporal behavior cannot be described on basis of a chemical reaction scheme alone. (c) The pressure dependence of the system's responses is due to transport phenomena of particles in the chamber. (d) The size distribution and the refractive indices of particles are time dependent and evolve on a timescale of minutes to hours. The rate of particle coagulation, involving coalescent growth and particle agglomeration, affects the observed oscillations. (e) The walls of the chamber act as a sink. The wall conditions (which could not be quantitatively characterized) have a profound influence on the dynamics of the system and on its slow return to an equilibrium state.

Observation of ionization enhancement in two-color circularly polarized laser fields

NASA Astrophysics Data System (ADS)

Mancuso, Christopher A.; Dorney, Kevin M.; Hickstein, Daniel D.; Chaloupka, Jan L.; Tong, Xiao-Min; Ellis, Jennifer L.; Kapteyn, Henry C.; Murnane, Margaret M.

2017-08-01

When atoms are irradiated by two-color circularly polarized laser fields the resulting strong-field processes are dramatically different than when the same atoms are irradiated by a single-color ultrafast laser. For example, electrons can be driven in complex two-dimensional trajectories before rescattering or circularly polarized high harmonics can be generated, which was once thought impossible. Here, we show that two-color circularly polarized lasers also enable control over the ionization process itself and make a surprising finding: the ionization rate can be enhanced by up to 700 % simply by switching the relative helicity of the two-color circularly polarized laser field. This enhancement is experimentally observed in helium, argon, and krypton over a wide range of intensity ratios of the two-color field. We use a combination of advanced quantum and fully classical calculations to explain this ionization enhancement as resulting in part due to the increased density of excited states available for resonance-enhanced ionization in counter-rotating fields compared with co-rotating fields. In the future, this effect could be used to probe the excited state manifold of complex molecules.

Progress in ultrafast laser processing and future prospects

NASA Astrophysics Data System (ADS)

Sugioka, Koji

2017-03-01

The unique characteristics of ultrafast lasers have rapidly revolutionized materials processing after their first demonstration in 1987. The ultrashort pulse width of the laser suppresses heat diffusion to the surroundings of the processed region, which minimizes the formation of a heat-affected zone and thereby enables ultrahigh precision micro- and nanofabrication of various materials. In addition, the extremely high peak intensity can induce nonlinear multiphoton absorption, which extends the diversity of materials that can be processed to transparent materials such as glass. Nonlinear multiphoton absorption enables three-dimensional (3D) micro- and nanofabrication by irradiation with tightly focused femtosecond laser pulses inside transparent materials. Thus, ultrafast lasers are currently widely used for both fundamental research and practical applications. This review presents progress in ultrafast laser processing, including micromachining, surface micro- and nanostructuring, nanoablation, and 3D and volume processing. Advanced technologies that promise to enhance the performance of ultrafast laser processing, such as hybrid additive and subtractive processing, and shaped beam processing are discussed. Commercial and industrial applications of ultrafast laser processing are also introduced. Finally, future prospects of the technology are given with a summary.

Coherence-Gated Sensorless Adaptive Optics Multiphoton Retinal Imaging

PubMed Central

Cua, Michelle; Wahl, Daniel J.; Zhao, Yuan; Lee, Sujin; Bonora, Stefano; Zawadzki, Robert J.; Jian, Yifan; Sarunic, Marinko V.

2016-01-01

Multiphoton microscopy enables imaging deep into scattering tissues. The efficient generation of non-linear optical effects is related to both the pulse duration (typically on the order of femtoseconds) and the size of the focused spot. Aberrations introduced by refractive index inhomogeneity in the sample distort the wavefront and enlarge the focal spot, which reduces the multiphoton signal. Traditional approaches to adaptive optics wavefront correction are not effective in thick or multi-layered scattering media. In this report, we present sensorless adaptive optics (SAO) using low-coherence interferometric detection of the excitation light for depth-resolved aberration correction of two-photon excited fluorescence (TPEF) in biological tissue. We demonstrate coherence-gated SAO TPEF using a transmissive multi-actuator adaptive lens for in vivo imaging in a mouse retina. This configuration has significant potential for reducing the laser power required for adaptive optics multiphoton imaging, and for facilitating integration with existing systems. PMID:27599635

Phase Sensitive Demodulation in Multiphoton Microscopy

NASA Astrophysics Data System (ADS)

Fisher, Walt G.; Piston, David W.; Wachter, Eric A.

2002-06-01

Multiphoton laser scanning microscopy offers advantages in depth of penetration into intact samples over other optical sectioning techniques. To achieve these advantages it is necessary to detect the emitted light without spatial filtering. In this nondescanned (nonconfocal) approach, ambient room light can easily contaminate the signal, forcing experiments to be performed in absolute darkness. For multiphoton microscope systems employing mode-locked lasers, signal processing can be used to reduce such problems by taking advantage of the pulsed characteristics of such lasers. Specifically, by recovering fluorescence generated at the mode-locked frequency, interference from stray light and other ambient noise sources can be significantly reduced. This technology can be adapted to existing microscopes by inserting demodulation circuitry between the detector and data collection system. The improvement in signal-to-noise ratio afforded by this approach yields a more robust microscope system and opens the possibility of moving multiphoton microscopy from the research lab to more demanding settings, such as the clinic.

Processing multiphoton states through operation on a single photon: Methods and applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lin Qing; He Bing; Bergou, Janos A.

2009-10-15

Multiphoton states are widely applied in quantum information technology. By the methods presented in this paper, the structure of a multiphoton state in the form of multiple single-photon qubit products can be mapped to a single-photon qudit, which could also be in a separable product with other photons. This makes possible the manipulation of such multiphoton states by processing single-photon states. The optical realization of unknown qubit discrimination [B. He, J. A. Bergou, and Y.-H. Ren, Phys. Rev. A 76, 032301 (2007)] is simplified with the transformation methods. Another application is the construction of quantum logic gates, where the inversemore » transformations back to the input state spaces are also necessary. We especially show that the modified setups to implement the transformations can realize the deterministic multicontrol gates (including Toffoli gate) operating directly on the products of single-photon qubits.« less

Coherence-Gated Sensorless Adaptive Optics Multiphoton Retinal Imaging.

PubMed

Cua, Michelle; Wahl, Daniel J; Zhao, Yuan; Lee, Sujin; Bonora, Stefano; Zawadzki, Robert J; Jian, Yifan; Sarunic, Marinko V

2016-09-07

Multiphoton microscopy enables imaging deep into scattering tissues. The efficient generation of non-linear optical effects is related to both the pulse duration (typically on the order of femtoseconds) and the size of the focused spot. Aberrations introduced by refractive index inhomogeneity in the sample distort the wavefront and enlarge the focal spot, which reduces the multiphoton signal. Traditional approaches to adaptive optics wavefront correction are not effective in thick or multi-layered scattering media. In this report, we present sensorless adaptive optics (SAO) using low-coherence interferometric detection of the excitation light for depth-resolved aberration correction of two-photon excited fluorescence (TPEF) in biological tissue. We demonstrate coherence-gated SAO TPEF using a transmissive multi-actuator adaptive lens for in vivo imaging in a mouse retina. This configuration has significant potential for reducing the laser power required for adaptive optics multiphoton imaging, and for facilitating integration with existing systems.

Polymer dots enable deep in vivo multiphoton fluorescence imaging of cerebrovascular architecture

NASA Astrophysics Data System (ADS)

Hassan, Ahmed M.; Wu, Xu; Jarrett, Jeremy W.; Xu, Shihan; Miller, David R.; Yu, Jiangbo; Perillo, Evan P.; Liu, Yen-Liang; Chiu, Daniel T.; Yeh, Hsin-Chih; Dunn, Andrew K.

2018-02-01

Deep in vivo imaging of vasculature requires small, bright, and photostable fluorophores suitable for multiphoton microscopy (MPM). Although semiconducting polymer dots (pdots) are an emerging class of highly fluorescent contrast agents with favorable advantages for the next generation of in vivo imaging, their use for deep multiphoton imaging has never before been demonstrated. Here we characterize the multiphoton properties of three pdot variants (CNPPV, PFBT, and PFPV) and demonstrate deep imaging of cortical microvasculature in C57 mice. Specifically, we measure the two- versus three-photon power dependence of these pdots and observe a clear three-photon excitation signature at wavelengths longer than 1300 nm, and a transition from two-photon to three-photon excitation within a 1060 - 1300 nm excitation range. Furthermore, we show that pdots enable in vivo two-photon imaging of cerebrovascular architecture in mice up to 850 μm beneath the pial surface using 800 nm excitation. In contrast with traditional multiphoton probes, we also demonstrate that the broad multiphoton absorption spectrum of pdots permits imaging at longer wavelengths (λex = 1,060 and 1225 nm). These wavelengths approach an ideal biological imaging wavelength near 1,300 nm and confer compatibility with a high-power ytterbium-fiber laser and a high pulse energy optical parametric amplifier, resulting in substantial improvements in signal-to-background ratio (>3.5-fold) and greater cortical imaging depths of 900 μm and 1300 μm. Ultimately, pdots are a versatile tool for MPM due to their extraordinary brightness and broad absorption, which will undoubtedly unlock the ability to interrogate deep structures in vivo.

Laser-Induced Ionization Efficiency Enhancement On A Filament For Thermal Ionization Mass Spectrometry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Siegfried, M.

2015-10-14

The evaluation of trace Uranium and Plutonium isotope ratios for nanogram to femtogram material quantities is a vital tool for nuclear counter-proliferation and safeguard activities. Thermal Ionization Mass Spectrometry (TIMS) is generally accepted as the state of the art technology for highly accurate and ultra-trace measurements of these actinide ratios. However, the very low TIMS ionization yield (typically less than 1%) leaves much room for improvement. Enhanced ionization of Nd and Sm from a TIMS filament was demonstrated using wavelength resonance with a nanosecond (pulse width) laser operating at 10 Hz when light was directed toward the filament.1 For thismore » study, femtosecond and picosecond laser capabilities were to be employed to study the dissociation and ionization mechanisms of actinides/lanthanides and measure the enhanced ionization of the metal of interest. Since the underlying chemistry of the actinide/lanthanide carbides produced and dissociated on a TIMS filament is not well understood, the experimental parameters affecting the photodissociation and photoionization with one and two laser beams were to be investigated.« less

Multiphoton microscopic imaging of human normal and cancerous oesophagus tissue.

PubMed

Chen, W S; Wang, Y; Liu, N R; Zhang, J X; Chen, R

2014-01-01

In this paper, microstructures of human oesophageal submucosa are evaluated using multiphoton microscopy, based on two-photon excited fluorescence and second harmonic generation. The content and distribution of collagen, elastic fibers and cancer cells in normal and cancerous submucosa layer have been distinctly obtained and briefly discussed. The variation of these components is very relevant to the pathology in oesophagus, especially in early oesophageal cancer. Our results further indicate that the multiphoton microscopy technique has the potential application in vivo in clinical diagnosis and monitoring of early oesophageal cancer. © 2013 The Authors Journal of Microscopy © 2013 Royal Microscopical Society.

Multiphoton microscopy for the in-situ investigation of cellular processes and integrity in cryopreservation.

PubMed

Doerr, Daniel; Stark, Martin; Ehrhart, Friederike; Zimmermann, Heiko; Stracke, Frank

2009-08-01

In this study we demonstrate a new noninvasive imaging method to monitor freezing processes in biological samples and to investigate life in the frozen state. It combines a laser scanning microscope with a computer-controlled cryostage. Nearinfrared (NIR) femtosecond laser pulses evoke the fluorescence of endogenous fluorophores and fluorescent labels due to multiphoton absorption.The inherent optical nonlinearity of multiphoton absorption allows 3D fluorescence imaging for optical tomography of frozen biological material in-situ. As an example for functional imaging we use fluorescence lifetime imaging (FLIM) to create images with chemical and physical contrast.

Multiphoton microscopy can visualize zonal damage and decreased cellular metabolic activity in hepatic ischemia-reperfusion injury in rats

NASA Astrophysics Data System (ADS)

Thorling, Camilla A.; Liu, Xin; Burczynski, Frank J.; Fletcher, Linda M.; Gobe, Glenda C.; Roberts, Michael S.

2011-11-01

Ischemia-reperfusion (I/R) injury is a common occurrence in liver surgery. In orthotopic transplantation, the donor liver is exposed to periods of ischemia and when oxygenated blood is reintroduced to the liver, oxidative stress may develop and lead to graft failure. The aim of this project was to investigate whether noninvasive multiphoton and fluorescence lifetime imaging microscopy, without external markers, were useful in detecting early liver damage caused by I/R injury. Localized hepatic ischemia was induced in rats for 1 h followed by 4 h reperfusion. Multiphoton and fluorescence lifetime imaging microscopy was conducted prior to ischemia and up to 4 h of reperfusion and compared to morphological and biochemical assessment of liver damage. Liver function was significantly impaired at 2 and 4 h of reperfusion. Multiphoton microscopy detected liver damage at 1 h of reperfusion, manifested by vacuolated cells and heterogeneous spread of damage over the liver. The damage was mainly localized in the midzonal region of the liver acinus. In addition, fluorescence lifetime imaging showed a decrease in cellular metabolic activity. Multiphoton and fluorescence lifetime imaging microscopy detected evidence of early I/R injury both structurally and functionally. This provides a simple noninvasive technique useful for following progressive liver injury without external markers.

Laser spectroscopic study of the Rydberg state structure of atomic lithium

NASA Astrophysics Data System (ADS)

Ballard, M. Kent

1998-07-01

Pulsed laser induced fluorescence spectroscopy was performed on both isotopic species of atomic lithium. Nonresonant multiphoton excitation spectra were recorded. The laser induced fluorescence of the lithium vapor was measured following excitation with a tunable, pulsed, nanosecond laser. Both two- and three-photon allowed transitions were observed resulting in four different transition series originating from the 22S and 22P levels, the latter likely originating from photodissociation products of the lithium dimer, Li2. Forty-seven identifiable transitions were assigned for 6Li. Evidence for a parity forbidden multiphoton transition is also present. For 7Li, fifty-three identifiable transitions were assigned including an additional series of parity forbidden multiphoton transitions. Laser polarization and power dependencies were measured and found to be consistent with the multiphoton transition probabilities. Due to the intense laser fields needed to produce the nonresonant multiphoton excitations, the lithium vapor was subjected to the laser induced ac Stark effect. The Autler-Townes doublets observed for the nF gets 2P transition series were found to exhibit normal asymmetry. The observed asymmetrical Autler-Townes profiles are explained in terms of the two-level and the three-level atomic systems which are based on different excitation schemes. A new computerized data acquisition system was developed as well as associated computer programs needed to analyze spectra.

Structure of multiphoton quantum optics. II. Bipartite systems, physical processes, and heterodyne squeezed states

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dell'Anno, Fabio; De Siena, Silvio; Illuminati, Fabrizio

2004-03-01

Extending the scheme developed for a single mode of the electromagnetic field in the preceding paper [F. Dell'Anno, S. De Siena, and F. Illuminati, Phys. Rev. A 69, 033812 (2004)], we introduce two-mode nonlinear canonical transformations depending on two heterodyne mixing angles. They are defined in terms of Hermitian nonlinear functions that realize heterodyne superpositions of conjugate quadratures of bipartite systems. The canonical transformations diagonalize a class of Hamiltonians describing nondegenerate and degenerate multiphoton processes. We determine the coherent states associated with the canonical transformations, which generalize the nondegenerate two-photon squeezed states. Such heterodyne multiphoton squeezed states are defined asmore » the simultaneous eigenstates of the transformed, coupled annihilation operators. They are generated by nonlinear unitary evolutions acting on two-mode squeezed states. They are non-Gaussian, highly nonclassical, entangled states. For a quadratic nonlinearity the heterodyne multiphoton squeezed states define two-mode cubic phase states. The statistical properties of these states can be widely adjusted by tuning the heterodyne mixing angles, the phases of the nonlinear couplings, as well as the strength of the nonlinearity. For quadratic nonlinearity, we study the higher-order contributions to the susceptibility in nonlinear media and we suggest possible experimental realizations of multiphoton conversion processes generating the cubic-phase heterodyne squeezed states.« less

Structure of multiphoton quantum optics. II. Bipartite systems, physical processes, and heterodyne squeezed states

NASA Astrophysics Data System (ADS)

dell'Anno, Fabio; de Siena, Silvio; Illuminati, Fabrizio

2004-03-01

Extending the scheme developed for a single mode of the electromagnetic field in the preceding paper [

Detection of the multiphoton signals in stained tissue using nonlinear optical microscopy

NASA Astrophysics Data System (ADS)

Zeng, Yaping; Xu, Jian; Kang, Deyong; Lin, Jiangbo; Chen, Jianxin

2016-10-01

Multiphoton microscopy (MPM) based on two-photon excited fluorescence (TPEF) and second harmonic generation (SHG) imaging, has become a powerful, important tool for tissue imaging at the molecular level. Recently, MPM is also used to image hematoxylin and eosin (H and E)-stained sections in cancer diagnostics. However, several studies have showed that the MPM images of tissue stained with H and E are significantly different from unstained tissue sections. Our aim was to detect of the multiphoton signals in stained tissue by using MPM. In this paper, MPM was used to image histological sections of esophageal invasive carcinoma tissues stained with H, E, H and E and fresh tissue. To detect of the multiphoton signals in stained tissue, the emission spectroscopic of tissue stained with H, E, H and E were obtained. For comparison, the fresh tissues were also investigated. Our results showed that the tissue stained with H, E, H and E could be detected by their TPEF signals. While the tissue stained with H and fresh tissue could be detected by their TPEF and SHG signals. In this work, we detect of the multiphoton signals in stained tissue. These findings will be useful for choosing suitable staining method so to improve the quality of MPM imaging in the future.

Ultrafast Structural Dynamics in Combustion Relevant Model Systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Weber, Peter M.

2014-03-31

The research project explored the time resolved structural dynamics of important model reaction system using an array of novel methods that were developed specifically for this purpose. They include time resolved electron diffraction, time resolved relativistic electron diffraction, and time resolved Rydberg fingerprint spectroscopy. Toward the end of the funding period, we also developed time-resolved x-ray diffraction, which uses ultrafast x-ray pulses at LCLS. Those experiments are just now blossoming, as the funding period expired. In the following, the time resolved Rydberg Fingerprint Spectroscopy is discussed in some detail, as it has been a very productive method. The binding energymore » of an electron in a Rydberg state, that is, the energy difference between the Rydberg level and the ground state of the molecular ion, has been found to be a uniquely powerful tool to characterize the molecular structure. To rationalize the structure sensitivity we invoke a picture from electron diffraction: when it passes the molecular ion core, the Rydberg electron experiences a phase shift compared to an electron in a hydrogen atom. This phase shift requires an adjustment of the binding energy of the electron, which is measurable. As in electron diffraction, the phase shift depends on the molecular, geometrical structure, so that a measurement of the electron binding energy can be interpreted as a measurement of the molecule’s structure. Building on this insight, we have developed a structurally sensitive spectroscopy: the molecule is first elevated to the Rydberg state, and the binding energy is then measured using photoelectron spectroscopy. The molecule’s structure is read out as the binding energy spectrum. Since the photoionization can be done with ultrafast laser pulses, the technique is inherently capable of a time resolution in the femtosecond regime. For the purpose of identifying the structures of molecules during chemical reactions, and for the analysis of molecular species in the hot environments of combustion processes, there are several features that make the Rydberg ionization spectroscopy uniquely useful. First, the Rydberg electron’s orbit is quite large and covers the entire molecule for most molecular structures of combustion interest. Secondly, the ionization does not change vibrational quantum numbers, so that even complicated and large molecules can be observed with fairly well resolved spectra. In fact, the spectroscopy is blind to vibrational excitation of the molecule. This has the interesting consequence for the study of chemical dynamics, where the molecules are invariably very energetic, that the molecular structures are observed unobstructed by the vibrational congestion that dominates other spectroscopies. This implies also that, as a tool to probe the time-dependent structural dynamics of chemically interesting molecules, Rydberg spectroscopy may well be better suited than electron or x-ray diffraction. With recent progress in calculating Rydberg binding energy spectra, we are approaching the point where the method can be evolved into a structure determination method. To implement the Rydberg ionization spectroscopy we use a molecular beam based, time-resolved pump-probe multi-photon ionization/photoelectron scheme in which a first laser pulse excites the molecule to a Rydberg state, and a probe pulse ionizes the molecule. A time-of-flight detector measures the kinetic energy spectrum of the photoelectrons. The photoelectron spectrum directly provides the binding energy of the electron, and thereby reveals the molecule’s time-dependent structural fingerprint. Only the duration of the laser pulses limits the time resolution. With a new laser system, we have now reached time resolutions better than 100 fs, although very deep UV wavelengths (down to 190 nm) have slightly longer instrument functions. The structural dynamics of molecules in Rydberg-excited states is obtained by delaying the probe ionization photon from the pump photon; the structural dynamics of molecules in their ground state or excited valence states is measured by inducing the dynamics using a near UV laser pulse, and employing a multi-photon ionization scheme via the Rydberg states as a probe process. Thus, the technique is capable of measuring the reaction dynamics in any electronic state of neutral molecules.« less

The Ar-NO van der Waals complex studied by resonant multiphoton ionization spectroscopy involving photoion and photoelectron measurements

NASA Astrophysics Data System (ADS)

Sato, Kenji; Achiba, Yohji; Kimura, Katsumi

1984-07-01

Using a 5% mixture of NO in Ar in a supersonic free jet, in the present work we have carried out measurements of the total ion current in the 380-385 nm laser wavelength region. We have also measured photoelectron kinetic energy spectra at individual ion current peaks. In the ion-current spectrum we have observed a new vibrational progression which consists of four peaks in the wavelength region longer than the peak of the two-photon transition of the free NO molecule NO(X, v″=0) →2hν NO(C,v'=0). It has been concluded that the new ion-current peaks are attributed to bound-to-bound transitions of the Ar-NO van der Waals complex from its ground state to the two-photon resonant state expressed by Ar-NO*(C 2Π, v'=0), in which the NO component is in the 3p Rydberg state. The whole resonant ionization process studied may be expressed by Ar-NO(X, v″=0) →2hνAr-NO*(C, v'=0) →hν Ar-NO+(X, v+=0). Each ion-current peak separation is about 50 cm-1, which may correspond to the frequency of the Ar-NO intermolecular stretching vibration, showing a strong anharmonicity. The dissociation energy (D0) of the Ar-NO*(C 2Π) state has been found to be 0.055±0.001 eV. From the photoelectron spectra, we also conclude that the adiabatic ionization energy of Ar-NO is Ia =9.148±0.005 eV and the dissociation energy of the Ar-NO+(X 1Σ) ion is D0=0.129±0.005 eV.

A novel flexible clinical multiphoton tomograph for early melanoma detection, skin analysis, testing of anti-age products, and in situ nanoparticle tracking

NASA Astrophysics Data System (ADS)

Weinigel, Martin; Breunig, Hans Georg; Gregory, Axel; Fischer, Peter; Kellner-Höfer, Marcel; Bückle, Rainer; König, Karsten

2010-02-01

High-resolution 3D microscopy based on multiphoton induced autofluorescence and second harmonic generation have been introduced in 1990. 13 years later, CE-marked clinical multiphoton systems for 3D imaging of human skin with subcellular resolution have first been launched by JenLab company with the tomography DermaInspect®. This year, the second generation of clinical multiphoton tomographs was introduced. The novel multiphoton tomograph MPTflex, equipped with a flexible articulated optical arm, provides an increased flexibility and accessibility especially for clinical and cosmetical examinations. Improved image quality and signal to noise ratio (SNR) are achieved by a very short source-drain spacing, by larger active areas of the detectors and by single photon counting (SPC) technology. Shorter image acquisition time due to improved image quality reduces artifacts and simplifies the operation of the system. The compact folded optical design and the light-weight structure of the optical head eases the handling. Dual channel detectors enable to distinguish between intratissue elastic fibers and collagenous structures simultaneously. Through the use of piezo-driven optics a stack of optical cross-sections (optical sectioning) can be acquired and 3D imaging can be performed. The multiphoton excitation of biomolecules like NAD(P)H, flavins, porphyrins, elastin, and melanin is done by picojoule femtosecond laser pulses from an tunable turn-key femtosescond near infrared laser system. The ability for rapid high-quality image acquisition, the user-friendly operation of the system and the compact and flexible design qualifies this system to be used for melanoma detection, diagnostics of dermatological disorders, cosmetic research and skin aging measurements as well as in situ drug monitoring and animal research.

Surface-plasmon resonance-enhanced multiphoton emission of high-brightness electron beams from a nanostructured copper cathode.

PubMed

Li, R K; To, H; Andonian, G; Feng, J; Polyakov, A; Scoby, C M; Thompson, K; Wan, W; Padmore, H A; Musumeci, P

2013-02-15

We experimentally investigate surface-plasmon assisted photoemission to enhance the efficiency of metallic photocathodes for high-brightness electron sources. A nanohole array-based copper surface was designed to exhibit a plasmonic response at 800 nm, fabricated using the focused ion beam milling technique, optically characterized and tested as a photocathode in a high power radio frequency photoinjector. Because of the larger absorption and localization of the optical field intensity, the charge yield observed under ultrashort laser pulse illumination is increased by more than 100 times compared to a flat surface. We also present the first beam characterization results (intrinsic emittance and bunch length) from a nanostructured photocathode.

Hindlimb heating increases vascular access of large molecules to murine tibial growth plates measured by in vivo multiphoton imaging

PubMed Central

Efaw, Morgan L.; Williams, Rebecca M.

2013-01-01

Advances in understanding the molecular regulation of longitudinal growth have led to development of novel drug therapies for growth plate disorders. Despite progress, a major unmet challenge is delivering therapeutic agents to avascular-cartilage plates. Dense extracellular matrix and lack of penetrating blood vessels create a semipermeable “barrier,” which hinders molecular transport at the vascular-cartilage interface. To overcome this obstacle, we used a hindlimb heating model to manipulate bone circulation in 5-wk-old female mice (n = 22). Temperatures represented a physiological range of normal human knee joints. We used in vivo multiphoton microscopy to quantify temperature-enhanced delivery of large molecules into tibial growth plates. We tested the hypothesis that increasing hindlimb temperature from 22°C to 34°C increases vascular access of large systemic molecules, modeled using 10, 40, and 70 kDa dextrans that approximate sizes of physiological regulators. Vascular access was quantified by vessel diameter, velocity, and dextran leakage from subperichondrial plexus vessels and accumulation in growth plate cartilage. Growth plate entry of 10 kDa dextrans increased >150% at 34°C. Entry of 40 and 70 kDa dextrans increased <50%, suggesting a size-dependent temperature enhancement. Total dextran levels in the plexus increased at 34°C, but relative leakage out of vessels was not temperature dependent. Blood velocity and vessel diameter increased 118% and 31%, respectively, at 34°C. These results demonstrate that heat enhances vascular carrying capacity and bioavailability of large molecules around growth plates, suggesting that temperature could be a noninvasive strategy for modulating delivery of therapeutics to impaired growth plates of children. PMID:24371019

Spin Multiphoton Antiresonance at Finite Temperatures

NASA Astrophysics Data System (ADS)

Hicke, Christian; Dykman, Mark

2007-03-01

Weakly anisotropic S>1 spin systems display multiphoton antiresonance. It occurs when an Nth overtone of the radiation frequency coincides with the distance between the ground and the Nth excited energy level (divided by ). The coherent response of the spin displays a sharp minimum or maximum as a function of frequency, depending on which state was initially occupied. We find the spectral shape of the response dips/peaks. We also study the stationary response for zero and finite temperatures. The response changes dramatically with increasing temperature, when excited states become occupied even in the absence of radiation. The change is due primarily to the increasing role of single-photon resonances between excited states, which occur at the same frequencies as multiphoton resonances. Single-photon resonances are broad, because the single-photon Rabi frequencies largely exceed the multi-photon ones. This allows us to separate different resonances and to study their spectral shape. We also study the change of the spectrum due to relaxational broadening of the peaks, with account taken of both decay and phase modulation.

High speed multiphoton imaging

NASA Astrophysics Data System (ADS)

Li, Yongxiao; Brustle, Anne; Gautam, Vini; Cockburn, Ian; Gillespie, Cathy; Gaus, Katharina; Lee, Woei Ming

2016-12-01

Intravital multiphoton microscopy has emerged as a powerful technique to visualize cellular processes in-vivo. Real time processes revealed through live imaging provided many opportunities to capture cellular activities in living animals. The typical parameters that determine the performance of multiphoton microscopy are speed, field of view, 3D imaging and imaging depth; many of these are important to achieving data from in-vivo. Here, we provide a full exposition of the flexible polygon mirror based high speed laser scanning multiphoton imaging system, PCI-6110 card (National Instruments) and high speed analog frame grabber card (Matrox Solios eA/XA), which allows for rapid adjustments between frame rates i.e. 5 Hz to 50 Hz with 512 × 512 pixels. Furthermore, a motion correction algorithm is also used to mitigate motion artifacts. A customized control software called Pscan 1.0 is developed for the system. This is then followed by calibration of the imaging performance of the system and a series of quantitative in-vitro and in-vivo imaging in neuronal tissues and mice.

Tuning single-photon sources for telecom multi-photon experiments.

PubMed

Greganti, Chiara; Schiansky, Peter; Calafell, Irati Alonso; Procopio, Lorenzo M; Rozema, Lee A; Walther, Philip

2018-02-05

Multi-photon state generation is of great interest for near-future quantum simulation and quantum computation experiments. To-date spontaneous parametric down-conversion is still the most promising process, even though two major impediments still exist: accidental photon noise (caused by the probabilistic non-linear process) and imperfect single-photon purity (arising from spectral entanglement between the photon pairs). In this work, we overcome both of these difficulties by (1) exploiting a passive temporal multiplexing scheme and (2) carefully optimizing the spectral properties of the down-converted photons using periodically-poled KTP crystals. We construct two down-conversion sources in the telecom wavelength regime, finding spectral purities of > 91%, while maintaining high four-photon count rates. We use single-photon grating spectrometers together with superconducting nanowire single-photon detectors to perform a detailed characterization of our multi-photon source. Our methods provide practical solutions to produce high-quality multi-photon states, which are in demand for many quantum photonics applications.

ARTICLES: Variation of the absorption cross section of high-power infrared laser radiation in homologous series of CnH2n+1OH molecules

NASA Astrophysics Data System (ADS)

Bagratashvili, Viktor N.; Brodskaya, E. A.; Vereshchagina, Lyudmila N.; Kuz'min, M. V.; Osmanov, R. R.; Putilin, F. N.; Stuchebryukhov, A. A.

1984-11-01

An experimental investigation was made of variation of the characteristics of infrared multiphoton absorption in a homologous series of CnH2n+1OH alcohols (n = 1-5) excited with CO2 laser pulses. The dependences of the energy absorbed by the molecules on the frequency and energy density of laser radiation were determined by the optoacoustic method. It was found that the multiphoton absorption cross section decreases on increase in the radiation energy density at a rate which becomes slower on increase in the molecular size. A model is proposed for multiphoton excitation of molecules in a homologous series. This model is based on an analysis of a resonant mode interacting with the infrared radiation field and coupled to a reservoir of modes that do not interact with the field. The model predicts correctly the change in the multiphoton absorption cross section on increase in the number of the degrees of freedom of a molecule.

Spatiotemporal focusing-based widefield multiphoton microscopy for fast optical sectioning.

PubMed

Cheng, Li-Chung; Chang, Chia-Yuan; Lin, Chun-Yu; Cho, Keng-Chi; Yen, Wei-Chung; Chang, Nan-Shan; Xu, Chris; Dong, Chen Yuan; Chen, Shean-Jen

2012-04-09

In this study, a microscope based on spatiotemporal focusing offering widefield multiphoton excitation has been developed to provide fast optical sectioning images. Key features of this microscope are the integrations of a 10 kHz repetition rate ultrafast amplifier featuring high instantaneous peak power (maximum 400 μJ/pulse at a 90 fs pulse width) and a TE-cooled, ultra-sensitive photon detecting, electron multiplying charge-coupled camera into a spatiotemporal focusing microscope. This configuration can produce multiphoton images with an excitation area larger than 200 × 100 μm² at a frame rate greater than 100 Hz (current maximum of 200 Hz). Brownian motions of fluorescent microbeads as small as 0.5 μm were observed in real-time with a lateral spatial resolution of less than 0.5 μm and an axial resolution of approximately 3.5 μm. Furthermore, second harmonic images of chicken tendons demonstrate that the developed widefield multiphoton microscope can provide high resolution z-sectioning for bioimaging.

Focal switching of photochromic fluorescent proteins enables multiphoton microscopy with superior image contrast.

PubMed

Kao, Ya-Ting; Zhu, Xinxin; Xu, Fang; Min, Wei

2012-08-01

Probing biological structures and functions deep inside live organisms with light is highly desirable. Among the current optical imaging modalities, multiphoton fluorescence microscopy exhibits the best contrast for imaging scattering samples by employing a spatially confined nonlinear excitation. However, as the incident laser power drops exponentially with imaging depth into the sample due to the scattering loss, the out-of-focus background eventually overwhelms the in-focus signal, which defines a fundamental imaging-depth limit. Herein we significantly improve the image contrast for deep scattering samples by harnessing reversibly switchable fluorescent proteins (RSFPs) which can be cycled between bright and dark states upon light illumination. Two distinct techniques, multiphoton deactivation and imaging (MPDI) and multiphoton activation and imaging (MPAI), are demonstrated on tissue phantoms labeled with Dronpa protein. Such a focal switch approach can generate pseudo background-free images. Conceptually different from wave-based approaches that try to reduce light scattering in turbid samples, our work represents a molecule-based strategy that focused on imaging probes.

Focal switching of photochromic fluorescent proteins enables multiphoton microscopy with superior image contrast

PubMed Central

Kao, Ya-Ting; Zhu, Xinxin; Xu, Fang; Min, Wei

2012-01-01

Probing biological structures and functions deep inside live organisms with light is highly desirable. Among the current optical imaging modalities, multiphoton fluorescence microscopy exhibits the best contrast for imaging scattering samples by employing a spatially confined nonlinear excitation. However, as the incident laser power drops exponentially with imaging depth into the sample due to the scattering loss, the out-of-focus background eventually overwhelms the in-focus signal, which defines a fundamental imaging-depth limit. Herein we significantly improve the image contrast for deep scattering samples by harnessing reversibly switchable fluorescent proteins (RSFPs) which can be cycled between bright and dark states upon light illumination. Two distinct techniques, multiphoton deactivation and imaging (MPDI) and multiphoton activation and imaging (MPAI), are demonstrated on tissue phantoms labeled with Dronpa protein. Such a focal switch approach can generate pseudo background-free images. Conceptually different from wave-based approaches that try to reduce light scattering in turbid samples, our work represents a molecule-based strategy that focused on imaging probes. PMID:22876358

Two-Step Single Particle Mass Spectrometry for On-Line Monitoring of Polycyclic Aromatic Hydrocarbons Bound to Ambient Fine Particulate Matter

NASA Astrophysics Data System (ADS)

Zimmermann, R.; Bente, M.; Sklorz, M.

2007-12-01

Polycyclic aromatic hydrocarbons (PAH) are formed as trace products in combustion processes and are emitted to the atmosphere. Larger PAH have low vapour pressure and are predominantly bound to the ambient fine particulate matter (PM). Upon inhalation, PAH show both, chronic human toxicity (i.e. many PAH are potent carcinogens) as well as acute human toxicity (i.e. inflammatory effects due to oxi-dative stress) and are discussed to be relevant for the observed health effect of ambient PM. Therefore a better understanding of the occurrence, dynamics and particle size dependence of particle bound-PAH is of great interest. On-line aerosol mass spectrometry in principle is the method of choice to investigate the size resolved changes in the chemical speciation of particles as well the status of internal vs. external mixing of chemical constituents. However the present available aerosol mass spectrometers (ATOFMS and AMS) do not allow detection of PAH from ambient air PM. In order to allow a single particle based monitoring of PAH from ambient PM a new single particle laser ionisation mass spectrometer was built and applied. The system is based on ATOFMS principle but uses a two- step photo-ionization. A tracked and sized particle firstly is laser desorbed (LD) by a IR-laser pulse (CO2-laser, λ=10.2 μm) and subsequently the released PAH are selectively ionized by an intense UV-laser pulse (ArF excimer, λ=248 nm) in a resonance enhanced multiphoton ionisation process (REMPI). The PAH-ions are detected in a time of flight mass spectrometer (TOFMS). A virtual impactor enrichment unit is used to increase the detection frequency of the ambient particles. With the current inlet system particles from about 400 nm to 10 μm are accessible. Single particle based temporal profiles of PAH containing particles ion (size distribution and PAH speciation) have been recorded in Oberschleissheim, Germany from ambient air. Furthermore profiles of relevant emission sources (e.g. gasoline and diesel engine, wood combustion) and the obtained chemical profiles were compared with the ones from the ambient PAH containing particles.

Real-time analysis of organic compounds in ship engine aerosol emissions using resonance-enhanced multiphoton ionisation and proton transfer mass spectrometry.

PubMed

Radischat, Christian; Sippula, Olli; Stengel, Benjamin; Klingbeil, Sophie; Sklorz, Martin; Rabe, Rom; Streibel, Thorsten; Harndorf, Horst; Zimmermann, Ralf

2015-08-01

Organic combustion aerosols from a marine medium-speed diesel engine, capable to run on distillate (diesel fuel) and residual fuels (heavy fuel oil), were investigated under various operating conditions and engine parameters. The online chemical characterisation of the organic components was conducted using a resonance-enhanced multiphoton ionisation time-of-flight mass spectrometer (REMPI TOF MS) and a proton transfer reaction-quadrupole mass spectrometer (PTR-QMS). Oxygenated species, alkenes and aromatic hydrocarbons were characterised. Especially the aromatic hydrocarbons and their alkylated derivatives were very prominent in the exhaust of both fuels. Emission factors of known health-hazardous compounds (e.g. mono- and poly-aromatic hydrocarbons) were calculated and found in higher amounts for heavy fuel oil (HFO) at typical engine loadings. Lower engine loads lead in general to increasing emissions for both fuels for almost every compound, e.g. naphthalene emissions varied for diesel fuel exhaust between 0.7 mg/kWh (75 % engine load, late start of injection (SOI)) and 11.8 mg/kWh (10 % engine load, late SOI) and for HFO exhaust between 3.3 and 60.5 mg/kWh, respectively. Both used mass spectrometric techniques showed that they are particularly suitable methods for online monitoring of combustion compounds and very helpful for the characterisation of health-relevant substances. Graphical abstract Three-dimensional REMPI data of organic species in diesel fuel and heavy fuel oil exhaust.

High-resolution multiphoton microscopy with a low-power continuous wave laser pump.

PubMed

Chen, Xiang-Dong; Li, Shen; Du, Bo; Dong, Yang; Wang, Ze-Hao; Guo, Guang-Can; Sun, Fang-Wen

2018-02-15

Multiphoton microscopy (MPM) has been widely used for three-dimensional biological imaging. Here, based on the photon-induced charge state conversion process, we demonstrated a low-power high-resolution MPM with a nitrogen vacancy (NV) center in diamond. Continuous wave green and orange lasers were used to pump and detect the two-photon charge state conversion, respectively. The power of the laser for multiphoton excitation was 40 μW. Both the axial and lateral resolutions were improved approximately 1.5 times compared with confocal microscopy. The results can be used to improve the resolution of the NV center-based quantum sensing and biological imaging.

Ionizing radiation changes the electronic properties of melanin and enhances the growth of melanized fungi.

PubMed

Dadachova, Ekaterina; Bryan, Ruth A; Huang, Xianchun; Moadel, Tiffany; Schweitzer, Andrew D; Aisen, Philip; Nosanchuk, Joshua D; Casadevall, Arturo

2007-05-23

Melanin pigments are ubiquitous in nature. Melanized microorganisms are often the dominating species in certain extreme environments, such as soils contaminated with radionuclides, suggesting that the presence of melanin is beneficial in their life cycle. We hypothesized that ionizing radiation could change the electronic properties of melanin and might enhance the growth of melanized microorganisms. Ionizing irradiation changed the electron spin resonance (ESR) signal of melanin, consistent with changes in electronic structure. Irradiated melanin manifested a 4-fold increase in its capacity to reduce NADH relative to non-irradiated melanin. HPLC analysis of melanin from fungi grown on different substrates revealed chemical complexity, dependence of melanin composition on the growth substrate and possible influence of melanin composition on its interaction with ionizing radiation. XTT/MTT assays showed increased metabolic activity of melanized C. neoformans cells relative to non-melanized cells, and exposure to ionizing radiation enhanced the electron-transfer properties of melanin in melanized cells. Melanized Wangiella dermatitidis and Cryptococcus neoformans cells exposed to ionizing radiation approximately 500 times higher than background grew significantly faster as indicated by higher CFUs, more dry weight biomass and 3-fold greater incorporation of (14)C-acetate than non-irradiated melanized cells or irradiated albino mutants. In addition, radiation enhanced the growth of melanized Cladosporium sphaerospermum cells under limited nutrients conditions. Exposure of melanin to ionizing radiation, and possibly other forms of electromagnetic radiation, changes its electronic properties. Melanized fungal cells manifested increased growth relative to non-melanized cells after exposure to ionizing radiation, raising intriguing questions about a potential role for melanin in energy capture and utilization.

Clinical combination of multiphoton tomography and high frequency ultrasound imaging for evaluation of skin diseases

NASA Astrophysics Data System (ADS)

König, K.; Speicher, M.; Koehler, M. J.; Scharenberg, R.; Elsner, P.; Kaatz, M.

2010-02-01

For the first time, high frequency ultrasound imaging, multiphoton tomography, and dermoscopy were combined in a clinical study. Different dermatoses such as benign and malign skin cancers, connective tissue diseases, inflammatory skin diseases and autoimmune bullous skin diseases have been investigated with (i) state-of-the-art and highly sophisticated ultrasound systems for dermatology, (ii) the femtosecond-laser multiphoton tomograph DermaInspectTM and (iii) dermoscopes. Dermoscopy provides two-dimensional color imaging of the skin surface with a magnification up to 70x. Ultrasound images are generated from reflections of the emitted ultrasound signal, based on inhomogeneities of the tissue. These echoes are converted to electrical signals. Depending on the ultrasound frequency the penetration depth varies from about 1 mm to 16 mm in dermatological application. The 100-MHz-ultrasound system provided an axial resolution down to 16 μm and a lateral resolution down to 32 μm. In contrast to the wide-field ultrasound images, multiphoton tomography provided horizontal optical sections of 0.36×0.36 mm2 down to 200 μm tissue depth with submicron resolution. The autofluorescence of mitochondrial coenzymes, melanin, and elastin as well as the secondharmonic- generation signal of the collagen network were imaged. The combination of ultrasound and multiphoton tomography provides a novel opportunity for diagnostics of skin disorders.

Photofragment slice imaging studies of pyrrole and the Xe…pyrrole cluster

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rubio-Lago, L.; Zaouris, D.; Sakellariou, Y.

The photolysis of pyrrole has been studied in a molecular beam at wavelengths 250 nm, 240 nm and 193.3 nm, using 2 different carrier gases, He and Xe. A broad bimodal distribution of H atom fragment velocities has been observed at all wavelengths. Near threshold at both 240 and 250 nm, , sharp features have been observed in the fast part of the H-atom distribution. Under appropriate molecular beam conditions, these sharp features and the photolysis of pyrrole at both 240 and 250 nm disappear when using Xe as opposed to He as the carrier gas. We attribute this phenomenonmore » to cluster formation between Xe and pyrrole, and this assumption is supported by observation of resonance enhanced multiphoton ionization spectra for the (Xe…pyrrole) cluster followed by photofragmentation of the nascent cation cluster. Ab initio calculations are performed to support the experimental data. Part of this work is supported by the transfer of knowledge program SOUTHERN DYNAMICS MTKD-CT-2004-014306. The experimental work was performed at the Ultraviolet Laser Facility operating at IESL-FORTH and has been supported in part by the European Commission through the Research Infrastructures activity of FP6 (“Laserlab- Europe” RII3-CT-2003-506350). We also wish to thank the graduate program Applied Molecular Spectroscopy (EPEAEK). Part of this work was supported by the Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, US Department of Energy with Battelle Memorial Institute, which operates the Pacific Northwest National Laboratory. Computer resources were provided by the Office of Science, US Department of Energy.« less

Watching proton transfer in real time: Ultrafast photoionization-induced proton transfer in phenol-ammonia complex cation.

PubMed

Shen, Ching-Chi; Tsai, Tsung-Ting; Wu, Jun-Yi; Ho, Jr-Wei; Chen, Yi-Wei; Cheng, Po-Yuan

2017-10-28

In this paper, we give a full account of our previous work [C. C. Shen et al., J. Chem. Phys. 141, 171103 (2014)] on the study of an ultrafast photoionization-induced proton transfer (PT) reaction in the phenol-ammonia (PhOH-NH 3 ) complex using ultrafast time-resolved ion photofragmentation spectroscopy implemented by the photoionization-photofragmentation pump-probe detection scheme. Neutral PhOH-NH 3 complexes prepared in a free jet are photoionized by femtosecond 1 + 1 resonance-enhanced multiphoton ionization via the S 1 state. The evolving cations are then probed by delayed pulses that result in ion fragmentation, and the ionic dynamics is followed by measuring the parent-ion depletion as a function of the pump-probe delay time. By comparing with systems in which PT is not feasible and the steady-state ion photofragmentation spectra, we concluded that the observed temporal evolutions of the transient ion photofragmentation spectra are consistent with an intracomplex PT reaction after photoionization from the initial non-PT to the final PT structures. Our experiments revealed that PT in [PhOH-NH 3 ] + cation proceeds in two distinct steps: an initial impulsive wave-packet motion in ∼70 fs followed by a slower relaxation of about 1 ps that stabilizes the system into the final PT configuration. These results indicate that for a barrierless PT system, even though the initial PT motions are impulsive and ultrafast, the time scale to complete the reaction can be much slower and is determined by the rate of energy dissipation into other modes.

Photodissociation of cis-, trans-, and 1,1-dichloroethylene in the ultraviolet range: characterization of Cl((2)P(J)) elimination.

PubMed

Hua, Linqiang; Zhang, Xiaopeng; Lee, Wei-Bin; Chao, Meng-Hsuan; Zhang, Bing; Lin, King-Chuen

2010-01-14

By using photofragment velocity imaging detection coupled with a (2 + 1) resonance-enhanced multiphoton ionization technique, the elimination channel of spin-orbit chlorine atoms in photodissociation of cis-, trans-, and 1,1-dichloroethylene at two photolysis wavelengths of 214.5 and 235 nm is investigated. Translational energy and angular distributions of Cl((2)P(J)) fragmentation are acquired. The Cl((2)P(J)) fragments are produced by two competing channels. The fast dissociation component with higher translational energy is characterized by a Gaussian distribution, resulting from a curve crossing of the initially excited (pi, pi*) state to nearby repulsive (pi, sigma*) and/or (n, sigma*). In contrast, the slow component with a lower translational energy is characterized by a Boltzmann distribution, which dissociates on the vibrationally hot ground state relaxed from the (pi, pi*) state via internal conversion. cis-C(2)H(2)Cl(2) is found to have a larger branching of Boltzmann component than the other two isomers. The fraction of available energy partitioning into translation increases along the trend of cis- < trans- < 1,1-C(2)H(2)Cl(2). This trend may be fitted by a rigid radical model and interpreted by means of a torque generated during the C-Cl bond cleavage. The anisotropy parameters are determined, and the transition dipole moments are expected to be essentially along the C horizontal lineC bond axis. The results are also predicted theoretically. The relative quantum yields of Cl((2)P(J)) have a similar value for the three isomers at the two photolysis wavelengths.

Probing cis-trans isomerization in the S{sub 1} state of C{sub 2}H{sub 2} via H-atom action and hot band-pumped IR-UV double resonance spectroscopies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Changala, P. Bryan; Baraban, Joshua H.; Field, Robert W., E-mail: rwfield@mit.edu

2015-08-28

We report novel experimental strategies that should prove instrumental in extending the vibrational and rotational assignments of the S{sub 1} state of acetylene, C{sub 2}H{sub 2}, in the region of the cis-trans isomerization barrier. At present, the assignments are essentially complete up to ∼500 cm{sup −1} below the barrier. Two difficulties arise when the assignments are continued to higher energies. One is that predissociation into C{sub 2}H + H sets in roughly 1100 cm{sup −1} below the barrier; the resulting quenching of laser-induced fluorescence (LIF) reduces its value for recording spectra in this region. The other difficulty is that tunnelingmore » through the barrier causes a staggering in the K-rotational structure of isomerizing vibrational levels. The assignment of these levels requires data for K values up to at least 3. Given the rotational selection rule K′ − ℓ{sup ′′} = ± 1, such data must be obtained via excited vibrational levels of the ground state with ℓ{sup ′′} > 0. In this paper, high resolution H-atom resonance-enhanced multiphoton ionization spectra are demonstrated to contain predissociated bands which are almost invisible in LIF spectra, while preliminary data using a hyperthermal pulsed nozzle show that ℓ{sup ′′} = 2 states can be selectively populated in a jet, giving access to K′ = 3 states in IR-UV double resonance.« less

Overview: MURI Center on spectroscopic and time domain detection of trace explosives in condensed and vapor phases

NASA Astrophysics Data System (ADS)

Spicer, James B.; Dagdigian, Paul; Osiander, Robert; Miragliotta, Joseph A.; Zhang, Xi-Cheng; Kersting, Roland; Crosley, David R.; Hanson, Ronald K.; Jeffries, Jay

2003-09-01

The research center established by Army Research Office under the Multidisciplinary University Research Initiative program pursues a multidisciplinary approach to investigate and advance the use of complementary analytical techniques for sensing of explosives and/or explosive-related compounds as they occur in the environment. The techniques being investigated include Terahertz (THz) imaging and spectroscopy, Laser-Induced Breakdown Spectroscopy (LIBS), Cavity Ring Down Spectroscopy (CRDS) and Resonance Enhanced Multiphoton Ionization (REMPI). This suite of techniques encompasses a diversity of sensing approaches that can be applied to detection of explosives in condensed phases such as adsorbed species in soil or can be used for vapor phase detection above the source. Some techniques allow for remote detection while others have highly specific and sensitive analysis capabilities. This program is addressing a range of fundamental, technical issues associated with trace detection of explosive related compounds using these techniques. For example, while both LIBS and THz can be used to carry-out remote analysis of condensed phase analyte from a distance in excess several meters, the sensitivities of these techniques to surface adsorbed explosive-related compounds are not currently known. In current implementations, both CRDS and REMPI require sample collection techniques that have not been optimized for environmental applications. Early program elements will pursue the fundamental advances required for these techniques including signature identification for explosive-related compounds/interferents and trace analyte extraction. Later program tasks will explore simultaneous application of two or more techniques to assess the benefits of sensor fusion.

Watching proton transfer in real time: Ultrafast photoionization-induced proton transfer in phenol-ammonia complex cation

NASA Astrophysics Data System (ADS)

Shen, Ching-Chi; Tsai, Tsung-Ting; Wu, Jun-Yi; Ho-Wei, Jr.; Chen, Yi-Wei; Cheng, Po-Yuan

2017-10-01

In this paper, we give a full account of our previous work [C. C. Shen et al., J. Chem. Phys. 141, 171103 (2014)] on the study of an ultrafast photoionization-induced proton transfer (PT) reaction in the phenol-ammonia (PhOH-NH3) complex using ultrafast time-resolved ion photofragmentation spectroscopy implemented by the photoionization-photofragmentation pump-probe detection scheme. Neutral PhOH-NH3 complexes prepared in a free jet are photoionized by femtosecond 1 + 1 resonance-enhanced multiphoton ionization via the S1 state. The evolving cations are then probed by delayed pulses that result in ion fragmentation, and the ionic dynamics is followed by measuring the parent-ion depletion as a function of the pump-probe delay time. By comparing with systems in which PT is not feasible and the steady-state ion photofragmentation spectra, we concluded that the observed temporal evolutions of the transient ion photofragmentation spectra are consistent with an intracomplex PT reaction after photoionization from the initial non-PT to the final PT structures. Our experiments revealed that PT in [PhOH-NH3]+ cation proceeds in two distinct steps: an initial impulsive wave-packet motion in ˜70 fs followed by a slower relaxation of about 1 ps that stabilizes the system into the final PT configuration. These results indicate that for a barrierless PT system, even though the initial PT motions are impulsive and ultrafast, the time scale to complete the reaction can be much slower and is determined by the rate of energy dissipation into other modes.

Preparation of Vibrationally Excited H2 in a Coherent Superposition of M-States Using Stark Induced Adiabatic Raman Passage (SARP)

NASA Astrophysics Data System (ADS)

Mukherjee, Nandini; Dong, Wenrui; Perreault, William; Zare, Richard

2017-04-01

We prepare a large ensemble of rovibrationally excited (v = 1, J = 2) H2 molecules in a coherent superposition of M-states using Stark-induced adiabatic Raman passage (SARP) with linearly polarized single mode pump (532 nm) and Stokes (699 nm) laser pulses of duration 6 ns and 4 ns. A biaxial superposition state, | ψ〉 = 1/ √2 [ | v = 1, J = 2, M = -2〉- | v = 1, J = 2, M = + 2〉], is prepared using SARP with a sequence of a pump laser pulse partially overlapping with a cross polarized Stokes laser pulse co-propagating along the quantization z-axis. The degree of phase coherence is measured by recording interference fringes in the ion signal produced using the O(2) line of 2 +1 resonance enhanced multiphoton ionization (REMPI) from the rovibrationally excited (v = 1, J = 2) level as a function of REMPI laser polarization angle. The ion signal is measured using a time-of-flight mass spectrometer. Nearly 60% population transfer from H2 (v = 0, J = 0) ground state to the superposition state in H2 (v = 1, J = 2) is measured from the depletion of Q(0) REMPI signal of the (v = 0, J = 0) ground state. The M-state superposition behaves much like a multi-slit interferometer where the number of slits, i.e. the number of M-states, and their separations, i.e. the relative phase, can be varied experimentally. This work has been supported by the U.S. Army Research Office.

USE OF MULTIPHOTON LASER SCANNING MICROSCOPY TO IMAGE BENZO[A]PYRENE AND METABOLITES IN FISH EGGS

EPA Science Inventory

Multiphoton laser scanning microscopy (MPLSM) is a promising tool to study the tissue distribution of environmental chemical contaminants during fish early life stages. One such chemical for which this is possible is benzo[a]pyrene (BaP), a polycyclic aromatic hydrocarbon that a...

Multiphoton Imaging of Rabbit Cornea Treated with Mitomycin C after Photorefractive Keratectomy

NASA Astrophysics Data System (ADS)

Hsueh, Chiu-Mei; Lo, Wen; Wang, Tsung-Jen; Hu, Fung-Rong; Dong, Chen-Yuan

2007-07-01

In this work we use multiphoton microscopy to observe the post surgery structure variation of rabbit cornea after photorefractive keratectomy (PRK). In addition, we added mitomycin C (MMC) to the post surgery rabbit cornea in order to investigate the effect of MMC treatment on the postoperative regeneration.

Enantiomer-specific analysis of multi-component mixtures by correlated electron imaging-ion mass spectrometry

NASA Astrophysics Data System (ADS)

Fanood, Mohammad M. Rafiee; Ram, N. Bhargava; Lehmann, C. Stefan; Powis, Ivan; Janssen, Maurice H. M.

2015-06-01

Simultaneous, enantiomer-specific identification of chiral molecules in multi-component mixtures is extremely challenging. Many established techniques for single-component analysis fail to provide selectivity in multi-component mixtures and lack sensitivity for dilute samples. Here we show how enantiomers may be differentiated by mass-selected photoelectron circular dichroism using an electron-ion coincidence imaging spectrometer. As proof of concept, vapours containing ~1% of two chiral monoterpene molecules, limonene and camphor, are irradiated by a circularly polarized femtosecond laser, resulting in multiphoton near-threshold ionization with little molecular fragmentation. Large chiral asymmetries (2-4%) are observed in the mass-tagged photoelectron angular distributions. These asymmetries switch sign according to the handedness (R- or S-) of the enantiomer in the mixture and scale with enantiomeric excess of a component. The results demonstrate that mass spectrometric identification of mixtures of chiral molecules and quantitative determination of enantiomeric excess can be achieved in a table-top instrument.

Photoemission of Energetic Hot Electrons Produced via Up-Conversion in Doped Quantum Dots.

PubMed

Dong, Yitong; Parobek, David; Rossi, Daniel; Son, Dong Hee

2016-11-09

The benefits of the hot electrons from semiconductor nanostructures in photocatalysis or photovoltaics result from their higher energy compared to that of the band-edge electrons facilitating the electron-transfer process. The production of high-energy hot electrons usually requires short-wavelength UV or intense multiphoton visible excitation. Here, we show that highly energetic hot electrons capable of above-threshold ionization are produced via exciton-to-hot-carrier up-conversion in Mn-doped quantum dots under weak band gap excitation (∼10 W/cm 2 ) achievable with the concentrated solar radiation. The energy of hot electrons is as high as ∼0.4 eV above the vacuum level, much greater than those observed in other semiconductor or plasmonic metal nanostructures, which are capable of performing energetically and kinetically more-challenging electron transfer. Furthermore, the prospect of generating solvated electron is unique for the energetic hot electrons from up-conversion, which can open a new door for long-range electron transfer beyond short-range interfacial electron transfer.

Enantiomer-specific analysis of multi-component mixtures by correlated electron imaging–ion mass spectrometry

PubMed Central

Fanood, Mohammad M Rafiee; Ram, N. Bhargava; Lehmann, C. Stefan; Powis, Ivan; Janssen, Maurice H. M.

2015-01-01

Simultaneous, enantiomer-specific identification of chiral molecules in multi-component mixtures is extremely challenging. Many established techniques for single-component analysis fail to provide selectivity in multi-component mixtures and lack sensitivity for dilute samples. Here we show how enantiomers may be differentiated by mass-selected photoelectron circular dichroism using an electron–ion coincidence imaging spectrometer. As proof of concept, vapours containing ∼1% of two chiral monoterpene molecules, limonene and camphor, are irradiated by a circularly polarized femtosecond laser, resulting in multiphoton near-threshold ionization with little molecular fragmentation. Large chiral asymmetries (2–4%) are observed in the mass-tagged photoelectron angular distributions. These asymmetries switch sign according to the handedness (R- or S-) of the enantiomer in the mixture and scale with enantiomeric excess of a component. The results demonstrate that mass spectrometric identification of mixtures of chiral molecules and quantitative determination of enantiomeric excess can be achieved in a table-top instrument. PMID:26104140

Below-threshold harmonic generation from strong non-uniform fields

NASA Astrophysics Data System (ADS)

Yavuz, I.

2017-10-01

Strong-field photoemission below the ionization threshold is a rich/complex region where atomic emission and harmonic generation may coexist. We studied the mechanism of below-threshold harmonics (BTH) from spatially non-uniform local fields near the metallic nanostructures. Discrete harmonics are generated due to the broken inversion symmetry, suggesting enriched coherent emission in the vuv frequency range. Through the numerical solution of the time-dependent Schrödinger equation, we investigate wavelength and intensity dependence of BTH. Wavelength dependence identifies counter-regular resonances; individual contributions from the multi-photon emission and channel-closing effects due to quantum path interferences. In order to understand the underlying mechanism of BTH, we devised a generalized semi-classical model, including the influence of Coulomb and non-uniform field interactions. As in uniform fields, Coulomb potential in non-uniform fields is the determinant of BTH; we observed that the generation of BTH are due to returning trajectories with negative energies. Due to large distance effectiveness of the non-uniformity, only long trajectories are noticeably affected.

Analytical model for atomic resonant attosecond transient absorption

NASA Astrophysics Data System (ADS)

Cariker, C.; Kjellson, T.; Lindroth, E.; Argenti, L.

2017-04-01

Recent advancements in ultrafast laser technology have made it possible to probe electron dynamics in highly excited atomic states that autoionize on a femtosecond timescale, thus giving insight into the dynamics of Auger decay and its interference with the continuum. These experiments provide a stringent test for time-resolved analytical models of autoionization. Here we present a finite-pulse, multi-photon perturbative model which is used in conjunction with ab-initio structure calculations to predict the attosecond transient absorption spectrum (ATAS) of an atom above the ionization threshold. We apply this model to compute the ATAS of argon in the vicinity of the 3s-1 4 p resonance as a function of the time delay between an extreme ultraviolet (XUV) and an infrared (IR) pulse, as well as of the angle between their polarization. We show that by modulating the parameters of the IR pulse it is possible to control the dipolar coupling between neighboring states and hence the lineshape of the 3s-1 4 p resonance. NSF Grant No. 1607588.

Experiment and simulation of novel liquid crystal plasma mirrors for high contrast, intense laser pulses

PubMed Central

Poole, P. L.; Krygier, A.; Cochran, G. E.; Foster, P. S.; Scott, G. G.; Wilson, L. A.; Bailey, J.; Bourgeois, N.; Hernandez-Gomez, C.; Neely, D.; Rajeev, P. P.; Freeman, R. R.; Schumacher, D. W.

2016-01-01

We describe the first demonstration of plasma mirrors made using freely suspended, ultra-thin films formed dynamically and in-situ. We also present novel particle-in-cell simulations that for the first time incorporate multiphoton ionization and dielectric models that are necessary for describing plasma mirrors. Dielectric plasma mirrors are a crucial component for high intensity laser applications such as ion acceleration and solid target high harmonic generation because they greatly improve pulse contrast. We use the liquid crystal 8CB and introduce an innovative dynamic film formation device that can tune the film thickness so that it acts as its own antireflection coating. Films can be formed at a prolonged, high repetition rate without the need for subsequent realignment. High intensity reflectance above 75% and low-field reflectance below 0.2% are demonstrated, as well as initial ion acceleration experimental results that demonstrate increased ion energy and yield on shots cleaned with these plasma mirrors. PMID:27557592

Electron-hydrogen collisions in a laser field. (Reannouncement with new availability information)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Smith, P.H.; Flannery, M.R.

1991-12-31

The Floquet treatment has already been successfully employed (Chu, Potvliege and Shakeshaft) in calculations of laser-induced multiphoton ionizations, where it provides dressed states for an atom in a laser field. The (perturbative) dressing of target states can have important consequences in laser-assisted scattering was illustrated by Byron and Joachain. These dressed states are useful, not only for laser-induced phenomena, but also as a collisional basis set for laser-assisted collisions. In this role they are in fact very appealing, since the Floquet treatment naturally lends itself to a time-independent analysis, and hence are compatible with present field-free scattering theories. Despite themore » apparent applicability of this approach, work along these lines has only just recently appeared (Sharma and Mohan, Smith and Flannery, Burke et al). Byron and Joachain have illustrated that perturbative dressing of the target states can have important consequences in laser-assisted scattering. Floquet dressing however provides a more complete description (Smith and Flannery).« less

Experiment and simulation of novel liquid crystal plasma mirrors for high contrast, intense laser pulses

DOE PAGES

Poole, P. L.; Krygier, A.; Cochran, G. E.; ...

2016-08-25

Here, we describe the first demonstration of plasma mirrors made using freely suspended, ultra-thin films formed dynamically and in-situ. We also present novel particle-in-cell simulations that for the first time incorporate multiphoton ionization and dielectric models that are necessary for describing plasma mirrors. Dielectric plasma mirrors are a crucial component for high intensity laser applications such as ion acceleration and solid target high harmonic generation because they greatly improve pulse contrast. We use the liquid crystal 8CB and introduce an innovative dynamic film formation device that can tune the film thickness so that it acts as its own antireflection coating.more » Films can be formed at a prolonged, high repetition rate without the need for subsequent realignment. High intensity reflectance above 75% and low-field reflectance below 0.2% are demonstrated, as well as initial ion acceleration experimental results that demonstrate increased ion energy and yield on shots cleaned with these plasma mirrors.« less

Infrared laser dissociation of single megadalton polymer ions in a gated electrostatic ion trap: the added value of statistical analysis of individual events.

PubMed

Halim, Mohammad A; Clavier, Christian; Dagany, Xavier; Kerleroux, Michel; Dugourd, Philippe; Dunbar, Robert C; Antoine, Rodolphe

2018-05-07

In this study, we report the unimolecular dissociation mechanism of megadalton SO 3 -containing poly(2-acrylamido-2-methyl-1-propanesulfonic acid) (PAMPS) polymer cations and anions with the aid of infrared multiphoton dissociation coupled to charge detection ion trap mass spectrometry. A gated electrostatic ion trap ("Benner trap") is used to store and detect single gaseous polymer ions generated by positive and negative polarity in an electrospray ionization source. The trapped ions are then fragmented due to the sequential absorption of multiple infrared photons produced from a continuous-wave CO 2 laser. Several fragmentation pathways having distinct signatures are observed. Highly charged parent ions characteristically adopt a distinctive "stair-case" pattern (assigned to the "fission" process) whereas low charge species take on a "funnel like" shape (assigned to the "evaporation" process). Also, the log-log plot of the dissociation rate constants as a function of laser intensity between PAMPS positive and negative ions is significantly different.

Nonlinear optical effects in semi-polar GaN micro-cavity emitter

NASA Astrophysics Data System (ADS)

Butler, Sween; Jiang, Hongxing; Lin, Jingyu; Neogi, Arup

Nonlinear optical (NLO) response of low dimensional emitters is of current interest because of the need for active elements in photonic applications. NLO effects in a selectively grown array of semi-polar GaN microcavity structures offer a promising route toward devices for integrated optical circuitry in optoelectronics and photonics field. Localized spatial excitation of a single hexagonal GaN microcavity with semipolar facets formed by selective area growth was optimized for nonlinear optical light generation due to second harmonic generation (SHG) and multi-photon luminescence(MPL). Multi-photon transition induced by tightly focused femtosecond NIR incident field results in ultra-violet and yellow luminescence for excitations above and below half bandgap energy, whereas SHG was observed for below half bandgap energy. We show that color and coherence of the light generation from the emitter can be controlled by selective onset of the nonlinear process which depends not only on the incident laser energy and intensity but also on the geometry of the microcavity. Quasi-WGM like modes were observed for off-resonant excitations from the GaN microcavity resulting in enhanced SHG. The directionality of MPL and SHG will be presented as a function of the pump polarization.

Generation of mechanical interference fringes by multi-photon counting

NASA Astrophysics Data System (ADS)

Ringbauer, M.; Weinhold, T. J.; Howard, L. A.; White, A. G.; Vanner, M. R.

2018-05-01

Exploring the quantum behaviour of macroscopic objects provides an intriguing avenue to study the foundations of physics and to develop a suite of quantum-enhanced technologies. One prominent path of study is provided by quantum optomechanics which utilizes the tools of quantum optics to control the motion of macroscopic mechanical resonators. Despite excellent recent progress, the preparation of mechanical quantum superposition states remains outstanding due to weak coupling and thermal decoherence. Here we present a novel optomechanical scheme that significantly relaxes these requirements allowing the preparation of quantum superposition states of motion of a mechanical resonator by exploiting the nonlinearity of multi-photon quantum measurements. Our method is capable of generating non-classical mechanical states without the need for strong single-photon coupling, is resilient against optical loss, and offers more favourable scaling against initial mechanical thermal occupation than existing schemes. Moreover, our approach allows the generation of larger superposition states by projecting the optical field onto NOON states. We experimentally demonstrate this multi-photon-counting technique on a mechanical thermal state in the classical limit and observe interference fringes in the mechanical position distribution that show phase super-resolution. This opens a feasible route to explore and exploit quantum phenomena at a macroscopic scale.

Peptides Labeled with Pyridinium Salts for Sensitive Detection and Sequencing by Electrospray Tandem Mass Spectrometry

NASA Astrophysics Data System (ADS)

Waliczek, Mateusz; Kijewska, Monika; Rudowska, Magdalena; Setner, Bartosz; Stefanowicz, Piotr; Szewczuk, Zbigniew

2016-11-01

Mass spectrometric analysis of trace amounts of peptides may be problematic due to the insufficient ionization efficiency resulting in limited sensitivity. One of the possible ways to overcome this problem is the application of ionization enhancers. Herein we developed new ionization markers based on 2,4,6-triphenylpyridinium and 2,4,6-trimethylpyridinium salts. Using of inexpensive and commercially available pyrylium salt allows selective derivatization of primary amino groups, especially those sterically unhindered, such as ɛ-amino group of lysine. The 2,4,6-triphenylpyridinium modified peptides generate in MS/MS experiments an abundant protonated 2,4,6-triphenylpyridinium ion. This fragment is a promising reporter ion for the multiple reactions monitoring (MRM) analysis. In addition, the fixed positive charge of the pyridinium group enhances the ionization efficiency. Other advantages of the proposed ionization enhancers are the simplicity of derivatization of peptides and the possibility of convenient incorporation of isotopic labels into derivatized peptides.

Tunable multiphoton Rabi oscillations in an electronic spin system

NASA Astrophysics Data System (ADS)

Bertaina, S.; Groll, N.; Chen, L.; Chiorescu, I.

2011-10-01

We report on multiphoton Rabi oscillations and controlled tuning of a multilevel system at room temperature (S=5/2 for Mn2+:MgO) in and out of a quasiharmonic level configuration. The anisotropy is much smaller than the Zeeman splittings, e.g., the six-level scheme shows only a small deviation from an equidistant diagram. This allows us to tune the spin dynamics by compensating for the cubic anisotropy with either a precise static-field orientation or a microwave field intensity. Using the rotating-frame approximation, the experiments are explained very well by both an analytical model and a generalized numerical model. The calculated multiphoton Rabi frequencies are in excellent agreement with the experimental data.

Moxifloxacin: Clinically compatible contrast agent for multiphoton imaging

NASA Astrophysics Data System (ADS)

Wang, Taejun; Jang, Won Hyuk; Lee, Seunghun; Yoon, Calvin J.; Lee, Jun Ho; Kim, Bumju; Hwang, Sekyu; Hong, Chun-Pyo; Yoon, Yeoreum; Lee, Gilgu; Le, Viet-Hoan; Bok, Seoyeon; Ahn, G.-One; Lee, Jaewook; Gho, Yong Song; Chung, Euiheon; Kim, Sungjee; Jang, Myoung Ho; Myung, Seung-Jae; Kim, Myoung Joon; So, Peter T. C.; Kim, Ki Hean

2016-06-01

Multiphoton microscopy (MPM) is a nonlinear fluorescence microscopic technique widely used for cellular imaging of thick tissues and live animals in biological studies. However, MPM application to human tissues is limited by weak endogenous fluorescence in tissue and cytotoxicity of exogenous probes. Herein, we describe the applications of moxifloxacin, an FDA-approved antibiotic, as a cell-labeling agent for MPM. Moxifloxacin has bright intrinsic multiphoton fluorescence, good tissue penetration and high intracellular concentration. MPM with moxifloxacin was demonstrated in various cell lines, and animal tissues of cornea, skin, small intestine and bladder. Clinical application is promising since imaging based on moxifloxacin labeling could be 10 times faster than imaging based on endogenous fluorescence.

Applications of multiphoton microscopy in the field of colorectal cancer

NASA Astrophysics Data System (ADS)

Wang, Shu; Li, Lianhuang; Zhu, Xiaoqin; Zheng, Liqin; Zhuo, Shuangmu; Chen, Jianxin

2018-06-01

Multiphoton microscopy (MPM) is a powerful tool for visualizing cellular and subcellular details within living tissue by its unique advantages of being label-free, its intrinsic optical sectioning ability, near-infrared excitation for deep penetration depth into tissue, reduced photobleaching and phototoxicity in the out-of-focus regions, and being capable of providing quantitative information. In this review, we focus on applications of MPM in the field of colorectal cancer, including monitoring cancer progression, detecting tumor metastasis and microenvironment, evaluating the cancer therapy response, and visualizing and ablating pre-invasive cancer cells. We also present one of the major challenges and the future research direction to exploit a colorectal multiphoton endoscope.

Ionizing Radiation Changes the Electronic Properties of Melanin and Enhances the Growth of Melanized Fungi

PubMed Central

Dadachova, Ekaterina; Bryan, Ruth A.; Huang, Xianchun; Moadel, Tiffany; Schweitzer, Andrew D.; Aisen, Philip; Nosanchuk, Joshua D.; Casadevall, Arturo

2007-01-01

Background Melanin pigments are ubiquitous in nature. Melanized microorganisms are often the dominating species in certain extreme environments, such as soils contaminated with radionuclides, suggesting that the presence of melanin is beneficial in their life cycle. We hypothesized that ionizing radiation could change the electronic properties of melanin and might enhance the growth of melanized microorganisms. Methodology/Principal Findings Ionizing irradiation changed the electron spin resonance (ESR) signal of melanin, consistent with changes in electronic structure. Irradiated melanin manifested a 4-fold increase in its capacity to reduce NADH relative to non-irradiated melanin. HPLC analysis of melanin from fungi grown on different substrates revealed chemical complexity, dependence of melanin composition on the growth substrate and possible influence of melanin composition on its interaction with ionizing radiation. XTT/MTT assays showed increased metabolic activity of melanized C. neoformans cells relative to non-melanized cells, and exposure to ionizing radiation enhanced the electron-transfer properties of melanin in melanized cells. Melanized Wangiella dermatitidis and Cryptococcus neoformans cells exposed to ionizing radiation approximately 500 times higher than background grew significantly faster as indicated by higher CFUs, more dry weight biomass and 3-fold greater incorporation of 14C-acetate than non-irradiated melanized cells or irradiated albino mutants. In addition, radiation enhanced the growth of melanized Cladosporium sphaerospermum cells under limited nutrients conditions. Conclusions/Significance Exposure of melanin to ionizing radiation, and possibly other forms of electromagnetic radiation, changes its electronic properties. Melanized fungal cells manifested increased growth relative to non-melanized cells after exposure to ionizing radiation, raising intriguing questions about a potential role for melanin in energy capture and utilization. PMID:17520016

Enhanced one-photon double ionization of atoms and molecules in an environment of different species.

PubMed

Stumpf, V; Kryzhevoi, N V; Gokhberg, K; Cederbaum, L S

2014-05-16

The correlated nature of electronic states in atoms and molecules is manifested in the simultaneous emission of two electrons after absorption of a single photon close to the respective threshold. Numerous observations in atoms and small molecules demonstrate that the double ionization efficiency close to threshold is rather small. In this Letter we show that this efficiency can be dramatically enhanced in the environment. To be specific, we concentrate on the case where the species in question has one or several He atoms as neighbors. The enhancement is achieved by an indirect process, where a He atom of the environment absorbs a photon and the resulting He(+) cation is neutralized fast by a process known as electron transfer mediated decay, producing thereby doubly ionized species. The enhancement of the double ionization is demonstrated in detail for the example of the Mg · He cluster. We show that the double ionization cross section of Mg becomes 3 orders of magnitude larger than the respective cross section of the isolated Mg atom. The impact of more neighbors is discussed and the extension to other species and environments is addressed.

The Multiphoton Interaction of Lambda Model Atom and Two-Mode Fields

NASA Technical Reports Server (NTRS)

Liu, Tang-Kun

1996-01-01

The system of two-mode fields interacting with atom by means of multiphotons is addressed, and the non-classical statistic quality of two-mode fields with interaction is discussed. Through mathematical calculation, some new rules of non-classical effects of two-mode fields which evolue with time, are established.

USE OF MULTIPHOTON LASER SCANNING MICROSCOPY TO IMAGE BENZO[A]PYRENE AND METABOLITES IN FISH EARLY LIFE STAGES

EPA Science Inventory

Multiphoton laser scanning micrsocopy holds promise as a tool to study the tissue distribution of environmental chemical contaminants during fish early life stage development. One such chemical for which this is possible is benzo[a]pyrene (BaP), a polyaromatic hydrocarbon that a...

Multi-Photon Absorption Spectra: A Comparison Between Transmittance Change and Fluorescence Methods

DTIC Science & Technology

2015-05-21

AFRL-OSR-VA-TR-2015-0134 multi-photon absorption spectra Cleber Mendonca INSTITUTO DE FISICA DE SAO CARLOS Final Report 05/21/2015 DISTRIBUTION A...5f. WORK UNIT NUMBER 7. PERFORMING ORGANIZATION NAME(S) AND ADDRESS(ES) Instituto de Fisica de Sao Carlos - Universidade de Sao Paulo Av

Real-time digital signal processing in multiphoton and time-resolved microscopy

NASA Astrophysics Data System (ADS)

Wilson, Jesse W.; Warren, Warren S.; Fischer, Martin C.

2016-03-01

The use of multiphoton interactions in biological tissue for imaging contrast requires highly sensitive optical measurements. These often involve signal processing and filtering steps between the photodetector and the data acquisition device, such as photon counting and lock-in amplification. These steps can be implemented as real-time digital signal processing (DSP) elements on field-programmable gate array (FPGA) devices, an approach that affords much greater flexibility than commercial photon counting or lock-in devices. We will present progress toward developing two new FPGA-based DSP devices for multiphoton and time-resolved microscopy applications. The first is a high-speed multiharmonic lock-in amplifier for transient absorption microscopy, which is being developed for real-time analysis of the intensity-dependence of melanin, with applications in vivo and ex vivo (noninvasive histopathology of melanoma and pigmented lesions). The second device is a kHz lock-in amplifier running on a low cost (50-200) development platform. It is our hope that these FPGA-based DSP devices will enable new, high-speed, low-cost applications in multiphoton and time-resolved microscopy.

Direct comparison between confocal and multiphoton microscopy for rapid histopathological evaluation of unfixed human breast tissue.

PubMed

Yoshitake, Tadayuki; Giacomelli, Michael G; Cahill, Lucas C; Schmolze, Daniel B; Vardeh, Hilde; Faulkner-Jones, Beverly E; Connolly, James L; Fujimoto, James G

2016-12-01

Rapid histopathological examination of surgical specimen margins using fluorescence microscopy during breast conservation therapy has the potential to reduce the rate of positive margins on postoperative histopathology and the need for repeat surgeries. To assess the suitability of imaging modalities, we perform a direct comparison between confocal fluorescence microscopy and multiphoton microscopy for imaging unfixed tissue and compare to paraffin-embedded histology. An imaging protocol including dual channel detection of two contrast agents to implement virtual hematoxylin and eosin images is introduced that provides high quality imaging under both one and two photon excitation. Corresponding images of unfixed human breast tissue show that both confocal and multiphoton microscopy can reproduce the appearance of conventional histology without the need for physical sectioning. We further compare normal breast tissue and invasive cancer specimens imaged at multiple magnifications, and assess the effects of photobleaching for both modalities using the staining protocol. The results demonstrate that confocal fluorescence microscopy is a promising and cost-effective alternative to multiphoton microscopy for rapid histopathological evaluation of ex vivo breast tissue.

Direct comparison between confocal and multiphoton microscopy for rapid histopathological evaluation of unfixed human breast tissue

PubMed Central

Yoshitake, Tadayuki; Giacomelli, Michael G.; Cahill, Lucas C.; Schmolze, Daniel B.; Vardeh, Hilde; Faulkner-Jones, Beverly E.; Connolly, James L.; Fujimoto, James G.

2016-01-01

Abstract. Rapid histopathological examination of surgical specimen margins using fluorescence microscopy during breast conservation therapy has the potential to reduce the rate of positive margins on postoperative histopathology and the need for repeat surgeries. To assess the suitability of imaging modalities, we perform a direct comparison between confocal fluorescence microscopy and multiphoton microscopy for imaging unfixed tissue and compare to paraffin-embedded histology. An imaging protocol including dual channel detection of two contrast agents to implement virtual hematoxylin and eosin images is introduced that provides high quality imaging under both one and two photon excitation. Corresponding images of unfixed human breast tissue show that both confocal and multiphoton microscopy can reproduce the appearance of conventional histology without the need for physical sectioning. We further compare normal breast tissue and invasive cancer specimens imaged at multiple magnifications, and assess the effects of photobleaching for both modalities using the staining protocol. The results demonstrate that confocal fluorescence microscopy is a promising and cost-effective alternative to multiphoton microscopy for rapid histopathological evaluation of ex vivo breast tissue. PMID:28032121

Multi-photon excited luminescence of magnetic FePt core-shell nanoparticles.

PubMed

Seemann, K M; Kuhn, B

2014-07-01

We present magnetic FePt nanoparticles with a hydrophilic, inert, and biocompatible silico-tungsten oxide shell. The particles can be functionalized, optically detected, and optically manipulated. To show the functionalization the fluorescent dye NOPS was bound to the FePt core-shell nanoparticles with propyl-triethoxy-silane linkers and fluorescence of the labeled particles were observed in ethanol (EtOH). In aqueous dispersion the NOPS fluorescence is quenched making them invisible using 1-photon excitation. However, we observe bright luminescence of labeled and even unlabeled magnetic core-shell nanoparticles with multi-photon excitation. Luminescence can be detected in the near ultraviolet and the full visible spectral range by near infrared multi-photon excitation. For optical manipulation, we were able to drag clusters of particles, and maybe also single particles, by a focused laser beam that acts as optical tweezers by inducing an electric dipole in the insulated metal nanoparticles. In a first application, we show that the luminescence of the core-shell nanoparticles is bright enough for in vivo multi-photon imaging in the mouse neocortex down to cortical layer 5.

Ultralow-threshold multiphoton-pumped lasing from colloidal nanoplatelets in solution

PubMed Central

Li, Mingjie; Zhi, Min; Zhu, Hai; Wu, Wen-Ya; Xu, Qing-Hua; Jhon, Mark Hyunpong; Chan, Yinthai

2015-01-01

Although multiphoton-pumped lasing from a solution of chromophores is important in the emerging fields of nonlinear optofluidics and bio-photonics, conventionally used organic dyes are often rendered unsuitable because of relatively small multiphoton absorption cross-sections and low photostability. Here, we demonstrate highly photostable, ultralow-threshold multiphoton-pumped biexcitonic lasing from a solution of colloidal CdSe/CdS nanoplatelets within a cuvette-based Fabry–Pérot optical resonator. We find that colloidal nanoplatelets surprisingly exhibit an optimal lateral size that minimizes lasing threshold. These nanoplatelets possess very large gain cross-sections of 7.3 × 10−14 cm2 and ultralow lasing thresholds of 1.2 and 4.3 mJ cm−2 under two-photon (λexc=800 nm) and three-photon (λexc=1.3 μm) excitation, respectively. The highly polarized emission from the nanoplatelet laser shows no significant photodegradation over 107 laser shots. These findings constitute a more comprehensive understanding of the utility of colloidal semiconductor nanoparticles as the gain medium in high-performance frequency-upconversion liquid lasers. PMID:26419950

Direct comparison between confocal and multiphoton microscopy for rapid histopathological evaluation of unfixed human breast tissue

NASA Astrophysics Data System (ADS)

Yoshitake, Tadayuki; Giacomelli, Michael G.; Cahill, Lucas C.; Schmolze, Daniel B.; Vardeh, Hilde; Faulkner-Jones, Beverly E.; Connolly, James L.; Fujimoto, James G.

2016-12-01

Rapid histopathological examination of surgical specimen margins using fluorescence microscopy during breast conservation therapy has the potential to reduce the rate of positive margins on postoperative histopathology and the need for repeat surgeries. To assess the suitability of imaging modalities, we perform a direct comparison between confocal fluorescence microscopy and multiphoton microscopy for imaging unfixed tissue and compare to paraffin-embedded histology. An imaging protocol including dual channel detection of two contrast agents to implement virtual hematoxylin and eosin images is introduced that provides high quality imaging under both one and two photon excitation. Corresponding images of unfixed human breast tissue show that both confocal and multiphoton microscopy can reproduce the appearance of conventional histology without the need for physical sectioning. We further compare normal breast tissue and invasive cancer specimens imaged at multiple magnifications, and assess the effects of photobleaching for both modalities using the staining protocol. The results demonstrate that confocal fluorescence microscopy is a promising and cost-effective alternative to multiphoton microscopy for rapid histopathological evaluation of ex vivo breast tissue.

Comparison of higher-order multiphoton signal generation and collection at the 1700-nm window based on transmittance measurement of objective lenses.

PubMed

Wen, Wenhui; Wang, Yuxin; Liu, Hongji; Wang, Kai; Qiu, Ping; Wang, Ke

2018-01-01

One benefit of excitation at the 1700-nm window is the more accessible modalities of multiphoton signal generation. It is demonstrated here that the transmittance performance of the objective lens is of vital importance for efficient higher-order multiphoton signal generation and collection excited at the 1700-nm window. Two commonly used objective lenses for multiphoton microscopy (MPM) are characterized and compared, one with regular coating and the other with customized coating for high transmittance at the 1700-nm window. Our results show that, fourth harmonic generation imaging of mouse tail tendon and 5-photon fluorescence of carbon quantum dots using the regular objective lens shows an order of magnitude signal higher than those using the customized objective lens. Besides, the regular objective lens also enables a 3-photon fluorescence imaging depth of >1600 μm in mouse brain in vivo. Our results will provide guidelines for objective lens selection for MPM at the 1700-nm window. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Equatorial ion composition, 140-200 km, based on Atmosphere Explorer E data

NASA Technical Reports Server (NTRS)

Miller, N. J.; Grebowsky, J. M.; Hedin, A. E.; Spencer, N. W.

1993-01-01

We have used in situ measurements of ion composition and horizontal winds, taken from equatorial orbiting Atmosphere Explorer E in eccentric orbit during 1975-1976 to investigate the bottomside ionosphere at altitudes 140-200 km. Representative daytime altitude profiles of ionization were stable against wide variations in horizontal wind patterns. Special features that sometimes appeared in the structured nightside ionization were apparent ion composition waves, intermediate layers of enhanced ionization, and ionization depletions similar to equatorial ionization bubbles. Apparent ion composition waves displayed a horizontal wave length of about 650 km. Enhanced layers of ionization appeared to be newly separated from the bottomside midnight F layer; its ions were primarily NO(+) and O2(+) without significant densities of metallic ions, an indication that metallic ions are not required to produce the layers at altitudes above 140 km. Equatorial ionization depletions were observed at lower altitudes than previously reported and displayed molecular ion depletions as well as O(+) depletions.

Raman Microscopy: A Noninvasive Method to Visualize the Localizations of Biomolecules in the Cornea.

PubMed

Kaji, Yuichi; Akiyama, Toshihiro; Segawa, Hiroki; Oshika, Tetsuro; Kano, Hideaki

2017-11-01

In vivo and in situ visualization of biomolecules without pretreatment will be important for diagnosis and treatment of ocular disorders in the future. Recently, multiphoton microscopy, based on the nonlinear interactions between molecules and photons, has been applied to reveal the localizations of various molecules in tissues. We aimed to use multimodal multiphoton microscopy to visualize the localizations of specific biomolecules in rat corneas. Multiphoton images of the corneas were obtained from nonlinear signals of coherent anti-Stokes Raman scattering, third-order sum frequency generation, and second-harmonic generation. The localizations of the adhesion complex-containing basement membrane and Bowman layer were clearly visible in the third-order sum frequency generation images. The fine structure of type I collagen was observed in the corneal stroma in the second-harmonic generation images. The localizations of lipids, proteins, and nucleic acids (DNA/RNA) was obtained in the coherent anti-Stokes Raman scattering images. Imaging technologies have progressed significantly and been applied in medical fields. Optical coherence tomography and confocal microscopy are widely used but do not provide information on the molecular structure of the cornea. By contrast, multiphoton microscopy provides information on the molecular structure of living tissues. Using this technique, we successfully visualized the localizations of various biomolecules including lipids, proteins, and nucleic acids in the cornea. We speculate that multiphoton microscopy will provide essential information on the physiological and pathological conditions of the cornea, as well as molecular localizations in tissues without pretreatment.

Multi-photon transitions and Rabi resonance in continuous wave EPR.

PubMed

Saiko, Alexander P; Fedaruk, Ryhor; Markevich, Siarhei A

2015-10-01

The study of microwave-radiofrequency multi-photon transitions in continuous wave (CW) EPR spectroscopy is extended to a Rabi resonance condition, when the radio frequency of the magnetic-field modulation matches the Rabi frequency of a spin system in the microwave field. Using the non-secular perturbation theory based on the Bogoliubov averaging method, the analytical description of the response of the spin system is derived for all modulation frequency harmonics. When the modulation frequency exceeds the EPR linewidth, multi-photon transitions result in sidebands in absorption EPR spectra measured with phase-sensitive detection at any harmonic. The saturation of different-order multi-photon transitions is shown to be significantly different and to be sensitive to the Rabi resonance. The noticeable frequency shifts of sidebands are found to be the signatures of this resonance. The inversion of two-photon lines in some spectral intervals of the out-of-phase first-harmonic signal is predicted under passage through the Rabi resonance. The inversion indicates the transition from absorption to stimulated emission or vice versa, depending on the sideband. The manifestation of the primary and secondary Rabi resonance is also demonstrated in the time evolution of steady-state EPR signals formed by all harmonics of the modulation frequency. Our results provide a theoretical framework for future developments in multi-photon CW EPR spectroscopy, which can be useful for samples with long spin relaxation times and extremely narrow EPR lines. Copyright © 2015 Elsevier Inc. All rights reserved.

Multiphoton fluorescence lifetime imaging of chemotherapy distribution in solid tumors

NASA Astrophysics Data System (ADS)

Carlson, Marjorie; Watson, Adrienne L.; Anderson, Leah; Largaespada, David A.; Provenzano, Paolo P.

2017-11-01

Doxorubicin is a commonly used chemotherapeutic employed to treat multiple human cancers, including numerous sarcomas and carcinomas. Furthermore, doxorubicin possesses strong fluorescent properties that make it an ideal reagent for modeling drug delivery by examining its distribution in cells and tissues. However, while doxorubicin fluorescence and lifetime have been imaged in live tissue, its behavior in archival samples that frequently result from drug and treatment studies in human and animal patients, and murine models of human cancer, has to date been largely unexplored. Here, we demonstrate imaging of doxorubicin intensity and lifetimes in archival formalin-fixed paraffin-embedded sections from mouse models of human cancer with multiphoton excitation and multiphoton fluorescence lifetime imaging microscopy (FLIM). Multiphoton excitation imaging reveals robust doxorubicin emission in tissue sections and captures spatial heterogeneity in cells and tissues. However, quantifying the amount of doxorubicin signal in distinct cell compartments, particularly the nucleus, often remains challenging due to strong signals in multiple compartments. The addition of FLIM analysis to display the spatial distribution of excited state lifetimes clearly distinguishes between signals in distinct compartments such as the cell nuclei versus cytoplasm and allows for quantification of doxorubicin signal in each compartment. Furthermore, we observed a shift in lifetime values in the nuclei of transformed cells versus nontransformed cells, suggesting a possible diagnostic role for doxorubicin lifetime imaging to distinguish normal versus transformed cells. Thus, data here demonstrate that multiphoton FLIM is a highly sensitive platform for imaging doxorubicin distribution in normal and diseased archival tissues.

Intravital multiphoton fluorescence imaging and optical manipulation of spinal cord in mice, using a compact fiber laser system.

PubMed

Oshima, Yusuke; Horiuch, Hideki; Honkura, Naoki; Hikita, Atsuhiko; Ogata, Tadanori; Miura, Hiromasa; Imamura, Takeshi

2014-09-01

Near-infrared ultrafast lasers are widely used for multiphoton excited fluorescence microscopy in living animals. Ti:Sapphire lasers are typically used for multiphoton excitation, but their emission wavelength is restricted below 1,000 nm. The aim of this study is to evaluate the performance of a compact Ytterbium-(Yb-) fiber laser at 1,045 nm for multiphoton excited fluorescence microscopy in spinal cord injury. In this study, we employed a custom-designed microscopy system with a compact Yb-fiber laser and evaluated the performance of this system in in vivo imaging of brain cortex and spinal cord in YFP-H transgenic mice. For in vivo imaging of brain cortex, sharp images of basal dendrites, and pyramidal cells expressing EYFP were successfully captured using the Yb-fiber laser in our microscopy system. We also performed in vivo imaging of axon fibers of spinal cord in the transgenic mice. The obtained images were almost as sharp as those obtained using a conventional ultrafast laser system. In addition, laser ablation and multi-color imaging could be performed simultaneously using the Yb-fiber laser. The high-peak pulse Yb-fiber laser is potentially useful for multimodal bioimaging methods based on a multiphoton excited fluorescence microscopy system that incorporates laser ablation techniques. Our results suggest that microscopy systems of this type could be utilized in studies of neuroscience and clinical use in diagnostics and therapeutic tool for spinal cord injury in the future. © 2014 Wiley Periodicals, Inc.

Improvement of depth resolution on photoacoustic imaging using multiphoton absorption

NASA Astrophysics Data System (ADS)

Yamaoka, Yoshihisa; Fujiwara, Katsuji; Takamatsu, Tetsuro

2007-07-01

Commercial imaging systems, such as computed tomography and magnetic resonance imaging, are frequently used powerful tools for observing structures deep within the human body. However, they cannot precisely visualized several-tens micrometer-sized structures for lack of spatial resolution. In this presentation, we propose photoacoustic imaging using multiphoton absorption technique to generate ultrasonic waves as a means of improving depth resolution. Since the multiphoton absorption occurs at only the focus point and the employed infrared pulses deeply penetrate living tissues, it enables us to extract characteristic features of structures embedded in the living tissue. When nanosecond pulses from a 1064-nm Nd:YAG laser were focused on Rhodamine B/chloroform solution (absorption peak: 540 nm), the peak intensity of the generated photoacoustic signal was proportional to the square of the input pulse energy. This result shows that the photoacoustic signals can be induced by the two-photon absorption of infrared nanosecond pulse laser and also can be detected by a commercial low-frequency MHz transducer. Furthermore, in order to evaluate the depth resolution of multiphoton-photoacoustic imaging, we investigated the dependence of photoacoustic signal on depth position using a 1-mm-thick phantom in a water bath. We found that the depth resolution of two-photon photoacoustic imaging (1064 nm) is greater than that of one-photon photoacoustic imaging (532 nm). We conclude that evolving multiphoton-photoacoustic imaging technology renders feasible the investigation of biomedical phenomena at the deep layer in living tissue.

Clinical multiphoton FLIM tomography

NASA Astrophysics Data System (ADS)

König, Karsten

2012-03-01

This paper gives an overview on current clinical high resolution multiphoton fluorescence lifetime imaging in volunteers and patients. Fluorescence lifetime imaging (FLIM) in Life Sciences was introduced in Jena/Germany in 1988/89 based on a ZEISS confocal picosecond dye laser scanning microscope equipped with a single photon counting unit. The porphyrin distribution in living cells and living tumor-bearing mice was studied with high spatial, temporal, and spectral resolution. Ten years later, time-gated cameras were employed to detect dental caries in volunteers based on one-photon excitation of autofluorescent bacteria with long fluorescence lifetimes. Nowadays, one-photon FLIM based on picosecond VIS laser diodes are used to study ocular diseases in humans. Already one decade ago, first clinical twophoton FLIM images in humans were taken with the certified clinical multiphoton femtosecond laser tomograph DermaInspectTM. Multiphoton tomographs with FLIM modules are now operating in hospitals at Brisbane, Tokyo, Berlin, Paris, London, Modena and other European cities. Multiple FLIM detectors allow spectral FLIM with a temporal resolution down to 20 ps (MCP) / 250 ps (PMT) and a spectral resolution of 10 nm. Major FLIM applications include the detection of intradermal sunscreen and tattoo nanoparticles, the detection of different melanin types, the early diagnosis of dermatitis and malignant melanoma, as well as the measurement of therapeutic effects in pateints suffering from dermatitis. So far, more than 1,000 patients and volunteers have been investigated with the clinical multiphoton FLIM tomographs DermaInspectTM and MPTflexTM.

Particle in cell simulation on plasma grating contrast enhancement induced by infrared laser pulse

NASA Astrophysics Data System (ADS)

Li, M.; Yuan, T.; Xu, Y. X.; Wang, J. X.; Luo, S. N.

2018-05-01

The dynamics of plasma grating contrast enhancement (PGCE) irradiated by an infrared laser pulse is investigated with one dimensional particle-in-cell simulation where field ionization and impact ionization are simultaneously considered for the first time. The numeric results show that the impact ionization dominates the PGCE process. Upon the interaction with the laser pulse, abundant free electrons are efficiently accelerated and subsequently triggered massive impact ionizations in the density ridges of the plasma grating for the higher local plasma energy density, which efficiently enhances the grating contrast. Besides the dynamic analysis of PGCE, we explore the parameter space of the incident infrared laser pulse to optimize the PGCE effect, which can provide useful guidance to experiments related to laser-plasma-grating interactions and may find applications in prolonging the duration of the plasma grating.

Investigation of ionized metal flux in enhanced high power impulse magnetron sputtering discharges

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stranak, Vitezslav, E-mail: stranak@prf.jcu.cz; Hubicka, Zdenek; Cada, Martin

2014-04-21

The metal ionized flux fraction and production of double charged metal ions Me{sup 2+} of different materials (Al, Cu, Fe, Ti) by High Power Impulse Magnetron Sputtering (HiPIMS) operated with and without a pre-ionization assistance is compared in the paper. The Electron Cyclotron Wave Resonance (ECWR) discharge was employed as the pre-ionization agent providing a seed of charge in the idle time of HiPIMS pulses. A modified grid-free biased quartz crystal microbalance was used to estimate the metal ionized flux fraction ξ. The energy-resolved mass spectrometry served as a complementary method to distinguish particular ion contributions to the total ionizedmore » flux onto the substrate. The ratio between densities of doubly Me{sup 2+} and singly Me{sup +} charged metal ions was determined. It is shown that ECWR assistance enhances Me{sup 2+} production with respect of absorbed rf-power. The ECWR discharge also increases the metal ionized flux fraction of about 30% especially in the region of lower pressures. Further, the suppression of the gas rarefaction effect due to enhanced secondary electron emission of Me{sup 2+} was observed.« less

Lanthanide heterometallic terephthalates: Concentration quenching and the principles of the "multiphotonic emission"

NASA Astrophysics Data System (ADS)

Utochnikova, V. V.; Grishko, A. Yu.; Koshelev, D. S.; Averin, A. A.; Lepnev, L. S.; Kuzmina, N. P.

2017-12-01

The principles of the "multiphotonic emission", i.e. multiple emission from one lanthanide ion, in heterometallic lanthanide terephthalates were determined. Thanks to it, another system with the same effect, namely EuxY1-x(dbm)3(Phen) (Hdbm - dibenzoylmethanate, Phen - o-phenanthroline (mistape)) was found. The criteria for concentration quenching appearance were formulated and demonstrated.

Limits to Sensitivity in Laser Enhanced Ionization.

ERIC Educational Resources Information Center

Travis, J. C.

1982-01-01

Laser enhanced ionization (LEI) occurs when a tunable dye laser is used to excite a specific atomic population in a flame. Explores the origin of LEI's high sensitivity and identifies possible avenues to higher sensitivity by describing instrument used and experimental procedures and discussing ion formation/detection. (Author/JN)

Modeling extracellular matrix (ECM) alterations in ovarian cancer by multiphoton excited fabrication of stromal models (Conference Presentation)

NASA Astrophysics Data System (ADS)

Campagnola, Paul J.; Ajeti, Visar; Lara, Jorge; Eliceiri, Kevin W.; Patankar, Mansh

2016-04-01

A profound remodeling of the extracellular matrix (ECM) occurs in human ovarian cancer but it unknown how this affects tumor growth, where this understanding could lead to better diagnostics and therapeutic approaches. We investigate the role of these ECM alterations by using multiphoton excited (MPE) polymerization to fabricate biomimetic models to investigate operative cell-matrix interactions in invasion/metastasis. First, we create nano/microstructured gradients mimicking the basal lamina to study adhesion/migration dynamics of ovarian cancer cells of differing metastatic potential. We find a strong haptotactic response that depends on both contact guidance and ECM binding cues. While we found enhanced migration for more invasive cells, the specifics of alignment and directed migration also depend on cell polarity. We further use MPE fabrication to create collagen scaffolds with complex, 3D submicron morphology. The stromal scaffold designs are derived directly from "blueprints" based on SHG images of normal, high risk, and malignant ovarian tissues. The models are seeded with different cancer cell lines and this allows decoupling of the roles of cell characteristics (metastatic potential) and ECM structure and composition (normal vs cancer) on adhesion/migration dynamics. We found the malignant stroma structure promotes enhanced migration and proliferation and also cytoskeletal alignment. Creating synthetic models based on fibers patterns further allows decoupling the topographic roles of the fibers themselves vs their alignment within the tissue. These models cannot be synthesized by other conventional fabrication methods and we suggest the MPE image-based fabrication method will enable a variety of studies in cancer biology.

High-Energy Laser Interaction with Gases, Droplets, and Bulk Liquids.

NASA Astrophysics Data System (ADS)

Jarzembski, Maurice Anthony

Breakdown threshold intensities (I_ {rm TH}) were measured as functions of wavelengths and pressure for air, He, Ar, and Xe using a Nd:YAG pulsed laser. Multiphoton absorption dominates in the UV and cascade collision ionization dominates in the IR; however, both can be affected by other electron gain and loss processes. Presence of droplets lowers breakdown of gases due to field enhancements. Breakdown is initiated either in the droplet material or in the gas. At lambda = 0.532mum for a 50 μm dia. water droplet in He, Ar, and air for p < 800 Torr, breakdown occurs inside the droplet and is independent of gas pressure. For droplet -in-Xe, at p < 140 Torr breakdown occurs inside the droplet and is independent of gas pressure. For droplet-in-Xe, at p < 140 Torr breakdown occurs inside the droplet but at p > 140 Torr, breakdown occurs outside the droplet and is dependent on gas pressure. Pressure dependence of breakdown was observed for 120mum dia. water droplets in Ar at p > 400 Torr. The required intensity for breakdown of droplet depends on I_{ rm TH} of bulk liquid and the effective field enhancement created by the droplet. The I _{rm TH} of droplet-in-air provides an upper limit to the propagation of a high energy laser beam in the atmosphere containing particles. By geometrical optics approach, a significant field enhancement located at the critical ring region, encircling the axis of the sphere in the forward direction at angle theta_{c}, was discovered where nonlinear processes can occur. This was confirmed experimentally and by Mie theory. Field enhancements calculated at the critical ring for water droplets of different sizes agree well with measurements. For a droplet of given size and real refractive index, the effective field enhancement and the volume over which it occurs are two important factors governing the occurrence of breakdown in droplets for both off resonance and on resonance conditions. Measurements of wavelength dependence of breakdown showed that in the UV, I_{rm TH} for droplets and bulk liquids were comparable and lower by few orders of magnitude from that of air. Transmittance and reflectance of bulk liquids in the UV change with intensity implying absorption due to nonlinear processes and consequent increase in the imaginary part of the refractive index of the liquids. In the IR, I_{rm TH} of air and bulk liquids are comparable but for droplets are considerably lower due to field enhancement.

Investigation of angiogenesis in bioactive 3-dimensional poly(d,l-lactide-co-glycolide)/nano-hydroxyapatite scaffolds by in vivo multiphoton microscopy in murine calvarial critical bone defect.

PubMed

Li, Jian; Xu, Qiang; Teng, Bin; Yu, Chen; Li, Jian; Song, Liang; Lai, Yu-Xiao; Zhang, Jian; Zheng, Wei; Ren, Pei-Gen

2016-09-15

Reconstruction of critical size bone defects remains a major clinical challenge because of poor bone regeneration, which is usually due to poor angiogenesis during repair. Satisfactory vascularization is a prerequisite for the survival of grafts and the integration of new tissue with existing tissue. In this work, we investigated angiogenesis in 3D scaffolds by in vivo multiphoton microscopy during bone formation in a murine calvarial critical bone defect model and evaluated bone regeneration 8weeks post-implantation. The continuous release of bioactive lentiviral vectors (LV-pdgfb) from the scaffolds could be detected for 5days in vitro. In vivo, the released LV-pdgfb transfected adjacent cells and expressed PDGF-BB, facilitating angiogenesis and enhancing bone regeneration. The expression of both pdgfb and the angiogenesis-related genes vWF and VEGFR2 was significantly increased in the pdgfb gene-carrying scaffold (PHp) group. In addition, microCT scanning and histomorphology results proved that there was more new bone ingrowth in the PHp group than in the PLGA/nHA (PH) and control groups. MicroCT parameters, including BMD, BV/TV, Tb.Sp, and Tb.N indicated that there was significantly more new bone formation in the PHp group than in the other groups. With regard to neovascularization, 8weeks post-implantation, blood vessel areas (BVAs) were 9428±944μm(2), 4090±680.3μm(2), and none in the PHp, PH, and control groups, respectively. At each time point, BVAs in the PHp scaffolds were significantly higher than in the PH scaffolds. To our knowledge, this is the first use of multiphoton microscopy in bone tissue-engineering to investigate angiogenesis in scaffolds in vivo. This method represents a valuable tool for investigating neovascularization in bone scaffolds to determine if a certain scaffold is beneficial to neovascularization. We also proved that delivery of the pdgfb gene alone can improve both angiogenesis and bone regeneration Acronyms. Reconstruction of critical size bone defects remains a major clinical challenge because of poor bone regeneration, which is usually due to poor angiogenesis during repair. Satisfactory vascularization is a prerequisite for the survival of grafts and the integration of new tissue with existing tissue. In this work, we investigated angiogenesis in 3D scaffolds by in vivo multiphoton microscopy during bone formation in a murine calvarial critical bone defect model and evaluated bone regeneration 8weeks post-implantation. To verify that pdgfb-expressing vectors carried by the scaffolds can promote angiogenesis in 3D-printed scaffolds in vivo, we monitored angiogenesis within the implants by multiphoton microscopy. To our knowledge, this is the first study to dynamically investigate angiogenesis in bone tissue engineering scaffolds in vivo. Copyright © 2016 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Small-signal modeling with direct parameter extraction for impact ionization effect in high-electron-mobility transistors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Guan, He; Lv, Hongliang; Guo, Hui, E-mail: hguan@stu.xidian.edu.cn

2015-11-21

Impact ionization affects the radio-frequency (RF) behavior of high-electron-mobility transistors (HEMTs), which have narrow-bandgap semiconductor channels, and this necessitates complex parameter extraction procedures for HEMT modeling. In this paper, an enhanced small-signal equivalent circuit model is developed to investigate the impact ionization, and an improved method is presented in detail for direct extraction of intrinsic parameters using two-step measurements in low-frequency and high-frequency regimes. The practicability of the enhanced model and the proposed direct parameter extraction method are verified by comparing the simulated S-parameters with published experimental data from an InAs/AlSb HEMT operating over a wide frequency range. The resultsmore » demonstrate that the enhanced model with optimal intrinsic parameter values that were obtained by the direct extraction approach can effectively characterize the effects of impact ionization on the RF performance of HEMTs.« less

Nanostructure and surface activation of mayenite (12CaO·7Al2O3) ceramics via femtosecond laser irradiation in solvents

NASA Astrophysics Data System (ADS)

Visbal, Heidy; Hirano, Minami; Omura, Takuya; Shimizu, Masahiro; Takaishi, Taigo; Hirao, Kazuyuki

2017-07-01

Mayenite (12CaO·7Al2O3) is a highly interesting functional material due to the wide variety of its possible future applications. In this study, we used femtosecond laser irradiation in several solvents with varying polarities to increase the specific surface area of 12CaO·7Al2O3 ceramics and reduce their particle size without any structural degradation or loss of crystallinity. We observed that when femtosecond laser irradiation was applied to solvents bearing hydroxyl groups, a smaller particle size was obtained with the particle size decreasing as the polarity of the solvent increased. Using infrared spectroscopy, we confirmed the presence of hydroxyl and carbonyl surface functional groups at the surface of 12CaO·7Al2O3 ceramics after femtosecond laser irradiation. This is attributed to the direct chemical bonds breaking of the solvent via multiphoton ionization and/or tunneling ionization, followed by the Coulomb explosion and the subsequent production of ions that are adsorbed on the surfaces of 12CaO·7Al2O3 ceramics. Femtosecond laser irradiation in polar solvents with hydroxyl groups can reduce the particle size and increase the specific surface area without degradation or loss of crystallinity of 12CaO·7Al2O3 ceramics. Additionally, this method can be used for the surface modification and introduction of functional groups on the 12CaO·7Al2O3 ceramics surface.

Enhanced ionization efficiency in TIMS analyses of plutonium and americium using porous ion emitters

DOE PAGES

Baruzzini, Matthew L.; Hall, Howard L.; Watrous, Matthew G.; ...

2016-12-05

Investigations of enhanced sample utilization in thermal ionization mass spectrometry (TIMS) using porous ion emitter (PIE) techniques for the analyses of trace quantities of americium and plutonium were performed. Repeat ionization efficiency (i.e., the ratio of ions detected to atoms loaded on the filament) measurements were conducted on sample sizes ranging from 10–100 pg for americium and 1–100 pg for plutonium using PIE and traditional (i.e., a single, zone-refined rhenium, flat filament ribbon with a carbon ionization enhancer) TIMS filament sources. When compared to traditional filaments, PIEs exhibited an average boost in ionization efficiency of ~550% for plutonium and ~1100%more » for americium. A maximum average efficiency of 1.09% was observed at a 1 pg plutonium sample loading using PIEs. Supplementary trials were conducted using newly developed platinum PIEs to analyze 10 pg mass loadings of plutonium. As a result, platinum PIEs exhibited an additional ~134% boost in ion yield over standard PIEs and ~736% over traditional filaments at the same sample loading level.« less

Enabling high-precision nonlinear three-dimensional photoprocessing of premeditated designs on a conventional multiphoton imaging system

NASA Astrophysics Data System (ADS)

Garsha, Karl E.

2004-06-01

There is an increasing amount of interest in functionalized microstructural, microphotonic and microelectromechanical systems (MEMS) for use in biological applications. By scanning a tightly focused ultra-short pulsed laser beam inside a wide variety of commercially available polymer systems, the flexibility of the multiphoton microscope can be extended to include routine manufacturing of micro-devices with feature sizes well below the diffraction limit. Compared with lithography, two-photon polymerization has the unique ability to additively realize designs with high resolution in three dimensions; this permits the construction of cross-linked components and structures with hollow cavities. In light of the increasing availability of multiphoton imaging systems at research facilities, femtosecond laser manufacturing becomes particularly attractive in that the modality provides a readily accessible, rapid and high-accuracy 3-D processing capability to biological investigators interested in culture scaffolds and biomimetic tissue engineering, bio-MEMS, biomicrophotonics and microfluidics applications. This manuscript overviews recent efforts towards to enabling user accessible 3-D micro-manufacturing capabilities on a conventional proprietary-based imaging system. Software which permits the off-line design of microstructures and leverages the extensibility of proprietary LCSM image acquisition software to realize designs is introduced. The requirements for multiphoton photo-disruption (ablation) are in some ways analogous to those for multiphoton polymerization. Hence, "beam-steering" also facilitates precision photo-disruption of biological tissues with 3-D resolution, and applications involving tissue microdissection and intracellular microsurgery or three-dimensionally resolved fluorescence recovery after photobleaching (FRAP) studies can benefit from this work as well.

IR and visible luminescence studies in the infrared multiphoton dissociation of 1,2-dibromo-1,1-difluoroethane

NASA Astrophysics Data System (ADS)

Pushpa, K. K.; Kumar, Awadhesh; Vatsa, R. K.; Naik, P. D.; Annaji Rao, K.; Mittal, J. P.; Parthasarathy, V.; Sarkar, S. K.

1995-07-01

The infrared multiphoton dissociation of 1,2-dibromo-1,1-difluoroethane gives rise to IR and visible luminescence. Vibrationally excited parent molecules dissociate via two primary channels yielding bromine and vibrationally excited HBr. The strong visible emission observed between 350 to 750 nm has been assigned to electronically excited carbene CF 2Br CH.

Mitochondrial Permeability Transition in Pathogenesis of Hemorrhagic Injury: Targeted Therapy with Minocycline

DTIC Science & Technology

2012-03-01

minocy- cline treatment (Figures 1-4). Minocycline also improved mitochondrial function as assessed by intravital multiphoton imaging of the...will make direct measurements by intravital multiphoton microscopy to determine whether onset of the mitochondrial permeability transition and...oxidative stress were assessed 6 h after resuscitation. Mitochondrial polarization were assessed by intravital microscopy. After H/R with vehicle or

Visualizing Viral Infection In Vivo by Multi-Photon Intravital Microscopy.

PubMed

Sewald, Xaver

2018-06-20

Viral pathogens have adapted to the host organism to exploit the cellular machinery for virus replication and to modulate the host cells for efficient systemic dissemination and immune evasion. Much of our knowledge of the effects that virus infections have on cells originates from in vitro imaging studies using experimental culture systems consisting of cell lines and primary cells. Recently, intravital microscopy using multi-photon excitation of fluorophores has been applied to observe virus dissemination and pathogenesis in real-time under physiological conditions in living organisms. Critical steps during viral infection and pathogenesis could be studied by direct visualization of fluorescent virus particles, virus-infected cells, and the immune response to viral infection. In this review, I summarize the latest research on in vivo studies of viral infections using multi-photon intravital microscopy (MP-IVM). Initially, the underlying principle of multi-photon microscopy is introduced and experimental challenges during microsurgical animal preparation and fluorescent labeling strategies for intravital imaging are discussed. I will further highlight recent studies that combine MP-IVM with optogenetic tools and transcriptional analysis as a powerful approach to extend the significance of in vivo imaging studies of viral pathogens.

Multiphoton fluorescence imaging of NADH to quantify metabolic changes in epileptic tissue in vitro

NASA Astrophysics Data System (ADS)

Chia, Thomas H.; Zinter, Joseph; Spencer, Dennis D.; Williamson, Anne; Levene, Michael J.

2007-02-01

A powerful advantage of multiphoton microscopy is its ability to image endogenous fluorophores such as the ubiquitous coenzyme NADH in discrete cellular populations. NADH is integral in both oxidative and non-oxidative cellular metabolism. NADH loses fluorescence upon oxidation to NAD +; thus changes in NADH fluorescence can be used to monitor metabolism. Recent studies have suggested that hypo metabolic astrocytes play an important role in cases of temporal lobe epilepsy (TLE). Current theories suggest this may be due to defective and/or a reduced number of mitochondria or dysfunction of the neuronal-astrocytic metabolic coupling. Measuring NADH fluorescence changes following chemical stimulation enables the quantification of the cellular distribution of metabolic anomalies in epileptic brain tissue compared to healthy tissue. We present what we believe to be the first multiphoton microscopy images of NADH from the human brain. We also present images of NADH fluorescence from the hippocampus of the kainate-treated rat TLE model. In some experiments, human and rat astrocytes were selectively labeled with the fluorescent dye sulforhodamine 101 (SR101). Our results demonstrate that multiphoton microscopy is a powerful tool for assaying the metabolic pathologies associated with temporal lobe epilepsy in humans and in rodent models.

Electrospray Post-Ionization Mass Spectrometry of Electrosurgical Aerosols

NASA Astrophysics Data System (ADS)

Guenther, Sabine; Schäfer, Karl-Christian; Balog, Júlia; Dénes, Júlia; Majoros, Tamás; Albrecht, Katalin; Tóth, Miklós; Spengler, Bernhard; Takáts, Zoltán

2011-11-01

The feasibility of electrospray (ES) ionization of aerosols generated by electrosurgical disintegration methods was investigated. Although electrosurgery itself was demonstrated to produce gaseous ions, post-ionization methods were implemented to enhance the ion yield, especially in those cases when the ion current produced by the applied electrosurgical method is not sufficient for MS analysis. Post-ionization was implemented by mounting an ES emitter onto a Venturi pump, which is used for ion transfer. The effect of various parameters including geometry, high voltage setting, flow parameters, and solvent composition was investigated in detail. Experimental setups were optimized accordingly. ES post-ionization was found to yield spectra similar to those obtained by the REIMS technique, featuring predominantly lipid-type species. Signal enhancement was 20- to 50-fold compared with electrosurgical disintegration in positive mode, while no improvement was observed in negative mode. ES post-ionization was also demonstrated to allow the detection of non-lipid type species in the electrosurgical aerosol, including drug molecules. Since the tissue specificity of the MS data was preserved in the ES post-ionization setup, feasibility of tissue identification was demonstrated using different electrosurgical methods.

Multiphoton tomography of intratissue tattoo nanoparticles

NASA Astrophysics Data System (ADS)

König, Karsten

2012-02-01

Most of today's intratissue tattoo pigments are unknown nanoparticles. So far, there was no real control of their use due to the absence of regulations. Some of the tattoo pigments contain carcinogenic amines e.g. azo pigment Red 22. Nowadays, the European Union starts to control the administration of tattoo pigments. There is an interest to obtain information on the intratissue distribution, their interaction with living cells and the extracellular matrix, and the mechanisms behind laser tattoo removal. Multiphoton tomographs are novel biosafety and imaging tools that can provide such information non-invasively and without further labeling. When using the spectral FLIM module, spatially-resolved emission spectra, excitation spectra, and fluorescence lifetimes can pr provided. Multiphoton tomographs are used by all major cosmetic comapanies to test the biosafety of sunscreen nanoparticles.

Multiphoton tomography to detect chemo- and biohazards

NASA Astrophysics Data System (ADS)

König, Karsten

2015-03-01

In vivo high-resolution multiphoton/CARS tomography provides optical biopsies with 300 nm lateral resolution with chemical fingerprints. Thousands of volunteers and patients have been investigated for early cancer diagnosis, evaluation of anti-ageing cosmetic products, and changes of cellular metabolism by UV exposure and decreased oxygen supply. The skin as the outermost and largest organ is also the major target of CB agents. Current UV-based sensors are useful for bio-aerosol sensing but not for evaluating exposed in vivo skin. Here we evaluate the use of 4D multiphoton/CARS tomographs based on near infrared femtosecond laser radiation, time-correlated single photon counting (FLIM) and white light generation by photonic crystal fibers to detect bio- and chemohazards in human in vivo skin using twophoton fluorescence, SHG, and Raman signals.

Derivatization reagents in liquid chromatography/electrospray ionization tandem mass spectrometry.

PubMed

Santa, Tomofumi

2011-01-01

Liquid chromatography/electrospray ionization tandem mass spectrometry (LC/ESI-MS/MS) is one of the most prominent analytical techniques owing to its inherent selectivity and sensitivity. In LC/ESI-MS/MS, chemical derivatization is often used to enhance the detection sensitivity. Derivatization improves the chromatographic separation, and enhances the mass spectrometric ionization efficiency and MS/MS detectability. In this review, an overview of the derivatization reagents which have been applied to LC/ESI-MS/MS is presented, focusing on the applications to low molecular weight compounds. 2010 John Wiley & Sons, Ltd.

Enhancing the photon-extraction efficiency of site-controlled quantum dots by deterministically fabricated microlenses

NASA Astrophysics Data System (ADS)

Kaganskiy, Arsenty; Fischbach, Sarah; Strittmatter, André; Rodt, Sven; Heindel, Tobias; Reitzenstein, Stephan

2018-04-01

We report on the realization of scalable single-photon sources (SPSs) based on single site-controlled quantum dots (SCQDs) and deterministically fabricated microlenses. The fabrication process comprises the buried-stressor growth technique complemented with low-temperature in-situ electron-beam lithography for the integration of SCQDs into microlens structures with high yield and high alignment accuracy. The microlens-approach leads to a broadband enhancement of the photon-extraction efficiency of up to (21 ± 2)% and a high suppression of multi-photon events with g (2)(τ = 0) < 0.06 without background subtraction. The demonstrated combination of site-controlled growth of QDs and in-situ electron-beam lithography is relevant for arrays of efficient SPSs which, can be applied in photonic quantum circuits and advanced quantum computation schemes.

Quantum-enhanced spectroscopy with entangled multiphoton states

NASA Astrophysics Data System (ADS)

Dinani, Hossein T.; Gupta, Manish K.; Dowling, Jonathan P.; Berry, Dominic W.

2016-06-01

Traditionally, spectroscopy is performed by examining the position of absorption lines. However, at frequencies near the transition frequency, additional information can be obtained from the phase shift. In this work we consider the information about the transition frequency obtained from both the absorption and the phase shift, as quantified by the Fisher information in an interferometric measurement. We examine the use of multiple single-photon states, NOON states, and numerically optimized states that are entangled and have multiple photons. We find the optimized states that improve over the standard quantum limit set by independent single photons for some atom number densities.

Reassigning the CaH+ 11Σ → 21Σ vibronic transition with CaD+

NASA Astrophysics Data System (ADS)

Condoluci, J.; Janardan, S.; Calvin, A. T.; Rugango, R.; Shu, G.; Sherrill, C. D.; Brown, K. R.

2017-12-01

We observe vibronic transitions in CaD+ between the 11Σ and 21Σ electronic states by resonance enhanced multiphoton photodissociation spectroscopy in a Coulomb crystal. The vibronic transitions are compared with previous measurements on CaH+. The result is a revised assignment of the CaH+ vibronic levels and a disagreement with multi-state-complete-active-space second-order perturbation theory theoretical calculations by approximately 700 cm-1. Updated high-level coupled-cluster calculations that include core-valence correlations reduce the disagreement between theory and experiment to 300 cm-1.

Biomass pyrolysis: Thermal decomposition mechanisms of furfural and benzaldehyde

NASA Astrophysics Data System (ADS)

Vasiliou, AnGayle K.; Kim, Jong Hyun; Ormond, Thomas K.; Piech, Krzysztof M.; Urness, Kimberly N.; Scheer, Adam M.; Robichaud, David J.; Mukarakate, Calvin; Nimlos, Mark R.; Daily, John W.; Guan, Qi; Carstensen, Hans-Heinrich; Ellison, G. Barney

2013-09-01

The thermal decompositions of furfural and benzaldehyde have been studied in a heated microtubular flow reactor. The pyrolysis experiments were carried out by passing a dilute mixture of the aromatic aldehydes (roughly 0.1%-1%) entrained in a stream of buffer gas (either He or Ar) through a pulsed, heated SiC reactor that is 2-3 cm long and 1 mm in diameter. Typical pressures in the reactor are 75-150 Torr with the SiC tube wall temperature in the range of 1200-1800 K. Characteristic residence times in the reactor are 100-200 μsec after which the gas mixture emerges as a skimmed molecular beam at a pressure of approximately 10 μTorr. Products were detected using matrix infrared absorption spectroscopy, 118.2 nm (10.487 eV) photoionization mass spectroscopy and resonance enhanced multiphoton ionization. The initial steps in the thermal decomposition of furfural and benzaldehyde have been identified. Furfural undergoes unimolecular decomposition to furan + CO: C4H3O-CHO (+ M) → CO + C4H4O. Sequential decomposition of furan leads to the production of HC≡CH, CH2CO, CH3C≡CH, CO, HCCCH2, and H atoms. In contrast, benzaldehyde resists decomposition until higher temperatures when it fragments to phenyl radical plus H atoms and CO: C6H5CHO (+ M) → C6H5CO + H → C6H5 + CO + H. The H atoms trigger a chain reaction by attacking C6H5CHO: H + C6H5CHO → [C6H6CHO]* → C6H6 + CO + H. The net result is the decomposition of benzaldehyde to produce benzene and CO.

Experimental investigation and computational modeling of hot filament diamond chemical vapor deposition

NASA Astrophysics Data System (ADS)

Zumbach, Volker; Schäfer, Jörg; Tobai, Jens; Ridder, Michael; Dreier, Thomas; Schaich, Thomas; Wolfrum, Jürgen; Ruf, Bernhard; Behrendt, Frank; Deutschman, Olaf; Warnatz, Jürgen

1997-10-01

A joint investigation has been undertaken of the gas-phase chemistry taking place in a hot-filament chemical vapor-deposition (HFCVD) process for diamond synthesis on silica surfaces by a detailed comparison of numerical modeling and experimental results. Molecular beam sampling using quadrupole mass spectroscopy and resonance-enhanced multiphoton ionization time of flight mass spectroscopy (REMPI-TOF-MS) has been used to determine absolute concentrations of stable hydrocarbons and radicals. Resulting species of a CH4/H2, a CH4/D2 (both 0.5%/99.5%) and a C2H2/H2 (0.25%/99.75%) feedgas mixture were investigated for varying filament and substrate temperatures. Spatially resolved temperature profiles at various substrate temperatures, obtained from coherent anti-Stokes Raman spectroscopy (CARS) of hydrogen, are used as input parameters for the numerical code to reproduce hydrogen atom, methyl radical, methane, acetylene, and ethylene concentration profiles in the boundary layer of the substrate. In addition, the concentration of vibrationally excited hydrogen is determined by CARS. Results reveal only qualitative agreement between measured data and simulations, concerning concentrations of stable species and radicals probed near the surface, on filament and substrate temperature dependence, respectively. Hydrogen and deuterium experiments show similar behaviour for all species. In the case of CH4 as feedgas the model describes measured concentration profiles of CH3, CH4, and C2H2 qualitatively well. Large differences between model and experiment occur for hydrogen atoms (factor of 2) and C2H4 (factor of 3). For acetylene as feedgas the model is not able to give any predictions because no conversion of C2H2 is seen in the model in contrast to the experiment.

Molecular Spectra of RbSr: Helium Droplet Assisted Preparation of a Diatomic Molecule

NASA Astrophysics Data System (ADS)

Lackner, Florian; Krois, Günter; Buchsteiner, Thomas; Pototschnig, Johann V.; Ernst, Wolfgang E.

2014-06-01

We report on the first spectroscopic investigation of the ground and excited states of RbSr. The molecules are prepared in their vibronic ground state (X^2Σ^+1/2, ν" = 0) in a sequential pickup process on the surface of helium nanodroplets, confined in a cold (0.38 K) and weakly perturbing superfluid environment. Utilizing resonance-enhanced multi-photon ionization time-of-flight (REMPI-TOF) spectroscopy and laser induced fluorescence (LIF) spectroscopy our investigations cover the spectral regime of 11500 cm-1 - 23000 cm-1. The weak interaction between molecules and helium droplets causes a broadening of the observed transitions. For spectrally resolved band systems the helium droplet isolation approach facilitates the determination of molecular constants. Our assignment is assisted by theoretical calculations of potential energy curves based on a multireference configuration interaction (MRCI) approach. Several strong transitions could be identified; the most prominent spectral feature is a vibrational resolved band system at 14000 cm-1. In contrast to the excitation spectra, dispersed fluorescence (DF) spectra are not influenced by the helium environment, because the molecules leave the droplets upon photoexcitation, revealing detailed insights into the electronic structure of the free RbSr molecule. G. Krois, J.V. Pototschnig, F. Lackner and W.E. Ernst, J. Phys. Chem. A, 117 (50), 13719-13731 (2013) C. Callegari and W. E. Ernst, Helium Droplets as Nanocryostats for Molecular Spectroscopy - from the Vacuum Ultraviolet to the Microwave Regime, in: Handbook of High-Resolution Spectroscopy, eds. M. Quack and F. Merkt, John Wiley & Sons, Chichester, (2011) P.S. Żuchowski, R. Guerout, and O. Dulieu, arXiv preprint arXiv:1402.0702 (2014) B. Pasquiou, A. Bayerle, S.M. Tzanova, S. Stellmer, J. Szczepkowski, M. Parigger, R. Grimm, and F. Schreck, Phys. Rev. A, 88 (2), 023601 (2013).

Electronic spectra and excited-state dynamics of acridine and its hydrated clusters

NASA Astrophysics Data System (ADS)

Harthcock, Colin; Zhang, Jie; Kong, Wei; Mitsui, Masaaki; Ohshima, Yasuhiro

2017-04-01

We combine results from several different experiments to investigate the photophysics of acridine (Ac) and its hydrated clusters in the gas phase. Our findings are also compared with results from condensed phase studies. Similar to measurements of Ac dissolved in hydrocarbons, the lifetime of the first electronically excited state of isolated Ac in vacuum is too short for typical resonantly enhanced multiphoton ionization (REMPI) and laser induced fluorescence (LIF) experiments, hence no signal from REMPI and LIF can be attributed to monomeric Ac. Instead, sensitized phosphorescence emission spectroscopy is more successful in revealing the electronic states of Ac. Upon clustering with water, on the other hand, the lifetimes of the excited states are substantially increased to the nanosecond scale, and with two water molecules attached to Ac, the lifetime of the hydrated cluster is essentially the same as that of Ac in aqueous solutions. Detailed REMPI and ultraviolet-ultraviolet hole-burning experiments are then performed to reveal the structural information of the hydrated clusters. Although the formation of hydrogen bonds results in energy level reversal and energy separation between the first two excited states of Ac, its effect on the internal geometry of Ac is minimal, and all clusters with 1-3 water molecules demonstrate consistent intramolecular vibrational modes. Theoretical calculations reveal just one stable structure for each cluster under supersonic molecular beam conditions. Furthermore, different from mono- and di-water clusters, tri-water clusters consist of a linear chain of three water molecules attached to Ac. Consequently, the fragmentation pattern in the REMPI spectrum of tri-water clusters seems to be dominated by water trimer elimination, since the REMPI spectrum of Ac+.W3 is largely reproduced in the Ac+ mass channel, but not in the Ac+.W1 or Ac+.W2 channel.

Tuning the Photon Statistics of a Strongly Coupled Nanophotonic System

NASA Astrophysics Data System (ADS)

Dory, C.; Fischer, K. A.; Müller, K.; Lagoudakis, K. G.; Sarmiento, T.; Rundquist, A.; Zhang, J. L.; Kelaita, Y.; Sapra, N. V.; Vučković, J.

Strongly coupled quantum-dot-photonic-crystal cavity systems provide a nonlinear ladder of hybridized light-matter states, which are a promising platform for non-classical light generation. The transmission of light through such systems enables light generation with tunable photon counting statistics. By detuning the frequencies of quantum emitter and cavity, we can tune the transmission of light to strongly enhance either single- or two-photon emission processes. However, these nanophotonic systems show a strongly dissipative nature and classical light obscures any quantum character of the emission. In this work, we utilize a self-homodyne interference technique combined with frequency-filtering to overcome this obstacle. This allows us to generate emission with a strong two-photon component in the multi-photon regime, where we measure a second-order coherence value of g (2) [ 0 ] = 1 . 490 +/- 0 . 034 . We propose rate equation models that capture the dominant processes of emission both in the single- and multi-photon regimes and support them by quantum-optical simulations that fully capture the frequency filtering of emission from our solid-state system. Finally, we simulate a third-order coherence value of g (3) [ 0 ] = 0 . 872 +/- 0 . 021 . Army Research Office (ARO) (W911NF1310309), National Science Foundation (1503759), Stanford Graduate Fellowship.

Multi-Photon Micro-Spectroscopy of Biological Specimens

DTIC Science & Technology

2000-07-01

Micro-spectroscopy, multi-photon fluorescence spectroscopy, second harmonic generation, plant tissues, stem, chloroplast, protoplast, maize, Arabidopsis...harmonic generation (SHG) in the plant cell 5wall. In this case, micro-spectroscopy provides a means of verification that, indeed, SHG occurs in plant ...fluorescence microscopy -the response of plant cells to high intensity illumination," Micron (in press) 2000. 3. H.-C. Huang and C. -C Chen, "Genome

Suppression in high-order above-threshold ionization: destructive interference from quantum orbits

NASA Astrophysics Data System (ADS)

Lai, Xuan Yang; Quan, Wei; Yu, Shao Gang; Huang, Yi Yi; Liu, Xiao Jun

2018-05-01

We experimentally study the above-threshold ionization (ATI) spectra of noble gas argon in an intense laser field and focus on a novel suppression structure in the high-order ATI (HATI) spectra. It is found that, when a well-documented resonancelike enhancement feature appears in the HATI spectra, a significant suppression structure is followed in a higher energy region of the spectra. The observation is well reproduced by a numerical solution of the time-dependent Schrödinger equation. In terms of quantum-orbit theory, the observed suppression structure can be ascribed to the destructive interference from longer quantum orbits. Furthermore, an intrinsic relation between the ionization suppression and the ionization enhancement in the HATI spectra is well established.

Thermal diffusion in partially ionized gases - The case of unequal temperatures. [in solar chromosphere

NASA Technical Reports Server (NTRS)

Geiss, J.; Burgi, A.

1987-01-01

Previous calculations of thermal diffusion coefficients in partially ionized gases are extended to the case of unequal neutral and ion temperatures and/or temperature gradients. Formulas are derived for the general case of a major gas as well as for minor atoms and ions. Strong enhancements of minor-ion thermal diffusion coefficients over their values in the fully ionized gas are found when the degree of ionization in the main gas is relatively low. However, compared to the case of equal temperatures, the enhancements are less strong when the neutrals are cooler than the ions. The specific case of the H-H(+) mixture, which is important in the study of solar and stellar atmospheres, is discussed as an application.

Infrared Multiphoton Dissociation Spectroscopy of a Gas-Phase Complex of Uranyl and 3-Oxa-Glutaramide: An Extreme Red-Shift of the [O=U=O]²⁺ Asymmetric Stretch

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gibson, John K.; Hu, Hanshi; Van Stipdonk, Michael J.

2015-04-09

The gas-phase complex UO₂(TMOGA)₂²⁺ (TMOGA = tetramethyl-3-oxa-glutaramide) prepared by electrospray ionization was characterized by infrared multiphoton dissociation (IRMPD) spectroscopy. The IRMPD spectrum from 700–1800 cm⁻¹ was interpreted using a computational study based on density functional theory. The predicted vibrational frequencies are in good agreement with the measured values, with an average deviation of only 8 cm⁻¹ (<1%) and a maximum deviation of 21 cm⁻¹ (<2%). The only IR peak assigned to the linear uranyl moiety was the asymmetric ν₃ mode, which appeared at 965 cm⁻¹ and was predicted by DFT as 953 cm⁻¹. This ν₃ frequency is red-shifted relative tomore » bare uranyl, UO₂²⁺, by ca. 150 cm⁻¹ due to electron donation from the TMOGA ligands. Based on the degree of red-shifting, it is inferred that two TMOGA oxygen-donor ligands have a greater effective gas basicity than the four monodentate acetone ligands in UO₂(acetone)₄²⁺. The uranyl ν₃ frequency was also computed for uranyl coordinated by two TMGA ligands, in which the central Oether of TMOGA has been replaced by CH₂. The computed ν₃ for UO₂(TMGA)₂²⁺, 950 cm⁻¹, is essentially the same as that for UO₂(TMOGA)₂²⁺, suggesting that electron donation to uranyl from the Oether of TMOGA is minor. The computed ν₃ asymmetric stretching frequencies for the three actinyl complexes, UO₂(TMOGA)₂²⁺, NpO₂(TMOGA)₂²⁺ and PuO₂(TMOGA)₂²⁺, are comparable. This similarity is discussed in the context of the relationship between ν₃ and intrinsic actinide-oxygen bond energies in actinyl complexes.« less

Thermoelectric power factor enhancement by ionized nanoparticle scattering

NASA Astrophysics Data System (ADS)

Bahk, Je-Hyeong; Bian, Zhixi; Zebarjadi, Mona; Santhanam, Parthiban; Ram, Rajeev; Shakouri, Ali

2011-08-01

We show theoretically that the thermoelectric power factor can be enhanced in degenerate semiconductors when embedded nanoparticles donate carriers to the matrix and replace conventional impurity dopants as scattering centers. Nanoparticle scattering rates calculated by the partial wave method indicate a mobility enhancement over materials with equivalent doping by isolated ionized impurities while the Seebeck coefficient remains nearly intact. We find that the thermoelectric power factor of In0.53Ga0.47As from 300 K to 800 K is enhanced by 15% - 30% by nanoparticles 3-4 nm in diameter.

Single- and multi-photon ionization studies of organosulfur species

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cheung, Yu -San

1999-02-12

Accurate ionization energies (IE`s) for molecular species are used for prediction of chemical reactivity and are of fundamental importance to chemists. The IE of a gaseous molecule can be determined routinely in a photoionization or a photoelectron experiment. IE determinations made in conventional photoionization and photoelectron studies have uncertainties in the range of 3--100 meV (25--250 cm -1). In the past decade, the most exciting development in the field of photoionization and photoelectron spectroscopy has been the availability of high resolution, tunable ultraviolet (UV) and vacuum ultraviolet (VUV) laser sources. The laser pulsed field ionization photoelectron (PFI-PE) scheme is currentlymore » the state-of-the-art photoelectron spectroscopic technique and is capable of providing photoelectron energy resolution close to the optical resolution. The author has focused attention on the photoionization processes of some sulfur-containing species. The studies of the photoionization and photodissociation on sulfur-containing compounds [such as CS 2, CH 3SH, CH 3SSCH 3, CH 3CH 2SCH 2CH 3, HSCH 2CH 2SH and C 4H 4S (thiophene) and sulfur-containing radicals, such as HS, CS, CH 3S, CH 3CH 2S and CH 3SS], have been the major subjects in the group because sulfur is an important species contributing to air pollution in the atmosphere. The modeling of the combustion and oxidation of sulfur compounds represents important steps for the control of both the production and the elimination of sulfur-containing pollutants. Chapter 1 is a general introduction of the thesis. Chapters 2 and 6 contain five papers published in, or accepted for publication in, academic periodicals. In Chapter 7, the progress of the construction in the laboratory of a new vacuum ultraviolet laser system equipped with a reflectron mass spectrometer is presented. Chapters 2 through 7 have been removed for separate processing. A general conclusion of these studies are given in Chapter 8 followed by an appendix.« less

Observation of fullerenes (C60-C70) associated with LDEF crater number 31

NASA Technical Reports Server (NTRS)

Radicatidibrozolo, Filippo; Fleming, R. H.; Bunch, T. E.

1992-01-01

The presence of fullerenes in and around the LDEF crater number 31 is reported. This crater has a high C level associated with it, and is interpreted as having been produced by the impact of a C-rich micrometeoroid. Fullerenes are large 3-D C structures, among which the species C sub 60 (MW 720) and C sub 70 (MW 840) are preeminent. Fullerenes have several UV absorption bands, hence fullerenes should be detectable using UV laser ionization time-of-flight mass spectrometry. We use a LIMA-2A instrument with pulsed UV laser (266 nm) to search for high mass C species associated with LDEF crater number 31. The mass range was 0 to 1200 amu. Low ablating laser power levels were used (less than or = 5 x 10 exp 7 W/sq. cm); 200 mass spectra were acquired and summed. We observed high mass signals near m/z 720, exhibiting 24 amu separation, which is characteristic of fullerenes. Alkali ion signals were also observed. Little or no C clusters of intermediate mass were observed. We interpret the signals around m/z 720 as fullerenes, mainly C sub 60+ with lower levels of C sub 70+. We propose that the mechanism that produces these signals is resonant multiphoton ionization (REMPI). This selective mechanism explains why low mass C cluster ions are not observed along with the fullerenes, since they have much higher ionization potentials. This finding is unexpected, since up to now the search for fullerenes in extraterrestrial materials has not been successful. We conclude that the fullerenes became associated with crater number 31 in space. Two alternative (and exciting) scenarios are being considered at this time: either the fullerenes were carried by the C-rich projectile that formed crater number 31, or the fullerenes formed upon impact with the LDEF. We show the results of experiments at the ARC Vertical Gun Facility, which may establish some constraints on the origin of the fullerenes.

Ionization rate from the electron precipitation during August 2011 storm

NASA Astrophysics Data System (ADS)

Huang, Y.; Huang, C. Y.; Su, Y.

2013-12-01

We apply a parameterization by Fang et al. [2010] (Fang2010) to the complex energy spectra measured by DMSP F16 satellites to calculate the ionization rate from electron precipitation during a moderate storm on August 6th, 2011. The DMSP electron flux measurements show that there is clear enhancement of electron fluxes in the polar cap. The mean energy in the polar cap is mostly above 100 eV, while the mean energy of auroral zone is above 1 keV. F16 also captures a strong Poynting flux enhancement in the polar cap. The electron impact ionization rates using thermospheric densities and temperatures from NRLMSISE-00, TIE-GCM and GITM show clear enhancement at F-region altitudes in the polar cap region due to the low-energy electrons precipitated. Using the default empirical formulations of electron impact ionization in GCMs, TIE-GCM and GITM do not capture the F-region ionization shown in the results of Fang2010 parameterization. Fang, X, C. E. Randall, D. Lummerzheim, W. Wang, G. Lu, S. C. Solomon, and R. A. Frahm (2010), Geophys. Res. Lett., 37, L22106, doi:10.1029/2010GL045406.

Towards in vivo breast skin characterization using multiphoton microscopy

NASA Astrophysics Data System (ADS)

Batista, Ana; Uchugonova, Aisada; Breunig, Hans Georg; König, Karsten

2017-02-01

Breast cancer, the most common type of cancer in women worldwide, as well as its treatment (e.g. radiation therapy) can affect the human skin. Multiphoton imaging could provide new insights into these skin alterations non-invasively and with high-resolution. As a preparation for a later investigation involving patients, areas of the breast and forearm skin of healthy volunteers were imaged using the clinically certified multiphoton imaging tomograph MPTflex based on endogenous skin autofluorescence and second-harmonic signals. Depth-resolved image stacks were acquired in consecutive weeks to explore the influence of hormonal variations on the skin properties. Both breasts were considered and up to three different areas were imaged per session. Acquisition parameters were optimized to minimize artifacts caused by breathing-motion. As a first result, skin properties, such as the epidermal thickness, appear to be influenced by hormonal variations.

Dirac Equation in (1 +1 )-Dimensional Curved Spacetime and the Multiphoton Quantum Rabi Model

NASA Astrophysics Data System (ADS)

Pedernales, J. S.; Beau, M.; Pittman, S. M.; Egusquiza, I. L.; Lamata, L.; Solano, E.; del Campo, A.

2018-04-01

We introduce an exact mapping between the Dirac equation in (1 +1 )-dimensional curved spacetime (DCS) and a multiphoton quantum Rabi model (QRM). A background of a (1 +1 )-dimensional black hole requires a QRM with one- and two-photon terms that can be implemented in a trapped ion for the quantum simulation of Dirac particles in curved spacetime. We illustrate our proposal with a numerical analysis of the free fall of a Dirac particle into a (1 +1 )-dimensional black hole, and find that the Zitterbewegung effect, measurable via the oscillatory trajectory of the Dirac particle, persists in the presence of gravity. From the duality between the squeezing term in the multiphoton QRM and the metric coupling in the DCS, we show that gravity generates squeezing of the Dirac particle wave function.

Assessing and benchmarking multiphoton microscopes for biologists

PubMed Central

Corbin, Kaitlin; Pinkard, Henry; Peck, Sebastian; Beemiller, Peter; Krummel, Matthew F.

2017-01-01

Multiphoton microscopy has become staple tool for tracking cells within tissues and organs due to superior depth of penetration, low excitation volumes, and reduced phototoxicity. Many factors, ranging from laser pulse width to relay optics to detectors and electronics, contribute to the overall ability of these microscopes to excite and detect fluorescence deep within tissues. However, we have found that there are few standard ways already described in the literature to distinguish between microscopes or to benchmark existing microscopes to measure the overall quality and efficiency of these instruments. Here, we discuss some simple parameters and methods that can either be used within a multiphoton facility or by a prospective purchaser to benchmark performance. This can both assist in identifying decay in microscope performance and in choosing features of a scope that are suited to experimental needs. PMID:24974026

Rapid in vivo vertical tissue sectioning by multiphoton tomography

NASA Astrophysics Data System (ADS)

Batista, Ana; Breunig, Hans Georg; König, Karsten

2018-02-01

A conventional tool in the pathological field is histology which involves the analysis of thin sections of tissue in which specific cellular structures are stained with different dyes. The process to obtain these stained tissue sections is time consuming and invasive as it requires tissue removal, fixation, sectioning, and staining. Moreover, imaging of live tissue is not possible. We demonstrate that multiphoton tomography can provide within seconds, non-invasive, label-free, vertical images of live tissue which are in quality similar to conventional light micrographs of histologic stained specimen. In contrast to conventional setups based on laser scanning which image horizontally sections, the vertical in vivo images are directly recorded by combined line scanning and timed adjustments of the height of the focusing optics. In addition, multiphoton tomography provides autofluorescence lifetimes which can be used to determine the metabolic states of cells.

Hybrid label-free multiphoton and optoacoustic microscopy (MPOM)

NASA Astrophysics Data System (ADS)

Soliman, Dominik; Tserevelakis, George J.; Omar, Murad; Ntziachristos, Vasilis

2015-07-01

Many biological applications require a simultaneous observation of different anatomical features. However, unless potentially harmful staining of the specimens is employed, individual microscopy techniques do generally not provide multi-contrast capabilities. We present a hybrid microscope integrating optoacoustic microscopy and multiphoton microscopy, including second-harmonic generation, into a single device. This combined multiphoton and optoacoustic microscope (MPOM) offers visualization of a broad range of structures by employing different contrast mechanisms and at the same time enables pure label-free imaging of biological systems. We investigate the relative performance of the two microscopy modalities and demonstrate their multi-contrast abilities through the label-free imaging of a zebrafish larva ex vivo, simultaneously visualizing muscles and pigments. This hybrid microscopy application bears great potential for developmental biology studies, enabling more comprehensive information to be obtained from biological specimens without the necessity of staining.

Note: a novel vacuum ultraviolet light source assembly with aluminum-coated electrodes for enhancing the ionization efficiency of photoionization mass spectrometry.

PubMed

Zhu, Zhixiang; Wang, Jian; Qiu, Keqing; Liu, Chengyuan; Qi, Fei; Pan, Yang

2014-04-01

A novel vacuum ultraviolet (VUV) light source assembly (VUVLSA) for enhancing the ionization efficiency of photoionization mass spectrometer has been described. The VUVLSA composes of a Krypton lamp and a pair of disk electrodes with circular center cavities. The two interior surfaces that face the photoionization region were aluminum-coated. VUV light can be reflected back and forth in the photoionization region between the electrodes, thus the photoionization efficiency can be greatly enhanced. The performances of two different shaped electrodes, the coated double flat electrodes (DFE), and double conical electrodes, were studied. We showed that the signal amplification of coated DFE is around 4 times higher than that of uncoated electrodes without VUV light reflection. The relationship between the pressure of ionization chamber and mass signal enhancement has also been studied.

Enhanced Biodegradability of Pharmaceuticals and Personal Care Products by Ionizing Radiation.

PubMed

Kim, Hyun Young; Lee, O-Mi; Kim, Tae-Hun; Yu, Seungho

2015-04-01

The radiolytic degradation of antibiotic compounds, including lincomycin (LMC), sulfamethoxazole (SMX), and tetracycline (TCN), and the change of biodegradability of the radiation-treated target compounds were evaluated. As a result, the degradation of target antibiotics by hydrolysis, biodegradation, and gamma irradiation showed a compound-dependent manner. However, the biodegradability of all target compounds was enhanced by the gamma irradiation. The enhanced biodegradability after gamma irradiation (2 kGy) followed the trend of LMC (18.89%)

Non-linear optical response by functionalized gold nanospheres: identifying design principles to maximize the molecular photo-release.

PubMed

Bergamini, Luca; Voliani, Valerio; Cappello, Valentina; Nifosì, Riccardo; Corni, Stefano

2015-08-28

In a recent study by Voliani et al. [Small, 2011, 7, 3271], the electromagnetic field enhancement in the vicinity of the gold nanoparticle surface has been exploited to achieve photocontrolled release of a molecular cargo conjugated to the nanoparticles via 1,2,3-triazole, a photocleavable moiety. The aim of the present study is to investigate the mechanism of the photorelease by characterizing the nanoparticle aggregation status within the cells and simulating the electric field enhancement in a range of experimentally realistic geometries, such as single Au nanoparticles, dimers, trimers and random aggregates. Two plasmon-enhanced processes are examined for triazole photocleavage, i.e. three-photon excitation and third-harmonic-generation (one-photon) excitation. Taking into account the absorption cross sections of the triazole, we conclude that the latter mechanism is more efficient, and provides a photocleavage rate that explains the experimental findings. Moreover, we determine which aggregate geometries are required to maximize the field enhancement, and the dependence of such enhancement on the excitation wavelength. Our results provide design principles for maximizing the multiphoton molecular photorelease by such functionalized gold nanoparticles.

Metabolic Mapping of Breast Cancer with Multiphoton Spectral and Lifetime Imaging

DTIC Science & Technology

2007-03-01

spectral and lifetime characterization of NADH may be used to reveal metabolic changes in vivo and has potential to be used as an early diagnostic...combined spectral lifetime imaging modality will help for 5 characterization of breast cancer cells from cell culture based models to a relevant in... spectral and lifetime system and integrated into a multiphoton fluorescence excitation microscopy system 7 • Calibrated and characterized this

Continuum generation in ultra high numerical aperture fiber with application to multiphoton microscopy

NASA Astrophysics Data System (ADS)

Sayler, Nicholas

Nonlinear microscopy benefits from broadband laser sources, enabling efficient excitation of an array of fluorophores, for example. This work demonstrates broadening of a narrow band input pulse (6 nm to 40 nm) centered at 1040 nm with excellent shot-to-shot stability. In a preliminary demonstration, multiphoton imaging with pulses from the fiber is performed. In particular second harmonic imaging of corn starch is performed.

First multiphoton tomography of brain in man

NASA Astrophysics Data System (ADS)

König, Karsten; Kantelhardt, Sven R.; Kalasauskas, Darius; Kim, Ella; Giese, Alf

2016-03-01

We report on the first two-photon in vivo brain tissue imaging study in man. High resolution in vivo histology by multiphoton tomography (MPT) including two-photon FLIM was performed in the operation theatre during neurosurgery to evaluate the feasibility to detect label-free tumor borders with subcellular resolution. This feasibility study demonstrates, that MPT has the potential to identify tumor borders on a cellular level in nearly real-time.

Label-free multiphoton microscopy reveals altered tissue architecture in hippocampal sclerosis.

PubMed

Uckermann, Ortrud; Galli, Roberta; Leupold, Susann; Coras, Roland; Meinhardt, Matthias; Hallmeyer-Elgner, Susanne; Mayer, Thomas; Storch, Alexander; Schackert, Gabriele; Koch, Edmund; Blümcke, Ingmar; Steiner, Gerald; Kirsch, Matthias

2017-01-01

The properties and structure of tissue can be visualized without labeling or preparation by multiphoton microscopy combining coherent anti-Stokes Raman scattering (CARS), addressing lipid content, second harmonic generation (SHG) showing collagen, and two-photon excited fluorescence (TPEF) of endogenous fluorophores. We compared samples of sclerotic and nonsclerotic human hippocampus to detect pathologic changes in the brain of patients with pharmacoresistant temporomesial epilepsy (n = 15). Multiphoton microscopy of cryosections and bulk tissue revealed hippocampal layering and micromorphologic details in accordance with reference histology: CARS displayed white and gray matter layering and allowed the assessment of axonal myelin. SHG visualized blood vessels based on adventitial collagen. In addition, corpora amylacea (CoA) were found to be SHG-active. Pyramidal cell bodies were characterized by intense cytoplasmic endogenous TPEF. Furthermore, diffuse TPEF around blood vessels was observed that co-localized with positive albumin immunohistochemistry and might indicate degeneration-associated vascular leakage. We present a label-free and fast optical approach that analyzes pathologic aspects of HS. Hippocampal layering, loss of pyramidal cells, and presence of CoA indicative of sclerosis are visualized. Label-free multiphoton microscopy has the potential to extend the histopathologic armamentarium for ex vivo assessment of changes of the hippocampal formation on fresh tissue and prospectively in vivo. Wiley Periodicals, Inc. © 2016 International League Against Epilepsy.

Multiphoton microscopy in every lab: the promise of ultrafast semiconductor disk lasers

NASA Astrophysics Data System (ADS)

Emaury, Florian; Voigt, Fabian F.; Bethge, Philipp; Waldburger, Dominik; Link, Sandro M.; Carta, Stefano; van der Bourg, Alexander; Helmchen, Fritjof; Keller, Ursula

2017-07-01

We use an ultrafast diode-pumped semiconductor disk laser (SDL) to demonstrate several applications in multiphoton microscopy. The ultrafast SDL is based on an optically pumped Vertical External Cavity Surface Emitting Laser (VECSEL) passively mode-locked with a semiconductor saturable absorber mirror (SESAM) and generates 170-fs pulses at a center wavelength of 1027 nm with a repetition rate of 1.63 GHz. We demonstrate the suitability of this laser for structural and functional multiphoton in vivo imaging in both Drosophila larvae and mice for a variety of fluorophores (including mKate2, tdTomato, Texas Red, OGB-1, and R-CaMP1.07) and for endogenous second-harmonic generation in muscle cell sarcomeres. We can demonstrate equivalent signal levels compared to a standard 80-MHz Ti:Sapphire laser when we increase the average power by a factor of 4.5 as predicted by theory. In addition, we compare the bleaching properties of both laser systems in fixed Drosophila larvae and find similar bleaching kinetics despite the large difference in pulse repetition rates. Our results highlight the great potential of ultrafast diode-pumped SDLs for creating a cost-efficient and compact alternative light source compared to standard Ti:Sapphire lasers for multiphoton imaging.

Clinical optical coherence tomography combined with multiphoton tomography for evaluation of several skin disorders

NASA Astrophysics Data System (ADS)

König, Karsten; Speicher, Marco; Bückle, Rainer; Reckfort, Julia; McKenzie, Gordon; Welzel, Julia; Koehler, Martin J.; Elsner, Peter; Kaatz, Martin

2010-02-01

The first clinical trial of optical coherence tomography (OCT) combined with multiphoton tomography (MPT) and dermoscopy is reported. State-of-the-art (i) OCT systems for dermatology (e.g. multibeam swept source OCT), (ii) the femtosecond laser multiphoton tomograph DermaInspectTM, and (iii) digital dermoscopes were applied to 47 patients with a diversity of skin diseases and disorders such as skin cancer, psoriasis, hemangioma, connective tissue diseases, pigmented lesions, and autoimmune bullous skin diseases. Dermoscopy, also called 'epiluminescent microscopy', provides two-dimensional color images of the skin surface. OCT imaging is based on the detection of optical reflections within the tissue measured interferometrically whereas nonlinear excitation of endogenous fluorophores and the second harmonic generation are the bases of MPT images. OCT cross sectional "wide field" image provides a typical field of view of 5 x 2 mm2 and offers fast information on the depth and the volume of the investigated lesion. In comparison, multiphoton tomography presents 0.36 x 0.36 mm2 horizontal or diagonal sections of the region of interest within seconds with submicron resolution and down to a tissue depth of 200 μm. The combination of OCT and MPT provides a synergistic optical imaging modality for early detection of skin cancer and other skin diseases.

Multiphoton in vivo imaging with a femtosecond semiconductor disk laser

PubMed Central

Voigt, Fabian F.; Emaury, Florian; Bethge, Philipp; Waldburger, Dominik; Link, Sandro M.; Carta, Stefano; van der Bourg, Alexander; Helmchen, Fritjof; Keller, Ursula

2017-01-01

We use an ultrafast diode-pumped semiconductor disk laser (SDL) to demonstrate several applications in multiphoton microscopy. The ultrafast SDL is based on an optically pumped Vertical External Cavity Surface Emitting Laser (VECSEL) passively mode-locked with a semiconductor saturable absorber mirror (SESAM) and generates 170-fs pulses at a center wavelength of 1027 nm with a repetition rate of 1.63 GHz. We demonstrate the suitability of this laser for structural and functional multiphoton in vivo imaging in both Drosophila larvae and mice for a variety of fluorophores (including mKate2, tdTomato, Texas Red, OGB-1, and R-CaMP1.07) and for endogenous second-harmonic generation in muscle cell sarcomeres. We can demonstrate equivalent signal levels compared to a standard 80-MHz Ti:Sapphire laser when we increase the average power by a factor of 4.5 as predicted by theory. In addition, we compare the bleaching properties of both laser systems in fixed Drosophila larvae and find similar bleaching kinetics despite the large difference in pulse repetition rates. Our results highlight the great potential of ultrafast diode-pumped SDLs for creating a cost-efficient and compact alternative light source compared to standard Ti:Sapphire lasers for multiphoton imaging. PMID:28717563

Clinical optical coherence tomography combined with multiphoton tomography of patients with skin diseases.

PubMed

König, Karsten; Speicher, Marco; Bückle, Rainer; Reckfort, Julia; McKenzie, Gordon; Welzel, Julia; Koehler, Martin J; Elsner, Peter; Kaatz, Martin

2009-07-01

We report on the first clinical study based on optical coherence tomography (OCT) in combination with multiphoton tomography (MPT) and dermoscopy. 47 patients with a variety of skin diseases and disorders such as skin cancer, psoriasis, hemangioma, connective tissue diseases, pigmented lesions, and autoimmune bullous skin diseases have been investigated with (i) state-of-the-art OCT systems for dermatology including multibeam swept source OCT, (ii) the femtosecond laser multiphoton tomograph, and (iii) dermoscopes. Dermoscopy provides two-dimensional color images of the skin surface. OCT images reflect modifications of the intratissue refractive index whereas MPT is based on nonlinear excitation of endogenous fluorophores and second harmonic generation. A stack of cross-sectional OCT "wide field" images with a typical field of view of 5 x 2 mm(2) gave fast information on the depth and the volume of the lesion. Multiphoton tomography provided 0.36 x 0.36 mm(2) horizontal/diagonal optical sections within seconds of a particular region of interest with superior submicron resolution down to a tissue depth of 200 mum. The combination of OCT and MPT provides a unique powerful optical imaging modality for early detection of skin cancer and other skin diseases as well as for the evaluation of the efficiency of treatments.

A single-photon fluorescence and multi-photon spectroscopic study of atherosclerotic lesions

NASA Astrophysics Data System (ADS)

Smith, Michael S. D.; Ko, Alex C. T.; Ridsdale, Andrew; Schattka, Bernie; Pegoraro, Adrian; Hewko, Mark D.; Shiomi, Masashi; Stolow, Albert; Sowa, Michael G.

2009-06-01

In this study we compare the single-photon autofluorescence and multi-photon emission spectra obtained from the luminal surface of healthy segments of artery with segments where there are early atherosclerotic lesions. Arterial tissue was harvested from atherosclerosis-prone WHHL-MI rabbits (Watanabe heritable hyperlipidemic rabbit-myocardial infarction), an animal model which mimics spontaneous myocardial infarction in humans. Single photon fluorescence emission spectra of samples were acquired using a simple spectrofluorometer set-up with 400 nm excitation. Samples were also investigated using a home built multi-photon microscope based on a Ti:sapphire femto-second oscillator. The excitation wavelength was set at 800 nm with a ~100 femto-second pulse width. Epi-multi-photon spectroscopic signals were collected through a fibre-optics coupled spectrometer. While the single-photon fluorescence spectra of atherosclerotic lesions show minimal spectroscopic difference from those of healthy arterial tissue, the multi-photon spectra collected from atherosclerotic lesions show marked changes in the relative intensity of two-photon excited fluorescence (TPEF) and second-harmonic generation (SHG) signals when compared with those from healthy arterial tissue. The observed sharp increase of the relative SHG signal intensity in a plaque is in agreement with the known pathology of early lesions which have increased collagen content.

Comparison of Cornea Module and DermaInspect for noninvasive imaging of ocular surface pathologies

NASA Astrophysics Data System (ADS)

Steven, Philipp; Müller, Maya; Koop, Norbert; Rose, Christian; Hüttmann, Gereon

2009-11-01

Minimally invasive imaging of ocular surface pathologies aims at securing clinical diagnosis without actual tissue probing. For this matter, confocal microscopy (Cornea Module) is in daily use in ophthalmic practice. Multiphoton microscopy is a new optical technique that enables high-resolution imaging and functional analysis of living tissues based on tissue autofluorescence. This study was set up to compare the potential of a multiphoton microscope (DermaInspect) to the Cornea Module. Ocular surface pathologies such as pterygia, papillomae, and nevi were investigated in vivo using the Cornea Module and imaged immediately after excision by DermaInspect. Two excitation wavelengths, fluorescence lifetime imaging and second-harmonic generation (SHG), were used to discriminate different tissue structures. Images were compared with the histopathological assessment of the samples. At wavelengths of 730 nm, multiphoton microscopy exclusively revealed cellular structures. Collagen fibrils were specifically demonstrated by second-harmonic generation. Measurements of fluorescent lifetimes enabled the highly specific detection of goblet cells, erythrocytes, and nevus-cell clusters. At the settings used, DermaInspect reaches higher resolutions than the Cornea Module and obtains additional structural information. The parallel detection of multiphoton excited autofluorescence and confocal imaging could expand the possibilities of minimally invasive investigation of the ocular surface toward functional analysis at higher resolutions.

Weak-field multiphoton femtosecond coherent control in the single-cycle regime.

PubMed

Chuntonov, Lev; Fleischer, Avner; Amitay, Zohar

2011-03-28

Weak-field coherent phase control of atomic non-resonant multiphoton excitation induced by shaped femtosecond pulses is studied theoretically in the single-cycle regime. The carrier-envelope phase (CEP) of the pulse, which in the multi-cycle regime does not play any control role, is shown here to be a new effective control parameter that its effect is highly sensitive to the spectral position of the ultrabroad spectrum. Rationally chosen position of the ultrabroadband spectrum coherently induces several groups of multiphoton transitions from the ground state to the excited state of the system: transitions involving only absorbed photons as well as Raman transitions involving both absorbed and emitted photons. The intra-group interference is controlled by the relative spectral phase of the different frequency components of the pulse, while the inter-group interference is controlled jointly by the CEP and the relative spectral phase. Specifically, non-resonant two- and three-photon excitation is studied in a simple model system within the perturbative frequency-domain framework. The developed intuition is then applied to weak-field multiphoton excitation of atomic cesium (Cs), where the simplified model is verified by non-perturbative numerical solution of the time-dependent Schrödinger equation. We expect this work to serve as a basis for a new line of femtosecond coherent control experiments.

Fast photodynamics of azobenzene probed by scanning excited-state potential energy surfaces using slow spectroscopy

NASA Astrophysics Data System (ADS)

Tan, Eric M. M.; Amirjalayer, Saeed; Smolarek, Szymon; Vdovin, Alexander; Zerbetto, Francesco; Buma, Wybren Jan

2015-01-01

Azobenzene, a versatile and polymorphic molecule, has been extensively and successfully used for photoswitching applications. The debate over its photoisomerization mechanism leveraged on the computational scrutiny with ever-increasing levels of theory. However, the most resolved absorption spectrum for the transition to S1(nπ*) has not followed the computational advances and is more than half a century old. Here, using jet-cooled molecular beam and multiphoton ionization techniques we report the first high-resolution spectra of S1(nπ*) and S2(ππ*). The photophysical characterization reveals directly the structural changes upon excitation and the timescales of dynamical processes. For S1(nπ*), we find that changes in the hybridization of the nitrogen atoms are the driving force that triggers isomerization. In combination with quantum chemical calculations we conclude that photoisomerization occurs along an inversion-assisted torsional pathway with a barrier of ~2 kcal mol-1. This methodology can be extended to photoresponsive molecular systems so far deemed non-accessible to high-resolution spectroscopy.

Vorticity generation and jetting caused by a laser-induced optical breakdown

NASA Astrophysics Data System (ADS)

Wang, Jonathan; Buchta, David; Freund, Jonathan

2017-11-01

A focused laser can cause optical breakdown of a gas that absorbs energy and can seed ignition. The local hydrodynamics are complex. The breakdown is observed to produce vorticity that subsequently collects into a jetting flow towards the laser source. The strength and the very direction of the jet is observed to be sensitive to the plasma kernel geometry. We use detailed numerical simulations to examine the short-time (< 1 μ s) dynamics leading to this vorticity and jetting. The simulation employs a two-temperature model, free-electron generation by multi-photon ionization, absorption of laser energy by inverse Bremsstrahlung, and 11 charged and neutral species for air. We quantify the early-time contributions of different thermodynamic and gas-dynamic effects to the baroclinic torque. It is found that the breakdown produces compression waves within the plasma kernel, and that the mismatch in their strengths precipitates the involution of the plasma remnants and yields the net vorticity that ultimately develops into the jet. We also quantify the temperature distribution and local strain rates and demonstrate their importance in seeding ignition in non-homogeneous hydrogen/air mixtures.

Heating the warm ionized medium

NASA Technical Reports Server (NTRS)

Reynolds, R. J.; Cox, D. P.

1992-01-01

If photoelectric heating by grains within the diffuse ionized component of the interstellar medium is 10 exp -25 ergs/s per H atom, the average value within diffuse H I regions, then grain heating equals or exceeds photoionization heating of the ionized gas. This supplemental heat source would obviate the need for energetic ionizing photons to balance the observed forbidden-line cooling and could be responsible in part for enhanced intensities of some of the forbidden lines.

Solution processed, white emitting tandem organic light-emitting diodes with inverted device architecture.

PubMed

Höfle, Stefan; Schienle, Alexander; Bernhard, Christoph; Bruns, Michael; Lemmer, Uli; Colsmann, Alexander

2014-08-13

Fully solution processed monochromatic and white-light emitting tandem or multi-photon polymer OLEDs with an inverted device architecture have been realized by employing WO3 /PEDOT:PSS/ZnO/PEI charge carrier generation layers. The luminance of the sub-OLEDs adds up in the stacked device indicating multi-photon emission. The white OLEDs exhibit a CRI of 75. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Characterizing multi-photon quantum interference with practical light sources and threshold single-photon detectors

NASA Astrophysics Data System (ADS)

Navarrete, Álvaro; Wang, Wenyuan; Xu, Feihu; Curty, Marcos

2018-04-01

The experimental characterization of multi-photon quantum interference effects in optical networks is essential in many applications of photonic quantum technologies, which include quantum computing and quantum communication as two prominent examples. However, such characterization often requires technologies which are beyond our current experimental capabilities, and today's methods suffer from errors due to the use of imperfect sources and photodetectors. In this paper, we introduce a simple experimental technique to characterize multi-photon quantum interference by means of practical laser sources and threshold single-photon detectors. Our technique is based on well-known methods in quantum cryptography which use decoy settings to tightly estimate the statistics provided by perfect devices. As an illustration of its practicality, we use this technique to obtain a tight estimation of both the generalized Hong‑Ou‑Mandel dip in a beamsplitter with six input photons and the three-photon coincidence probability at the output of a tritter.

Effect Of Molecular Rotations On High Intensity Absorption In CO2

NASA Astrophysics Data System (ADS)

Bandrauk, Andre D.; Claveau, Lorraine

1986-10-01

In intense fields, the Rabi frequency ωR = pE/h can easily be of the order of rotational and vibrational energies of molecules. This means that rotations as well as vibrations become strongly perturbed so that perturbative methods no longer apply. We will show that nonperturbative methods can be derived from the concept of the dressed molecule. This leads to coupled equations which are used ko simulate numerically the multiphoton processes which will occur at intensities > 108 W/cm2. Furthermore, for multiphoton rotational tran-sitions, one can derive analytical models which help one understand the temporal behaviour of energy flow in a molecule in terms of its dressed spectrum, such as chaotic or regular (nonchaotic) behaviour. These results are of relevance to the manifestation of multiphoton coherences in a CO2 spectrum at very high intensities (I % 1012 W/cm2).

Pushing the Limit of Infrared Multiphoton Dissociation to Megadalton-Size DNA Ions.

PubMed

Doussineau, Tristan; Antoine, Rodolphe; Santacreu, Marion; Dugourd, Philippe

2012-08-16

We report the use of infrared multiphoton dissociation (IRMPD) for the determination of relative activation energies for unimolecular dissociation of megadalton DNA ions. Single ions with masses in the megadalton range were stored in an electrostatic ion trap for a few tens of milliseconds and the image current generated by the roundtrips of ions in the trap was recorded. While being trapped, single ions were irradiated by a CO2 laser and fragmented, owing to multiphoton IR activation. The analysis of the single-ion image current during the heating period allows us to measure changes in the charge of the trapped ion. We estimated the activation energy associated with the dissociation of megadalton-size DNA ions in the frame of an Arrhenius-like model by analyzing a large set of individual ions in order to construct a frequency histogram of the dissociation rates for a collection of ions.

Protocol for generating multiphoton entangled states from quantum dots in the presence of nuclear spin fluctuations

NASA Astrophysics Data System (ADS)

Denning, Emil V.; Iles-Smith, Jake; McCutcheon, Dara P. S.; Mork, Jesper

2017-12-01

Multiphoton entangled states are a crucial resource for many applications in quantum information science. Semiconductor quantum dots offer a promising route to generate such states by mediating photon-photon correlations via a confined electron spin, but dephasing caused by the host nuclear spin environment typically limits coherence (and hence entanglement) between photons to the spin T2* time of a few nanoseconds. We propose a protocol for the deterministic generation of multiphoton entangled states that is inherently robust against the dominating slow nuclear spin environment fluctuations, meaning that coherence and entanglement is instead limited only by the much longer spin T2 time of microseconds. Unlike previous protocols, the present scheme allows for the generation of very low error probability polarization encoded three-photon GHZ states and larger entangled states, without the need for spin echo or nuclear spin calming techniques.

Highly Resolved Intravital Striped-illumination Microscopy of Germinal Centers

PubMed Central

Andresen, Volker; Sporbert, Anje

2014-01-01

Monitoring cellular communication by intravital deep-tissue multi-photon microscopy is the key for understanding the fate of immune cells within thick tissue samples and organs in health and disease. By controlling the scanning pattern in multi-photon microscopy and applying appropriate numerical algorithms, we developed a striped-illumination approach, which enabled us to achieve 3-fold better axial resolution and improved signal-to-noise ratio, i.e. contrast, in more than 100 µm tissue depth within highly scattering tissue of lymphoid organs as compared to standard multi-photon microscopy. The acquisition speed as well as photobleaching and photodamage effects were similar to standard photo-multiplier-based technique, whereas the imaging depth was slightly lower due to the use of field detectors. By using the striped-illumination approach, we are able to observe the dynamics of immune complex deposits on secondary follicular dendritic cells – on the level of a few protein molecules in germinal centers. PMID:24748007

Characteristics of subgingival calculus detection by multiphoton fluorescence microscopy

NASA Astrophysics Data System (ADS)

Tung, Oi-Hong; Lee, Shyh-Yuan; Lai, Yu-Lin; Chen, How-Foo

2011-06-01

Subgingival calculus has been recognized as a major cause of periodontitis, which is one of the main chronic infectious diseases of oral cavities and a principal cause of tooth loss in humans. Bacteria deposited in subgingival calculus or plaque cause gingival inflammation, function deterioration, and then periodontitis. However, subgingival calculus within the periodontal pocket is a complicated and potentially delicate structure to be detected with current dental armamentaria, namely dental x-rays and dental probes. Consequently, complete removal of subgingival calculus remains a challenge to periodontal therapies. In this study, the detection of subgingival calculus employing a multiphoton autofluorescence imaging method was characterized in comparison with a one-photon confocal fluorescence imaging technique. Feasibility of such a system was studied based on fluorescence response of gingiva, healthy teeth, and calculus with and without gingiva covered. The multiphoton fluorescence technology perceived the tissue-covered subgingival calculus that cannot be observed by the one-photon confocal fluorescence method.

Distribution of hybrid entanglement and hyperentanglement with time-bin for secure quantum channel under noise via weak cross-Kerr nonlinearity.

PubMed

Heo, Jino; Kang, Min-Sung; Hong, Chang-Ho; Yang, Hyung-Jin; Choi, Seong-Gon; Hong, Jong-Phil

2017-08-31

We design schemes to generate and distribute hybrid entanglement and hyperentanglement correlated with degrees of freedom (polarization and time-bin) via weak cross-Kerr nonlinearities (XKNLs) and linear optical devices (including time-bin encoders). In our scheme, the multi-photon gates (which consist of XKNLs, quantum bus [qubus] beams, and photon-number-resolving [PNR] measurement) with time-bin encoders can generate hyperentanglement or hybrid entanglement. And we can also purify the entangled state (polarization) of two photons using only linear optical devices and time-bin encoders under a noisy (bit-flip) channel. Subsequently, through local operations (using a multi-photon gate via XKNLs) and classical communications, it is possible to generate a four-qubit hybrid entangled state (polarization and time-bin). Finally, we discuss how the multi-photon gate using XKNLs, qubus beams, and PNR measurement can be reliably performed under the decoherence effect.

Adaptive multiphoton endomicroscopy through a dynamically deformed multicore optical fiber using proximal detection.

PubMed

Warren, Sean C; Kim, Youngchan; Stone, James M; Mitchell, Claire; Knight, Jonathan C; Neil, Mark A A; Paterson, Carl; French, Paul M W; Dunsby, Chris

2016-09-19

This paper demonstrates multiphoton excited fluorescence imaging through a polarisation maintaining multicore fiber (PM-MCF) while the fiber is dynamically deformed using all-proximal detection. Single-shot proximal measurement of the relative optical path lengths of all the cores of the PM-MCF in double pass is achieved using a Mach-Zehnder interferometer read out by a scientific CMOS camera operating at 416 Hz. A non-linear least squares fitting procedure is then employed to determine the deformation-induced lateral shift of the excitation spot at the distal tip of the PM-MCF. An experimental validation of this approach is presented that compares the proximally measured deformation-induced lateral shift in focal spot position to an independent distally measured ground truth. The proximal measurement of deformation-induced shift in focal spot position is applied to correct for deformation-induced shifts in focal spot position during raster-scanning multiphoton excited fluorescence imaging.

Extending the fundamental imaging-depth limit of multi-photon microscopy by imaging with photo-activatable fluorophores.

PubMed

Chen, Zhixing; Wei, Lu; Zhu, Xinxin; Min, Wei

2012-08-13

It is highly desirable to be able to optically probe biological activities deep inside live organisms. By employing a spatially confined excitation via a nonlinear transition, multiphoton fluorescence microscopy has become indispensable for imaging scattering samples. However, as the incident laser power drops exponentially with imaging depth due to scattering loss, the out-of-focus fluorescence eventually overwhelms the in-focal signal. The resulting loss of imaging contrast defines a fundamental imaging-depth limit, which cannot be overcome by increasing excitation intensity. Herein we propose to significantly extend this depth limit by multiphoton activation and imaging (MPAI) of photo-activatable fluorophores. The imaging contrast is drastically improved due to the created disparity of bright-dark quantum states in space. We demonstrate this new principle by both analytical theory and experiments on tissue phantoms labeled with synthetic caged fluorescein dye or genetically encodable photoactivatable GFP.

Label-free identification of intestinal metaplasia in the stomach using multiphoton microscopy

NASA Astrophysics Data System (ADS)

Wu, G.; Wei, J.; Zheng, Z.; Ye, J.; Zeng, S.

2014-06-01

The early diagnosis of intestinal metaplasia (IM) in the stomach together with effective therapeutic interventions is crucial to reducing the mortality-rates of the patients associated with gastric cancer. However, it is challenging during conventional white-light endoscopy, and histological analysis remains the ‘gold standard’ for the final diagnosis. Here, we describe a label-free imaging method, multiphoton microscopy (MPM), for the identification of IM in the stomach. It was found that multiphoton imaging provides cellular and subcellular details to the identification of IM from normal gastric tissues. In particular, there is significant difference in the population density of goblet cells between normal and IM gastric tissues, providing substantial potential to become a quantitative intrinsic marker for in vivo clinical diagnosis of early gastric lesions. To our knowledge, this is the first demonstration of the potential of MPM for the identification of IM.

Theoretical derivation of laser-dressed atomic states by using a fractal space

NASA Astrophysics Data System (ADS)

Duchateau, Guillaume

2018-05-01

The derivation of approximate wave functions for an electron submitted to both a Coulomb and a time-dependent laser electric fields, the so-called Coulomb-Volkov (CV) state, is addressed. Despite its derivation for continuum states does not exhibit any particular problem within the framework of the standard theory of quantum mechanics (QM), difficulties arise when considering an initially bound atomic state. Indeed the natural way of translating the unperturbed momentum by the laser vector potential is no longer possible since a bound state does not exhibit a plane wave form explicitly including a momentum. The use of a fractal space permits to naturally define a momentum for a bound wave function. Within this framework, it is shown how the derivation of laser-dressed bound states can be performed. Based on a generalized eikonal approach, a new expression for the laser-dressed states is also derived, fully symmetric relative to the continuum or bound nature of the initial unperturbed wave function. It includes an additional crossed term in the Volkov phase which was not obtained within the standard theory of quantum mechanics. The derivations within this fractal framework have highlighted other possible ways to derive approximate laser-dressed states in QM. After comparing the various obtained wave functions, an application to the prediction of the ionization probability of hydrogen targets by attosecond XUV pulses within the sudden approximation is provided. This approach allows to make predictions in various regimes depending on the laser intensity, going from the non-resonant multiphoton absorption to tunneling and barrier-suppression ionization.

Unified model of plasma formation, bubble generation and shock wave emission in water for fs to ns laser pulses (Conference Presentation)

NASA Astrophysics Data System (ADS)

Liang, Xiao-Xuan; Freidank, Sebastian; Linz, Norbert; Paltauf, Günther; Zhang, Zhenxi; Vogel, Alfred

2017-03-01

We developed modeling tools for optical breakdown events in water that span various phases reaching from breakdown initiation via solvated electron generation, through laser induced-plasma formation and temperature evolution in the focal spot to the later phases of cavitation bubble dynamics and shock wave emission and applied them to a large parameter space of pulse durations, wavelengths, and pulse energies. The rate equation model considers the interplay of linear absorption, photoionization, avalanche ionization and recombination, traces thermalization and temperature evolution during the laser pulse, and portrays the role of thermal ionization that becomes relevant for T > 3000 K. Modeling of free-electron generation includes recent insights on breakdown initiation in water via multiphoton excitation of valence band electrons into a solvated state at Eini = 6.6 eV followed by up-conversion into the conduction band level that is located at 9.5 eV. The ability of tracing the temperature evolution enabled us to link the model of laser-induced plasma formation with a hydrodynamic model of plasma-induced pressure evolution and phase transitions that, in turn, traces bubble generation and dynamics as well as shock wave emission. This way, the amount of nonlinear energy deposition in transparent dielectrics and the resulting material modifications can be assessed as a function of incident laser energy. The unified model of plasma formation and bubble dynamics yields an excellent agreement with experimental results over the entire range of investigated pulse durations (femtosecond to nanosecond), wavelengths (UV to IR) and pulse energies.

Use of 3-nitrobenzonitrile as an additive for improved sensitivity in sonic-spray ionization mass spectrometry.

PubMed

Kanaki, Katerina; Pergantis, Spiros A

2014-12-15

Sonic-spray ionization (SSI) has been shown to produce gas-phase ions for a wide range of compounds, without the application of voltage or a laser. However, it remains to be shown that it can also provide similar sensitivities to those obtained by electrospray ionization mass spectrometry (ESI-MS). Here we report on an attempt to further improve the sensitivity of SSI-MS, more specifically a version of SSI that is referred to as Venturi easy ambient sonic-spray ionization (V-EASI) MS, by adding a signal-enhancing additive to the sample solution. The additive used is 3-nitrobenzonitrile (3-NBN), which has recently been used with success in a new ionization approach named matrix-assisted ionization vacuum. In order to conduct this study we have analyzed a range of compounds, including peptides, metalloproteins, and some organometalloids. During the V-EASI-MS analyses molecular ion and protonated molecule signal intensities as well as their corresponding signal-to-noise (S/N) ratios, obtained in the presence and absence of the 3-NBN, were compared. The 3-NBN-assisted V-EASI-MS approach developed here provides significant improvement in sensitivity relative to conventional V-EASI-MS for almost all compounds tested. More specifically, for peptides a 1.6- to 4-fold enhancement was realized, for proteins the enhancements were from 2- to 5-fold, and for some metalloid species enhancements reached up to 10-fold. However, optimum additive concentration and ion transfer capillary temperature were found to be compound-dependent and thus require optimization in order for maximum enhancements to be achieved. In most cases the 3-NBN-assisted V-EASI-MS approach provides comparable sensitivities and S/N ratios to ESI-MS on the same ion trap mass spectrometer. The use of 3-NBN with V-EASI-MS gives rise to a novel 3-NBN-assisted MS technique, which has demonstrated considerable signal enhancement for most of the compounds analyzed, thus improving its competitiveness towards the well-established and dominating ESI-MS technique. Copyright © 2014 John Wiley & Sons, Ltd.

Weakly ionized cosmic gas: Ionization and characterization

NASA Technical Reports Server (NTRS)

Rosenberg, M.; Mendis, D. A.; Chow, V. W.

1994-01-01

Since collective plasma behavior may determine important transport processes (e.g., plasma diffusion across a magnetic field) in certain cosmic environments, it is important to delineate the parameter space in which weakly ionized cosmic gases may be characterized as plasmas. In this short note, we do so. First, we use values for the ionization fraction given in the literature, wherein the ionization is generally assumed to be due primarily to ionization by cosmic rays. We also discuss an additional mechanism for ionization in such environments, namely, the photoelectric emission of electrons from cosmic dust grains in an interstellar Far Ultra Violet (FUV) radiation field. Simple estimates suggest that under certain conditions this mechanism may dominate cosmic ray ionization, and possibly also the photoionization of metal atoms by the interstellar FUV field, and thereby lead to an enhanced ionization level.

Extreme ionization of Xe clusters driven by ultraintense laser fields

DOE Office of Scientific and Technical Information (OSTI.GOV)

Heidenreich, Andreas; Last, Isidore; Jortner, Joshua

We applied theoretical models and molecular dynamics simulations to explore extreme multielectron ionization in Xe{sub n} clusters (n=2-2171, initial cluster radius R{sub 0}=2.16-31.0 A ring ) driven by ultraintense infrared Gaussian laser fields (peak intensity I{sub M}=10{sup 15}-10{sup 20} W cm{sup -2}, temporal pulse length {tau}=10-100 fs, and frequency {nu}=0.35 fs{sup -1}). Cluster compound ionization was described by three processes of inner ionization, nanoplasma formation, and outer ionization. Inner ionization gives rise to high ionization levels (with the formation of (Xe{sup q+}){sub n} with q=2-36), which are amenable to experimental observation. The cluster size and laser intensity dependence of themore » inner ionization levels are induced by a superposition of barrier suppression ionization (BSI) and electron impact ionization (EII). The BSI was induced by a composite field involving the laser field and an inner field of the ions and electrons, which manifests ignition enhancement and screening retardation effects. EII was treated using experimental cross sections, with a proper account of sequential impact ionization. At the highest intensities (I{sub M}=10{sup 18}-10{sup 20} W cm{sup -2}) inner ionization is dominated by BSI. At lower intensities (I{sub M}=10{sup 15}-10{sup 16} W cm{sup -2}), where the nanoplasma is persistent, the EII contribution to the inner ionization yield is substantial. It increases with increasing the cluster size, exerts a marked effect on the increase of the (Xe{sup q+}){sub n} ionization level, is most pronounced in the cluster center, and manifests a marked increase with increasing the pulse length (i.e., becoming the dominant ionization channel (56%) for Xe{sub 2171} at {tau}=100 fs). The EII yield and the ionization level enhancement decrease with increasing the laser intensity. The pulse length dependence of the EII yield at I{sub M}=10{sup 15}-10{sup 16} W cm{sup -2} establishes an ultraintense laser pulse length control mechanism of extreme ionization products.« less

Searching for Axionlike Particles with Ultraperipheral Heavy-Ion Collisions.

PubMed

Knapen, Simon; Lin, Tongyan; Lou, Hou Keong; Melia, Tom

2017-04-28

We show that ultraperipheral heavy-ion collisions at the Large Hadron Collider (LHC) can be used to search for axionlike particles with mass below 100 GeV. The Z^{4} enhanced photon-photon luminosity from the ions provides a large exclusive production rate, with a signature of a resonant pair of back-to-back photons and no other activity in the detector. In addition, we present both new and updated limits from recasting multiphoton searches at LEP II and the LHC, which are more stringent than those currently in the literature for the mass range 100 MeV to 100 GeV.

Wavefront correction in two-photon microscopy with a multi-actuator adaptive lens.

PubMed

Bueno, Juan M; Skorsetz, Martin; Bonora, Stefano; Artal, Pablo

2018-05-28

A multi-actuator adaptive lens (AL) was incorporated into a multi-photon (MP) microscope to improve the quality of images of thick samples. Through a hill-climbing procedure the AL corrected for the specimen-induced aberrations enhancing MP images. The final images hardly differed when two different metrics were used, although the sets of Zernike coefficients were not identical. The optimized MP images acquired with the AL were also compared with those obtained with a liquid-crystal-on-silicon spatial light modulator. Results have shown that both devices lead to similar images, which corroborates the usefulness of this AL for MP imaging.

Atom-Resonant Heralded Single Photons by Interaction-Free Measurement

NASA Astrophysics Data System (ADS)

Wolfgramm, Florian; de Icaza Astiz, Yannick A.; Beduini, Federica A.; Cerè, Alessandro; Mitchell, Morgan W.

2011-02-01

We demonstrate the generation of rubidium-resonant heralded single photons for quantum memories. Photon pairs are created by cavity-enhanced down-conversion and narrowed in bandwidth to 7 MHz with a novel atom-based filter operating by “interaction-free measurement” principles. At least 94% of the heralded photons are atom-resonant as demonstrated by a direct absorption measurement with rubidium vapor. A heralded autocorrelation measurement shows gc(2)(0)=0.040±0.012, i.e., suppression of multiphoton contributions by a factor of 25 relative to a coherent state. The generated heralded photons can readily be used in quantum memories and quantum networks.

Holes generation in glass using large spot femtosecond laser pulses

NASA Astrophysics Data System (ADS)

Berg, Yuval; Kotler, Zvi; Shacham-Diamand, Yosi

2018-03-01

We demonstrate high-throughput, symmetrical, holes generation in fused silica glass using a large spot size, femtosecond IR-laser irradiation which modifies the glass properties and yields an enhanced chemical etching rate. The process relies on a balanced interplay between the nonlinear Kerr effect and multiphoton absorption in the glass which translates into symmetrical glass modification and increased etching rate. The use of a large laser spot size makes it possible to process thick glasses at high speeds over a large area. We have demonstrated such fabricated holes with an aspect ratio of 1:10 in a 1 mm thick glass samples.

Improved modeling on the RF behavior of InAs/AlSb HEMTs

NASA Astrophysics Data System (ADS)

Guan, He; Lv, Hongliang; Zhang, Yuming; Zhang, Yimen

2015-12-01

The leakage current and the impact ionization effect causes a drawback for the performance of InAs/AlSb HEMTs due to the InAs channel with a very narrow band gap of 0.35 eV. In this paper, the conventional HEMT small-signal model was enhanced to characterize the RF behavior for InAs/AlSb HEMTs. The additional gate leakage current induced by the impact ionization was modeled by adding two resistances RGh1 and RGh2 shunting the Cgs-Ri and Cgd-Rj branches, respectively, and the ionized-drain current was characterized by an additional resistance Rmi parallel with the output resistance Rds, meanwhile the influence of the impact ionization on the transconductance was modeled by an additional current source gmi controlled by Vgs. The additional inductance, evaluated as a function of f(ω, R), was introduced to characterize the frequency dependency of impact ionization by using the impact ionization effective rate 1/τi and a new frequency response rate factor n, which guaranteed the enhanced model reliable for a wide frequency range. As a result, the enhanced model achieved good agreement with the measurements of the S-parameters and Y-parameters for a wide frequency range, moreover, the simulated results of the stability factor K, the cutoff frequency fT, the maximum frequency of oscillation fmax, and the unilateral Mason's gain U were estimated to approach the experimental results with a high degree.

Optical Spectroscopy and Multiphoton Imaging for the Diagnosis and Characterization of Hyperplasias in the Mouse Mammary

DTIC Science & Technology

2006-09-01

was inhibited with 3 - bromopyruvate , which inhibits glyceraldehyde- 3 -phosphate dehydrogenase and 3 -phosphoglycerate kinase in a competitive manner (8...consistent with FAD fluorescence (12). Multiphoton FLIM of NADH showed that 3 - bromopyruvate caused an increase in the fluorescence lifetime of protein...images from 4 dishes), cells treated with 3 - bromopyruvate (n=6 images from 2 dishes), which inhibits glycolysis, and cells treated with CoCl2 (n=6

Multiphoton Process and Anomalous Potential of Cell Membrane by Laser Radiation

NASA Technical Reports Server (NTRS)

Zhang, Kaixi; Zhao, Qingxun; Cui, Zhiyun; Zhar, Ping; Dong, Lifang

1996-01-01

In this paper, by the use of quantum biology and quantum optics, the laser induced potential variation of cell membrane has been studied. Theoretically, we have found a method of calculating the monophoton and multiphoton processes in the formation of the anomalous potential of cell membrane. In contrast with the experimental results, our numerical result is in the same order. Therefore, we have found the possibility of cancer caused by the laser induced anomalous cell potential.

Multiphoton spectroscopy of human skin in vivo

NASA Astrophysics Data System (ADS)

Breunig, Hans G.; Weinigel, Martin; König, Karsten

2012-03-01

In vivo multiphoton-intensity images and emission spectra of human skin are reported. Optical sections from different depths of the epidermis and dermis have been measured with near-infrared laser-pulse excitation. While the intensity images reveal information on the morphology, the spectra show emission characteristics of main endogenous skin fluorophores like keratin, NAD(P)H, melanin, elastin and collagen as well as of second harmonic generation induced by the excitation-light interaction with the dermal collagen network.

All-near-infrared multiphoton microscopy interrogates intact tissues at deeper imaging depths than conventional single- and two-photon near-infrared excitation microscopes

PubMed Central

Sarder, Pinaki; Yazdanfar, Siavash; Akers, Walter J.; Tang, Rui; Sudlow, Gail P.; Egbulefu, Christopher

2013-01-01

Abstract. The era of molecular medicine has ushered in the development of microscopic methods that can report molecular processes in thick tissues with high spatial resolution. A commonality in deep-tissue microscopy is the use of near-infrared (NIR) lasers with single- or multiphoton excitations. However, the relationship between different NIR excitation microscopic techniques and the imaging depths in tissue has not been established. We compared such depth limits for three NIR excitation techniques: NIR single-photon confocal microscopy (NIR SPCM), NIR multiphoton excitation with visible detection (NIR/VIS MPM), and all-NIR multiphoton excitation with NIR detection (NIR/NIR MPM). Homologous cyanine dyes provided the fluorescence. Intact kidneys were harvested after administration of kidney-clearing cyanine dyes in mice. NIR SPCM and NIR/VIS MPM achieved similar maximum imaging depth of ∼100  μm. The NIR/NIR MPM enabled greater than fivefold imaging depth (>500  μm) using the harvested kidneys. Although the NIR/NIR MPM used 1550-nm excitation where water absorption is relatively high, cell viability and histology studies demonstrate that the laser did not induce photothermal damage at the low laser powers used for the kidney imaging. This study provides guidance on the imaging depth capabilities of NIR excitation-based microscopic techniques and reveals the potential to multiplex information using these platforms. PMID:24150231

Compensation of temporal and spatial dispersion for multiphoton acousto-optic laser-scanning microscopy

NASA Astrophysics Data System (ADS)

Iyer, Vijay; Saggau, Peter

2003-10-01

In laser-scanning microscopy, acousto-optic (AO) deflection provides a means to quickly position a laser beam to random locations throughout the field-of-view. Compared to conventional laser-scanning using galvanometer-driven mirrors, this approach increases the frame rate and signal-to-noise ratio, and reduces time spent illuminating sites of no interest. However, random-access AO scanning has not yet been combined with multi-photon microscopy, primarily because the femtosecond laser pulses employed are subject to significant amounts of both spatial and temporal dispersion upon propagation through common AO materials. Left uncompensated, spatial dispersion reduces the microscope"s spatial resolution while temporal dispersion reduces the multi-photon excitation efficacy. In previous work, we have demonstrated, 1) the efficacy of a single diffraction grating scheme which reduces the spatial dispersion at least 3-fold throughout the field-of-view, and 2) the use of a novel stacked-prism pre-chirper for compensating the temporal dispersion of a pair of AODs using a shorter mechanical path length (2-4X) than standard prism-pair arrangements. In this work, we demonstrate for the first time the use of these compensation approaches with a custom-made large-area slow-shear TeO2 AOD specifically suited for the development of a high-resolution 2-D random-access AO scanning multi-photon laser-scanning microscope (AO-MPLSM).

Video-rate resonant scanning multiphoton microscopy

PubMed Central

Kirkpatrick, Nathaniel D.; Chung, Euiheon; Cook, Daniel C.; Han, Xiaoxing; Gruionu, Gabriel; Liao, Shan; Munn, Lance L.; Padera, Timothy P.; Fukumura, Dai; Jain, Rakesh K.

2013-01-01

The abnormal tumor microenvironment fuels tumor progression, metastasis, immune suppression, and treatment resistance. Over last several decades, developments in and applications of intravital microscopy have provided unprecedented insights into the dynamics of the tumor microenvironment. In particular, intravital multiphoton microscopy has revealed the abnormal structure and function of tumor-associated blood and lymphatic vessels, the role of aberrant tumor matrix in drug delivery, invasion and metastasis of tumor cells, the dynamics of immune cell trafficking to and within tumors, and gene expression in tumors. However, traditional multiphoton microscopy suffers from inherently slow imaging rates—only a few frames per second, thus unable to capture more rapid events such as blood flow, lymphatic flow, and cell movement within vessels. Here, we report the development and implementation of a video-rate multiphoton microscope (VR-MPLSM) based on resonant galvanometer mirror scanning that is capable of recording at 30 frames per second and acquiring intravital multispectral images. We show that the design of the system can be readily implemented and is adaptable to various experimental models. As examples, we demonstrate the utility of the system to directly measure flow within tumors, capture metastatic cancer cells moving within the brain vasculature and cells in lymphatic vessels, and image acute responses to changes in a vascular network. VR-MPLSM thus has the potential to further advance intravital imaging and provide new insight into the biology of the tumor microenvironment. PMID:24353926

Single-photon counting multicolor multiphoton fluorescence microscope.

PubMed

Buehler, Christof; Kim, Ki H; Greuter, Urs; Schlumpf, Nick; So, Peter T C

2005-01-01

We present a multicolor multiphoton fluorescence microscope with single-photon counting sensitivity. The system integrates a standard multiphoton fluorescence microscope, an optical grating spectrograph operating in the UV-Vis wavelength region, and a 16-anode photomultiplier tube (PMT). The major technical innovation is in the development of a multichannel photon counting card (mC-PhCC) for direct signal collection from multi-anode PMTs. The electronic design of the mC-PhCC employs a high-throughput, fully-parallel, single-photon counting scheme along with a high-speed electrical or fiber-optical link interface to the data acquisition computer. There is no electronic crosstalk among the detection channels of the mC-PhCC. The collected signal remains linear up to an incident photon rate of 10(8) counts per second. The high-speed data interface offers ample bandwidth for real-time readout: 2 MByte lambda-stacks composed of 16 spectral channels, 256 x 256 pixel image with 12-bit dynamic range can be transferred at 30 frames per second. The modular design of the mC-PhCC can be readily extended to accommodate PMTs of more anodes. Data acquisition from a 64-anode PMT has been verified. As a demonstration of system performance, spectrally resolved images of fluorescent latex spheres and ex-vivo human skin are reported. The multicolor multiphoton microscope is suitable for highly sensitive, real-time, spectrally-resolved three-dimensional imaging in biomedical applications.

Visualizing radiofrequency-skin interaction using multiphoton microscopy in vivo.

PubMed

Tsai, Tsung-Hua; Lin, Sung-Jan; Lee, Woan-Ruoh; Wang, Chun-Chin; Hsu, Chih-Ting; Chu, Thomas; Dong, Chen-Yuan

2012-02-01

Redundant skin laxity is a major feature of aging. Recently, radiofrequency has been introduced for nonablative tissue tightening by volumetric heating of the deep dermis. Despite the wide range of application based on this therapy, the effect of this technique on tissue and the subsequent tissue remodeling have not been investigated in detail. Our objective is to evaluate the potential of non-linear optics, including multiphoton autofluorescence and second harmonic generation (SHG) microscopy, as a non-invasive imaging modality for the real-time study of radiofrequency-tissue interaction. Electro-optical synergy device (ELOS) was used as the radiofrequency source in this study. The back skin of nude mouse was irradiated with radiofrequency at different passes. We evaluated the effect on skin immediately and 1 month after treatment with multiphoton microscopy. Corresponding histology was performed for comparison. We found that SHG is negatively correlated to radiofrequency passes, which means that collagen structural disruption happens immediately after thermal damage. After 1 month of collagen remodeling, SHG signals increased above baseline, indicating that collagen regeneration has occurred. Our findings may explain mechanism of nonablative skin tightening and were supported by histological examinations. Our work showed that monitoring the dermal heating status of RF and following up the detailed process of tissue reaction can be imaged and quantified with multiphoton microscopy non-invasively in vivo. Copyright © 2011. Published by Elsevier Ireland Ltd.

Resonant Pump-dump Quantum Control of Solvated Dye Molecules with Phase Jumps

NASA Astrophysics Data System (ADS)

Konar, Arkaprabha; Lozovoy, Vadim; Dantus, Marcos

2014-03-01

Quantum coherent control of two photon and multiphoton excitation processes in atomic and condensed phase systems employing phase jumps has been well studied and understood. Here we demonstrate coherent quantum control of a two photon resonant pump-dump process in a complex solvated dye molecule. Phase jump in the frequency domain via a pulse shaper is employed to coherently enhance the stimulated emission by an order of magnitude when compared to transform limited pulses. Red shifted stimulated emission from successive low energy Stokes shifted excited states leading to narrowband emission are observed upon scanning the pi step across the excitation spectrum. A binary search space routine was also employed to investigate the effects of other types of phase jumps on stimulated emission and to determine the optimum phase that maximizes the emission. Understanding the underlying mechanism of this kind of enhancement will guide us in designing pulse shapes for enhancing stimulated emission, which can be further applied in the field of imaging.