High-rotational symmetry lattices fabricated by moiré nanolithography.

PubMed

Lubin, Steven M; Zhou, Wei; Hryn, Alexander J; Huntington, Mark D; Odom, Teri W

2012-09-12

This paper describes a new nanofabrication method, moiré nanolithography, that can fabricate subwavelength lattices with high-rotational symmetries. By exposing elastomeric photomasks sequentially at multiple offset angles, we created arrays with rotational symmetries as high as 36-fold, which is three times higher than quasiperiodic lattices (≤12-fold) and six times higher than two-dimensional periodic lattices (≤6-fold). Because these moiré nanopatterns can be generated over wafer-scale areas, they are promising for a range of photonic applications, especially those that require broadband, omnidirectional absorption of visible light.

Exciton absorption of entangled photons in semiconductor quantum wells

NASA Astrophysics Data System (ADS)

Rodriguez, Ferney; Guzman, David; Salazar, Luis; Quiroga, Luis; Condensed Matter Physics Group Team

2013-03-01

The dependence of the excitonic two-photon absorption on the quantum correlations (entanglement) of exciting biphotons by a semiconductor quantum well is studied. We show that entangled photon absorption can display very unusual features depending on space-time-polarization biphoton parameters and absorber density of states for both bound exciton states as well as for unbound electron-hole pairs. We report on the connection between biphoton entanglement, as quantified by the Schmidt number, and absorption by a semiconductor quantum well. Comparison between frequency-anti-correlated, unentangled and frequency-correlated biphoton absorption is addressed. We found that exciton oscillator strengths are highly increased when photons arrive almost simultaneously in an entangled state. Two-photon-absorption becomes a highly sensitive probe of photon quantum correlations when narrow semiconductor quantum wells are used as two-photon absorbers. Research funds from Facultad de Ciencias, Universidad de los Andes

Picosecond absorption spectroscopy of self-trapped excitons and transient Ce states in LaBr3 and LaBr3:Ce

NASA Astrophysics Data System (ADS)

Li, Peiyun; Gridin, Sergii; Ucer, K. Burak; Williams, Richard T.; Menge, Peter R.

2018-04-01

Picosecond time-resolved optical absorption spectra induced by two-photon interband excitation of LaBr3 are reported. The spectra are similar in general characteristics to self-trapped exciton (STE) absorption previously measured in alkali halides and alkaline-earth halides. A broad ultraviolet absorption band results from excitation of the self-trapped hole within the STE. A series of infrared and red-visible bands results from excitation of the bound outer electron within the STE similar to bands found in alkali halides corresponding to different degrees of "off-center" relaxation. Induced absorption in cerium-doped LaBr3 after band-gap excitation of the host exhibits similar STE spectra, except it decays faster on the tens-of-picoseconds scale in proportion to the Ce concentration. This is attributed to dipole-dipole energy transfer from STE to Ce3 + dopant ions. The absorption spectra were also measured after direct excitation of the Ce3 + ions with sufficient intensity to drive two- and three-photon resonantly enhanced excitation. In this case, the spectrum attributed to STEs created adjacent to Ce3 + ions decays in 1 ps suggesting dipole-dipole transfer from the nearest-neighbor separation. A transient absorption band at 2.1 eV growing with Ce concentration is found and attributed to a charge-transfer excitation of the Ce3 +* excited state responsible for scintillation in LaBr3:Ce crystals. This study concludes that the energy transport from host to activator responsible for the scintillation of LaBr3:Ce proceeds by STE creation and dipole-dipole transfer more than by sequential trapping of holes and electrons on Ce3 + ions.

Sequential double photodetachment of He- in elliptically polarized laser fields

NASA Astrophysics Data System (ADS)

Génévriez, Matthieu; Dunseath, Kevin M.; Terao-Dunseath, Mariko; Urbain, Xavier

2018-02-01

Four-photon double detachment of the helium negative ion is investigated experimentally and theoretically for photon energies where the transient helium atom is in the 1 s 2 s 3S or 1 s 2 p P3o states, which subsequently ionize by absorption of three photons. Ionization is enhanced by intermediate resonances, giving rise to series of peaks in the He+ spectrum, which we study in detail. The He+ yield is measured in the wavelength ranges from 530 to 560 nm and from 685 to 730 nm and for various polarizations of the laser light. Double detachment is treated theoretically as a sequential process, within the framework of R -matrix theory for the first step and effective Hamiltonian theory for the second step. Experimental conditions are accurately modeled, and the measured and simulated yields are in good qualitative and, in some cases, quantitative agreement. Resonances in the double detachment spectra can be attributed to well-defined Rydberg states of the transient atom. The double detachment yield exhibits a strong dependence on the laser polarization which can be related to the magnetic quantum number of the intermediate atomic state. We also investigate the possibility of nonsequential double detachment with a two-color experiment but observe no evidence for it.

Two-photon absorption by spectrally shaped entangled photons

NASA Astrophysics Data System (ADS)

Oka, Hisaki

2018-03-01

We theoretically investigate two-photon excitation by spectrally shaped entangled photons with energy anticorrelation in terms of how the real excitation of an intermediate state affects two-photon absorption by entangled photons. Spectral holes are introduced in the entangled photons around the energy levels of an intermediate state so that two-step excitation via the real excitation of the intermediated state can be suppressed. Using a three-level atomic system as an example, we show that the spectral holes well suppress the real excitation of the intermediate state and recover two-photon absorption via a virtual state. Furthermore, for a short pulse close to a monocycle, we show that the excitation efficiency by the spectrally shaped entangled photons can be enhanced a thousand times as large as that by uncorrelated photons.

Absorption bleaching of squarylium dye J aggregates via a two-photon excitation process

NASA Astrophysics Data System (ADS)

Furuki, Makoto; Tian, Minquan; Sato, Yasuhiro; Pu, Lyong Sun; Tatsuura, Satoshi; Abe, Shuji

2001-08-01

Squarylium dye J aggregates exhibit ultrafast nonlinear optical response of absorption saturation at the resonant wavelength of 770 nm. We studied the two-photon excitation process of J aggregates. By fluorescence measurement, we found the two-photon absorption band at 1.3 μm, which was different from that of the dye solution at 1.2 μm. Absorption saturation at 770 nm via a two-photon excitation process was observed by two-photon resonant excitation at 1.3 μm and also by off-resonant excitation at 1.55 μm, suggesting the possibility of J aggregates for optical switching materials working at the wavelength used in optical communications.

Sub-diffraction limit laser ablation via multiple exposures using a digital micromirror device.

PubMed

Heath, Daniel J; Grant-Jacob, James A; Feinaeugle, Matthias; Mills, Ben; Eason, Robert W

2017-08-01

We present the use of digital micromirror devices as variable illumination masks for pitch-splitting multiple exposures to laser machine the surfaces of materials. Ultrafast laser pulses of length 150 fs and 800 nm central wavelength were used for the sequential machining of contiguous patterns on the surface of samples in order to build up complex structures with sub-diffraction limit features. Machined patterns of tens to hundreds of micrometers in lateral dimensions with feature separations as low as 270 nm were produced in electroless nickel on an optical setup diffraction limited to 727 nm, showing a reduction factor below the Abbe diffraction limit of ∼2.7×. This was compared to similar patterns in a photoresist optimized for two-photon absorption, which showed a reduction factor of only 2×, demonstrating that multiple exposures via ablation can produce a greater resolution enhancement than via two-photon polymerization.

Two-Photon Activation of p-Hydroxyphenacyl Phototriggers: Toward Spatially Controlled Release of Diethyl Phosphate and ATP.

PubMed

Houk, Amanda L; Givens, Richard S; Elles, Christopher G

2016-03-31

Two-photon activation of the p-hydroxyphenacyl (pHP) photoactivated protecting group is demonstrated for the first time using visible light at 550 nm from a pulsed laser. Broadband two-photon absorption measurements reveal a strong two-photon transition (>10 GM) near 4.5 eV that closely resembles the lowest-energy band at the same total excitation energy in the one-photon absorption spectrum of the pHP chromophore. The polarization dependence of the two-photon absorption band is consistent with excitation to the same S3 ((1)ππ*) excited state for both one- and two-photon activation. Monitoring the progress of the uncaging reaction under nonresonant excitation at 550 nm confirms a quadratic intensity dependence and that two-photon activation of the uncaging reaction is possible using visible light in the range 500-620 nm. Deprotonation of the pHP chromophore under mildly basic conditions shifts the absorption band to lower energy (3.8 eV) in both the one- and two-photon absorption spectra, suggesting that two-photon activation of the pHP chromophore may be possible using light in the range 550-720 nm. The results of these measurements open the possibility of spatially and temporally selective release of biologically active compounds from the pHP protecting group using visible light from a pulsed laser.

Two-photon absorption measurements of deep UV transmissible materials at 213 nm

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

Patankar, S.; Yang, S. T.; Moody, J. D.

We report on two photon absorption measurements at 213nm of deep UV transmissible media including LiF, MgF 2, CaF 2, BaF 2, Sapphire (Al 2O 3) and high purity grades of fused-silica (SiO 2). A high stability 24ps Nd:YAG laser operating at the 5th harmonic (213nm) was used to generate a high intensity, long Rayleigh length Gaussian focus inside the samples. The measurements of the Fluoride crystals and Sapphire indicate two photon absorption coefficients between 0.004 and 0.82 cm/GW. We find that different grades of fused silica performed near identically for two photon absorption, however, there are differences in linearmore » losses associated with purity. A low two photon absorption cross section is measured for MgF 2 making it an ideal material for the propagation of high intensity deep UV lasers.« less

Two-photon absorption measurements of deep UV transmissible materials at 213 nm

DOE PAGES

Patankar, S.; Yang, S. T.; Moody, J. D.; ...

2017-09-19

We report on two photon absorption measurements at 213nm of deep UV transmissible media including LiF, MgF 2, CaF 2, BaF 2, Sapphire (Al 2O 3) and high purity grades of fused-silica (SiO 2). A high stability 24ps Nd:YAG laser operating at the 5th harmonic (213nm) was used to generate a high intensity, long Rayleigh length Gaussian focus inside the samples. The measurements of the Fluoride crystals and Sapphire indicate two photon absorption coefficients between 0.004 and 0.82 cm/GW. We find that different grades of fused silica performed near identically for two photon absorption, however, there are differences in linearmore » losses associated with purity. A low two photon absorption cross section is measured for MgF 2 making it an ideal material for the propagation of high intensity deep UV lasers.« less

Upconversion single-microbelt photodetector via two-photon absorption simultaneous

NASA Astrophysics Data System (ADS)

Lou, Guanlin; Wu, Yanyan; Zhu, Hai; Li, Jinyu; Chen, Anqi; Chen, Zhiyang; Liang, Yunfeng; Ren, Yuhao; Gui, Xuchun; Zhong, Dingyong; Qiu, Zhiren; Tang, Zikang; Su, Shi C.

2018-05-01

Single microbelt (MB) photodetectors with metal–semiconductor-metal structure have been demonstrated and characterized comprehensively. For single-photon absorption, the maximum responsivity of ZnO-MB photodetector can reach as high as 1.4  ×  105 A W‑1 at 20 V bias. The results about photoresponse of MB-detector reveals that two relaxation mechanisms contribute to the carrier decay time. Moreover, the two-photon absorption upconversion photoresponsivity in the single-MB detector has also been realized, which is the first report about the two-photon absorption detector to the best of our knowledge. The excellent two-photon absorption photoresponsivity characteristic of the MB device can be available not only for detector but also for solar cell and biomedical imaging. The above results present a significant step towards future fabrication of single micro/nano-structure based multiphoton excitation optoelectronic devices.

Two-photon absorption measurements of deep UV transmissible materials at 213  nm.

PubMed

Patankar, S; Yang, S T; Moody, J D; Swadling, G F; Erlandson, A C; Bayramian, A J; Barker, D; Datte, P; Acree, R L; Pepmeier, B; Madden, R E; Borden, M R; Ross, J S

2017-10-20

We report on two-photon absorption measurements at 213 nm of deep UV transmissible media, including LiF, MgF 2 , CaF 2 , BaF 2 , sapphire (Al 2 O 3 ), and high-purity grades of fused-silica (SiO 2 ). A high-stability 24 ps Nd:YAG laser operating at the 5th harmonic (213 nm) was used to generate a high-intensity, long-Rayleigh-length Gaussian focus inside the samples. The measurements of the fluoride crystals and sapphire indicate two-photon absorption coefficients between 0.004 and 0.82 cm/GW. We find that different grades of fused silica performed near identically for two-photon absorption; however, there are differences in linear losses associated with purity. A low two-photon absorption cross section is measured for MgF 2 , making it an ideal material for the propagation of high-intensity deep UV lasers.

Quantum Entanglement Molecular Absorption Spectrum Simulator

NASA Technical Reports Server (NTRS)

Nguyen, Quang-Viet; Kojima, Jun

2006-01-01

Quantum Entanglement Molecular Absorption Spectrum Simulator (QE-MASS) is a computer program for simulating two photon molecular-absorption spectroscopy using quantum-entangled photons. More specifically, QE-MASS simulates the molecular absorption of two quantum-entangled photons generated by the spontaneous parametric down-conversion (SPDC) of a fixed-frequency photon from a laser. The two-photon absorption process is modeled via a combination of rovibrational and electronic single-photon transitions, using a wave-function formalism. A two-photon absorption cross section as a function of the entanglement delay time between the two photons is computed, then subjected to a fast Fourier transform to produce an energy spectrum. The program then detects peaks in the Fourier spectrum and displays the energy levels of very short-lived intermediate quantum states (or virtual states) of the molecule. Such virtual states were only previously accessible using ultra-fast (femtosecond) laser systems. However, with the use of a single-frequency continuous wave laser to produce SPDC photons, and QEMASS program, these short-lived molecular states can now be studied using much simpler laser systems. QE-MASS can also show the dependence of the Fourier spectrum on the tuning range of the entanglement time of any externally introduced optical-path delay time. QE-MASS can be extended to any molecule for which an appropriate spectroscopic database is available. It is a means of performing an a priori parametric analysis of entangled photon spectroscopy for development and implementation of emerging quantum-spectroscopic sensing techniques. QE-MASS is currently implemented using the Mathcad software package.

Mid-infrared two-photon absorption in an extended-wavelength InGaAs photodetector

NASA Astrophysics Data System (ADS)

Piccardo, Marco; Rubin, Noah A.; Meadowcroft, Lauren; Chevalier, Paul; Yuan, Henry; Kimchi, Joseph; Capasso, Federico

2018-01-01

We investigate the nonlinear optical response of a commercial extended-wavelength In0.81Ga0.19As uncooled photodetector. Degenerate two-photon absorption in the mid-infrared range is observed using a quantum cascade laser emitting at λ = 4.5 μm as the excitation source. From the measured two-photon photocurrent signal, we extract a two-photon absorption coefficient β(2) = 0.6 ± 0.2 cm/MW, in agreement with the theoretical value obtained from the Eg-3 scaling law. Considering the wide spectral range covered by extended-wavelength InxGa1-xAs alloys, this result holds promise for applications based on two-photon absorption for this family of materials at wavelengths between 1.8 and 5.6 μm.

Two-photon absorption resonance in 3-(1,1-dicyanoethenyl)-1-phenyl-4,5-dihydro-1H-pyrazole (DCNP)

NASA Astrophysics Data System (ADS)

Miniewicz, Andrzej; Delysse, Stéphane; Nunzi, Jean-Michel; Kajzar, François

1998-04-01

A two-photon absorption spectrum of 3-(1,1-dicyanoethenyl)-1-phenyl-4,5-dihydro-1H-pyrazole (DCNP) in tetrahydrofuran solution has been studied by the Kerr ellipsometry technique. The spectral shape and amplitude of the imaginary part of the dominant molecular hyperpolarizability term Im( γXXXX) is compared with the relevant linear absorption spectrum within a simple two-level model. Agreement between the measured γXXXX=2.0×10 -48 m 5 V -2 and calculated γXXXX=(1.2-1.5)×10 -48 m 5 V -2 two-photon absorption molecular hyperpolarizabilties in the vicinity of the two-photon resonance transition is satisfactory.

Two Photon Absorption in II-VI Semiconductors: The Influence of Dimensionality and Size.

PubMed

Scott, Riccardo; Achtstein, Alexander W; Prudnikau, Anatol; Antanovich, Artsiom; Christodoulou, Sotirios; Moreels, Iwan; Artemyev, Mikhail; Woggon, Ulrike

2015-08-12

We report a comprehensive study on the two-photon absorption cross sections of colloidal CdSe nanoplatelets, -rods, and -dots of different sizes by the means of z-scan and two-photon excitation spectroscopy. Platelets combine large particle volumes with ultra strong confinement. In contrast to weakly confined nanocrystals, the TPA cross sections of CdSe nanoplatelets scale superlinearly with volume (V(∼2)) and show ten times more efficient two-photon absorption than nanorods or dots. This unexpectedly strong shape dependence goes well beyond the effect of local fields. The larger the particles' aspect ratio, the greater is the confinement related electronic contribution to the increased two-photon absorption. Both electronic confinement and local field effects favor the platelets and make them unique two-photon absorbers with outstanding cross sections of up to 10(7) GM, the largest ever reported for (colloidal) semiconductor nanocrystals and ideally suited for two-photon imaging and nonlinear optoelectronics. The obtained results are confirmed by two independent techniques as well as a new self-referencing method.

Pseudopotential calculations and photothermal lensing measurements of two-photon absorption in solids

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

White, W.T. III

1985-11-04

We have studied two-photon absorption in solids theoretically and experimentally. We have shown that it is possible to use accurate band structure techniques to compute two-photon absorption spectra within 15% of measured values in a wide band-gap material, ZnS. The empirical pseudopotential technique that we used is significantly more accurate than previous models of two-photon absorption in zinc blende materials, including present tunneling theories (which are essentially parabolic-band results in disguise) and the nonparabolic-band formalism of Pidgeon et al. and Weiler. The agreement between our predictions and previous measurements allowed us to use ZnS as a reference material in ordermore » to validate a technique for measuring two-photon absorption that was previously untried in solids, pulsed dual-beam thermal lensing. With the validated technique, we examined nonlinear absorption in one other crystal (rutile) and in several glasses, including silicates, borosilicates, and one phosphate glass. Initially, we believed that the absorption edges of all the materials were comparable; however, subsequent evidence suggested that the effective band-gap energies of the glasses were above the energy of two photons in our measurement. Therefore, we attribute the nonlinear absorption that we observed in glasses to impurities or defects. The measured nonlinear absorption coefficients were of the order of a few cm/TW in the glasses and of the order of 10 cm/GW in the crystals, four orders of magnitude higher than in glasses. 292 refs.« less

Two-photon absorption of [2.2]paracyclophane derivatives in solution: A theoretical investigation

NASA Astrophysics Data System (ADS)

Ferrighi, Lara; Frediani, Luca; Fossgaard, Eirik; Ruud, Kenneth

2007-12-01

The two-photon absorption of a class of [2.2]paracyclophane derivatives has been studied using quadratic response and density functional theories. For the molecules investigated, several effects influencing the two-photon absorption spectra have been investigated, such as side-chain elongation, hydrogen bonding, the use of ionic species, and solvent effects, the latter described by the polarizable continuum model. The calculations have been carried out using a recent parallel implementation of the polarizable continuum model in the DALTON code. Special attention is given to those aspects that could explain the large solvent effect on the two-photon absorption cross sections observed experimentally for this class of compounds.

Preparation, one- and two-photon properties of carbazole derivatives containing nitrogen heterocyclic ring

NASA Astrophysics Data System (ADS)

Zhang, Yichi; Wang, Ping; Li, Liang; Chen, Zhimin; He, Chunying; Wu, Yiqun

Preparation of recording materials with high two-photon absorption activities is one of the important issues to superhigh- density two-photon absorption (TPA) three-dimensional (3D) optical data storage. In this paper, three new carbazole derivatives containing nitrogen heterocyclic ring with symmetric and asymmetric structures are prepared using ethylene as the π bridge between the carbazole unit and nitrogen heterocyclic ring, namely, 9-butyl-3-(2-(1,8- naphthyridin)vinyl)-carbazole (material 1), 9-butyl-3,6-bis(2-(1,8-naphthyl)vinyl)-carbazole (material 2) and 9-butyl-3,6- bis(2-(quinolin)vinyl)-carbazole (material 3). Their one photon properties including linear absorption spectra, fluorescence emission spectra, and fluorescence quantum yields are studied. The fluorescence excited by 120 fs pulse at 800 nm Ti: sapphire laser operating at 1 kHz repetition rate with different incident powers of 9-butyl-3-(2-(quinolin) vinyl)-carbazole (material 3) was investigated, and two-photon absorption cross-sections has been obtained. It is shown that material 3 containing quinoline rings as electron acceptor with symmetric structure exhibit high two-photon absorption activity. The result implies that material 3 (9-butyl-3-(2-(quinolin) vinyl)-carbazole) is a good candidate as a promising recording material for super-high-density two-photon absorption (TPA) three-dimensional (3D) optical data storage. The influence of chemical structure of the materials on the optical properties is discussed.

Two-photon absorption in layered transition metal dichalcogenides

NASA Astrophysics Data System (ADS)

Dong, Ningning; Zhang, Saifeng; Li, Yuanxin; Wang, Jun

2018-02-01

Two-dimensional (2D) layered transition metal dichalcogenides (TMDCs) exhibit unique nonlinear optical (NLO) features and have becoming intriguing and promising candidate materials for photonic and optoelectronic devices with high performance and unique functions. Owing to layered geometry and the thickness-dependent bandgap, we studied the ultrafast NLO properties of a range of TMDCs. TMDCs with high-quality layered nanosheets were prepared through chemical vapor deposition (CVD) technique and vapor-phase growth method. Saturable absorption, two photon absorption (TPA) and two photon pumped frequency up-converted luminescence were observed from these 2D nanostructures. The exciting results open up the door to 2D photonic devices, such as passive mode-lockers, Q-switchers, optical limiters, light emitters, etc.

Mammographic x-ray unit kilovoltage test tool based on k-edge absorption effect.

PubMed

Napolitano, Mary E; Trueblood, Jon H; Hertel, Nolan E; David, George

2002-09-01

A simple tool to determine the peak kilovoltage (kVp) of a mammographic x-ray unit has been designed. Tool design is based on comparing the effect of k-edge discontinuity of the attenuation coefficient for a series of element filters. Compatibility with the mammography accreditation phantom (MAP) to obtain a single quality control film is a second design objective. When the attenuation of a series of sequential elements is studied simultaneously, differences in the absorption characteristics due to the k-edge discontinuities are more evident. Specifically, when the incident photon energy is higher than the k-edge energy of a number of the elements and lower than the remainder, an inflection may be seen in the resulting attenuation data. The maximum energy of the incident photon spectra may be determined based on this inflection point for a series of element filters. Monte Carlo photon transport analysis was used to estimate the photon transmission probabilities for each of the sequential k-edge filter elements. The photon transmission corresponds directly to optical density recorded on mammographic x-ray film. To observe the inflection, the element filters chosen must have k-edge energies that span a range greater than the expected range of the end point energies to be determined. For the design, incident x-ray spectra ranging from 25 to 40 kVp were assumed to be from a molybdenum target. Over this range, the k-edge energy changes by approximately 1.5 keV between sequential elements. For this design 21 elements spanning an energy range from 20 to 50 keV were chosen. Optimum filter element thicknesses were calculated to maximize attenuation differences at the k-edge while maintaining optical densities between 0.10 and 3.00. Calculated relative transmission data show that the kVp could be determined to within +/-1 kV. To obtain experimental data, a phantom was constructed containing 21 different elements placed in an acrylic holder. MAP images were used to determine appropriate exposure techniques for a series of end point energies from 25 to 35 kVp. The average difference between the kVp determination and the calibrated dial setting was 0.8 and 1.0 kV for a Senographe 600 T and a Senographe DMR, respectively. Since the k-edge absorption energies of the filter materials are well known, independent calibration or a series of calibration curves is not required.

Two-photon absorption of soft X-ray free electron laser radiation by graphite near the carbon K-absorption edge

NASA Astrophysics Data System (ADS)

Lam, Royce K.; Raj, Sumana L.; Pascal, Tod A.; Pemmaraju, C. D.; Foglia, Laura; Simoncig, Alberto; Fabris, Nicola; Miotti, Paolo; Hull, Christopher J.; Rizzuto, Anthony M.; Smith, Jacob W.; Mincigrucci, Riccardo; Masciovecchio, Claudio; Gessini, Alessandro; De Ninno, Giovanni; Diviacco, Bruno; Roussel, Eleonore; Spampinati, Simone; Penco, Giuseppe; Di Mitri, Simone; Trovò, Mauro; Danailov, Miltcho B.; Christensen, Steven T.; Sokaras, Dimosthenis; Weng, Tsu-Chien; Coreno, Marcello; Poletto, Luca; Drisdell, Walter S.; Prendergast, David; Giannessi, Luca; Principi, Emiliano; Nordlund, Dennis; Saykally, Richard J.; Schwartz, Craig P.

2018-07-01

We have examined the transmission of soft X-ray pulses from the FERMI free electron laser through carbon films of varying thickness, quantifying nonlinear effects of pulses above and below the carbon K-edge. At typical of soft X-ray free electron laser intensities, pulses exhibit linear absorption at photon energies above and below the K-edge, ∼308 and ∼260 eV, respectively; whereas two-photon absorption becomes significant slightly below the K-edge, ∼284.2 eV. The measured two-photon absorption cross section at 284.18 eV (∼6 × 10-48 cm4 s) is 7 orders of magnitude above what is expected from a simple theory based on hydrogen-like atoms - a result of resonance effects.

Counterfactual Rydberg gate for photons

NASA Astrophysics Data System (ADS)

Garcia-Escartin, Juan Carlos; Chamorro-Posada, Pedro

2012-03-01

Quantum computation with photons requires efficient two-photon gates. We put forward a two-photon entangling gate which uses an intermediate atomic system. The system includes a single Rydberg atom which can switch on and off photon absorption in an ensemble using the dipole blockade. The gate is based in a counterfactual protocol. The mere possibility of an absorption that can only occur with a vanishing probability steers the photons to the desired final state.

Nonsequential two-photon absorption from the K shell in solid zirconium

DOE PAGES

Ghimire, Shambhu; Fuchs, Matthias; Hastings, Jerry; ...

2016-10-21

Here, we report the observation of nonsequential two-photon absorption from the K shell of solid Zr (atomic number Z=40) using intense x-ray pulses from the Spring-8 Angstrom Compact Free-Electron Laser (SACLA). We determine the generalized nonlinear two-photon absorption cross section at the two-photon threshold in the range of 3.9–57 ×10 –60 cm 4s bounded by the estimated uncertainty in the absolute intensity. The lower limit is consistent with the prediction of 3.1 ×10 –60 cm 4s from the nonresonant Z –6 scaling for hydrogenic ions in the nonrelativistic, dipole limit.

Development of novel two-photon absorbing chromophores

NASA Astrophysics Data System (ADS)

Rogers, Joy E.; Slagle, Jonathan E.; McLean, Daniel G.; Sutherland, Richard L.; Krein, Douglas M.; Cooper, Thomas M.; Brant, Mark; Heinrichs, James; Kannan, Ramamurthi; Tan, Loon-Seng; Urbas, Augustine M.; Fleitz, Paul A.

2006-08-01

There has been much interest in the development of two-photon absorbing materials and many efforts to understand the nonlinear absorption properties of these dyes but this area is still not well understood. A computational model has been developed in our lab to understand the nanosecond nonlinear absorption properties that incorporate all of the measured one-photon photophysical parameters of a class of materials called AFX. We have investigated the nonlinear and photophysical properties of the AFX chromophores including the two-photon absorption cross-section, the excited state cross-section, the intersystem crossing quantum yield, and the singlet and triplet excited state lifetimes using a variety of experimental techniques that include UV-visible, fluorescence and phosphorescence spectroscopy, time correlated single photon counting, ultrafast transient absorption, and nanosecond laser flash photolysis. The model accurately predicts the nanosecond nonlinear transmittance data using experimentally measured parameters. Much of the strong nonlinear absorption has been shown to be due to excited state absorption from both the singlet and triplet excited states. Based on this understanding of the nonlinear absorption and the importance of singlet and triplet excited states we have begun to develop new two-photon absorbing molecules within the AFX class as well as linked to other classes of nonlinear absorbing molecules. This opens up the possibilities of new materials with unique and interesting properties. Specifically we have been working on a new class of two-photon absorbing molecules linked to platinum poly-ynes. In the platinum poly-yne chromophores the photophysics are more complicated and we have just started to understand what drives both the linear and non-linear photophysical properties.

Dual photon effects in nitrogen dioxide photolysis

NASA Technical Reports Server (NTRS)

Hakala, D.; Harteck, P.; Reeves, R. R.

1974-01-01

A previous study demonstrated two-photon consecutive absorption as being the most probable mechanism for the photodissociation of NO2 using a pulsed ruby laser at 6943 A. Additional data discussed here confirmed this and also examined an associated phenomenon, that of multiphoton induced fluorescence. The dissociation of NO2 by ON-O bond cleavage requires 3.4 eV, while the laser energy corresponds to 1.785 eV. The pooling of the energy of two photons would give more than enough energy to dissociate the NO2 into NO + O. Several mechanisms including (1) simultaneous absorption of two photons; (2) reaction of two singly excited NO2; (3) reaction of a singly excited NO2 with a ground state NO2; and (4) consecutive absorption of two photons were examined.

Dual Mechanism Nonlinear Response of Selected Metal Organic Chromophores

DTIC Science & Technology

2007-10-01

emission was observed due to the high quantum efficiency of the free ligand despite having a relatively low two photon cross section at this wavelength...nonlinear absorbing chromophores. .............................30 2-1 Beer’s Law relationships of linear absorption...optical processes; (4) structure-property relationships of nonlinear absorption as it relates to two photon absorption and reverse saturable absorption

Two-Photon Absorption of Soft X-Ray Free Electron Laser Radiation by Graphite Near the Carbon K-Absorption Edge

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

Christensen, Steven T; Lam, Royce K.; Raj, Sumana L.

We have examined the transmission of soft X-ray pulses from the FERMI free electron laser through carbon films of varying thickness, quantifying nonlinear effects of pulses above and below the carbon K-edge. At typical of soft X-ray free electron laser intensities, pulses exhibit linear absorption at photon energies above and below the K-edge, ~308 and ~260 eV, respectively; whereas two-photon absorption becomes significant slightly below the K-edge, ~284.2 eV. The measured two-photon absorption cross section at 284.18 eV (~6 x 10-48 cm4 s) is 7 orders of magnitude above what is expected from a simple theory based on hydrogen-like atomsmore » - a result of resonance effects.« less

Vibrational spectra and structures of neutral Si(m)C(n) clusters (m + n = 6): sequential doping of silicon clusters with carbon atoms.

PubMed

Savoca, Marco; Lagutschenkov, Anita; Langer, Judith; Harding, Dan J; Fielicke, André; Dopfer, Otto

2013-02-14

Vibrational spectra of mixed silicon carbide clusters Si(m)C(n) with m + n = 6 in the gas phase are obtained by resonant infrared-vacuum-ultraviolet two-color ionization (IR-UV2CI for n ≤ 2) and density functional theory (DFT) calculations. Si(m)C(n) clusters are produced in a laser vaporization source, in which the silicon plasma reacts with methane. Subsequently, they are irradiated with tunable IR light from an IR free electron laser before they are ionized with UV photons from an F(2) laser. Resonant absorption of one or more IR photons leads to an enhanced ionization efficiency for Si(m)C(n) and provides the size-specific IR spectra. IR spectra measured for Si(6), Si(5)C, and Si(4)C(2) are assigned to their most stable isomers by comparison with calculated linear absorption spectra. The preferred Si(m)C(n) structures with m + n = 6 illustrate the systematic transition from chain-like geometries for bare C(6) to three-dimensional structures for bare Si(6). In contrast to bulk SiC, carbon atom segregation is observed already for the smallest n (n = 2).

Absolute Two-Photon Absorption Coefficients in UltraViolet Window Materials

DTIC Science & Technology

1977-12-01

fvtt* tld » II ntctHB,-y md Idtnlll’ by block number; The absolute two-photon absorption coefficiehts of u. v. transmitting materials have been...measured using well-calibrated single picosecond pulses, at the third and fourth harmonic of a mode locked Nd:YAG laser systems. Twc photon...30, 1977. Work in the area of laser induced breakdown and multiphoton absorption in ultraviolet and infrared laser window materials was carried

Excitation of photosystem I by 760 nm femtosecond laser pulses: transient absorption spectra and intermediates

NASA Astrophysics Data System (ADS)

Cherepanov, Dmitry A.; Shelaev, Ivan V.; Gostev, Fedor E.; Mamedov, Mahir D.; Petrova, Anastasia A.; Aybush, Arseniy V.; Shuvalov, Vladimir A.; Semenov, Alexey Yu; Nadtochenko, Victor A.

2017-09-01

Excitation of photosystem I (PS I) by a femtosecond 760 nm pump leads to one- and two-photon absorption. The one-photon excitation produces intermediates with transient absorption spectra similar to the spectra of the primary [{{{P}}700}+{{{A}}0}-{{A}}1] and secondary [{{{P}}700}+{{A}}0{{{A}}1}-] ion-radical pairs in the PS I reaction center. The two-photon absorption generates the upper level excited states of chlorophyll (Chl) and carotenoid molecules in the antenna. These excited states are converted into the long-lived intermediates and can be tentatively attributed to the excited and charge-transfer ion-radical states of Chl molecules and to the excited states of carotenoids in the antenna. The transient spectra of intermediates generated by two-photon excitation differ from the transient one-photon spectra of the primary and secondary ion-radical pairs.

Two-photon or higher-order absorbing optical materials and methods of use

NASA Technical Reports Server (NTRS)

Marder, Seth (Inventor); Perry, Joseph (Inventor)

2012-01-01

Compositions capable of simultaneous two-photon absorption and higher order absorptivities are provided. Compounds having a donor-pi-donor or acceptor-pi-acceptor structure are of particular interest, where the donor is an electron donating group, acceptor is an electron accepting group, and pi is a pi bridge linking the donor and/or acceptor groups. The pi bridge may additionally be substituted with electron donating or withdrawing groups to alter the absorptive wavelength of the structure. Also disclosed are methods of generating an excited state of such compounds through optical stimulation with light using simultaneous absorption of photons of energies individually insufficient to achieve an excited state of the compound, but capable of doing so upon simultaneous absorption of two or more such photons. Applications employing such methods are also provided, including controlled polymerization achieved through focusing of the light source(s) used.

Polarization-dependent two-photon absorption for the determination of protein secondary structure: A theoretical study

NASA Astrophysics Data System (ADS)

Wanapun, Duangporn; Wampler, Ronald D.; Begue, Nathan J.; Simpson, Garth J.

2008-03-01

A new method for sensitive determination of protein secondary structure via multi-photon absorption is considered theoretically. Perturbation theory is developed to describe the polarization-dependent two-photon absorption (TPA) of α-helix and β-sheet protein secondary structures. The exciton coupling interactions responsible for relatively weak electronic circular dichroism in one-photon absorption are predicted to give rise to large changes in the TPA cross-section (>200%) for circular versus linear incident polarizations, defined as CLD. The CLD effect in TPA is electric dipole-allowed, which explains the much greater sensitivity. These predictions suggest TPA should be a viable means of sensitively probing protein secondary structure.

Two-photon absorption dispersion spectrometer for 1.53 μm eye-safe Doppler LIDAR.

PubMed

Vance, J D

2012-07-01

Based upon resonant two-photon absorption within a rubidium cell and 780 nm pump light, a birefringent medium for 1.530 μm is induced that changes rapidly with frequency. The birefringence is exploited to build a spectrometer that is capable of measuring the Doppler shift of scattered photons.

Optical nonlinearities of colloidal InP@ZnS core-shell quantum dots probed by Z-scan and two-photon excited emission

NASA Astrophysics Data System (ADS)

Wawrzynczyk, Dominika; Szeremeta, Janusz; Samoc, Marek; Nyk, Marcin

2015-11-01

Spectrally resolved nonlinear optical properties of colloidal InP@ZnS core-shell quantum dots of various sizes were investigated with the Z-scan technique and two-photon fluorescence excitation method using a femtosecond laser system tunable in the range from 750 nm to 1600 nm. In principle, both techniques should provide comparable results and can be interchangeably used for determination of the nonlinear optical absorption parameters, finding maximal values of the cross sections and optimizing them. We have observed slight differences between the two-photon absorption cross sections measured by the two techniques and attributed them to the presence of non-radiative paths of absorption or relaxation. The most significant value of two-photon absorption cross section σ2 for 4.3 nm size InP@ZnS quantum dot was equal to 2200 GM, while the two-photon excitation action cross section σ2Φ was found to be 682 GM at 880 nm. The properties of these cadmium-free colloidal quantum dots can be potentially useful for nonlinear bioimaging.

Strong-field two-photon transition by phase shaping

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

Lee, Sangkyung; Lim, Jongseok; Ahn, Jaewook

2010-08-15

We demonstrate the ultrafast coherent control of a nonlinear two-photon absorption in a dynamically shifted energy level structure. We use a spectrotemporal laser-pulse shaping that is programed to preserve the resonant absorption condition during the intense laser-field interaction. Experiments carried out in the strong-field regime of two-photon absorption in the ground state of atomic cesium reveal that the analytically obtained offset and curvature of a laser spectrum compensate the effect of both static and dynamic energy shifts of the given light-atom interaction.

All-inorganic colloidal upconversion quantum dots (Conference Presentation)

NASA Astrophysics Data System (ADS)

Oron, Dan; Teitelboim, Ayelet

2017-02-01

Upconversion (UC) is a nonlinear process in which two, or more, long wavelength photons are converted to a shorter wavelength photon. This process is based on sequential absorption of two or more photons, involving metastable, long lived intermediate energy states, thus is not restricted to ultrashort pulsed excitation. Hence, requirements for UC processes are long lived excited states, a ladder like arrangement of energy levels and a mechanism inhibiting cooling of the hot charge carrier. UC holds great promise for bioimaging, enabling to perform multiphoton imaging in scattering specimen at very low powers. Rare-earth-doped nanocrystals, the most commonly used ones for UC, typically require a minimal particle diameter of several tens of nanometers and have a limited action spectrum. Here, we present a novel luminescence upconversion nano-system based on colloidal semiconductor double quantum dots, consisting of a NIR-absorbing component and a visible emitting component separated by a tunneling barrier in a spherical onion-like geometry. These dual near-infrared and visible core/shell/shell PbSe/CdSe/CdS nanocrystals are shown to efficiently upconvert a broad range of NIR wavelengths up to 1.2 microns to visible emission at room temperature, covering a spectral range where there are practically no alternative upconversion systems. The particle diameter is less than ten nanometers, and the synthesis enables versatility and tunability of both the visible emission color and the NIR absorption edge. The physical mechanism for upconversion in this type of structures, as well as potential advances and extensions on this system will be discussed.

Photonic polymer-blend structures and method for making

DOEpatents

Barnes, Michael D.

2004-06-29

The present invention comprises the formation of photonic polymer-blend structures having tunable optical and mechanical properties. The photonic polymer-blend structures comprise monomer units of spherical microparticles of a polymer-blend material wherein the spherical microparticles have surfaces partially merged with one another in a robust inter-particle bond having a tunable inter-particle separation or bond length sequentially attached in a desired and programmable architecture. The photonic polymer-blend structures of the present invention can be linked by several hundred individual particles sequentially linked to form complex three-dimensional structures or highly ordered two-dimensional arrays of 3D columns with 2D spacing.

A Successful Attempt to Obtain the Linear Dependence Between One-Photon and Two-Photon Spectral Properties and Hammett Parameters of Various Aromatic Substituents in New π-Extended Asymmetric Organic Chromophores.

PubMed

Hu, Nvdan; Gong, Yulong; Wang, Xinchao; Lu, Yao; Peng, Guangyue; Yang, Long; Zhang, Shengtao; Luo, Ziping; Li, Hongru; Gao, Fang

2015-11-01

A series of new asymmetric chromophores containing aromatic substituents and possessing the excellent π-extension in space were prepared through multi-steps routes. One-photon and two-photon spectral properties of these new chromophores could be tuned by these substituents finely and simultaneously. The linear correlation of the wave numbers of the one-photon absorption and emission maxima to Hammett parameters of these substituents was presented. Near infrared two-photon absorption emission integrated areas of the target chromophores were correlated linearly to Hammett constants of these substituted groups.

Two Photon Absorption in a Novel Nano-optical Material Based on the Nonconjugated Conductive Polymer, Poly(beta-pinene)

NASA Astrophysics Data System (ADS)

Titus, Jitto; Thakur, Mrinal

2006-03-01

As recently reported, the electrical conductivity of the nonconjugated polymer, poly(beta-pinene) increases by more than ten orders of magnitude upon doping with iodine [1]. The FTIR, optical absorption and EPR measurements have shown that radical cations are formed upon doping and charge-transfer involving the isolated double-bond in poly(beta-pinene). In this report, exceptionally large two-photon absorption in iodine-doped poly(beta-pinene) will be discussed. The linear absorption spectrum of medium-doped poly(beta-pinene) have peaks at about 4 eV and 3.1 eV. The first peak is due to the radical cation and the second due to the charge-transfer between the double bond and the dopant. The two-photon absorption of the medium-doped polymer has been measured at 730-860 nm using open-aperture z-scan with 150 femtosecond pulses from a Ti:Sapphire laser. A two-photon peak at about 1.5 eV with a magnitude of more than 1 cm/MW has been observed. The large magnitude of the two-photon absorption coefficient which is proportional to the imaginary part of the third order susceptibility has been attributed to the special structure of the radical cation and the confinement within a sub-nanometer dimension. [1] Vippa, Rajagopalan and Thakur, J. Poly. Sci. Part B: Poly. Phys., 43, 3695 (2005).

Opacity from two-photon processes

DOE PAGES

More, Richard M.; Hansen, Stephanie B.; Nagayama, Taisuke

2017-07-22

Here, the recent iron opacity measurements performed at Sandia National Laboratory by Bailey and collaborators have raised questions about the completeness of the physical models normally used to understand partially ionized hot dense plasmas. We describe calculations of two-photon absorption, which is a candidate for the observed extra opacity. Our calculations do not yet match the experiments but show that the two-photon absorption process is strong enough to require careful consideration.

Two-color two-photon excited fluorescence of indole: Determination of wavelength-dependent molecular parameters

NASA Astrophysics Data System (ADS)

Herbrich, Sebastian; Al-Hadhuri, Tawfik; Gericke, Karl-Heinz; Shternin, Peter S.; Smolin, Andrey G.; Vasyutinskii, Oleg S.

2015-01-01

We present a detailed study of two-color two-photon excited fluorescence in indole dissolved in propylene glycol. Femtosecond excitation pulses at effective wavelengths from 268 to 293.33 nm were used to populate the two lowest indole excited states 1La and 1Lb and polarized fluorescence was then detected. All seven molecular parameters and the two-photon polarization ratio Ω containing information on two-photon absorption dynamics, molecular lifetime τf, and rotation correlation time τrot have been determined from experiment and analyzed as a function of the excitation wavelength. The analysis of the experimental data has shown that 1Lb-1La inversion occurred under the conditions of our experiment. The two-photon absorption predominantly populated the 1La state at all excitation wavelengths but in the 287-289 nm area which contained an absorption hump of the 1Lb state 0-0 origin. The components of the two-photon excitation tensor S were analyzed giving important information on the principal tensor axes and absorption symmetry. The results obtained are in a good agreement with the results reported by other groups. The lifetime τf and the rotation correlation time τrot showed no explicit dependence on the effective excitation wavelength. Their calculated weighted average values were found to be τf = 3.83 ± 0.14 ns and τrot = 0.74 ± 0.06 ns.

Non-degenerate two-photon absorption in silicon waveguides. Analytical and experimental study

DOE PAGES

Zhang, Yanbing; Husko, Chad; Lefrancois, Simon; ...

2015-06-22

We theoretically and experimentally investigate the nonlinear evolution of two optical pulses in a silicon waveguide. We provide an analytic solution for the weak probe wave undergoing non-degenerate two-photon absorption (TPA) from the strong pump. At larger pump intensities, we employ a numerical solution to study the interplay between TPA and photo-generated free carriers. We develop a simple and powerful approach to extract and separate out the distinct loss contributions of TPA and free-carrier absorption from readily available experimental data. Our analysis accounts accurately for experimental results in silicon photonic crystal waveguides.

Change of electric dipole moment in charge transfer transitions of ferrocene oligomers studied by ultrafast two-photon absorption

NASA Astrophysics Data System (ADS)

Mikhaylov, Alexander; Arias, Eduardo; Moggio, Ivana; Ziolo, Ronald; Uudsemaa, Merle; Trummal, Aleksander; Cooper, Thomas; Rebane, Aleksander

2017-02-01

Change of permanent electric dipole moment in the lower-energy charge transfer transitions for a series of symmetrical and non-symmetrical ferrocene-phenyleneethynylene oligomers were studied by measuring the corresponding femtosecond two-photon absorption cross section spectra, and were determined to be in the range Δμ = 3 - 10 D. Quantum-chemical calculations of Δμ for the non-symmetrical oligomers show good quantitative agreement with the experimental results, thus validating two-photon absorption spectroscopy as a viable experimental approach to study electrostatic properties of organometallics and other charge transfer systems.

Two-photon interband absorption coefficients in tungstate and molybdate crystals

NASA Astrophysics Data System (ADS)

Lukanin, V. I.; Karasik, A. Ya.

2015-02-01

Two-photon absorption (TPA) coefficients were measured in tungstate and molybdate crystals - BaWO4, KGW, CaMoO4, BaMoO4, CaWO4, PbWO4 and ZnWO4 upon different orientations of excitation polarization with respect to the crystallographic axes. Trains of 25 ps pulses with variable radiation intensities of third (349 nm) harmonics of passively mode-locked 1047 nm Nd:YLF laser were used for interband two-photon excitation of the crystals. It was suggested that in the case, when 349 nm radiation pumping energy exceeds the bandgap width (hν>Eg), the nonlinear excitation process can be considered as two-step absorption. The interband two-photon absorption in all the studied crystals induces the following one-photon absorption from the exited states, which affects the nonlinear process dynamics and leads to a hysteresis in the dependence of the transmission on the excitation intensity. This fact was taken into account under analysis of the experimental dependences of the reciprocal transmission on the excitation intensity. Laser excitation in the transparency region of the crystals caused stimulated Raman scattering (SRS) not for all the crystals studied. The measured nonlinear coefficients allowed us to explain the suppression of SRS in crystals as a result of competition between the SRS and TPA.

A novel flurophore-cyano-carboxylic-Ag microhybrid: Enhanced two photon absorption for two-photon photothermal therapy of HeLa cancer cells by targeting mitochondria.

PubMed

Kong, Lin; Yang, Li; Xin, Chen-Qi; Zhu, Shu-Juan; Zhang, Hui-Hui; Zhang, Ming-Zhu; Yang, Jia-Xiang; Li, Lin; Zhou, Hong-Ping; Tian, Yu-Peng

2018-06-15

In this study, a novel two-photon photothermal therapy (TP-PTT) agent based on an organic-metal microhybrid with surface Plasmon resonance (SPR) enhanced two-photon absorption (TPA) characteristic was designed and synthesized using a fluorescent cyano-carboxylic derivative 2-cyano-3-(9-ethyl-9H-carbazol-3-yl) -acrylic acid (abbreviated as CECZA) and silver nanoparticles through self-assembly process induced by the interfacial coordination interactions between the O/N atom of CECZA and Ag + ion at the surface of Ag nanoparticles. The coordination interactions caused electron transfer from the Ag nanoparticles to CECZA molecules at the excited state, resulting in a decreased fluorescence quantum yield. The interfacial coordination interactions also enhanced the nonlinear optical properties, including 13 times increase in the TPA cross-section (δ). The decreased fluorescence quantum yield and increased two photon absorption caused by the SPR effect led excellent two-photon photothermal conversion, which was beneficial for the TP-PTT effect on HeLa cancer cells. Copyright © 2018 Elsevier B.V. All rights reserved.

Two-Photon Absorption in Organometallic Bromide Perovskites.

PubMed

Walters, Grant; Sutherland, Brandon R; Hoogland, Sjoerd; Shi, Dong; Comin, Riccardo; Sellan, Daniel P; Bakr, Osman M; Sargent, Edward H

2015-09-22

Organometallic trihalide perovskites are solution-processed semiconductors that have made great strides in third-generation thin film light-harvesting and light-emitting optoelectronic devices. Recently, it has been demonstrated that large, high-purity single crystals of these perovskites can be synthesized from the solution phase. These crystals' large dimensions, clean bandgap, and solid-state order have provided us with a suitable medium to observe and quantify two-photon absorption in perovskites. When CH3NH3PbBr3 single crystals are pumped with intense 800 nm light, we observe band-to-band photoluminescence at 572 nm, indicative of two-photon absorption. We report the nonlinear absorption coefficient of CH3NH3PbBr3 perovskites to be 8.6 cm GW(-1) at 800 nm, comparable to epitaxial single-crystal semiconductors of similar bandgap. We have leveraged this nonlinear process to electrically autocorrelate a 100 fs pulsed laser using a two-photon perovskite photodetector. This work demonstrates the viability of organometallic trihalide perovskites as a convenient and low-cost nonlinear absorber for applications in ultrafast photonics.

Optical nonlinearities of colloidal InP@ZnS core-shell quantum dots probed by Z-scan and two-photon excited emission

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

Wawrzynczyk, Dominika; Szeremeta, Janusz; Samoc, Marek

Spectrally resolved nonlinear optical properties of colloidal InP@ZnS core-shell quantum dots of various sizes were investigated with the Z-scan technique and two-photon fluorescence excitation method using a femtosecond laser system tunable in the range from 750 nm to 1600 nm. In principle, both techniques should provide comparable results and can be interchangeably used for determination of the nonlinear optical absorption parameters, finding maximal values of the cross sections and optimizing them. We have observed slight differences between the two-photon absorption cross sections measured by the two techniques and attributed them to the presence of non-radiative paths of absorption or relaxation.more » The most significant value of two-photon absorption cross section σ{sub 2} for 4.3 nm size InP@ZnS quantum dot was equal to 2200 GM, while the two-photon excitation action cross section σ{sub 2}Φ was found to be 682 GM at 880 nm. The properties of these cadmium-free colloidal quantum dots can be potentially useful for nonlinear bioimaging.« less

Transient absorption study of two-photon excitation mechanism in the LH2 complex from purple bacterium Rhodobacter sphaeroides.

PubMed

Stepanenko, Ilya; Kompanetz, Viktor; Makhneva, Zoya; Chekalin, Sergey; Moskalenko, Andrei; Razjivin, Andrei

2012-03-08

The mechanism of two-photon excitation of a peripheral light-harvesting complex LH2 (B800-850) from purple bacterium Rhodobacter sphaeroides was explained on the basis of femtosecond transient absorption data. Fast bleaching of the B850 absorption band was measured under two-photon excitation by 1350 nm femtosecond pulses, showing fast subpicosecond arrival of excitation energy to B850 circular aggregates. Any spectral changes connected with the B800 absorption band of B800-BChl molecules were absent. A similar picture was observed under one-photon excitation of the LH2 complex by 675 nm femtosecond pulses. We believe these effects may be attributed to direct excitation of high-energy excitonic states of a B850 circular aggregate or its vibrational manifold in accordance with the model of Abe [Chem. Phys. 2001, 264, 355-363].

Physics-based, Bayesian sequential detection method and system for radioactive contraband

DOEpatents

Candy, James V; Axelrod, Michael C; Breitfeller, Eric F; Chambers, David H; Guidry, Brian L; Manatt, Douglas R; Meyer, Alan W; Sale, Kenneth E

2014-03-18

A distributed sequential method and system for detecting and identifying radioactive contraband from highly uncertain (noisy) low-count, radionuclide measurements, i.e. an event mode sequence (EMS), using a statistical approach based on Bayesian inference and physics-model-based signal processing based on the representation of a radionuclide as a monoenergetic decomposition of monoenergetic sources. For a given photon event of the EMS, the appropriate monoenergy processing channel is determined using a confidence interval condition-based discriminator for the energy amplitude and interarrival time and parameter estimates are used to update a measured probability density function estimate for a target radionuclide. A sequential likelihood ratio test is then used to determine one of two threshold conditions signifying that the EMS is either identified as the target radionuclide or not, and if not, then repeating the process for the next sequential photon event of the EMS until one of the two threshold conditions is satisfied.

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.

Influence of Two-Photon Absorption Anisotropy on Terahertz Emission Through Optical Rectification in Zinc-Blende Crystals

NASA Astrophysics Data System (ADS)

Sanjuan, Federico; Gaborit, Gwenaël; Coutaz, Jean-Louis

2018-04-01

We report for the first time on the observation of an angular anisotropy of the THz signal generated by optical rectification in a < 111 > ZnTe crystal. This cubic (zinc-blende) crystal in the < 111 > orientation exhibits both transverse isotropy for optical effects involving the linear χ (1) and nonlinear χ (2) susceptibilities. Thus, the observed anisotropy can only be related to χ (3) effect, namely two-photon absorption, which leads to the photo-generation of free carriers that absorb the generated THz signal. Two-photon absorption in zinc-blende crystals is known to be due to a spin-orbit interaction between the valence and higher-conduction bands. We perform a couple of measurements that confirm our hypothesis, as well as we fit the recorded data with a simple model. This two-photon absorption effect makes difficult an efficient generation, through optical rectification in < 111 > zinc-blende crystals, of THz beams of any given polarization state by only monitoring the laser pump polarization.

Infrared reduction, an efficient method to control the non-linear optical property of graphene oxide in femtosecond regime

NASA Astrophysics Data System (ADS)

Bhattacharya, S.; Maiti, R.; Saha, S.; Das, A. C.; Mondal, S.; Ray, S. K.; Bhaktha, S. B. N.; Datta, P. K.

2016-04-01

Graphene Oxide (GO) has been prepared by modified Hummers method and it has been reduced using an IR bulb (800-2000 nm). Both as grown GO and reduced graphene oxide (RGO) have been characterized using Raman spectroscopy and X-ray photoelectron spectroscopy (XPS). Raman spectra shows well documented Dband and G-band for both the samples while blue shift of G-band confirms chemical functionalization of graphene with different oxygen functional group. The XPS result shows that the as-prepared GO contains 52% of sp2 hybridized carbon due to the C=C bonds and 33% of carbon atoms due to the C-O bonds. As for RGO, increment of the atomic % of the sp2 hybridized carbon atom to 83% and rapid decrease in atomic % of C=O bonds confirm an efficient reduction with infrared radiation. UV-Visible absorption spectrum also confirms increment of conjugation with increased reduction. Non-linear optical properties of both GO and RGO are measured using single beam open aperture Z-Scan technique in femtosecond regime. Intensity dependent nonlinear phenomena are observed. Depending upon the intensity, both saturable absorption and two photon absorption contribute to the non-linearity of both the samples. Saturation dominates at low intensity (~ 127 GW/cm2) while two photon absorption become prominent at higher intensities (from 217 GW/cm2 to 302 GW/cm2). We have calculated the two-photon absorption co-efficient and saturation intensity for both the samples. The value of two photon absorption co-efficient (for GO~ 0.0022-0.0037 cm/GW and for RGO~ 0.0128-0.0143 cm/GW) and the saturation intensity (for GO~57 GW/cm2 and for RGO~ 194GW/cm2) is increased with reduction. Increase in two photon absorption coefficient with increasing intensity can also suggest that there may be multi-photon absorption is taking place.

Vibrational excitation of hydrogen molecules by two-photon absorption and third-harmonic generation

NASA Astrophysics Data System (ADS)

Miyamoto, Yuki; Hara, Hideaki; Hiraki, Takahiro; Masuda, Takahiko; Sasao, Noboru; Uetake, Satoshi; Yoshimi, Akihiro; Yoshimura, Koji; Yoshimura, Motohiko

2018-01-01

We report the coherent excitation of the vibrational state of hydrogen molecules by two-photon absorption and the resultant third-harmonic generation (THG). Parahydrogen molecules cooled by liquid nitrogen are irradiated by mid-infrared nanosecond pulses at 4.8 μm with a nearly Fourier-transform-limited linewidth. The first excited vibrational state of parahydrogen is populated by two-photon absorption of the mid-infrared photons. Because of the narrow linewidth of the mid-infrared pulses, coherence between the ground and excited states is sufficient to induce higher-order processes. Near-infrared photons from the THG are observed at 1.6 μm. The dependence of the intensity of the near-infrared radiation on mid-infrared pulse energy, target pressure, and cell length is determined. We used a simple formula for THG with consideration of realistic experimental conditions to explain the observed results.

Two-photon absorption in SiO{sub 2}- and (SiO{sub 2} + GeO{sub 2})-based fibres at a wavelength of 349 nm

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

Chunaev, D S; Karasik, A Ya

2014-06-30

The nonlinear two-photon light absorption coefficients have been measured in an optical fibre with a quartz glass (SiO{sub 2}) core and in a fibre with a germanosilicate glass (SiO{sub 2} + GeO{sub 2}) core. The two-photon absorption coefficient β measured at a wavelength of 349 nm in the (SiO{sub 2} + GeO{sub 2})-based fibre (13.7 cm TW{sup -1}) multiply exceeds that for the pure quartz glass optical fibre (0.54 cm TW{sup -1}). (nonlinear optical phenomena)

Facile synthesis of a two-photon fluorescent probe based on pyrimidine 2-isothiocyanate and its application in bioimaging.

PubMed

Yang, Jie; Hu, Wei; Li, Huirong; Hou, Hanna; Tu, Yi; Liu, Bo

2018-04-18

Two-photon microscopy imaging has been widely applied in biological imaging, but the development of two-photon absorption probes is obviously lagging behind in the development of imaging technology. In this paper, a two-photon fluorescent probe (1) based on pyrimidine 2-isothiocyanate has been designed and synthesized through a simple method for two-photon biological imaging. Probe 1 was able to couple effectively with the amino groups on biomolecules. To verify the reactivity of the isothiocyanate group on probe 1 and the amine groups on the biomolecules, d-glucosamine was chosen as a model biomolecule to conjugate with probe 1. The result showed that probe 1 could effectively conjugate with d-glucosamine to synthesize probe 2, and the yield of probe 2 was 83%. After conjugating with d-glucosamine, linear absorption spectra, single-photon fluorescence spectra, and two-photon fluorescence spectra of probes 1 and 2 did not present significant changes. Probes 1 and 2 exhibited high fluorescence quantum yields (0.71-0.79) in toluene and chloroform. They also exhibited different photo-physical properties in solvents with different polarities. The two-photon absorption cross-section of probe 1 was 953 GM in toluene. In addition, probe 1 could be effectively conjugated with transferrin, and the conjugated probe (Tf-1) could be transported into Hep G2 cells through a receptor-mediated process for biological imaging. These results demonstrate that such probes are expected to have great potential applications in two-photon fluorescence bioimaging.

Multi-photon absorption limits to heralded single photon sources

PubMed Central

Husko, Chad A.; Clark, Alex S.; Collins, Matthew J.; De Rossi, Alfredo; Combrié, Sylvain; Lehoucq, Gaëlle; Rey, Isabella H.; Krauss, Thomas F.; Xiong, Chunle; Eggleton, Benjamin J.

2013-01-01

Single photons are of paramount importance to future quantum technologies, including quantum communication and computation. Nonlinear photonic devices using parametric processes offer a straightforward route to generating photons, however additional nonlinear processes may come into play and interfere with these sources. Here we analyse spontaneous four-wave mixing (SFWM) sources in the presence of multi-photon processes. We conduct experiments in silicon and gallium indium phosphide photonic crystal waveguides which display inherently different nonlinear absorption processes, namely two-photon (TPA) and three-photon absorption (ThPA), respectively. We develop a novel model capturing these diverse effects which is in excellent quantitative agreement with measurements of brightness, coincidence-to-accidental ratio (CAR) and second-order correlation function g(2)(0), showing that TPA imposes an intrinsic limit on heralded single photon sources. We build on these observations to devise a new metric, the quantum utility (QMU), enabling further optimisation of single photon sources. PMID:24186400

Undistorted 3D microstructures in SU8 formed through two-photon polymerization

NASA Astrophysics Data System (ADS)

Ohlinger, Kris; Lin, Yuankun; Poole, Zsolt; Chen, Kevin P.

2011-09-01

This paper presents the wavelength dependence of two-photon polymerization in SU-8 between 720-780 nm. The study is performed by microstructuring SU-8 through a single-shot exposure of SU-8 to 140 fs tunable laser pulses with 80 MHz repetition rate, or by laser direct writing. Two-photon absorption is closely related to one-photon absorption in pristine SU-8. By careful design of the neighboring micro-structures, or by varying wet-processing parameters during development, undistorted and unbended 3D micro-structures have been fabricated through direct laser writing.

Two-photon-excited fluorescence spectroscopy of atomic fluorine at 170 nm

NASA Technical Reports Server (NTRS)

Herring, G. C.; Dyer, Mark J.; Jusinski, Leonard E.; Bischel, William K.

1988-01-01

Two-photon-excited fluorescence spectroscopy of atomic fluorine is reported. A doubled dye laser at 286-nm is Raman shifted in H2 to 170 nm (sixth anti-Stokes order) to excite ground-state 2P(0)J fluorine atoms to the 2D(0)J level. The fluorine atoms are detected by one of two methods: observing the fluorescence decay to the 2PJ level or observing F(+) production through the absorption of an additional photon by the excited atoms. Relative two-photon absorption cross sections to and the radiative lifetimes of the 2D(0)J states are measured.

Broadband two-photon absorption cross sections of benzothiazole derivatives and benzobisthiazolium salts

NASA Astrophysics Data System (ADS)

Noskovičova, Eva; Lorenc, Dušan; Magdolen, Peter; Sigmundová, Ivica; Zahradník, Pavol; Velič, Dušan

2018-05-01

Two-photon absorption (TPA) cross sections of conjugated donor-π-acceptor dipolar structures containing benzothiazole or benzobisthiazolium moieties are determined in a broad spectral range from 700 nm to 1000 nm using two-photon induced fluorescence technique. The TPA cross section values range from 150 GM to 4600 GM. The largest values are observed in near-infrared region. The dipolar derivative of benzothiazole has the largest TPA cross section of 4600 GM at wavelength of 890 nm. A combination of the large TPA in the near-infrared region and the high emission quantum yield makes these compounds excellent candidates for two-photon fluorescence microscopy.

Two photon spectroscopy and microscopy of the fluorescent flavoprotein, iLOV.

PubMed

Homans, Rachael J; Khan, Raja U; Andrews, Michael B; Kjeldsen, Annemette E; Natrajan, Louise S; Marsden, Steven; McKenzie, Edward A; Christie, John M; Jones, Alex R

2018-06-06

LOV-domains are ubiquitous photosensory proteins that are commonly re-engineered to serve as powerful and versatile fluorescent proteins and optogenetic tools. The photoactive, flavin chromophore, however, is excited using short wavelengths of light in the blue and UV regions, which have limited penetration into biological samples and can cause photodamage. Here, we have used non-linear spectroscopy and microscopy of the fluorescent protein, iLOV, to reveal that functional variants of LOV can be activated to great effect by two non-resonant photons of lower energy, near infrared light, not only in solution but also in biological samples. The two photon cross section of iLOV has a significantly blue-shifted S0 → S1 transition compared with the one photon absorption spectrum, suggesting preferential population of excited vibronic states. It is highly likely, therefore, that the two photon absorption wavelength of engineered, LOV-based tools is tuneable. We also demonstrate for the first time two photon imaging using iLOV in human epithelial kidney cells. Consequently, two photon absorption by engineered, flavin-based bio-molecular tools can enable non-invasive activation with high depth resolution and the potential for not only improved image clarity but also enhanced spatiotemporal control for optogenetic applications.

Photon absorption potential coefficient as a tool for materials engineering

NASA Astrophysics Data System (ADS)

Akande, Raphael Oluwole; Oyewande, Emmanuel Oluwole

2016-09-01

Different atoms achieve ionizations at different energies. Therefore, atoms are characterized by different responses to photon absorption in this study. That means there exists a coefficient for their potential for photon absorption from a photon source. In this study, we consider the manner in which molecular constituents (atoms) absorb photon from a photon source. We observe that there seems to be a common pattern of variation in the absorption of photon among the electrons in all atoms on the periodic table. We assume that the electrons closest to the nucleus (En) and the electrons closest to the outside of the atom (Eo) do not have as much potential for photon absorption as the electrons at the middle of the atom (Em). The explanation we give to this effect is that the En electrons are embedded within the nuclear influence, and similarly, Eo electrons are embedded within the influence of energies outside the atom that there exists a low potential for photon absorption for them. Unlike En and Eo, Em electrons are conditioned, such that there is a quest for balance between being influenced either by the nuclear force or forces external to the atom. Therefore, there exists a higher potential for photon absorption for Em electrons than for En and Eo electrons. The results of our derivations and analysis always produce a bell-shaped curve, instead of an increasing curve as in the ionization energies, for all elements in the periodic table. We obtained a huge data of PAPC for each of the several materials considered. The point at which two or more PAPC values cross one another is termed to be a region of conflicting order of ionization, where all the atoms absorb equal portion of the photon source at the same time. At this point, a greater fraction of the photon source is pumped into the material which could lead to an explosive response from the material. In fact, an unimaginable and unreported phenomenon (in physics) could occur, when two or more PAPCs cross, and the material is able to absorb more than that the photon source could provide, at this point. These resulting effects might be of immense materials engineering applications.

Tandem-layered quantum dot solar cells: tuning the photovoltaic response with luminescent ternary cadmium chalcogenides.

PubMed

Santra, Pralay K; Kamat, Prashant V

2013-01-16

Photon management in solar cells is an important criterion as it enables the capture of incident visible and infrared photons in an efficient way. Highly luminescent CdSeS quantum dots (QDs) with a diameter of 4.5 nm were prepared with a gradient structure that allows tuning of absorption and emission bands over the entire visible region without varying the particle size. These crystalline ternary cadmium chalcogenides were deposited within a mesoscopic TiO(2) film by electrophoretic deposition with a sequentially-layered architecture. This approach enabled us to design tandem layers of CdSeS QDs of varying band gap within the photoactive anode of a QD solar cell (QDSC). An increase in power conversion efficiency of 1.97-2.81% with decreasing band gap was observed for single-layer CdSeS, thus indicating varying degrees of photon harvesting. In two- and three-layered tandem QDSCs, we observed maximum power conversion efficiencies of 3.2 and 3.0%, respectively. These efficiencies are greater than the values obtained for the three individually layered photoanodes. The synergy of using tandem layers of the ternary semiconductor CdSeS in QDSCs was systematically evaluated using transient spectroscopy and photoelectrochemistry.

Polarized two-photon photoselection in EGFP: Theory and experiment

NASA Astrophysics Data System (ADS)

Masters, T. A.; Marsh, R. J.; Blacker, T. S.; Armoogum, D. A.; Larijani, B.; Bain, A. J.

2018-04-01

In this work, we present a complete theoretical description of the excited state order created by two-photon photoselection from an isotropic ground state; this encompasses both the conventionally measured quadrupolar (K = 2) and the "hidden" degree of hexadecapolar (K = 4) transition dipole alignment, their dependence on the two-photon transition tensor and emission transition dipole moment orientation. Linearly and circularly polarized two-photon absorption (TPA) and time-resolved single- and two-photon fluorescence anisotropy measurements are used to determine the structure of the transition tensor in the deprotonated form of enhanced green fluorescent protein. For excitation wavelengths between 800 nm and 900 nm, TPA is best described by a single element, almost completely diagonal, two-dimensional (planar) transition tensor whose principal axis is collinear to that of the single-photon S0 → S1 transition moment. These observations are in accordance with assignments of the near-infrared two-photon absorption band in fluorescent proteins to a vibronically enhanced S0 → S1 transition.

Polarized two-photon photoselection in EGFP: Theory and experiment.

PubMed

Masters, T A; Marsh, R J; Blacker, T S; Armoogum, D A; Larijani, B; Bain, A J

2018-04-07

In this work, we present a complete theoretical description of the excited state order created by two-photon photoselection from an isotropic ground state; this encompasses both the conventionally measured quadrupolar (K = 2) and the "hidden" degree of hexadecapolar (K = 4) transition dipole alignment, their dependence on the two-photon transition tensor and emission transition dipole moment orientation. Linearly and circularly polarized two-photon absorption (TPA) and time-resolved single- and two-photon fluorescence anisotropy measurements are used to determine the structure of the transition tensor in the deprotonated form of enhanced green fluorescent protein. For excitation wavelengths between 800 nm and 900 nm, TPA is best described by a single element, almost completely diagonal, two-dimensional (planar) transition tensor whose principal axis is collinear to that of the single-photon S 0 → S 1 transition moment. These observations are in accordance with assignments of the near-infrared two-photon absorption band in fluorescent proteins to a vibronically enhanced S 0 → S 1 transition.

Two-Photon Absorption and Two-Photon-Induced Gain in Perovskite Quantum Dots.

PubMed

Nagamine, Gabriel; Rocha, Jaqueline O; Bonato, Luiz G; Nogueira, Ana F; Zaharieva, Zhanet; Watt, Andrew A R; de Brito Cruz, Carlos H; Padilha, Lazaro A

2018-06-21

Perovskite quantum dots (PQDs) emerged as a promising class of material for applications in lighting devices, including light emitting diodes and lasers. In this work, we explore nonlinear absorption properties of PQDs showing the spectral signatures and the size dependence of their two-photon absorption (2PA) cross-section, which can reach values higher than 10 6 GM. The large 2PA cross section allows for low threshold two-photon induced amplified spontaneous emission (ASE), which can be as low as 1.6 mJ/cm 2 . We also show that the ASE properties are strongly dependent on the nanomaterial size, and that the ASE threshold, in terms of the average number of excitons, decreases for smaller PQDs. Investigating the PQDs biexciton binding energy, we observe strong correlation between the increasing on the biexciton binding energy and the decreasing on the ASE threshold, suggesting that ASE in PQDs is a biexciton-assisted process.

Photoactive high explosives: linear and nonlinear photochemistry of petrin tetrazine chloride.

PubMed

Greenfield, Margo T; McGrane, Shawn D; Bolme, Cindy A; Bjorgaard, Josiah A; Nelson, Tammie R; Tretiak, Sergei; Scharff, R Jason

2015-05-21

Pentaerythritol tetranitrate (PETN), a high explosive, initiates with traditional shock and thermal mechanisms. In this study, the tetrazine-substituted derivative of PETN, pentaerythritol trinitrate chlorotetrazine (PetrinTzCl), is being investigated for a photochemical initiation mechanism that could allow control over the chemistry contributing to decomposition leading to initiation. PetrinTzCl exhibits a photochemical quantum yield (QYPC) at 532 nm not evident with PETN. Using static spectroscopic methods, we observe energy absorption on the tetrazine (Tz) ring that results in photodissociation yielding N2, Cl-CN, and Petrin-CN as the major photoproducts. The QYPC was enhanced with increasing irradiation intensity. Experiment and theoretical calculations imply this excitation mechanism follows sequential photon absorption. Dynamic simulations demonstrate that the relaxation mechanism leading to the observed photochemistry in PetrinTzCl is due to vibrational excitation during internal conversion. PetrinTzCl's single photon stability and intensity dependence suggest this material could be stable in ambient lighting, yet possible to initiate with short-pulsed lasers.

Direct Observation of Two-Step Photon Absorption in an InAs/GaAs Single Quantum Dot for the Operation of Intermediate-Band Solar Cells.

PubMed

Nozawa, Tomohiro; Takagi, Hiroyuki; Watanabe, Katsuyuki; Arakawa, Yasuhiko

2015-07-08

We present the first direct observation of two-step photon absorption in an InAs/GaAs single quantum dot (QD) using photocurrent spectroscopy with two lasers. The sharp peaks of the photocurrent are shifted due to the quantum confined Stark effect, indicating that the photocurrent from a single QD is obtained. In addition, the intensity of the peaks depends on the power of the secondary laser. These results reveal the direct demonstration of the two-step photon absorption in a single QD. This is an essential result for both the fundamental operation and the realization of ultrahigh solar-electricity energy conversion in quantum dot intermediate-band solar cells.

Two-Photon Absorption in Pentacene Dimers: The Importance of the Spacer Using Upconversion as an Indirect Route to Singlet Fission.

PubMed

Garoni, Eleonora; Zirzlmeier, Johannes; Basel, Bettina S; Hetzer, Constantin; Kamada, Kenji; Guldi, Dirk M; Tykwinski, Rik R

2017-10-11

In this proof of concept study, we show that intramolecular singlet fission (iSF) can be initiated from a singlet excited state accessed by two-photon absorption, rather than through a traditional route of direct one-photon excitation (OPE). Thus, iSF in pentacene dimers 2 and 3 is enabled through NIR irradiation at 775 nm, a wavelength where neither dimer exhibits linear absorption of light. The adamantyl and meta-phenylene spacers 2 and 3, respectively, are designed to feature superimposable geometries, which establishes that the electronic coupling between the two pentacenes is the significant structural feature that dictates iSF efficiency.

Synthesis, spectral and third-order nonlinear optical properties of terpyridine Zn(II) complexes based on carbazole derivative with polyether group

NASA Astrophysics Data System (ADS)

Kong, Ming; Liu, Yanqiu; Wang, Hui; Luo, Junshan; Li, Dandan; Zhang, Shengyi; Li, Shengli; Wu, Jieying; Tian, Yupeng

2015-01-01

Four novel Zn(II) terpyridine complexes (ZnLCl2, ZnLBr2, ZnLI2, ZnL(SCN)2) based on carbazole derivative group were designed, synthesized and fully characterized. Their photophysical properties including absorption and one-photon excited fluorescence, two-photon absorption (TPA) and optical power limiting (OPL) were further investigated systematically and interpreted on the basis of theoretical calculations (TD-DFT). The influences of different solvents on the absorption and One-Photon Excited Fluorescence (OPEF) spectral behavior, quantum yields and the lifetime of the chromophores have been investigated in detail. The third-order nonlinear optical (NLO) properties were investigated by open/closed aperture Z-scan measurements using femtosecond pulse laser in the range from 680 to 1080 nm. These results revealed that ZnLCl2 and ZnLBr2 exhibited strong two-photon absorption and ZnLCl2 showed superior optical power limiting property.

Two-color two-photon excited fluorescence of indole: Determination of wavelength-dependent molecular parameters

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

Herbrich, Sebastian; Al-Hadhuri, Tawfik; Gericke, Karl-Heinz, E-mail: k.Gericke@tu-bs.de

2015-01-14

We present a detailed study of two-color two-photon excited fluorescence in indole dissolved in propylene glycol. Femtosecond excitation pulses at effective wavelengths from 268 to 293.33 nm were used to populate the two lowest indole excited states {sup 1}L{sub a} and {sup 1}L{sub b} and polarized fluorescence was then detected. All seven molecular parameters and the two-photon polarization ratio Ω containing information on two-photon absorption dynamics, molecular lifetime τ{sub f}, and rotation correlation time τ{sub rot} have been determined from experiment and analyzed as a function of the excitation wavelength. The analysis of the experimental data has shown that {supmore » 1}L{sub b}–{sup 1}L{sub a} inversion occurred under the conditions of our experiment. The two-photon absorption predominantly populated the {sup 1}L{sub a} state at all excitation wavelengths but in the 287–289 nm area which contained an absorption hump of the {sup 1}L{sub b} state 0-0 origin. The components of the two-photon excitation tensor S were analyzed giving important information on the principal tensor axes and absorption symmetry. The results obtained are in a good agreement with the results reported by other groups. The lifetime τ{sub f} and the rotation correlation time τ{sub rot} showed no explicit dependence on the effective excitation wavelength. Their calculated weighted average values were found to be τ{sub f} = 3.83 ± 0.14 ns and τ{sub rot} = 0.74 ± 0.06 ns.« less

Ag@Aggregation-induced emission dye core/shell nanostructures with enhanced one- and two-photon fluorescence

NASA Astrophysics Data System (ADS)

Wang, Cheng; Li, Yang; Xu, Qiujin; Luo, Liang

2017-10-01

Combining plasmonic nanostructures with two-photon fluorescence materials is a promising way to significantly enhance two-photon fluorescence. Ag@1,4-bis(2-cyano-2-phenylethenyl) benzene (BCPEB) core/shell nanostructures were fabricated by simply incubating the isolated Ag nanoparticles with BCPEB microrods in ethanol. BCPEB was chosen as the fluorescent organic molecule owing to the aggregation-induced-emission (AIE) nature which would reduce the emission loss as being practically applied in solid phase. By utilizing the match of the extinction spectrum of Ag nanoparticles and BCPEB's absorption band, the target Ag@BCPEB core/shell nanostructures showed an enhanced one-photon (12×) fluorescence, integrating with SERS signal as well. Moreover, the resultant second harmonic generation of Ag nanoparticles under two-photon excitation also well matched with the absorption band of BCPEB, and significant enhanced two-photon (17×) fluorescence was obtained. The confocal images of NIH-3T3 cells with these nanostructures under one- and two-photon excitation showed good contrast and brightness for bio-imaging.

Fluorenyl benzothiadiazole and benzoselenadiazole near-IR fluorescent probes for two-photon fluorescence imaging (Conference Presentation)

NASA Astrophysics Data System (ADS)

Belfield, Kevin D.; Yao, Sheng; Kim, Bosung; Yue, Xiling

2016-03-01

Imaging biological samples with two-photon fluorescence (2PF) microscopy has the unique advantage of resulting high contrast 3D resolution subcellular image that can reach up to several millimeters depth. 2PF probes that absorb and emit at near IR region need to be developed. Two-photon excitation (2PE) wavelengths are less concerned as 2PE uses wavelengths doubles the absorption wavelength of the probe, which means 2PE wavelengths for probes even with absorption at visible wavelength will fall into NIR region. Therefore, probes that fluoresce at near IR region with high quantum yields are needed. A series of dyes based on 5-thienyl-2, 1, 3-benzothiadiazole and 5-thienyl-2, 1, 3-benzoselenadiazole core were synthesized as near infrared two-photon fluorophores. Fluorescence maxima wavelengths as long as 714 nm and fluorescence quantum yields as high as 0.67 were achieved. The fluorescence quantum yields of the dyes were nearly constant, regardless of solvents polarity. These diazoles exhibited large Stokes shift (<114nm), high two-photon absorption cross sections (up to 2,800 GM), and high two-photon fluorescence figure of merit (FM , 1.04×10-2 GM). Cells incubated on a 3D scaffold with one of the new probes (encapsulated in Pluronic micelles) exhibited bright fluorescence, enabling 3D two-photon fluorescence imaging to a depth of 100 µm.

Enantiopure distorted ribbon-shaped nanographene combining two-photon absorption-based upconversion and circularly polarized luminescence.

PubMed

Cruz, Carlos M; Márquez, Irene R; Mariz, Inês F A; Blanco, Victor; Sánchez-Sánchez, Carlos; Sobrado, Jesús M; Martín-Gago, José A; Cuerva, Juan M; Maçôas, Ermelinda; Campaña, Araceli G

2018-04-28

Herein we describe a distorted ribbon-shaped nanographene exhibiting unprecedented combination of optical properties in graphene-related materials, namely upconversion based on two-photon absorption (TPA-UC) together with circularly polarized luminescence (CPL). The compound is a graphene molecule of ca. 2 nm length and 1 nm width with edge defects that promote the distortion of the otherwise planar lattice. The edge defects are an aromatic saddle-shaped ketone unit and a [5]carbohelicene moiety. This system is shown to combine two-photon absorption and circularly polarized luminescence and a remarkably long emission lifetime of 21.5 ns. The [5]helicene is responsible for the chiroptical activity while the push-pull geometry and the extended network of sp 2 carbons are factors favoring the nonlinear absorption. Electronic structure theoretical calculations support the interpretation of the results.

Two-photon or higher-order absorbing optical materials for generation of reactive species

NASA Technical Reports Server (NTRS)

Marder, Seth R. (Inventor); Cumpston, Brian (Inventor); Lipson, Matthew (Inventor); Perry, Joseph W. (Inventor)

2003-01-01

Disclosed are highly efficient multiphoton absorbing compounds and methods of their use. The compounds generally include a bridge of pi-conjugated bonds connecting electron donating groups or electron accepting groups. The bridge may be substituted with a variety of substituents as well. Solubility, lipophilicity, absorption maxima and other characteristics of the compounds may be tailored by changing the electron donating groups or electron accepting groups, the substituents attached to or the length of the pi-conjugated bridge. Numerous photophysical and photochemical methods are enabled by converting these compounds to electronically excited states upon simultaneous absorption of at least two photons of radiation. The compounds have large two-photon or higher-order absorptivities such that upon absorption, one or more Lewis acidic species, Lewis basic species, radical species or ionic species are formed.

Two-photon or higher-order absorbing optical materials for generation of reactive species

NASA Technical Reports Server (NTRS)

Perry, Joseph W (Inventor); Cumpston, Brian (Inventor); Lipson, Matthew (Inventor); Marder, Seth R (Inventor)

2007-01-01

Disclosed are highly efficient multiphoton absorbing compounds and methods of their use. The compounds generally include a bridge of pi-conjugated bonds connecting electron donating groups or electron accepting groups. The bridge may be substituted with a variety of substituents as well. Solubility, lipophilicity, absorption maxima and other characteristics of the compounds may be tailored by changing the electron donating groups or electron accepting groups, the substituents attached to or the length of the pi-conjugated bridge. Numerous photophysical and photochemical methods are enabled by converting these compounds to electronically excited states upon simultaneous absorption of at least two photons of radiation. The compounds have large two-photon or higher-order absorptivities such that upon absorption, one or more Lewis acidic species, Lewis basic species, radical species or ionic species are formed.

Two-Photon or Higher-Order Absorbing Optical Materials for Generation of Reactive Species

NASA Technical Reports Server (NTRS)

Perry, Joseph W. (Inventor); Cumpston, Brian (Inventor); Lipson, Matthew (Inventor); Marder, Seth R. (Inventor)

2013-01-01

Disclosed are highly efficient multiphoton absorbing compounds and methods of their use. The compounds generally include a bridge of pi-conjugated bonds connecting electron donating groups or electron accepting groups. The bridge may be substituted with a variety of substituents as well. Solubility, lipophilicity, absorption maxima and other characteristics of the compounds may be tailored by changing the electron donating groups or electron accepting groups, the substituents attached to or the length of the pi-conjugated bridge. Numerous photophysical and photochemical methods are enabled by converting these compounds to electronically excited states upon simultaneous absorption of at least two photons of radiation. The compounds have large two-photon or higher-order absorptivities such that upon absorption, one or more Lewis acidic species, Lewis basic species, radical species or ionic species are formed.

Optical Kerr effect and two-photon absorption in monolayer black phosphorus

NASA Astrophysics Data System (ADS)

Margulis, Vl A.; Muryumin, E. E.; Gaiduk, E. A.

2018-05-01

A theoretical treatment of nonlinear refraction and two-photon absorption is presented for a novel two-dimensional material, monolayer black phosphorus (or phosphorene), irradiated by a normally incident and linearly polarized coherent laser beam of frequency ω. It is found that both the nonlinear refractive index n 2(ω) and the two-photon absorption coefficient α 2(ω) of phosphorene depend upon the polarization of the radiation field relative to phosphorene’s crystallographic axes. For the two principal polarization directions considered—viz, the armchair ({ \\mathcal A }{ \\mathcal C }) and zigzag ({ \\mathcal Z }{ \\mathcal Z }), the calculated values of n 2 and α 2 are distinguished by the order of their magnitude, with the n 2 and α 2 values being greater for the { \\mathcal A }{ \\mathcal C } direction. Furthermore, for almost all the incident photon energies below the fundamental absorption edge, except its neighborhood, the signs of n 2 as well as α 2 for the { \\mathcal A }{ \\mathcal C } and { \\mathcal Z }{ \\mathcal Z } polarization directions are opposed to each other. Also, for both the directions, the change of sign of n 2 is predicted to occur in the way between the two-photon absorption edge and the fundamental absorption edge, as well as in the near vicinity of the latter, where the Kerr nonlinearity has a pronounced resonant character and the magnitude of n 2 for the { \\mathcal A }{ \\mathcal C } and { \\mathcal Z }{ \\mathcal Z } polarization directions reaches its largest positive values of the order of 10‑9 and 10‑10 cm2 W‑1, respectively. The implications of the findings for practical all-optical switching applications are discussed.

LASERS IN MEDICINE: Two-photon excitation of aluminium phthalocyanines

NASA Astrophysics Data System (ADS)

Meshalkin, Yu P.; Alfimov, E. E.; Vasil'ev, N. E.; Denisov, A. N.; Makukha, V. K.; Ogirenko, A. P.

1999-12-01

A demonstration is given of the feasibility of two-photon excitation of aluminium phthalocyanine and of the pharmaceutical preparation 'Fotosens', used in photodynamic therapy. The excitation source was an Nd:YAG laser emitting at the 1064 nm wavelength. The spectra of the two-photon-excited luminescence were obtained and the two-photon absorption cross sections were determined.

Microfabrication technology by femtosecond laser direct scanning using two-photon photo-polymerization

NASA Astrophysics Data System (ADS)

Zhou, Ming; Liu, Li-Peng; Dai, Qi-Xun; Pan, Chuan-Peng

2005-01-01

Two-photon absorption (TPA) is confined at the focus under tight-focusing conditions, which provides a novel concept for micro-fabrication using two-photon photo-polymerization in resin. The development of three-dimensional micro-fabrication by femtosecond laser was introduced at first, then the merits of femtosecond two-photon photo-polymerization was expatiated. Femtosecond laser direct scanning three-dimensional (3D) micro-fabrication system was set up and corresponding controlling software was developed. We demonstrated a fabrication of three-dimensional microstructures using photo-polymerization of resin by two-photon absorption. The precision of micro-machining and the spatial resolution reached 1um because of TPA. The dependence of fabricated line width to the micro-fabrication speed was investigated. Benzene ring, CHINA and layer-by-layer of log structures were fabricated in this 3D- micro-fabrication system as examples.

Mid-infrared two photon absorption sensitivity of commercial detectors

NASA Astrophysics Data System (ADS)

Boiko, D. L.; Antonov, A. V.; Kuritsyn, D. I.; Yablonskiy, A. N.; Sergeev, S. M.; Orlova, E. E.; Vaks, V. V.

2017-10-01

We report on broad-band two-photon absorption (TPA) in several commercially available MIR inter-band bulk semiconductor photodetectors with the spectral cutoff in the range of 4.5-6 μm. The highest TPA responsivity of 2 × 10-5 A.mm2/W2 is measured for a nitrogen-cooled InSb photovoltaic detector. Its performance as a two-photon detector is validated by measuring the second-order interferometric autocorrelation function of a multimode quantum cascade laser emitting at the wavelength of 8 μm.

Two-photon absorption properties of cationic 1,4-bis(styryl)benzene derivative and its inclusion complexes with cyclodextrins.

PubMed

Nag, Okhil Kumar; Nayak, Rati Ranjan; Lim, Chang Su; Kim, In Hong; Kyhm, Kwangseuk; Cho, Bong Rae; Woo, Han Young

2010-07-29

Two-photon absorption properties of 1,4-bis{4'-[N,N-bis(6''-trimethylammoniumhexyl)amino]styryl}benzene tetrabromide (C1) and its inclusion complexes (ICs) with cyclodextrins (CDs) have been studied. Upon complexation with CDs, the absorption spectra of C1 showed a slight red shift, whereas the emission spectra showed a blue shift with concomitant increase in the fluorescence quantum efficiency. A Stern-Volmer study using K(3)Fe(CN)(6) as a quencher revealed significant reduction in the photoinduced charge transfer quenching, in accord with the IC formation. Comparison of the spectroscopic results reveals that C1 forms increasingly more stable ICs in the order C1/beta-CD < C1/gamma-CD < C1/(3gamma:beta)-CD (gamma-CD/beta-CD 3:1, mole ratio). Moreover, the two-photon action cross section of C1 increased from 200 GM for C1 to 400 GM for C1/beta-CD, 460 GM for C1/gamma-CD, and 650 GM for C1/(3gamma:beta)-CD, respectively. Furthermore, the two-photon microscopy images of HeLa cells stained with C1 emitted strong two-photon excited fluorescence in the plasma membrane. These results provide a useful guideline for the development of efficient two-photon materials for bioimaging applications.

Double-mode Two-photon Absorption and Enhanced Photon Antibunching Due to Interference

NASA Astrophysics Data System (ADS)

Bandilla, A.; Ritze, H.-H.

Inspired by results of interfering signal and idler from a nondegenerate parametric amplifier we investigate the photon statistics of the resulting field after interference of two components subjected to double-mode two-photon absorption. This absorption process leads to a strong correlation of the participating modes, which can be used to generate fields with photon antibunching in interference experiments. In addition the photon number can be made small, which produces enhanced antibunching.Translated AbstractZwei-Photonen-Absorption aus zwei Moden und durch Interferenz verstärktes photon antibunchingDie quantenmechanische Betrachtung der Interferenz führt zu neuen Ergebnissen, wenn Felder ohne klassisches Analogon betrachtet werden. Insbesondere ergibt sich durch die Reduktion der Photonenzahl durch Interferenz eine effektive Verstärkung des Photon Antibunching, wie von den Verfassern in vorhergehenden Arbeiten gezeigt wurde. Die vorliegende Untersuchung betrachtet die Interferenz von zwei korrelierten Moden, wobei die Korrelation durch Zwei-Photonen-Absorption aus den beiden Moden zustande kommt. In jeder einzelnen Mode ergibt sich lediglich ein gewisses Bunching, wenn man mit kohärentem Licht in beiden Moden beginnt. Es wird die Interferenz der Feldstärke-Komponenten in bestimmten Polarisationsrichtungen untersucht. Zur Vereinfachung wird in den betrachteten Moden die gleiche Anfangsphotonenzahl vorausgesetzt und der Analysator auf minimale Transmittanz gebracht. Das eigentliche Signal entsteht dann durch Einführung einer endlichen Phasenverschiebung zwischen den beiden Moden. Dieses Signal zeigt Antibunching und kann in seiner Intensität beliebig variiert werden, was wegen des (1/n)-Charakters des Antibunching zu seiner Verstärkung führt. Ferner wird gezeigt, daß die zunächst für zwei linear polarisierte Moden durchgeführte Rechnung auf zwei zirkulare Moden sowie auf zwei gegenläufige Strahlen bei der dopplerfreien Zwei-Quanten-Absorption übertragen werden kann. Die Ergebnisse werden durch numerische Rechnungen gestützt und schließlich durch approximative Methoden reproduziert und erweitert.

Carcinogenic damage to deoxyribonucleic acid is induced by near-infrared laser pulses in multiphoton microscopy via combination of two- and three-photon absorption

NASA Astrophysics Data System (ADS)

Nadiarnykh, Oleg; Thomas, Giju; Van Voskuilen, Johan; Sterenborg, Henricus J. C. M.; Gerritsen, Hans C.

2012-11-01

Nonlinear optical imaging modalities (multiphoton excited fluorescence, second and third harmonic generation) applied in vivo are increasingly promising for clinical diagnostics and the monitoring of cancer and other disorders, as they can probe tissue with high diffraction-limited resolution at near-infrared (IR) wavelengths. However, high peak intensity of femtosecond laser pulses required for two-photon processes causes formation of cyclobutane-pyrimidine-dimers (CPDs) in cellular deoxyribonucleic acid (DNA) similar to damage from exposure to solar ultraviolet (UV) light. Inaccurate repair of subsequent mutations increases the risk of carcinogenesis. In this study, we investigate CPD damage that results in Chinese hamster ovary cells in vitro from imaging them with two-photon excited autofluorescence. The CPD levels are quantified by immunofluorescent staining. We further evaluate the extent of CPD damage with respect to varied wavelength, pulse width at focal plane, and pixel dwell time as compared with more pronounced damage from UV sources. While CPD damage has been expected to result from three-photon absorption, our results reveal that CPDs are induced by competing two- and three-photon absorption processes, where the former accesses UVA absorption band. This finding is independently confirmed by nonlinear dependencies of damage on laser power, wavelength, and pulse width.

Two-Photon Excitation, Fluorescence Microscopy, and Quantitative Measurement of Two-Photon Absorption Cross Sections

NASA Astrophysics Data System (ADS)

DeArmond, Fredrick Michael

As optical microscopy techniques continue to improve, most notably the development of super-resolution optical microscopy which garnered the Nobel Prize in Chemistry in 2014, renewed emphasis has been placed on the development and use of fluorescence microscopy techniques. Of particular note is a renewed interest in multiphoton excitation due to a number of inherent properties of the technique including simplified optical filtering, increased sample penetration, and inherently confocal operation. With this renewed interest in multiphoton fluorescence microscopy, comes an increased demand for robust non-linear fluorescent markers, and characterization of the associated tool set. These factors have led to an experimental setup to allow a systematized approach for identifying and characterizing properties of fluorescent probes in the hopes that the tool set will provide researchers with additional information to guide their efforts in developing novel fluorophores suitable for use in advanced optical microscopy techniques as well as identifying trends for their synthesis. Hardware was setup around a software control system previously developed. Three experimental tool sets were set up, characterized, and applied over the course of this work. These tools include scanning multiphoton fluorescence microscope with single molecule sensitivity, an interferometric autocorrelator for precise determination of the bandwidth and pulse width of the ultrafast Titanium Sapphire excitation source, and a simplified fluorescence microscope for the measurement of two-photon absorption cross sections. Resulting values for two-photon absorption cross sections and two-photon absorption action cross sections for two standardized fluorophores, four commercially available fluorophores, and ten novel fluorophores are presented as well as absorption and emission spectra.

Pushing the limits of CMOS optical parametric amplifiers with USRN:Si7N3 above the two-photon absorption edge

PubMed Central

Ooi, K. J. A.; Ng, D. K. T.; Wang, T.; Chee, A. K. L.; Ng, S. K.; Wang, Q.; Ang, L. K.; Agarwal, A. M.; Kimerling, L. C.; Tan, D. T. H.

2017-01-01

CMOS platforms operating at the telecommunications wavelength either reside within the highly dissipative two-photon regime in silicon-based optical devices, or possess small nonlinearities. Bandgap engineering of non-stoichiometric silicon nitride using state-of-the-art fabrication techniques has led to our development of USRN (ultra-silicon-rich nitride) in the form of Si7N3, that possesses a high Kerr nonlinearity (2.8 × 10−13 cm2 W−1), an order of magnitude larger than that in stoichiometric silicon nitride. Here we experimentally demonstrate high-gain optical parametric amplification using USRN, which is compositionally tailored such that the 1,550 nm wavelength resides above the two-photon absorption edge, while still possessing large nonlinearities. Optical parametric gain of 42.5 dB, as well as cascaded four-wave mixing with gain down to the third idler is observed and attributed to the high photon efficiency achieved through operating above the two-photon absorption edge, representing one of the largest optical parametric gains to date on a CMOS platform. PMID:28051064

X-ray two-photon absorption with high fluence XFEL pulses

DOE PAGES

Hoszowska, Joanna; Szlachetko, J.; Dousse, J. -Cl.; ...

2015-09-07

Here, we report on nonlinear interaction of solid Fe with intense femtosecond hard x-ray free-electron laser (XFEL) pulses. The experiment was performed at the CXI end-station of the Linac Coherent Light Source (LCLS) by means of high- resolution x-ray emission spectroscopy. The focused x-ray beam provided extreme fluence of ~10 5 photons/Å 2. Two-photon absorption leading to K-shell hollow atom formation and to single K-shell ionization of solid Fe was investigated.

Highly Efficient and Excitation Tunable Two-Photon Luminescence Platform For Targeted Multi-Color MDRB Imaging Using Graphene Oxide

NASA Astrophysics Data System (ADS)

Pramanik, Avijit; Fan, Zhen; Chavva, Suhash Reddy; Sinha, Sudarson Sekhar; Ray, Paresh Chandra

2014-08-01

Multiple drug-resistance bacteria (MDRB) infection is one of the top three threats to human health according to the World Health Organization (WHO). Due to the large penetration depth and reduced photodamage, two-photon imaging is an highly promising technique for clinical MDRB diagnostics. Since most commercially available water-soluble organic dyes have low two-photon absorption cross-section and rapid photobleaching tendency, their applications in two-photon imaging is highly limited. Driven by the need, in this article we report extremely high two-photon absorption from aptamer conjugated graphene oxide (σ2PA = 50800 GM) which can be used for highly efficient two-photon fluorescent probe for MDRB imaging. Reported experimental data show that two-photon photoluminescence imaging color, as well as luminescence peak position can be tuned from deep blue to red, just by varying the excitation wavelength without changing its chemical composition and size. We have demonstrated that graphene oxide (GO) based two-photon fluorescence probe is capable of imaging of multiple antibiotics resistance MRSA in the first and second biological transparency windows using 760-1120 nm wavelength range.

Absorption spectroscopy at the ultimate quantum limit from single-photon states

NASA Astrophysics Data System (ADS)

Whittaker, R.; Erven, C.; Neville, A.; Berry, M.; O'Brien, J. L.; Cable, H.; Matthews, J. C. F.

2017-02-01

Absorption spectroscopy is routinely used to characterise chemical and biological samples. For the state-of-the-art in laser absorption spectroscopy, precision is theoretically limited by shot-noise due to the fundamental Poisson-distribution of photon number in laser radiation. In practice, the shot-noise limit can only be achieved when all other sources of noise are eliminated. Here, we use wavelength-correlated and tuneable photon pairs to demonstrate how absorption spectroscopy can be performed with precision beyond the shot-noise limit and near the ultimate quantum limit by using the optimal probe for absorption measurement—single photons. We present a practically realisable scheme, which we characterise both the precision and accuracy of by measuring the response of a control feature. We demonstrate that the technique can successfully probe liquid samples and using two spectrally similar types of haemoglobin we show that obtaining a given precision in resolution requires fewer heralded single probe photons compared to using an idealised laser.

Excited-State Structure of Oligothiophene Dendrimers: Computational and Experimental Study

DTIC Science & Technology

2010-01-01

REPORT Excited-State Structure of Oligothiophene Dendrimers : Computational and Experimental Study 14. ABSTRACT 16. SECURITY CLASSIFICATION OF: The...nature of one and two-photon absorption enhancement in a series of oligothiophene dendrimers , recently proposed for applications in entangled photon...upconversion measurements). The linear absorption spectra exhibit a red shift of the absorption maxima and broadening as a function of dendrimer generations

A self-assembled nanohybrid composed of fluorophore-phenylamine nanorods and Ag nanocrystals: energy transfer, wavelength shift of fluorescence and TPEF applications for live-cell imaging.

PubMed

Kong, Lin; Yang, Jia-xiang; Li, Sheng-li; Zhang, Qiong; Xue, Zhao-ming; Zhou, Hong-ping; Wu, Jie-ying; Jin, Bao-kang; Tian, Yu-peng

2013-12-02

A fluorophore-phenylamine derivative (L) has been coupled with silver nanocrystals (NCs) to construct an L-Ag nanohybrid. Owing to synergic effects of the L and Ag components, the exciton-plasmon interactions between L and Ag increase the strength of the donor-acceptor interaction within the nanohybrid, a fact that results in an energy-transfer process and further brings about a dramatic redshift of single-photon absorption and fluorescence, and a decreased fluorescence FL lifetime. The coupling effect also leads to enhancement of a series of nonlinear optical properties, including two-photon-excited fluorescence (TPEF), two-photon-absorption (TPA) cross section (δ), two-photon-absorption coefficient (β), nonlinear refractive index (γ), and third order nonlinear optical susceptibility (χ((3))). The enhanced two-photon fluorescence of the nanohybrid is proven to be potentially useful for two-photon microscopy of live cells, such as HepG2. Moreover, cytotoxicity tests show that the low-micromolar concentrations of the nanohybrid do not cause significant reduction in cell viability over a period of at least 24 h and should be safe for further biological studies. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Mitochondria-targeted cationic porphyrin-triphenylamine hybrids for enhanced two-photon photodynamic therapy.

PubMed

Hammerer, Fabien; Poyer, Florent; Fourmois, Laura; Chen, Su; Garcia, Guillaume; Teulade-Fichou, Marie-Paule; Maillard, Philippe; Mahuteau-Betzer, Florence

2018-01-01

The proof of concept for two-photon activated photodynamic therapy has already been achieved for cancer treatment but the efficiency of this approach still heavily relies on the availability of photosensitizers combining high two-photon absorption and biocompatibility. In this line we recently reported on a series of porphyrin-triphenylamine hybrids which exhibit high singlet oxygen production quantum yield as well as high two-photon absorption cross-sections but with a very poor cellular internalization. We present herein new photosensitizers of the same porphyrin-triphenylamine hybrid series but bearing cationic charges which led to strongly enhanced water solubility and thus cellular penetration. In addition the new compounds have been found localized in mitochondria that are preferential target organelles for photodynamic therapy. Altogether the strongly improved properties of the new series combined with their specific mitochondrial localization lead to a significantly enhanced two-photon activated photodynamic therapy efficiency. Copyright © 2017 Elsevier Ltd. All rights reserved.

Two-photon or higher-order absorbing optical materials and methods of use

NASA Technical Reports Server (NTRS)

Perry, Joseph (Inventor); Marder, Seth (Inventor)

2001-01-01

Compositions capable of simultaneous two-photon absorption and higher order absorptivities are disclosed. Many of these compositions are compounds satisfying the formulae D-.PI.-D, A-.PI.-A, D-A-D and A-D-A, wherein D is an electron donor group, A is an electron acceptor group and .PI. comprises a bridge of .pi.-conjugated bonds connecting the electron donor groups and electron acceptor groups. In A-D-A and D-A-D compounds, the .pi. bridge is substituted with electron donor groups and electron acceptor groups, respectively. Also disclosed are methods that generate an electronically excited state of a compound, including those satisfying one of these formulae. The electronically excited state is achieved in a method that includes irradiating the compound with light. Then, the compound is converted to a multi-photon electronically excited state upon simultaneous absorption of at least two photons of light. The sum of the energies of all of the absorbed photons is greater than or equal to the transition energy from a ground state of the compound to the multi-photon excited state. The energy of each absorbed photon is less than the transition energy between the ground state and the lowest single-photon excited state of the compound is less than the transition energy between the multi-photon excited state and the ground state.

Ligand-core NLO-phores: a combined experimental and theoretical approach to the two-photon absorption and two-photon excited emission properties of small-ligated silver nanoclusters.

PubMed

Russier-Antoine, Isabelle; Bertorelle, Franck; Calin, Nathalie; Sanader, Željka; Krstić, Marjan; Comby-Zerbino, Clothilde; Dugourd, Philippe; Brevet, Pierre-François; Bonačić-Koutecký, Vlasta; Antoine, Rodolphe

2017-01-19

We report a combined experimental and theoretical study of the two-photon absorption and excited emission properties of monodisperse ligand stabilized Ag 11 , Ag 15 and Ag 31 nanoclusters in aqueous solutions. The nanoclusters were synthesized using a cyclic reduction under oxidative conditions and separated by vertical gel electrophoresis. The two-photon absorption cross-sections of these protected noble metal nanoclusters measured within the biologically attractive 750-900 nm window are several orders of magnitude larger than that reported for commercially available standard organic dyes. The two-photon excited fluorescence spectra are also presented for excitation wavelengths within the same excitation spectral window. They exhibit size-tunability. Because the fundamental photophysical mechanisms underlying these multiphoton processes in ligand protected clusters with only a few metal atoms are not fully understood yet, a theoretical model is proposed to identify the key driving elements. Elements that regulate the dipole moments and the nonlinear optical properties are the nanocluster size, its structure and the charge distribution on both the metal core and the bound ligands. We coined this new class of NLO materials as "Ligand-Core" NLO-phores.

Two-photon absorption of KBe2BO3F2 and CsLiB6O10 at 193 nm

NASA Astrophysics Data System (ADS)

Nakazato, Tomoharu; Wang, Xiaoyang; Chen, Chuangtian; Watanabe, Shuntaro

2017-12-01

We measured the two-photon absorption coefficients of KBe2BO3F2 (KBBF) and CsLiB6O10 (CLBO) at 193.5 nm using CaF2 as a reference. This is the first report about KBBF measurement at any wavelength. The two-photon absorption coefficients of KBBF, CLBO, and CaF2 were 1.3 × 10-9, 1.0 × 10-9, and 0.8 × 10-9 cm/W, respectively. We also measured the fluorescence spectra of KBBF, CLBO, and CaF2 excited by 193.5 nm light. The observed spectrum of KBBF had a broad peak at 322 nm, similar to that of CaF2. The luminescence intensity showed a quadratic dependence on incident laser intensity for KBBF and CaF2, indicating a two-photon process, but showed a linear dependence for CLBO. Taken together, we conclude that the two-photon fluorescence of KBBF originates, as in the case of CaF2, from the transition of a self-trapped exciton formed by a F2 - ion (self-trapped hole), which captures an electron.

Absorption and emission properties of photonic crystals and metamaterials

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

Peng, Lili

We study the emission and absorption properties of photonic crystals and metamaterials using Comsol Multiphysics and Ansoft HFSS as simulation tools. We calculate the emission properties of metallic designs using drude model and the results illustrate that an appropriate termination of the surface of the metallic structure can significantly increase the absorption and therefore the thermal emissivity. We investigate the spontaneous emission rate modifications that occur for emitters inside two-dimensional photonic crystals and find the isotropic and directional emissions with respect to different frequencies as we have expected.

Two-photon-absorption line strengths for nitric oxide: Comparison of theory and sub-Doppler, laser-induced fluorescence measurements

NASA Astrophysics Data System (ADS)

Kulatilaka, Waruna D.; Lucht, Robert P.

2017-03-01

We discuss the results of high-resolution, sub-Doppler two-photon-absorption laser-induced fluorescence (TPALIF) spectroscopy of nitric oxide at low pressure and room temperature. The measurements were performed using the single-longitudinal mode output of a diode-laser-seeded optical parametric generator (OPG) system with a measured frequency bandwidth of 220 MHz. The measurements were performed using a counter-propagating pump beam geometry, resulting in sub-Doppler TPALIF spectra of NO for various rotational transitions in the (0,0) vibrational band of the A2Σ+ - X2Π electronic transition. The experimental results are compared with the results of a perturbative treatment of the rotational line strengths for the 20 different rotational branches of the X2Π(v″ = 0) → A2Σ+(v' = 0) two-photon absorption band. In the derivation of the expressions for the two-photon transition absorption strength, the closure relation is used for rotational states in the intermediate levels of the two-photon transition in analogy with the Placzek treatment of Raman transitions. The theoretical treatment of the effect of angular momentum coupling on the two-photon rotational line strengths features the use of irreducible spherical tensors and 3j symbols. The final results are expressed in terms of the Hund's case (a) coupling coefficients aJ and bJ for the X2Π(v″ = 0) rotational level wavefunctions, which are intermediate between Hund's case (a) and case (b). Considerable physical insight is provided by this final form of the equations for the rotational line strengths. Corrections to the two-photon absorption rotational line strength for higher order effects such as centrifugal stretching can be included in a straightforward fashion in the analysis by incorporating higher order terms in these coupling coefficients aJ and bJ, although these corrections are essentially negligible for J < 50. The theoretical calculations of relative line intensities are in good agreement both with our experiment and with published experimental results. In addition, the calculated line shapes and relative intensities for closely spaced main branch and satellite transitions are in excellent agreement with our experimental measurements.

Superior optical nonlinearity of an exceptional fluorescent stilbene dye

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

He, Tingchao; Division of Physics and Applied Physics, Centre for Disruptive Photonic Technologies; Sreejith, Sivaramapanicker

2015-03-16

Strong multiphoton absorption and harmonic generation in organic fluorescent chromophores are, respectively, significant in many fields of research. However, most of fluorescent chromophores fall short of the full potential due to the absence of the combination of such different nonlinear upconversion behaviors. Here, we demonstrate that an exceptional fluorescent stilbene dye could exhibit efficient two- and three-photon absorption under the excitation of femtosecond pulses in solution phase. Benefiting from its biocompatibility and strong excited state absorption behavior, in vitro two-photon bioimaging and superior optical limiting have been exploited, respectively. Simultaneously, the chromophore could generate efficient three-photon excited fluorescence and third-harmonicmore » generation (THG) when dispersed into PMMA film, circumventing the limitations of classical fluorescent chromophores. Such chromophore may find application in the production of coherent light sources of higher photon energy. Moreover, the combination of three-photon excited fluorescence and THG can be used in tandem to provide complementary information in biomedical studies.« less

Design, synthesis, and characterization of photoinitiators for two-photon polymerization

NASA Astrophysics Data System (ADS)

Whitby, Reece; MacMillan, Ryan; Janssens, Stefaan; Raymond, Sebastiampillai; Clarke, Dave; Kay, Andrew; Jin, Jianyong; Simpson, Cather M.

2016-09-01

A series of dipolar and quadrupolar two-photon absorption (2PA) photoinitiators (PIs) based around the well-known triphenylamine (TPA) core and tricyanofuran (TCF) acceptors have been prepared for use in two-photon polymerisation (TPP). The synthesised dipolar species are designated as 5 and 7, and the remaining quadrupolar species are 6, 8, 9 and 10. Large two-photon absorption cross-sections (δ2PA) ranging between 333 - 507 GM were measured at 780 nm using the z-scan technique. Fluorescence quantum yields (ΦF) were below 3% across the series when compared to Rhodamine 6G as a reference standard. Finally, TPP tests were conducted on PIs 7 and 8 to assess their ability to initiate the polymerisation of acrylate monomers using an 800 nm femtosecond Ti:Sapphire laser system.

The physics of heterodyne detection in the far-infrared: Transition from electric-field to photon-absorption detection in a simple system

NASA Technical Reports Server (NTRS)

Teich, M. C.

1980-01-01

The history of heterodyne detection is reviewed from the radiowave to the optical regions of the electromagnetic spectrum with emphasion the submillimeter/far infrared. The transition from electric field to photon absorption detection in a simple system is investigated. The response of an isolated two level detector to a coherent source of incident radiation is calculated for both heterodyne and video detection. When the processes of photon absorption and photon emission cannot be distinguished, the relative detected power at double- and sum-frequencies is found to be multiplied by a coefficient, which is less than or equal to unity, and which depends on the incident photon energy and on the effective temperature of the system.

Platinum Acetylide Two-Photon Chromophores (Postprint)

DTIC Science & Technology

2007-01-01

two lower- energy photons results in initiation of the same photophysical processes as one-photon absorption (1PA) of one high- energy photon. This is...advantageous for two reasons. First, by using lower- energy photons, a material will be protected from photodegradation effects. Second, the quadratic...D. L.; Ehrlich, J. E.; Erskine , L. L.; Heikal, A. A.; Kuebler, S. M.; Le, I. Y. S.; McCord-Maughon, D.; Qin, J.; Rockel, H.; Rumi, M.; Wu, X. L

L(alpha)-induced two-photon absorption of visible light emitted from an O-type star by H2(+) ions located near the surface of the Stromgren sphere surrounding the star: A possible explanation for the diffuse interstellar absorption bands (DIDs)

NASA Technical Reports Server (NTRS)

Glownia, James H.; Sorokin, Peter P.

1994-01-01

In this paper, a new model is proposed to account for the DIB's (Diffuse Interstellar Bands). In this model, the DIB's result from a non-linear effect: resonantly-enhanced two-photon absorption of H(2+) ions located near the surface of the Stromgren sphere that surrounds an O- or B- type star. The strong light that is required to 'drive' the two-photon transition is provided by L(alpha) light emerging from the Stromgren sphere that bounds the H II region surrounding the star. A value of approximately 100 micro W/sq cm is estimated for the L(alpha) flux at the Stromgren radius, R(s), of a strong (O5) star. It is shown that a c.w. L(alpha) flux of this intensity should be sufficient to induce a few percent absorption for visible light radiated by the same star at a frequency (omega2) that completes an allowed two-photon transition, provided (1) the L(alpha) radiation happens to be nearly resonant with the frequency of a fully-allowed absorber transition that effectively represents the first step in the two-photon transition, and (2) an effective column density approximately 10(sup18)/sq cm of the absorber is present near the Stromgren sphere radius, R(sub s).

The optical biomedical sensors for DNA detection and imaging based on two-photon excited luminescent styryl dyes: phototoxic influence on the DNA

NASA Astrophysics Data System (ADS)

Yashchuk, Valeriy M.; Kudrya, Vladislav Yu.; Losytskyy, Mykhaylo Yu.; Tokar, Valentyna P.; Yarmoluk, Sergiy M.; Dmytruk, Igor M.; Prokopets, Vadym M.; Kovalska, Vladyslava B.; Balanda, Anatoliy O.; Kryvorotenko, Dmytro V.; Ogul'chansky, Tymish Yu.

2007-06-01

The optical absorption, fluorescence and phosphorescence of the novel styryl dyes developed for the fluorescent detection of DNA were investigated. The energy structures of dye molecules as well as spectral manifestations of the dyes aggregate formation and interaction with DNA were studied. The dramatic increase (up to 1000 times) of the fluorescence intensity of dyes in the presence of DNA was observed. The photostability and phototoxic influence on the DNA of several styryl dyes were studied by analyzing absorption, fluorescence and phosphorescence spectra of these dyes and dye-DNA systems. Changes of the optical density value of dye-DNA solutions caused by the visible light irradiation were fixed in the wavelength regions of the DNA absorption and of the dye absorption. Fluorescence emission of dye-DNA complexes upon two-photon excitation (TPE) at wavelength 1064 nm with the 20 ns pulsed YAG: Nd3+ laser and at 840 nm with the 90 fs pulsed Ti:sapphire laser was registered. The values of two-photon absorption cross-sections of dye-DNA complexes were evaluated.

Two and four photon absorption and nonlinear refraction in undoped, chromium doped and copper doped ZnS quantum dots

NASA Astrophysics Data System (ADS)

Sharma, Dimple; Malik, B. P.; Gaur, Arun

2015-12-01

The ZnS quantum dots (QDs) with Cr and Cu doping were synthesized by chemical co-precipitation method. The nanostructures of the prepared undoped and doped ZnS QDs were characterized by UV-vis spectroscopy, Transmission electron microscopy (TEM) and X-ray diffraction (XRD). The sizes of QDs were found to be within 3-5 nm range. The nonlinear parameters viz. Two photon absorption coefficient (β2), nonlinear refractive index (n2), third order nonlinear susceptibility (χ3) at wavelength 532 nm and Four photon absorption coefficient (β4) at wavelength 1064 nm have been calculated by Z-scan technique using nanosecond Nd:YAG laser in undoped, Cr doped and Cu doped ZnS QDs. Higher values of nonlinear parameters for doped ZnS infer that they are potential material for the development of photonics devices and sensor protection applications.

Tuning the nonlinear optical absorption of reduced graphene oxide by chemical reduction.

PubMed

Shi, Hongfei; Wang, Can; Sun, Zhipei; Zhou, Yueliang; Jin, Kuijuan; Redfern, Simon A T; Yang, Guozhen

2014-08-11

Reduced graphene oxides with varying degrees of reduction have been produced by hydrazine reduction of graphene oxide. The linear and nonlinear optical properties of both graphene oxide as well as the reduced graphene oxides have been measured by single beam Z-scan measurement in the picosecond region. The results reveal both saturable absorption and two-photon absorption, strongly dependent on the intensity of the pump pulse: saturable absorption occurs at lower pump pulse intensity (~1.5 GW/cm2 saturation intensity) whereas two-photon absorption dominates at higher intensities (≥5.7 GW/cm2). Intriguingly, we find that the two-photon absorption coefficient (from 1.5 cm/GW to 4.5cm/GW) and the saturation intensity (from 1 GW/cm2 to 2 GW/cm2) vary with chemical reduction, which is ascribed to the varying concentrations of sp2 domains and sp2 clusters in the reduced graphene oxides. Our results not only provide an insight into the evolution of the nonlinear optical coefficient in reduced graphene oxide, but also suggest that chemical engineering techniques may usefully be applied to tune the nonlinear optical properties of various nano-materials, including atomically thick graphene sheets.

Efficient control of ultrafast optical nonlinearity of reduced graphene oxide by infrared reduction

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

Bhattachraya, S.; Maiti, R.; Das, A. C.

Simultaneous occurrence of saturable absorption nonlinearity and two-photon absorption nonlinearity in the same medium is well sought for the devices like optical limiter and laser mode-locker. Pristine graphene sheet consisting entirely of sp{sup 2}-hybridized carbon atoms has already been identified having large optical nonlinearity. However, graphene oxide (GO), a precursor of graphene having both sp{sup 2} and sp{sup 3}-hybridized carbon atom, is increasingly attracting cross-discipline researchers for its controllable properties by reduction of oxygen containing groups. In this work, GO has been prepared by modified Hummers method, and it has been further reduced by infrared (IR) radiation. Characterization of reducedmore » graphene oxide (RGO) by means of Raman spectroscopy, X-ray photoelectron spectroscopy, and UV-Visible absorption measurements confirms an efficient reduction with infrared radiation. Here, we report precise control of non-linear optical properties of RGO in femtosecond regime with increased degrees of IR reduction measured by open aperture z-scan technique. Depending on the intensity, both saturable absorption and two-photon absorption effects are found to contribute to the non-linearity of all the samples. Saturation dominates at low intensity (∼127 GW/cm{sup 2}) while two-photon absorption becomes prominent at higher intensities (from 217 GW/cm{sup 2} to 302 GW/cm{sup 2}). The values of two-photon absorption co-efficient (∼0.0022–0.0037 cm/GW for GO, and ∼0.0128–0.0143 cm/GW for RGO) and the saturation intensity (∼57 GW/cm{sup 2} for GO, and ∼194 GW/cm{sup 2} for RGO) increase with increasing reduction, indicating GO and RGO as novel tunable photonic devices. We have also explained the reason of tunable nonlinear optical properties by using amorphous carbon model.« less

Synthesis of Photoresponsive Dual NIR Two-Photon Absorptive [60]Fullerene Triads and Tetrads

PubMed Central

Jeon, Seaho; Wang, Min; Tan, Loon-Seng; Cooper, Thomas; Hamblin, Michael R.; Chiang, Long Y.

2013-01-01

Broadband nonlinear optical (NLO) organic nanostructures exhibiting both ultrafast photoresponse and a large cross-section of two-photon absorption throughout a wide NIR spectrum may make them suitable for use as nonlinear biophotonic materials. We report here the synthesis and characterization of two C60-(antenna)x analogous compounds as branched triad C60(>DPAF-C18)(>CPAF-C2M) and tetrad C60(>DPAF-C18)(>CPAF-C2M)2 nanostructures. These compounds showed approximately equal extinction coefficients of optical absorption over 400–550 nm that corresponds to near-IR two-photon based excitation wavelengths at 780–1,100 nm. Accordingly, they may be utilized as potential precursor candidates to the active-core structures of photosensitizing nanodrugs for 2γ-PDT in the biological optical window of 800–1,050 nm. PMID:23941881

Bio-Inspired Photon Absorption and Energy Transfer for Next Generation Photovoltaic Devices

NASA Astrophysics Data System (ADS)

Magsi, Komal

Nature's solar energy harvesting system, photosynthesis, serves as a model for photon absorption, spectra broadening, and energy transfer. Photosynthesis harvests light far differently than photovoltaic cells. These differences offer both engineering opportunity and scientific challenges since not all of the natural photon absorption mechanisms have been understood. In return, solar cells can be a very sensitive probe for the absorption characteristics of molecules capable of transferring charge to a conductive interface. The objective of this scientific work is the advancement of next generation photovoltaics through the development and application of natural photo-energy transfer processes. Two scientific methods were used in the development and application of enhancing photon absorption and transfer. First, a detailed analysis of photovoltaic front surface fluorescent spectral modification and light scattering by hetero-structure was conducted. Phosphor based spectral down-conversion is a well-known laser technology. The theoretical calculations presented here indicate that parasitic losses and light scattering within the spectral range are large enough to offset any expected gains. The second approach for enhancing photon absorption is based on bio-inspired mechanisms. Key to the utilization of these natural processes is the development of a detailed scientific understanding and the application of these processes to cost effective systems and devices. In this work both aspects are investigated. Dye type solar cells were prepared and tested as a function of Chlorophyll (or Sodium-Copper Chlorophyllin) and accessory dyes. Forster has shown that the fluorescence ratio of Chlorophyll is modified and broadened by separate photon absorption (sensitized absorption) through interaction with nearby accessory pigments. This work used the dye type solar cell as a diagnostic tool by which to investigate photon absorption and photon energy transfer. These experiments shed some doubt on the Foster Resonant Energy Transfer mechanism since energy relay dye architecture-photosensitizer mixtures do not broaden the response of solar cells. Spectral absorption characterization of chromophore-Chlorophyll solutions in varying solvent polarity confirm the lack of cooperative absorption via a Foster-like mechanism and point the way to new concepts of cooperative absorption in natural systems and the development of a new photovoltaic paradigm.

Off-Resonant Two-Photon Absorption Cross-Section Enhancement of an Organic Chromophore on Gold Nanorods

PubMed Central

Sivapalan, Sean T.; Vella, Jarrett H.; Yang, Timothy K.; Dalton, Matthew J.; Haley, Joy E.; Cooper, Thomas M.; Urbas, Augustine M.; Tan, Loon-Seng; Murphy, Catherine J.

2013-01-01

Surface-plasmon-initiated interference effects of polyelectrolyte-coated gold nanorods on the two-photon absorption of an organic chromophore were investigated. With polyelectrolyte bearing gold nanorods of 2,4,6 and 8 layers, the role of the plasmonic fields as function of distance on such effects was examined. An unusual distance dependence was found: enhancements in the two-photon cross-section were at a minimum at an intermediate distance, then rose again at a further distance. The observed values of enhancement were compared to theoretical predictions using finite element analysis and showed good agreementdue to constructive and destructive interference effects. PMID:23687561

Three-photon absorption process in organic dyes enhanced by surface plasmon resonance

NASA Astrophysics Data System (ADS)

Cohanoschi, Ion

2006-07-01

Multi-photon absorption processes have received significant attention from the scientific community during the last decade, mainly because of their potential applications in optical limiting, data storage and biomedical fields. Perhaps, one of the most investigated processes studied so far has been two-photon absorption (2PA). These investigations have resulted in successful applications in all the fields mentioned above. However, 2PA present some limitations in the biomedical field when pumping at typical 2PA wavelengths. In order to overcome these limitations, three-photon absorption (3PA) process has been proposed. However, 3PA in organic molecules has a disadvantage, typical values of sigma3' are small (10-81 cm6s 2/photon2), therefore, 3PA excitation requires high irradiances to induce the promotion of electrons from the ground state to the final excited state. To overcome this obstacle, specific molecules that exhibit large 3PA cross-section must be designed. Thus far, there is a lack of systematic studies that correlate 3PA processes with the molecular structure of organic compounds. In order to fill the existent gap in 3PA molecular engineering, in this dissertation we have investigated the structure/property relationship for a new family of fluorene derivatives with very high three-photon absorption cross-sections. We demonstrated that the symmetric intramolecular charge transfer as well as the pi-electron conjugation length enhances the 3PA cross-section of fluorene derivatives. In addition, we showed that the withdrawing electron character of the attractor groups in a pull-pull geometry proved greater 3PA cross-section. After looking for alternative ways to enhance the effective sigma 3' of organic molecules, we investigated the enhancement of two- and three-photon absorption processes by means of Surface Plasmon. We demonstrated an enhancement of the effective two- and three-photon absorption cross-section of an organic compound of 480 and 30 folds, respectively. We proved that the enhancement is a direct consequence of the electric field enhancement at a metal/buffer interface. Next, motivated by the demands for new materials with enhanced nonlinear optical properties, we studied the 3PA of Hematoporphyrin IX and J-aggregate supramolecular systems. As a result, we were able to propose the use of 3PA in photodynamic therapy using Photofrin, the only drug approved by the FDA for PDT.

Novel carbazole derivatives with quinoline ring: synthesis, electronic transition, and two-photon absorption three-dimensional optical data storage.

PubMed

Li, Liang; Wang, Ping; Hu, Yanlei; Lin, Geng; Wu, Yiqun; Huang, Wenhao; Zhao, Quanzhong

2015-03-15

We designed carbazole unit with an extended π conjugation by employing Vilsmeier formylation reaction and Knoevenagel condensation to facilitate the functional groups of quinoline from 3- or 3,6-position of carbazole. Two compounds doped with poly(methyl methacrylate) (PMMA) films were prepared. To explore the electronic transition properties of these compounds, one-photon absorption properties were experimentally measured and theoretically calculated by using the time-dependent density functional theory. We surveyed these films by using an 800 nm Ti:sapphire 120-fs laser with two-photon absorption (TPA) fluorescence emission properties and TPA coefficients to obtain the TPA cross sections. A three-dimensional optical data storage experiment was conducted by using a TPA photoreaction with an 800 nm-fs laser on the film to obtain a seven-layer optical data storage. The experiment proves that these carbazole derivatives are well suited for two-photon 3D optical storage, thus laying the foundation for the research of multilayer high-density and ultra-high-density optical information storage materials. Copyright © 2014 Elsevier B.V. All rights reserved.

Calculation of the spatial resolution in two-photon absorption spectroscopy applied to plasma diagnosis

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

Garcia-Lechuga, M.; Laser Processing Group, Instituto de Óptica “Daza de Valdés,” CSIC, 28006-Madrid; Fuentes, L. M.

2014-10-07

We report a detailed characterization of the spatial resolution provided by two-photon absorption spectroscopy suited for plasma diagnosis via the 1S-2S transition of atomic hydrogen for optogalvanic detection and laser induced fluorescence (LIF). A precise knowledge of the spatial resolution is crucial for a correct interpretation of measurements, if the plasma parameters to be analysed undergo strong spatial variations. The present study is based on a novel approach which provides a reliable and realistic determination of the spatial resolution. Measured irradiance distribution of laser beam waists in the overlap volume, provided by a high resolution UV camera, are employed tomore » resolve coupled rate equations accounting for two-photon excitation, fluorescence decay and ionization. The resulting three-dimensional yield distributions reveal in detail the spatial resolution for optogalvanic and LIF detection and related saturation due to depletion. Two-photon absorption profiles broader than the Fourier transform-limited laser bandwidth are also incorporated in the calculations. The approach allows an accurate analysis of the spatial resolution present in recent and future measurements.« less

Synthesis of Dual NIR Two-photon Absorptive [60]fullerenyl Multiadducts for Nonlinear Light-transmittance Reduction Application

DTIC Science & Technology

2014-11-01

INTRODUCTION Nonlinear optical characteristics of [60] fullerene -derived C60-(antenna)x nanostructure conjugates are based on excited singlet state...two-photon absorption (2PA) processes in the NIR region [3]. Fullerene cages exhibit high electronegativity and electron-accepting characteristics...photoenergy by the donor DPAF-Cn antenna was able to undergo efficient intramolecular electron- or energy-transfer to the fullerene acceptor moiety in

One- and two-photon photosensitized singlet oxygen production: characterization of aromatic ketones as sensitizer standards.

PubMed

Arnbjerg, Jacob; Paterson, Martin J; Nielsen, Christian B; Jørgensen, Mikkel; Christiansen, Ove; Ogilby, Peter R

2007-07-05

Singlet molecular oxygen, O2(a1Deltag), can be efficiently produced in a photosensitized process using either one- or two-photon irradiation. The aromatic ketone 1-phenalenone (PN) is an established one-photon singlet oxygen sensitizer with many desirable attributes for use as a standard. In the present work, photophysical properties of two other aromatic ketones, pyrene-1,6-dione (PD) and benzo[cd]pyren-5-one (BP), are reported and compared to those of PN. Both PD and BP sensitize the production of singlet oxygen with near unit quantum efficiency in a nonpolar (toluene) and a polar (acetonitrile) solvent. With their more extensive pi networks, the one-photon absorption spectra for PD and BP extend out to longer wavelengths than that for PN, thus providing increased flexibility for sensitizer excitation over the range approximately 300-520 nm. Moreover, PD and BP have much larger two-photon absorption cross sections than PN over the range 655-840 nm which, in turn, results in amounts of singlet oxygen that are readily detected in optical experiments. One- and two-photon absorption spectra of PD and BP obtained using high-level calculations model the salient features of the experimental data well. In particular, the ramifications of molecular symmetry are clearly reflected in both the experimental and calculated spectra. The use of PD and BP as standards for both the one- and two-photon photosensitized production of singlet oxygen is expected to facilitate the development of new sensitizers for application in singlet-oxygen-based imaging experiments.

Nonlinear Optical Spectroscopy of Two-Dimensional Materials

NASA Astrophysics Data System (ADS)

Cui, Qiannan

Nonlinear optical properties of two-dimensional (2D) materials, such as transition metal dichalcogenides (TMDs), graphene, black phosphorus, and so on, play a key role of understanding nanoscale light-matter interactions, as well as developing nanophotonics applications from solar cells to quantum computation. With ultrafast lasers, we experimentally study nonlinear optical properties of 2D materials. Employing transient absorption microscopy, we study several members of 2D materials, such as WSe2, TiS3 and ReS2. The dynamical saturable absorption process of 2D excitons is spatiotemporally resolved. Intrinsic parameters of these 2D materials, such as exciton lifetime, exciton diffusion coefficient, and exciton mobility, are effectively measured. Especially, in-plane anisotropy of transient absorption and diffusive transport is observed for 2D excitons in monolayer ReS2, demonstrating the in-plane degree of freedom. Furthermore, with quantum interference and control nanoscopy, we all-optically inject, detect and manipulate nanoscale ballistic charge currents in a ReS2 thin film. By tuning the phase difference between one photon absorption and two photon absorption transition paths, sub-picosecond timescale of ballistic currents is coherently controlled for the first time in TMDs. In addition, the spatial resolution is two-order of magnitude smaller than optical diffraction limit. The second-order optical nonlinearity of 2D monolayers is resolved by second harmonic generation (SHG) microscopy. We measure the second-order susceptibility of monolayer MoS 2. The angular dependence of SHG in monolayer MoS2 shows strong symmetry dependence on its crystal lattice structure. Hence, second harmonic generation microscopy can serve as a powerful tool to noninvasively determine the crystalline directions of 2D monolayers. The real and imaginary parts of third-order optical nonlinearity of 2D monolayers are resolved by third harmonic generation (THG) microscopy and two-photon transient absorption microscopy, respectively. With third harmonic generation microscopy, we observe strong and anisotropic THG in monolayer and multilayer ReS2. Comparing with 2D materials with hexagonal lattice, such as MoS2, the third-order susceptibility is higher by one order of magnitude in ReS2 with a distorted 1T structure. The in-plane anisotropy of THG is attributed to the lattice distortion in ReS2 after comparing with a symmetry analysis. With two-photon transient absorption microscopy, we observe a giant two-photon absorption coefficient of monolayer WS2.

Data reading with the aid of one-photon and two-photon luminescence in three-dimensional optical memory devices based on photochromic materials

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

Akimov, Denis A; Zheltikov, Aleksei M; Koroteev, Nikolai I

1998-06-30

The problem of nondestructive reading of the data stored in the interior of a photochromic sample was analysed. A comparison was made of the feasibility of reading based on one-photon and two-photon luminescence. A model was proposed for the processes of reading the data stored in photochromic molecules with the aid of one-photon and two-photon luminescence. In addition to photochromic transitions, account was taken of the transfer of populations between optically coupled transitions in molecules under the action of the exciting radiation. This model provided a satisfactory description of the kinetics of decay of the coloured form of bulk samplesmore » of spiropyran and made it possible to determine experimentally the quantum yield of the reverse photoreaction as well as the two-photon absorption cross section of the coloured form. Measurements were made of the characteristic erasure times of the data stored in a photochromic medium under one-photon and two-photon luminescence reading conditions. It was found that the use of two-photon luminescence made it possible to enhance considerably the contrast and localisation of the optical data reading scheme in three-dimensional optical memory devices. The experimental results were used to estimate the two-photon absorption cross section of the coloured form of a sample of indoline spiropyran in a polymethyl methacrylate matrix. (laser applications and other topics in quantum electronics)« less

LASER APPLICATIONS AND OTHER TOPICS IN QUANTUM ELECTRONICS: Data reading with the aid of one-photon and two-photon luminescence in three-dimensional optical memory devices based on photochromic materials

NASA Astrophysics Data System (ADS)

Akimov, Denis A.; Zheltikov, Aleksei M.; Koroteev, Nikolai I.; Magnitskiy, Sergey A.; Naumov, A. N.; Sidorov-Biryukov, D. A.; Sokolyuk, N. T.; Fedotov, Andrei B.

1998-06-01

The problem of nondestructive reading of the data stored in the interior of a photochromic sample was analysed. A comparison was made of the feasibility of reading based on one-photon and two-photon luminescence. A model was proposed for the processes of reading the data stored in photochromic molecules with the aid of one-photon and two-photon luminescence. In addition to photochromic transitions, account was taken of the transfer of populations between optically coupled transitions in molecules under the action of the exciting radiation. This model provided a satisfactory description of the kinetics of decay of the coloured form of bulk samples of spiropyran and made it possible to determine experimentally the quantum yield of the reverse photoreaction as well as the two-photon absorption cross section of the coloured form. Measurements were made of the characteristic erasure times of the data stored in a photochromic medium under one-photon and two-photon luminescence reading conditions. It was found that the use of two-photon luminescence made it possible to enhance considerably the contrast and localisation of the optical data reading scheme in three-dimensional optical memory devices. The experimental results were used to estimate the two-photon absorption cross section of the coloured form of a sample of indoline spiropyran in a polymethyl methacrylate matrix.

Polarization dependent two-photon absorption spectroscopy on a naturally occurring biomarker (curcumin) in solution: A theoretical-experimental study

NASA Astrophysics Data System (ADS)

Tiburcio-Moreno, Jose A.; Alvarado-Gil, J. J.; Diaz, Carlos; Echevarria, Lorenzo; Hernández, Florencio E.

2013-09-01

We report on the theoretical-experimental analysis of the two-photon absorption (TPA) and two-photon circular-linear dichroism (TPCLD) spectra of (1E,6E)-1,7-bis(4-hydroxy-3-methoxyphenyl)-1,6-heptadiene-3,5-dione (curcumin) in Tetrahydrofuran (THF) solution. The measurement of the full TPA spectrum of this molecule reveals a maximum TPA cross-section at 740 nm, i.e. more than 10 times larger than the maximum reported in the literature at 800 nm for the application of curcumin in bioimaging. The TPCLD spectrum exposes the symmetry of the main excited-states involved in the two-photon excitation process. TD-DFT calculations support the experimental results. These outcomes are expected to expand the application of natural-occurring dyes in bioimaging.

Imaging of molecular hydrogen and oxygen by single and two-photon fluorescence using laser and flashlamp sources

NASA Technical Reports Server (NTRS)

Diskin, Glenn S.; Lempert, Walter R.; Miles, Richard B.; Kumar, Vinod; Glesk, Ivan

1991-01-01

Two flow visualization techniques, i.e., simultaneous two-dimensional fluorescence imaging of H2 and O2 in a diffusion flame, and quasi-linear fluorescence imaging of O2, are presented. The first uses an injection-locked argon-fluoride excimer laser and a partial overlap of a two-photon ground state absorption in H2 with a single photon absorption from a vibrational level in O2. The second uses a simple, high-intensity ultraviolet flashlamp which provides a flux of photons in the 180-195 nm range, sufficient to produce a quasi-one-dimensional fluorescence image of hot/room temperature oxygen. Both techniques do not require that a seed material be introduced into the flow, they can image major flow constituents, and provide an instantaneous snapshot of the flow.

NIR-emitting molecular-based nanoparticles as new two-photon absorbing nanotools for single particle tracking

NASA Astrophysics Data System (ADS)

Daniel, J.; Godin, A. G.; Clermont, G.; Lounis, B.; Cognet, L.; Blanchard-Desce, M.

2015-07-01

In order to provide a green alternative to QDs for bioimaging purposes and aiming at designing bright nanoparticles combining both large one- and two-photon brightness, a bottom-up route based on the molecular engineering of dedicated red to NIR emitting dyes that spontaneously form fluorescent organic nanoparticles (FONs) has been implemented. These fully organic nanoparticles built from original quadrupolar dyes are prepared using a simple, expeditious and green protocol that yield very small molecular-based nanoparticles (radius ~ 7 nm) suspension in water showing a nice NIR emission (λem=710 nm). These FONs typically have absorption coefficient more than two orders larger than popular NIR-emitting dyes (such as Alexa Fluor 700, Cy5.5 ….) and much larger Stokes shift values (i.e. up to over 5500 cm-1). They also show very large two-photon absorption response in the 800-1050 nm region (up to about 106 GM) of major promise for two-photon excited fluorescence microscopy. Thanks to their brightness and enhanced photostability, these FONs could be imaged as isolated nanoparticles and tracked using wide-field imaging. As such, thanks to their size and composition (absence of heavy metals), they represent highly promising alternatives to NIR-emitting QDs for use in bioimaging and single particle tracking applications. Moreover, efficient FONs coating was achieved by using a polymeric additive built from a long hydrophobic (PPO) and a short hydrophilic (PEO) segment and having a cationic head group able to interact with the highly negative surface of FONs. This electrostatically-driven interaction promotes both photoluminescence and two-photon absorption enhancement leading to an increase of two-photon brightness of about one order of magnitude. This opens the way to wide-field single particle tracking under two-photon excitation

Demonstration of an all-optical feed-forward delay line buffer using the quadratic Stark effect and two-photon absorption in an SOA.

PubMed

Soto, Horacio; Tong, Miriam A; Domínguez, Juan C; Muraoka, Ramón

2017-09-04

We have inserted into an unbiased semiconductor optical amplifier (SOA) a powerful control beam, with photon energy slightly smaller than that of the band-gap of its active region, for exciting two-photon absorption and the quadratic Stark effect. For the available SOA, we estimated these phenomena generated a nonlinear absorption coefficient β= -865 cm/GW and induced an appreciable birefringence inside the amplifier waveguide, which significantly modified the polarization-state of a probe beam. Based on these effects, we have experimentally demonstrated the operation of an all-optical buffer, using an 80 Gb/s optical pulse comb, as well as an unbiased SOA, which was therefore, devoid of amplified spontaneous emission and pattern effects.

New Materials, Techniques and Device Concepts for Organic NLO Chromophore-based Electrooptic Devices. Part 1

DTIC Science & Technology

2006-08-23

polarization the electric field vector is parallel to the substrate, for TM polarization the magnetic field vector is parallel to the substrate. Figure...section can be obtained for the case of the two electromagnetic field polarization vectors λ and µ describing the two photons being absorbed (of the same or... polarization effects on two-photon absorption as investigated by the technique of thermal lensing detected absorption of a mode- locked laser beam. This

pH-Induced Modulation of One- and Two-Photon Absorption Properties in a Naphthalene-Based Molecular Probe.

PubMed

Murugan, N Arul; Kongsted, Jacob; Ågren, Hans

2013-08-13

Presently, there is a great demand for small probe molecules that can be used for two-photon excitation microscopy (TPM)-based monitoring of intracellular and intraorganelle activity and pH. The candidate molecules should ideally possess a large two-photon absorption cross section with optical properties sensitive to pH changes. In the present work, we investigate the potential of a methoxy napthalene (MONAP) derivative for its suitability to serve as a pH sensor using TPM. Using an integrated approach rooted in hybrid quantum mechanics/molecular mechanics, the structures, dynamics, and the one- and two-photon properties of the probe in dimethylformamide solvent are studied. It is found that the protonated form is responsible for the optical property of MONAP at moderately low pH, for which the calculated pH-induced red shift is in good agreement with experiments. A 2-fold increase in the two-photon absorption cross section in the IR region of the spectrum is predicted for the moderately low pH form of the probe, suggesting that this can be a potential probe for pH monitoring of living cells. We also propose some design principles aimed at obtaining control of the absorption spectral range of the probe by structural tuning. Our work indicates that the integrated approach employed is capable of capturing the pH-induced changes in structure and optical properties of organic molecular probes and that such in silico tools can be used to draw structure-property relationships to design novel molecular probes suitable for a specific application.

Probing the SEB Sensitive Depth of a Power MOSFET Using a Two-Photon Absorption Laser Method

NASA Technical Reports Server (NTRS)

Lauenstein, Jean-Marie; Liu, Sandra; Titus, Jeffrey L.; McMorrow, Dale; Casey, Megan C.; Buchner, Stephen P.; Warner, Jeffrey; Phan, Anthony M.; Topper, Alyson D.; Kim, Hak S.;

Merged beam laser design for reduction of gain-saturation and two-photon absorption in high power single mode semiconductor lasers.

PubMed

Lysevych, M; Tan, H H; Karouta, F; Fu, L; Jagadish, C

2013-04-08

In this paper we report a method to overcome the limitations of gain-saturation and two-photon absorption faced by developers of high power single mode InP-based lasers and semiconductor optical amplifiers (SOA) including those based on wide-waveguide or slab-coupled optical waveguide laser (SCOWL) technology. The method is based on Y-coupling design of the laser cavity. The reduction in gain-saturation and two-photon absorption in the merged beam laser structures (MBL) are obtained by reducing the intensity of electromagnetic field in the laser cavity. Standard ridge-waveguide lasers and MBLs were fabricated, tested and compared. Despite a slightly higher threshold current, the reduced gain-saturation in MBLs results in higher output power. The MBLs also produced a single spatial mode, as well as a strongly dominating single spectral mode which is the inherent feature of MBL-type cavity.

Photoinduced electron transfer in a molecular dyad by nanosecond pump-pump-probe spectroscopy.

PubMed

Ha-Thi, M-H; Pham, V-T; Pino, T; Maslova, V; Quaranta, A; Lefumeux, C; Leibl, W; Aukauloo, A

2018-06-01

The design of robust and inexpensive molecular photocatalysts for the conversion of abundant stable molecules like H2O and CO2 into an energetic carrier is one of the major fundamental questions for scientists nowadays. The outstanding challenge is to couple single photoinduced charge separation events with the sequential accumulation of redox equivalents at the catalytic unit for performing multielectronic catalytic reactions. Herein, double excitation by nanosecond pump-pump-probe experiments was used to interrogate the photoinduced charge transfer and charge accumulation on a molecular dyad composed of a porphyrin chromophore and a ruthenium-based catalyst in the presence of a reversible electron acceptor. An accumulative charge transfer state is unattainable because of rapid reverse electron transfer to the photosensitizer upon the second excitation and the low driving force of the forward photodriven electron transfer reaction. Such a method allows the fundamental understanding of the relaxation mechanism after two sequential photon absorptions, deciphering the undesired electron transfer reactions that limit the charge accumulation efficiency. This study is a step toward the improvement of synthetic strategies of molecular photocatalysts for light-induced charge accumulation and more generally, for solar energy conversion.

Production of photocurrent due to intermediate-to-conduction-band transitions: a demonstration of a key operating principle of the intermediate-band solar cell.

PubMed

Martí, A; Antolín, E; Stanley, C R; Farmer, C D; López, N; Díaz, P; Cánovas, E; Linares, P G; Luque, A

2006-12-15

We present intermediate-band solar cells manufactured using quantum dot technology that show for the first time the production of photocurrent when two sub-band-gap energy photons are absorbed simultaneously. One photon produces an optical transition from the intermediate-band to the conduction band while the second pumps an electron from the valence band to the intermediate-band. The detection of this two-photon absorption process is essential to verify the principles of operation of the intermediate-band solar cell. The phenomenon is the cornerstone physical principle that ultimately allows the production of photocurrent in a solar cell by below band gap photon absorption, without degradation of its output voltage.

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).

Two-photon excitation cross-section in light and intermediate atoms

NASA Technical Reports Server (NTRS)

Omidvar, K.

1980-01-01

The method of explicit summation over the intermediate states is used along with LS coupling to derive an expression for two-photon absorption cross section in light and intermediate atoms in terms of integrals over radial wave functions. Two selection rules, one exact and one approximate, are also derived. In evaluating the radial integrals, for low-lying levels, the Hartree-Fock wave functions, and for high-lying levels, hydrogenic wave functions obtained by the quantum defect method are used. A relationship between the cross section and the oscillator strengths is derived. Cross sections due to selected transitions in nitrogen, oxygen, and chlorine are given. The expression for the cross section is useful in calculating the two-photon absorption in light and intermediate atoms.

Two-photon excitation cross section in light and intermediate atoms in frozen-core LS-coupling approximation

NASA Technical Reports Server (NTRS)

Omidvar, K.

1980-01-01

Using the method of explicit summation over the intermediate states two-photon absorption cross sections in light and intermediate atoms based on the simplistic frozen-core approximation and LS coupling have been formulated. Formulas for the cross section in terms of integrals over radial wave functions are given. Two selection rules, one exact and one approximate, valid within the stated approximations are derived. The formulas are applied to two-photon absorptions in nitrogen, oxygen, and chlorine. In evaluating the radial integrals, for low-lying levels, the Hartree-Fock wave functions, and for high-lying levels, hydrogenic wave functions obtained by the quantum-defect method have been used. A relationship between the cross section and the oscillator strengths is derived.

Polarized two-photon fluorescence excitation spectra of indole and benzimidazole

NASA Astrophysics Data System (ADS)

Anderson, Bruce E.; Jones, Richard D.; Rehms, Aden A.; Ilich, Predrag; Callis, Patrik R.

1986-03-01

Polarized two-photon fluorescence excitation spectra of indole in hexane, benzimidazole in isopropanol, and benzimidazole cation in methanol-H 2SO 4, all at 0.2 M and 25°C are reported for the excitation range 470-600 nm, the region of their L b, and L a bands. Relative two-photon absorptivities are deduced by correcting for different fluorescence response and are compared to toluene's L b band. The indole integrated absorptivity is about 10 times greater than that of toluene. The L a band of indole appears less dominant than in one-photon but still outweighs the L b band by a factor of 4. The two-photon polarization spectrum for indole indicates that the L a origin lies ≈500-1000 cm -1 above the L b origin in hexane. The benzimidazoles absorb only about twice as strongly as toluene and show strong vibronic peaks; the L a, bands are only faintly seen. Two-photon properties calculated from INDO/S CI wavefunctions with doubly excited configurations are in good agreement with those of indole, but predict the benzimidazole TPA to be several times stronger than observed. For the cation, the predicted results are nearly two orders of magnitude too high.

Synthesis, prodigious two-photon absorption cross sections and electrochemical properties of a series of triphenylamine-based chromophores

NASA Astrophysics Data System (ADS)

Li, Rui; Li, Dandan; Fei, Wenwen; Tan, Jingyun; Li, Shengli; Zhou, Hongping; Zhang, Shengyi; Wu, Jieying; Tian, Yupeng

2014-06-01

A series of triphenylamine-based chromophores (L1-3) with donor-π-donor (D-π-D) model have been designed and synthesized via solid phase Wittig reaction. Their one/two-photon fluorescence and electrochemical properties have been investigated. The results show that L2 and L3 exhibited strong and wide-dispersed two-photon-excited fluorescence (TPEF) in different solvents. Chromophore L3 displays the strongest intensity two-photon absorption activity and large cross-sections (>3600 GM) in the range of 680-840 nm in THF, the largest δ up to 8899 GM in the near-IR range, and the measured maximum TPA cross-sections per molecular weight (δmax/MW) is 8.64 GM/g (L3) in THF. Significantly, it also exhibits good solubility in common organic solvents when the chromophore was modified by polyether units as peripheral groups.

Two-photon absorption and upconversion luminescence of colloidal CsPbX3 quantum dots

NASA Astrophysics Data System (ADS)

Han, Qiuju; Wu, Wenzhi; Liu, Weilong; Yang, Qingxin; Yang, Yanqiang

2018-01-01

The nonlinear optical and the upconversion luminescence (UCL) properties of CsPbX3 (X = Br or its binary mixtures with Cl, I) quantum dots (QDs) are investigated by femtosecond open-aperture (OA) Z-scan and time-resolved luminescence techniques in nonresonant spectral region. The OA Z-scan results show that CsPbX3 QDs have strong reverse saturable absorption (RSA), which is ascribed to two-photon absorption. Partially changing halide composition from Cl to Br, to I, two-photon absorption cross sections become larger at the same laser excitation intensity. The composition-tunable nonlinear absorption should be attributed to the gradual decrease of the lowest direct band gaps with the halide substitute. Moreover, the strong UCL can be observed under near infrared femtosecond laser excitation. Halide composition-tunable UCL dynamics of CsPbX3 QDs is analyzed by use of two-exponential fitting with deconvolution. When CsPbX3 QDs have similar sizes (10-13 nm), with partially changing halide composition from Cl to Br, to I, the average UCL lifetime becomes longer due to the variation of Kane energy. Our findings suggest all-inorganic perovskite QDs can be used as excellent gain medium for high-performance frequency-upconversion lasers and provide reference to engineer such QDs toward practical optoelectronic applications.

Selective two-photon absorption in carbon dots: a piece of the photoluminescence emission puzzle.

PubMed

Santos, Carla I M; Mariz, Inês F A; Pinto, Sandra N; Gonçalves, Gil; Bdikin, Igor; Marques, Paula A A P; Neves, Maria Graça P M S; Martinho, José M G; Maçôas, Ermelinda M S

2018-06-22

Carbon nanodots (Cdots) are now emerging as promising nonlinear fluorophores for applications in biological environments. A thorough and systematic approach to the two-photon induced emission of Cdots that could provide design guidelines to control their nonlinear emission properties is still missing. In this work, we address the nonlinear optical spectroscopy of Cdots prepared by controlled chemical cutting of graphene oxide (GO). The two-photon absorption in the 700-1000 nm region and the corresponding emission spectrum are carefully investigated. The highest two-photon absorption cross-section estimated was 130 GM at 720 nm. This value is comparable with the one reported for graphene nanoribbons with push-pull architecture. The emission spectrum depends on the excitation mode. At the same excitation energy, nonlinear excitation results in excitation-wavelength independent emission, while upon linear excitation the emission is excitation-wavelength dependent. The biphotonic interaction seems to be selective towards sp2 clusters bearing electron donor and acceptor groups found in push-pull architectures. Both linear and nonlinear emission can be understood based on the existence of isolated sp2 clusters involved in π-π stacking interactions with clusters in adjacent layers.

Novel D-π-A-π-D type organic chromophores for second harmonic generation and multi-photon absorption applications

NASA Astrophysics Data System (ADS)

Aditya, Pusala; Kumar, Hari; Kumar, Sunil; Rajashekar, Muralikrishna, M.; Muthukumar, V. Sai; Kumar, B. Siva; Sai, S. Siva Sankara; Rao, G. Nageshwar

2013-06-01

We report here the optical and non-linear optical properties of six different novel bis-chalcones of D-π-A-π-D derivatives of diarylideneacetone (DBA). These derivatives have been synthesized by Claisen-Schmidt condensation reaction and were well characterized by using FTIR, 1HNMR, 13CNMR, UV-Visible absorption and mass spectroscopic techniques. The optical bandgap for each of the DBA derivatives were determined both experimentally (UV-Visible spectra & Tauc Plot) and theoretically by ab intio DFT calculations using SIESTA software package. They were found to be in close agreement with each other. The Second Harmonic Generation from these organic chromophores were studied by standard Kurtz and Perry Powder SHG method at 1064 nm. They were found to have superior SHG conversion efficiency when compared to urea (standard sample). Further, we investigated the Multi-Photon absorption properties were using conventional open aperture z-scan technique. These DBA derivatives exhibited strong two photon absorption in the order of 1e-11m/W. Hence, these are potential candidate for various photonic applications like optical power limiting, photonic switching and frequency conversion.

Two-photon sensitized recording materials for multilayer optical disk

NASA Astrophysics Data System (ADS)

Akiba, M.; Goto-Takahashi, E.; Takizawa, H.; Sasaki, T.; Mochizuki, H.; Mikami, T.; Kitahara, T.

2010-06-01

Two types of novel two-photon sensitized recording material writable at 405 nm and 522nm were developed. The fluorescent dye generation type (F-type) material consists of at least two-photon absorption dye (TPAD) and fluorescent dye precursor (FDP), which is non-fluorescent before two-photon recording and fluorescent after two-photon recording due to fluorescent dye generation. The fluorescence quench type (Q-type) material, on the other hand, consists of at least TPAD, fluorescent dye (FD) and fluorescent quencher precursor (QP), which is fluorescent before two-photon recording and the fluorescence intensity is reduced after two-photon recording at the recorded spot due to fluorescent quencher generation. Both types of material showed quadratic dependency of recording light intensity at 522 and 405 nm. A twenty-layer two-photon recording media was fabricated with the Q-type material, and two-photon recording and onephoton fluorescent signal readout was successfully conducted.

Enhanced optical limiting effect in fluorine-functionalized graphene oxide

NASA Astrophysics Data System (ADS)

Zhang, Fang; Wang, Zhengping; Wang, Duanliang; Wang, Shenglai; Xu, Xinguang

2017-09-01

Nonlinear optical absorption of fluorine-functionalized graphene oxide (F-GO) solution was researched by the open-aperture Z-scan method using 1064 and 532 nm lasers as the excitation sources. The F-GO dispersion exhibited strong optical limiting property and the fitted results demonstrated that the optical limiting behavior was the result of a two-photon absorption process. For F-GO nanosheets, the two-photon absorption coefficients at 1064 nm excitation are 20% larger than the values at 532 nm excitation and four times larger than that of pure GO nanosheets. It indicates that the doping of fluorine can effectively improve the nonlinear optical property of GO especially in infrared waveband, and fluorine-functionalized graphene oxide is an excellent nonlinear absorption material in infrared waveband.

Two-Photon Fluorescence Microscope for Microgravity Research

NASA Technical Reports Server (NTRS)

Fischer, David G.; Zimmerli, Gregory A.; Asipauskas, Marius

2005-01-01

A two-photon fluorescence microscope has been developed for the study of biophysical phenomena. Two-photon microscopy is a novel form of laser-based scanning microscopy that enables three-dimensional imaging without many of the problems inherent in confocal microscopy. Unlike one-photon optical microscopy, two-photon microscopy utilizes the simultaneous nonlinear absorption of two near-infrared photons. However, the efficiency of two-photon absorption is much lower than that of one-photon absorption, so an ultra-fast pulsed laser source is typically employed. On the other hand, the critical energy threshold for two-photon absorption leads to fluorophore excitation that is intrinsically localized to the focal volume. Consequently, two-photon microscopy enables optical sectioning and confocal performance without the need for a signal-limiting pinhole. In addition, there is a reduction (relative to one-photon optical microscopy) in photon-induced damage because of the longer excitation wavelength. This reduction is especially advantageous for in vivo studies. Relative to confocal microscopy, there is also a reduction in background fluorescence, and, because of a reduction in Rayleigh scattering, there is a 4 increase of penetration depth. The prohibitive cost of a commercial two-photon fluorescence-microscope system, as well as a need for modularity, has led to the construction of a custom-built system (see Figure 1). This system includes a coherent mode-locked titanium: sapphire laser emitting 120-fs-duration pulses at a repetition rate of 80 MHz. The pulsed laser has an average output power of 800 mW and a wavelength tuning range of 700 to 980 nm, enabling the excitation of a variety of targeted fluorophores. The output from the laser is attenuated, spatially filtered, and then directed into a confocal scanning head that has been modified to provide for side entry of the laser beam. The laser output coupler has been replaced with a dichroic filter that reflects the longer-wavelength excitation light and passes the shorter-wavelength fluorescence light. Also, the confocal pinhole has been removed to increase the signal strength. The laser beam is scanned by a twoperpendicular- axis pair of galvanometer mirrors through a pupil transfer lens into the side port of an inverted microscope. Finally, the beam is focused by a 63-magnification, 1.3-numerical- aperture oil-immersion objective lens onto a specimen. The pupil transfer lens serves to match the intermediate image planes of the scanning head and the microscope, and its location is critical. In order to maximize the quality of the image, (that is, the point spread function of the objective lens for all scan positions), the entire system was modeled in optical-design software, and the various free design parameters (the parameters of the spatial-filter components as well as the separations of all of the system components) were determined through an iterative optimization process. A modular design was chosen to facilitate access to the optical train for future fluorescence correlation spectroscopy and fluorescence-lifetime experiments.

Measuring upconversion nanoparticles photoluminescence lifetime with FastFLIM and phasor plots

NASA Astrophysics Data System (ADS)

Sun, Yuansheng; Lee, Hsien-Ming; Qiu, Hailin; Liao, Shih-Chu Jeff; Coskun, Ulas; Barbieri, Beniamino

2018-02-01

Photon upconversion is a nonlinear process in which the sequential of absorption of two or more photons leads to the anti-stoke emission. Different than the conventional multiphoton excitation process, upconversion can be efficiently performed at low excitation densities. Recent developments in lanthanide-doped upconversion nanoparticles (UCNPs) have led to a diversity of applications, including detecting and sensing of biomolecules, imaging of live cells, tissues and animals, cancer diagnostic and therapy, etc. Measuring the upconversion lifetime provides a new dimension of its imaging and opens a new window for its applications. Due to the long metastable intermediate excited state, UCNP typically has a long excited state lifetime ranging from sub-microseconds to milliseconds. Here, we present a novel development using the FastFLIM technique to measure UCNP lifetime by laser scanning confocal microscopy. FastFLIM is capable of measuring lifetime from 100 ps to 100 ms and features the high data collection efficiency (up to 140-million counts per second). Other than the traditional nonlinear least-square fitting analysis, the raw data acquired by FastFLIM can be directly processed by the model-free phasor plots approach for instant and unbiased lifetime results, providing the ideal routine for the UCNP photoluminescence lifetime microscopy imaging.

Two-Photon Fluorescence Microscopy Developed for Microgravity Fluid Physics

NASA Technical Reports Server (NTRS)

Fischer, David G.; Zimmerli, Gregory A.; Asipauskas, Marius

2004-01-01

Recent research efforts within the Microgravity Fluid Physics Branch of the NASA Glenn Research Center have necessitated the development of a microscope capable of high-resolution, three-dimensional imaging of intracellular structure and tissue morphology. Standard optical microscopy works well for thin samples, but it does not allow the imaging of thick samples because of severe degradation caused by out-of-focus object structure. Confocal microscopy, which is a laser-based scanning microscopy, provides improved three-dimensional imaging and true optical sectioning by excluding the out-of-focus light. However, in confocal microscopy, out-of-focus object structure is still illuminated by the incoming beam, which can lead to substantial photo-bleaching. In addition, confocal microscopy is plagued by limited penetration depth, signal loss due to the presence of a confocal pinhole, and the possibility of live-cell damage. Two-photon microscopy is a novel form of laser-based scanning microscopy that allows three-dimensional imaging without many of the problems inherent in confocal microscopy. Unlike one-photon microscopy, it utilizes the nonlinear absorption of two near-infrared photons. However, the efficiency of two-photon absorption is much lower than that of one-photon absorption because of the nonlinear (i.e., quadratic) electric field dependence, so an ultrafast pulsed laser source must typically be employed. On the other hand, this stringent energy density requirement effectively localizes fluorophore excitation to the focal volume. Consequently, two-photon microscopy provides optical sectioning and confocal performance without the need for a signal-limiting pinhole. In addition, there is a reduction in photo-damage because of the longer excitation wavelength, a reduction in background fluorescence, and a 4 increase in penetration depth over confocal methods because of the reduction in Rayleigh scattering.

Two-photon absorption and transient photothermal imaging of pigments in tissues

NASA Astrophysics Data System (ADS)

Ye, Tong; Fu, Dan; Matthews, Thomas E.; Hong, Lian; Simon, John D.; Warren, Warren S.

2008-02-01

As a main pigment in skin tissues, melanin plays an important role in photo-protecting skin from UV radiation. However, melanogenesis may be altered due to disease or environmental factors; for example, sun exposure may cause damage and mutation of melanocytes and induce melanoma. Imaging pigmentation changes may provide invaluable information to catch the malignant transformation in its early stage and in turn improve the prognosis of patients. We have demonstrated previously that transmission mode, two-photon, one- or two-color absorption microscopy could provide remarkable contrast in imaging melanin in skin. In this report we demonstrate significantly improved sensitivity, so that we are now able to image in epi-mode (or back reflection) in two-photon absorption. This improvement makes possible for us to characterize the different types of pigmentation on the skin in vivo at virtually any location. Another finding is that we can also image transient photothermal dynamics due to the light absorption of melanin. By carefully choosing excitation and probe wavelengths, we might be able to image melanin in different structures under different micro-environments in skin, which could provide useful photochemical and photophysical insights in understanding how pigments are involved in photoprotection and photodamage of cells.

Enhancement of broadband optical absorption in photovoltaic devices by band-edge effect of photonic crystals.

PubMed

Tanaka, Yoshinori; Kawamoto, Yosuke; Fujita, Masayuki; Noda, Susumu

2013-08-26

We numerically investigate broadband optical absorption enhancement in thin, 400-nm thick microcrystalline silicon (µc-Si) photovoltaic devices by photonic crystals (PCs). We realize absorption enhancement by coupling the light from the free space to the large area resonant modes at the photonic band-edge induced by the photonic crystals. We show that multiple photonic band-edge modes can be produced by higher order modes in the vertical direction of the Si photovoltaic layer, which can enhance the absorption on multiple wavelengths. Moreover, we reveal that the photonic superlattice structure can produce more photonic band-edge modes that lead to further optical absorption. The absorption average in wavelengths of 500-1000 nm weighted to the solar spectrum (AM 1.5) increases almost twice: from 33% without photonic crystal to 58% with a 4 × 4 period superlattice photonic crystal; our result outperforms the Lambertian textured structure.

Entangled Two Photon Absorption Cross Section on the 808 nm Region for the Common Dyes Zinc Tetraphenylporphyrin and Rhodamine B.

PubMed

Villabona-Monsalve, Juan P; Calderón-Losada, Omar; Nuñez Portela, M; Valencia, Alejandra

2017-10-19

We report the measurement of the entangled two-photon absorption (ETPA) cross section, σ E , at 808 nm on organic chromophores in solution in a low photon flux regime. We performed measurements on zinc tetraphenylporphyrin (ZnTPP) in toluene and rhodamine B (RhB) in methanol. This is, to the best of our knowledge, the first time that σ E is measured for RhB. Additionally, we report a study of the dependence of σ E on the molecular concentration for both molecular systems. In contrast to previous experiments, our measurements are based on detecting the pairs of photons that are transmitted by the molecular system. By using a coincidence count circuit it was possible to improve the signal-to-noise ratio. This type of work is important for the development of spectroscopic and microscopic techniques using entangled photons.

Non linear optical investigations of silver nanoparticles synthesised by curcumin reduction

NASA Astrophysics Data System (ADS)

Dhanya, N. P.

2017-11-01

Metal nanoparticles have considerable applications in assorted fields like medicine, biology, photonics, metallurgy etc. Optical applications of Silver nanoparticles are of significant interest among researchers nowadays. In this paper, we report a single step chemical reduction of silver nanoparticles with Curcumin both as a reducing and stabilising agent at room temperature. Structural, plasmonic and non linear optical properties of the prepared nanoparticles are explored using Scanning Electron Microscope, Transmission Electron Microscope, UV absorption spectrometry, Spectroflurometry and Z scan. UV-Vis absorption studies affirm the Surface Plasmon Resonance (SPR) absorption and spectroflurometric studies announce the emission spectrum of the prepared silvernanoparticles at 520 nm. SEM and TEM images uphold the existence of uniform sized, spherical silvernanoparticles. Nonlinear optical studies are accomplished with the open aperture z scan technique in the nanosecond regime. The nonlinearity is in virtue of saturable absorption, two-photon absorption and excited state absorption. The marked nonlinearity and optical limiting of the Curcumin reduced silvernanoparticles enhances its photonic applications.

Development of Thermally Stable and Highly Fluorescent IR Dyes

NASA Technical Reports Server (NTRS)

Bu, Xiu R.

2004-01-01

Fluorophores are the core component in various optical applications such as sensors and probes. Fluorphores with low-energy or long wavelength emission, in particular, in NIR region, possess advantages of low interference and high sensitivity. In this study, we has explored several classes of imidazole-based compounds for NIR fluorescent properties and concluded: (1) thiazole-based imidazole compounds are fluorescent; (2) emission energy is tunable by additional donor groups; (3) they also possess impressive two- photon absorption properties; and (4) fluorescence emission can be induced by two- photon input. This report summarizes (1) synthesis of new series of fluorophore; (2) impact of electron-withdrawing groups on fluorescent property; (3) unique property of two-photon absorption; and (4) on-going development.

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

Xue, B.; Japan Science and Technology Agency, CREST, 5 Sanbancho, Chiyoda-ku, Tokyo, 102-0075; Katan, C.

This study demonstrates a measurement system for a non-degenerate two-photon absorption (NDTPA) spectrum. The NDTPA light sources are a white light super continuum beam (WLSC, 500 ∼ 720 nm) and a fundamental beam (798 nm) from a Ti:Sapphire laser. A reliable broadband NDTPA spectrum is acquired in a single-shot detection procedure using a 128-channel lock-in amplifier. The NDTPA spectra for several common laser dyes are measured. Two photon absorption cross section enhancements are found in the experiment and validated by theoretical calculation for all of the chromophores.

Observation of non-classical correlations in sequential measurements of photon polarization

NASA Astrophysics Data System (ADS)

Suzuki, Yutaro; Iinuma, Masataka; Hofmann, Holger F.

2016-10-01

A sequential measurement of two non-commuting quantum observables results in a joint probability distribution for all output combinations that can be explained in terms of an initial joint quasi-probability of the non-commuting observables, modified by the resolution errors and back-action of the initial measurement. Here, we show that the error statistics of a sequential measurement of photon polarization performed at different measurement strengths can be described consistently by an imaginary correlation between the statistics of resolution and back-action. The experimental setup was designed to realize variable strength measurements with well-controlled imaginary correlation between the statistical errors caused by the initial measurement of diagonal polarizations, followed by a precise measurement of the horizontal/vertical polarization. We perform the experimental characterization of an elliptically polarized input state and show that the same complex joint probability distribution is obtained at any measurement strength.

Photoionization of environmentally polluting aromatic chlorides and nitrides on the water surface by laser and synchrotron radiations.

PubMed

Sato, Miki; Maeda, Yuki; Ishioka, Toshio; Harata, Akira

2017-11-20

The detection limits and photoionization thresholds of polycyclic aromatic hydrocarbons and their chlorides and nitrides on the water surface are examined using laser two-photon ionization and single-photon ionization, respectively. The laser two-photon ionization methods are highly surface-selective, with a high sensitivity for aromatic hydrocarbons tending to accumulate on the water surface in the natural environment due to their highly hydrophobic nature. The dependence of the detection limits of target aromatic molecules on their physicochemical properties (photoionization thresholds relating to excess energy, molar absorptivity, and the octanol-water partition coefficient) is discussed. The detection limit clearly depends on the product of the octanol-water partition coefficient and molar absorptivity, and no clear dependence was found on excess energy. The detection limits of laser two-photon ionization for these types of molecules on the water surface are formulated.

A series of fluorene-based two-photon absorbing molecules: synthesis, linear and nonlinear characterization, and bioimaging

PubMed Central

Andrade, Carolina D.; Yanez, Ciceron O.; Rodriguez, Luis; Belfield, Kevin D.

2010-01-01

The synthesis, structural, and photophysical characterization of a series of new fluorescent donor–acceptor and acceptor-acceptor molecules, based on the fluorenyl ring system, with two-photon absorbing properties is described. These new compounds exhibited large Stokes shifts, high fluorescent quantum yields, and, significantly, high two-photon absorption cross sections, making them well suited for two-photon fluorescence microscopy (2PFM) imaging. Confocal and two-photon fluorescence microscopy imaging of COS-7 and HCT 116 cells incubated with probe I showed endosomal selectivity, demonstrating the potential of this class of fluorescent probes in multiphoton fluorescence microscopy. PMID:20481596

Two-dimensional imaging of molecular hydrogen in H2-air diffusion flames using two-photon laser-induced fluorescence

NASA Technical Reports Server (NTRS)

Lempert, W.; Kumar, V.; Glesk, I.; Miles, R.; Diskin, G.

1991-01-01

The use of a tunable ArF laser at 193.26 nm to record simultaneous single-laser-shot, planar images of molecular hydrogen and hot oxygen in a turbulent H2-air diffusion flame. Excitation spectra of fuel and oxidant-rich flame zones confirm a partial overlap of the two-photon H2 and single-photon O2 Schumann-Runge absorption bands. UV Rayleigh scattering images of flame structure and estimated detection limits for the H2 two-photon imaging are also presented.

Two-photon absorption induced stimulated Rayleigh-Bragg scattering

NASA Astrophysics Data System (ADS)

He, Guang S.; Prasad, Paras N.

2005-01-01

A frequency-unshifted and backward stimulated scattering can be efficiently generated in one-photon-absorption free but two-photon absorbing materials. Using a number of novel two-photon absorbing dye solutions as the scattering media and nanosecond pulsed laser as the pump beams, a highly directional backward stimulated scattering at the exact pump wavelength can be readily observed once the pump intensity is higher than a certain threshold level. The spectral and spatial structures as well as the temporal behavior and optical phase-conjugation property of this new type of backward stimulated scattering have been experimentally studied. This stimulated scattering phenomenon can be explained by using a model of two-photon-excitation enhanced standing-wave Bragg grating initially formed by the strong forward pump beam and much weaker backward Rayleigh scattering beam; the partial reflection of the pump beam from this grating provides an positive feedback to the initial backward Rayleigh scattering beam without suffering linear attenuation influence. Comparing to other known stimulated (Raman, Brillouin, Rayleigh-wing, and Kerr) scattering effects, the stimulated Rayleigh-Bragg scattering exhibits the advantages of no frequency-shift, low pump threshold, and low spectral linewidth requirement.

Synthesis, characterization, and nonlinear optical (NLO) properties of truxene-cored diphenylamine derivatives

NASA Astrophysics Data System (ADS)

Li, Fusheng; Zhao, Baodong; Chen, Yu; Zhang, Yufei; Wang, Tao; Xue, Song

2017-10-01

Three star-shaped compounds based on a truxene core (FS11, FS12 and FS13) were prepared. The truxene core is incorporating with asymmetric diphenylamines, including one phenyl of diphenylamine substituted by methoxy group and the other phenyl substituted by tolyl, fluorophenyl and phenylethynyl for FS11, FS12 and FS13, respectively. Their one-photon, two-photon absorption, geometric structures, electrochemical behavior and thermal properties were investigated. The absorption maxima of charge transfer band for FS11, FS12 and FS13 are 375 nm, 373 nm and 383 nm, and the corresponding molar extinction coefficients of FS11, FS12 and FS13 is 79,950 M- 1 cm- 1, 67,220 M- 1 cm- 1 and 108,780 M- 1 cm- 1. The ;pull-push; structure promotes charge transfer between asymmetric diphenylamine branches and the truxene core. Their two-photon absorbtion property is measured by two-photon induced fluorescence. The maximum two-photon cross-sections values of FS11, FS12 and FS13 are excited at 750 nm, which are 260 GM, 204GM and 367 GM, respectively.

Investigation of third-order nonlinear and optical power limiting properties of terphenyl derivatives

NASA Astrophysics Data System (ADS)

Kamath, Laxminarayana; Manjunatha, K. B.; Shettigar, Seetharam; Umesh, G.; Narayana, B.; Samshuddin, S.; Sarojini, B. K.

2014-03-01

A series of new chalcones containing terphenyl as a core and with different functional groups has been successfully synthesized by Claisen-Schmidt condensation method in search of new nonlinear optical (NLO) materials. Molecular structural characterization for the compounds was achieved by FTIR and single crystal X-ray diffraction. The third-order NLO absorption and refraction coefficients were simultaneously determined by Z-scan technique. The measurements were performed at 532 nm with 7 ns laser pulses using a Nd:YAG laser in solution form. The Z-scan experiments reveal that the compounds exhibit strong nonlinear refraction coefficient of the order 10-11 esu and the molecular two photon absorption cross section is 10-46 cm4 s/photon. The results also show that the structures of the compounds have great impact on NLO properties. The compounds show optical power limiting behavior due to two-photon absorption (TPA).

Sensitive measurement of nonlinear absorption and optical limiting in undoped and Fe-doped ZnO quantum dots using pulsed laser

NASA Astrophysics Data System (ADS)

Sharma, D.; Malik, B. P.; Gaur, A.

2016-11-01

Zinc oxide quantum dots (QDs) with Fe-doping at different concentrations were prepared by chemical co-precipitation method. The prepared QDs were characterized by UV-Vis spectroscopy, X-ray diffraction and Z-scan technique. The sizes of QDs were found to be within 4.6-6.6 nm range. The nonlinear parameters viz. two-photon absorption coefficient (βTPA) and two-photon absorption cross-section (σTPA) were extracted with the help of open aperture Z-scan technique using nanosecond Nd:YAG laser operating at wavelength 532 nm. Higher values of βTPA and σTPA for Fe doped ZnO implied that they were potential materials for development of photonics devices and sensor protection applications. Fe doped sample (3 % by wt) was found to be the best optical limiter with limiting threshold intensity of 0.64 TW/cm2.

Silicon-nanomembrane-based photonic crystal nanostructures for chip-integrated open sensor systems

NASA Astrophysics Data System (ADS)

Chakravarty, Swapnajit; Lai, Wei-Cheng; Zou, Yi; Lin, Cheyun; Wang, Xiaolong; Chen, Ray T.

2011-11-01

We experimentally demonstrate two devices on the photonic crystal platform for chip-integrated optical absorption spectroscopy and chip-integrated biomolecular microarray assays. Infrared optical absorption spectroscopy and biomolecular assays based on conjugate-specific binding principles represent two dominant sensing mechanisms for a wide spectrum of applications in environmental pollution sensing in air and water, chem-bio agents and explosives detection for national security, microbial contamination sensing in food and beverages to name a few. The easy scalability of photonic crystal devices to any wavelength ensures that the sensing principles hold across a wide electromagnetic spectrum. Silicon, the workhorse of the electronics industry, is an ideal platform for the above optical sensing applications.

Two-photon absorption laser-induced fluorescence measurements of atomic nitrogen in a radio-frequency atmospheric-pressure plasma jet

NASA Astrophysics Data System (ADS)

Wagenaars, E.; Gans, T.; O'Connell, D.; Niemi, K.

2012-08-01

The first direct measurements of atomic nitrogen species in a radio-frequency atmospheric-pressure plasma jet (APPJ) are presented. Atomic nitrogen radicals play a key role in new plasma medicine applications of APPJs. The measurements were performed with a two-photon absorption laser-induced fluorescence diagnostic, using 206.65 nm laser photons for the excitation of ground-state N atoms and observing fluorescence light around 744 nm. The APPJ was run with a helium gas flow of 1 slm and varying small admixtures of molecular nitrogen of 0-0.7 vol%. A maximum in the measured N concentration was observed for an admixture of 0.25 vol% N2.

Coherent perfect absorption in deeply subwavelength films in the single-photon regime

PubMed Central

Roger, Thomas; Vezzoli, Stefano; Bolduc, Eliot; Valente, Joao; Heitz, Julius J. F.; Jeffers, John; Soci, Cesare; Leach, Jonathan; Couteau, Christophe; Zheludev, Nikolay I.; Faccio, Daniele

2015-01-01

The technologies of heating, photovoltaics, water photocatalysis and artificial photosynthesis depend on the absorption of light and novel approaches such as coherent absorption from a standing wave promise total dissipation of energy. Extending the control of absorption down to very low light levels and eventually to the single-photon regime is of great interest and yet remains largely unexplored. Here we demonstrate the coherent absorption of single photons in a deeply subwavelength 50% absorber. We show that while the absorption of photons from a travelling wave is probabilistic, standing wave absorption can be observed deterministically, with nearly unitary probability of coupling a photon into a mode of the material, for example, a localized plasmon when this is a metamaterial excited at the plasmon resonance. These results bring a better understanding of the coherent absorption process, which is of central importance for light harvesting, detection, sensing and photonic data processing applications. PMID:25991584

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.

A theoretical study of a series of water-soluble triphenylamine photosensitizers for two-photon photodynamic therapy.

PubMed

Wang, Xin; Yin, Xue; Lai, Xiao-Yong; Liu, Ying-Tao

2018-10-05

In this study, the therapeutic activity of a series of water-soluble triphenylamine (TP) photosensitizers (Ps) was explored by using theoretical simulations. The key photophysical parameters which determined the efficiency of Ps, such as absorption electronic spectra, singlet-triplet energy gaps and spin-orbit matrix elements were calculated at density functional theory and its time-dependent extension (DFT, TD-DFT). The calculated results showed that these TP photosensitizers possessed large two-photon absorption cross-section in the near-infrared region (NIR), efficient intersystem crossing (ISC) transition from the first singlet excited state to the low lying triplet excited states and sufficient energy for generating reactive oxygen species (ROS). These suitable features made these TP series holding great promise for applications in two-photon photodynamic therapy (PDT). These TP photosensitizers studied here in principle extended the application range of two-photon PDT in water solution. Copyright © 2018 Elsevier B.V. All rights reserved.

Open-Ended Recursive Approach for the Calculation of Multiphoton Absorption Matrix Elements

PubMed Central

2015-01-01

We present an implementation of single residues for response functions to arbitrary order using a recursive approach. Explicit expressions in terms of density-matrix-based response theory for the single residues of the linear, quadratic, cubic, and quartic response functions are also presented. These residues correspond to one-, two-, three- and four-photon transition matrix elements. The newly developed code is used to calculate the one-, two-, three- and four-photon absorption cross sections of para-nitroaniline and para-nitroaminostilbene, making this the first treatment of four-photon absorption in the framework of response theory. We find that the calculated multiphoton absorption cross sections are not very sensitive to the size of the basis set as long as a reasonably large basis set with diffuse functions is used. The choice of exchange–correlation functional, however, significantly affects the calculated cross sections of both charge-transfer transitions and other transitions, in particular, for the larger para-nitroaminostilbene molecule. We therefore recommend the use of a range-separated exchange–correlation functional in combination with the augmented correlation-consistent double-ζ basis set aug-cc-pVDZ for the calculation of multiphoton absorption properties. PMID:25821415

Cross-phase modulation-induced spectral broadening in silicon waveguides.

PubMed

Zhang, Yanbing; Husko, Chad; Lefrancois, Simon; Rey, Isabella H; Krauss, Thomas F; Schröder, Jochen; Eggleton, Benjamin J

2016-01-11

We analytically and experimentally investigate cross-phase modulation (XPM) in silicon waveguides. In contrast to the well known result in pure Kerr media, the spectral broadening ratio of XPM to self-phase modulation is not two in the presence of either two-photon absorption (TPA) or free carriers. The physical origin of this change is different for each effect. In the case of TPA, this nonlinear absorption attenuates and slightly modifies the pulse shape due to differential absorption in the pulse peak and wings. When free carriers are present two different mechanisms modify the dynamics. First, free-carrier absorption performs a similar role to TPA, but is additionally asymmetric due to the delayed free-carrier response. Second, free-carrier dispersion induces an asymmetric blue phase shift which competes directly with the symmetric Kerr-induced XPM red shift. We confirm this analysis with pump-probe experiments in a silicon photonic crystal waveguide.

Stimulated emission and lasing from all-inorganic perovskite quantum dots

NASA Astrophysics Data System (ADS)

Sun, Handong; Wang, Yue; Li, Xiaoming; Haibo, Zeng

We present superior optical gain and lasing properties in a new class of emerging quantum materials, the colloidal all-inorganic cesium lead halide perovskite quantum dots (IPQDs) (CsPbX3, X = Cl, Br, I). Our result has indicated that such material system show combined merits of both colloidal quantum dots and halide perovskites. Low-threshold and ultrastable stimulated emission was demonstrated under atmospheric condition. The flexibility and advantageous optical gain properties of these CsPbX3 IPQDs were manifested by demonstration of an optically pumped micro-laser. The nonlinear optical properties including the multi-photon absorption and resultant photoluminescence of the CsPbX3 nanocrystals were investigated. A large two-photon absorption cross-section of up to ~1.2×105 GM is determined from 9 nm-sized CsPbBr3 nanocrystals. Moreover, low-threshold frequency-upconverted stimulated emission by two-photon absorption was observed from the thin films of close-packed CsPbBr3 nanocrystals. We further realize the three-photon pumped stimulated emission in green spectra range from colloidal IPQD.

Ultrafast responses of dipolar and V-shaped dipicolinate derivatives with potential applications in the labeling of biomolecules

NASA Astrophysics Data System (ADS)

Wang, Yaochuan; Liu, Siyuan; Liu, Dajun; Wang, Guiqiu; Xiao, Haibo

2016-02-01

A dipolar dipicolinate derivative, trans-dimethyl-4-[4'-(N,N-diphenylamino)-styry1]-pyridin-2,6-dicarboxylate (P-1), and a P-1based V-shaped compound, {4-[(E)-2-(2,6-dimethoxycarbonylpyridin-4-yl) vinyl]}-N-phenyl-N-{4-[(E)-2-(2,6-dimethoxycarbonylpyridin-4-yl)vinylphenyl]}aniline (P-2), with intense two-photon fluorescence emission properties were systematically investigated by using steady-state absorption and fluorescence spectroscopy, open-aperture Z-scans, and two-photon excited fluorescence (TPF). The two-photon absorption cross-section of the V-shaped compound P-2 in tetrahydrofuran (THF) was determined to be 208 GM, which represents a 6.5-fold enhancement compared with its dipolar counterpart P-1 (32 GM). Extension of the intramolecular charge transfer (ICT) in the V-shaped dipicolinate derivative has been suggested as the mechanism of enhancement. The excited state dynamics from transient absorption spectroscopy were analyzed and discussed. The formation and relaxation lifetimes of the ICT state for these dipicolinate derivatives in THF solutions were found to be several picoseconds and several hundred picoseconds, respectively. The results show an increased ICT character of the V-shaped compound and a potential application for this compound in two-photon fluorescence imaging fields.

Nano-photonic light trapping near the Lambertian limit in organic solar cell architectures.

PubMed

Biswas, Rana; Timmons, Erik

2013-09-09

A critical step to achieving higher efficiency solar cells is the broad band harvesting of solar photons. Although considerable progress has recently been achieved in improving the power conversion efficiency of organic solar cells, these cells still do not absorb upto ~50% of the solar spectrum. We have designed and developed an organic solar cell architecture that can boost the absorption of photons by 40% and the photo-current by 50% for organic P3HT-PCBM absorber layers of typical device thicknesses. Our solar cell architecture is based on all layers of the solar cell being patterned in a conformal two-dimensionally periodic photonic crystal architecture. This results in very strong diffraction of photons- that increases the photon path length in the absorber layer, and plasmonic light concentration near the patterned organic-metal cathode interface. The absorption approaches the Lambertian limit. The simulations utilize a rigorous scattering matrix approach and provide bounds of the fundamental limits of nano-photonic light absorption in periodically textured organic solar cells. This solar cell architecture has the potential to increase the power conversion efficiency to 10% for single band gap organic solar cells utilizing long-wavelength absorbers.

Measurement of the Two-photon Absorption Coefficient of Gallium Phosphide (GaP) Using a Dispersion-minimized Sub-10 Femtosecond Z-scan Measurement System

DTIC Science & Technology

2012-09-01

bandwidth of the pulse. Using the standard laboratory and analysis methods of Sheik- Bahae et al., we obtain a two-photon absorption coefficient, β, of...organic thin-film materials deposited on various substrates. 15 6. References 1. Sheik- Bahae , M.; Said, A. A.; Van Stryland, E. W. High...sensitivity, Single-beam n2 Measurements. Optics Letters 1989, 14 (17). 2. Sheik- Bahae , M.; Said, A. A.; Van Stryland, E. W.; Wei, T-H; Hagan, D. J

Studies of Interactions Between Nano-Objects and Polarized Light

NASA Astrophysics Data System (ADS)

Xie, Dan

Optical studies of nano-objects that have dimensions 10--1000 nm have become a flourishing field of research. This special dimension category, connecting the smaller (molecular) world and the larger (cellular) world, have enabled these nano-objects to be widely utilized as novel optical tools in many fields. In addition to the extensive applications of nano objects, increasing efforts are also being put to better understand their interactions with light at a fundamental level. The work presented in this dissertation is part of such efforts, in which I selected three types of nano-objects and studied their optical properties both in theory and experiment. Second-harmonic and sum-frequency generations are among the most well-known nonlinear optical processes. Dielectric nanocrystals that are SHG- and SFG-active are favored tools in bioimaging. For a nanocrystal, its SHG/SFG intensity depends on the geometry of the light-particle system, i.e., the relationship between the nanocrystal orientation and the laser polarization. Using BaTiO 3 nanocrystals as an example, I carried out an in-depth, theoretical investigation of such dependence. Particularly, I studied the possibility of selectively maximizing the contrast between light signals from two or more nanocrystals by manipulating laser polarization. I will present a discussion on how the capacity of this selective illumination depends on the relative orientation between the two nanocrystals and the polarization of the excitation field. The optical responses of non-spherical plasmonic particles, being dynamic and complex, are only partially understood. Gold nanorods (AuNRs) are one of the most popular members in this nanoparticle family. They can produce two-photon luminescence (TPL) and amplify molecular events occurring at their surface. Both phenomena are known to be associated with surface plasmon resonances (SPR) of AuNRs, but details of the mechanisms are yet to be understood and quantified. I constructed a two-photon laser-scanning microscopy system to study these phenomena at the single-particle level. In the experiment, I measured the polarization-dependent TPL emissions from single nanorods that are triggered by time-resolved two-photon excitations. The observation indicates that, different from what was generally believed, the TPL in AuNRs is resulted from two sequentially one-photon absorption process that are both coupled to the longitudinal SPR mode. The studies on the two-photon fluorescence in dyes conjugated with AuNRs confirmed the coherent nature of the two-photon absorption process and provided an estimate of the fluorescence enhancement due to the presence of AuNRs. Molecules with cross-conjugated structures have a special role in molecular electronics. Their inherent quantum interference property can be utilized to create molecular switches with excellent on/off ratio. When a molecular junction is exposed to light, photons may open extra pathways for electron tunneling, and thus modify the conduction properties of the junction. Such modification depends on the electronic structure of the molecule, as well as on the frequency, amplitude, and polarization of the driving field. In collaboration with my colleague, I simulated electron tunneling properties of junctions with cross-conjugated molecules and discussed their dependence on light properties. It is noteworthy that symmetry plays a major role in zero-bias tunneling: the molecule-field systems with general parity show distinct tunneling behaviors from their counterparts without general parity.

Effect of marine derived deoxyribonucleic acid on nonlinear optical properties of PicoGreen dye

NASA Astrophysics Data System (ADS)

Pradeep, C.; Mathew, S.; Nithyaja, B.; Radhakrishnan, P.; Nampoori, V. P. N.

2013-06-01

We have investigated the effect of DNA on nonlinear absorption of PicoGreen dye using single beam open aperture Z-scan technique in nanosecond regime. We observed reverse saturable absorption at 532 nm for PicoGreen without DNA. In the presence of DNA, the sample begins to behave like saturable absorbers and this effect increased as the concentration of DNA was increased. The dye-intercalated DNA showed SA characteristics near the focus but exhibited RSA characteristics at the focus. Theoretical analysis has been performed using a two-photon absorption model based on nonlinear absorption coefficient and saturation intensity. Such tailoring of optical nonlinear absorption in PicoGreen makes it a potential candidate for photonic application.

Energy transfer and energy absorption in photon interactions with matter revisited: A step-by-step illustrated approach

NASA Astrophysics Data System (ADS)

Abdel-Rahman, W.; Podgorsak, E. B.

2010-05-01

A clear understanding of energy transfer and energy absorption in photon interactions with matter is essential for the understanding of radiation dosimetry and development of new dosimetry techniques. The concepts behind the two quantities have been enunciated many years ago and described in many scientific papers, review articles, and textbooks. Data dealing with energy transfer and energy absorption as well as the associated mass energy transfer coefficient and the mass energy absorption coefficient are readily available in web-based tabular forms. However, tables, even when available in detailed and easy to access form, do not lend themselves to serve as visual aid to promote better understanding of the dosimetric quantities related to energy transfer and energy absorption as well as their relationship to the photon energy and absorber atomic number. This paper uses graphs and illustrations, in addition to well-known mathematical relationships, to guide the reader in a systematic manner through the various stages involved in the derivation of energy absorbed in medium and its associated quantity, the mass energy absorption coefficient, from the mass attenuation coefficient.

Two-Photon Absorbing Phosphorescent Metalloporphyrins: Effects of π-Extension and Peripheral Substitution.

PubMed

Esipova, Tatiana V; Rivera-Jacquez, Héctor J; Weber, Bruno; Masunov, Artëm E; Vinogradov, Sergei A

2016-12-07

The ability to form triplet excited states upon two-photon excitation is important for several applications of metalloporphyrins, including two-photon phosphorescence lifetime microscopy (2PLM) and two-photon photodynamic therapy (PDT). Here we analyzed one-photon (1P) and degenerate two-photon (2P) absorption properties of several phosphorescent Pt (II) porphyrins, focusing on the effects of aromatic π-extension and peripheral substitution on triplet emissivity and two-photon absorption (2PA). Our 2PA measurements for the first time made use of direct time-resolved detection of phosphorescence, having the ability to efficiently reject laser background through microsecond time gating. π-Extension of the porphyrin macrocycle by way of syn-fusion with two external aromatic fragments, such as in syn-dibenzo- (DBP) and syn-dinaphthoporphyrins (DNP), lowers the symmetry of the porphyrin skeleton. As a result, DBPs and DNPs exhibit stronger 2PA into the one-photon-allowed B (Soret) and Q states than fully symmetric (D 4h ) nonextended porphyrins. However, much more 2P-active states lie above the B state and cannot be accessed due to the interfering linear absorption. Alkoxycarbonyl groups (CO 2 R) in the benzo-rings dramatically enhance 2PA near the B state level. Time-dependent density functional theory (TDDFT) calculations in combinations with the sum-over-states (SOS) formalism revealed that the enhancement is due to the stabilization of higher-lying 2P-active states, which are dominated by the excitations involving orbitals extending onto the carbonyl groups. Furthermore, calculations predicted even stronger stabilization of the 2P-allowed gerade-states in symmetric Pt octaalkoxycarbonyl-tetrabenzoporphyrins. Experiments confirmed that the 2PA cross-section of PtTBP(CO 2 Bu) 8 near 810 nm reaches above 500 GM in spite of its completely centrosymmetric structure. Combined with exceptionally bright phosphorescence (ϕ phos = 0.45), strong 2PA makes Pt(II) complexes of π-extended porphyrins a valuable class of chromophores for 2P applications. Another important advantage of these porphyrinoids is their compact size and easily scalable synthesis.

Modified two-photon absorption and dispersion of ultrafast third-order polarization beats via twin noisy driving fields

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

Zhang Yanpeng; Department of Electronic Science and Technology, Xi'an Jiaotong University, Xi'an 710049; Gan Chenli

2006-05-15

We investigate the color-locked twin-noisy-field correlation effects in third-order nonlinear absorption and dispersion of ultrafast polarization beats. We demonstrate a phase-sensitive method for studying the two-photon nondegenerate four-wave mixing (NDFWM) due to atomic coherence in a multilevel system. The reference signal is another one-photon degenerate four-wave-mixing signal, which propagates along the same optical path as the NDFWM signal. This method is used for studying the phase dispersion of the third-order susceptibility and for the optical heterodyne detection of the NDFWM signal. The third-order nonlinear response can be controlled and modified through the color-locked correlation of twin noisy fields.

Measuring Incompatible Observables by Exploiting Sequential Weak Values.

PubMed

Piacentini, F; Avella, A; Levi, M P; Gramegna, M; Brida, G; Degiovanni, I P; Cohen, E; Lussana, R; Villa, F; Tosi, A; Zappa, F; Genovese, M

2016-10-21

One of the most intriguing aspects of quantum mechanics is the impossibility of measuring at the same time observables corresponding to noncommuting operators, because of quantum uncertainty. This impossibility can be partially relaxed when considering joint or sequential weak value evaluation. Indeed, weak value measurements have been a real breakthrough in the quantum measurement framework that is of the utmost interest from both a fundamental and an applicative point of view. In this Letter, we show how we realized for the first time a sequential weak value evaluation of two incompatible observables using a genuine single-photon experiment. These (sometimes anomalous) sequential weak values revealed the single-operator weak values, as well as the local correlation between them.

Measuring Incompatible Observables by Exploiting Sequential Weak Values

NASA Astrophysics Data System (ADS)

Piacentini, F.; Avella, A.; Levi, M. P.; Gramegna, M.; Brida, G.; Degiovanni, I. P.; Cohen, E.; Lussana, R.; Villa, F.; Tosi, A.; Zappa, F.; Genovese, M.

2016-10-01

One of the most intriguing aspects of quantum mechanics is the impossibility of measuring at the same time observables corresponding to noncommuting operators, because of quantum uncertainty. This impossibility can be partially relaxed when considering joint or sequential weak value evaluation. Indeed, weak value measurements have been a real breakthrough in the quantum measurement framework that is of the utmost interest from both a fundamental and an applicative point of view. In this Letter, we show how we realized for the first time a sequential weak value evaluation of two incompatible observables using a genuine single-photon experiment. These (sometimes anomalous) sequential weak values revealed the single-operator weak values, as well as the local correlation between them.

Dynamical Evolution of Properties for Atom and Field in the Process of Two-Photon Absorption and Emission Between Atomic Levels

NASA Astrophysics Data System (ADS)

Wang, Jian-ming; Xu, Xue-xiang

2018-04-01

Using dressed state method, we cleverly solve the dynamics of atom-field interaction in the process of two-photon absorption and emission between atomic levels. Here we suppose that the atom is initially in the ground state and the optical field is initially in Fock state, coherent state or thermal state, respectively. The properties of the atom, including the population in excited state and ground state, the atom inversion, and the properties for optical field, including the photon number distribution, the mean photon number, the second-order correlation function and the Wigner function, are discussed in detail. We derive their analytical expressions and then make numerical analysis for them. In contrast with Jaynes-Cummings model, some similar results, such as quantum Rabi oscillation, revival and collapse, are also exhibit in our considered model. Besides, some novel nonclassical states are generated.

Optimal mode transformations for linear-optical cluster-state generation

DOE PAGES

Uskov, Dmitry B.; Lougovski, Pavel; Alsing, Paul M.; ...

2015-06-15

In this paper, we analyze the generation of linear-optical cluster states (LOCSs) via sequential addition of one and two qubits. Existing approaches employ the stochastic linear-optical two-qubit controlled-Z (CZ) gate with success rate of 1/9 per operation. The question of optimality of the CZ gate with respect to LOCS generation has remained open. We report that there are alternative schemes to the CZ gate that are exponentially more efficient and show that sequential LOCS growth is indeed globally optimal. We find that the optimal cluster growth operation is a state transformation on a subspace of the full Hilbert space. Finally,more » we show that the maximal success rate of postselected entangling n photonic qubits or m Bell pairs into a cluster is (1/2) n-1 and (1/4) m-1, respectively, with no ancilla photons, and we give an explicit optical description of the optimal mode transformations.« less

Up-conversion in rare-earth doped micro-particles applied to new emissive two-dimensional displays

NASA Astrophysics Data System (ADS)

Milliez, Anne Janet

Up-conversion (UC) in rare-earth co-doped fluorides to convert diode laser light in the near infrared to red, green and blue visible light is applied to make possible high performance emissive displays. The infrared-to-visible UC in the materials we study is a sequential form of non-linear two photon absorption in which a strong absorbing constituent absorbs two low energy photons and transfers this energy to another constituent which emits visible light. Some of the UC emitters' most appealing characteristics for displays are: a wide color gamut with very saturated colors, very high brightness operation without damage to the emitters, long lifetimes and efficiencies comparable to those of existing technologies. Other advantages include simplicity of fabrication, versatility of operating modes, and the potential for greatly reduced display weight and depth. Thanks to recent advances in material science and diode laser technology at the excitation wavelength, UC selected materials can be very efficient visible emitters. However, optimal UC efficiencies strongly depend on chosing proper operating conditions. In this thesis, we studied the conditions required for optimization. We demonstrated that high efficiency UC depends on high pump irradiance, low temperature and low scattering. With this understanding we can predict how to optimally use UC emitters in a wide range of applications. In particular, we showed how our very efficient UC emitters can be applied to make full color displays and very efficient white light sources.

Two-Photon Pumped Synchronously Mode-Locked Bulk GaAs Laser

NASA Astrophysics Data System (ADS)

Cao, W. L.; Vaucher, A. M.; Ling, J. D.; Lee, C. H.

1982-04-01

Pulses 7 picoseconds or less in duration have been generated from a bulk GaAs crystal by a synchronous mode-locking technique. The GaAs crystal was optically pumped by two-photon absorption of the emission from a mode-locked Nd:glass laser. Two-photon absorption as the means of excitation increases the volume of the gain medium by increasing the pene-tration depth of the pump intensity, enabling generation of intra-cavity pulses with peak power in the megawatt range. Tuning of the wavelength of the GaAs emission is achieved by varying the temperature. A tuning range covering 840 nm to 885 nm has been observed over a temperature range from 97°K to 260°K. The intensity of the GaAs emission has also been observed to decrease as the temperature of the crystal is increased.

Molecular photosensitisers for two-photon photodynamic therapy.

PubMed

Bolze, F; Jenni, S; Sour, A; Heitz, V

2017-11-30

Two-photon excitation has attracted the attention of biologists, especially after the development of two-photon excited microscopy in the nineties. Since then, new applications have rapidly emerged such as the release of biologically active molecules and photodynamic therapy (PDT) using two-photon excitation. PDT, which requires a light-activated drug (photosensitiser), is a clinically approved and minimally invasive treatment for cancer and for non-malignant diseases. This feature article focuses on the engineering of molecular two-photon photosensitisers for PDT, which should bring important benefits to the treatment, increase the treatment penetration depth with near-infrared light excitation, improve the spatial selectivity and reduce the photodamage to healthy tissues. After an overview of the two-photon absorption phenomenon and the methods to evaluate two-photon induced phototoxicity on cell cultures, the different classes of photosensitisers described in the literature are discussed. The two-photon PDT performed with historical one-photon sensitisers are briefly presented, followed by specifically engineered cyclic tetrapyrrole photosensitisers, purely organic photosensitisers and transition metal complexes. Finally, targeted two-photon photosensitisers and theranostic agents that should enhance the selectivity and efficiency of the treatment are discussed.

Novel xenon calibration scheme for two-photon absorption laser induced fluorescence of hydrogen

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

Elliott, Drew; Scime, Earl; Short, Zachary, E-mail: zdshort@mix.wvu.edu

Two photon absorption laser induced fluorescence (TALIF) measurements of neutral hydrogen and its isotopes are typically calibrated by performing TALIF measurements on krypton with the same diagnostic system and using the known ratio of the absorption cross sections [K. Niemi et al., J. Phys. D 34, 2330 (2001)]. Here we present the measurements of a new calibration method based on a ground state xenon scheme for which the fluorescent emission wavelength is nearly identical to that of hydrogen, thereby eliminating chromatic effects in the collection optics and simplifying detector calibration. We determine that the ratio of the TALIF cross sectionsmore » of xenon and hydrogen is 0.024 ± 0.001.« less

Precise Two-Photon Photodynamic Therapy using an Efficient Photosensitizer with Aggregation-Induced Emission Characteristics.

PubMed

Gu, Bobo; Wu, Wenbo; Xu, Gaixia; Feng, Guangxue; Yin, Feng; Chong, Peter Han Joo; Qu, Junle; Yong, Ken-Tye; Liu, Bin

2017-07-01

Two-photon photodynamic therapy (PDT) is able to offer precise 3D manipulation of treatment volumes, providing a target level that is unattainable with current therapeutic techniques. The advancement of this technique is greatly hampered by the availability of photosensitizers with large two-photon absorption (TPA) cross section, high reactive-oxygen-species (ROS) generation efficiency, and bright two-photon fluorescence. Here, an effective photosensitizer with aggregation-induced emission (AIE) characteristics is synthesized, characterized, and encapsulated into an amphiphilic block copolymer to form organic dots for two-photon PDT applications. The AIE dots possess large TPA cross section, high ROS generation efficiency, and excellent photostability and biocompatibility, which overcomes the limitations of many conventional two-photon photosensitizers. Outstanding therapeutic performance of the AIE dots in two-photon PDT is demonstrated using in vitro cancer cell ablation and in vivo brain-blood-vessel closure as examples. This shows therapy precision up to 5 µm under two-photon excitation. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Multiphoton-gated cycloreversion reaction of a fluorescent diarylethene derivative as revealed by transient absorption spectroscopy.

PubMed

Nagasaka, Tatsuhiro; Kunishi, Tomohiro; Sotome, Hikaru; Koga, Masafumi; Morimoto, Masakazu; Irie, Masahiro; Miyasaka, Hiroshi

2018-06-07

The one- and two-photon cycloreversion reactions of a fluorescent diarylethene derivative with oxidized benzothiophene moieties were investigated by means of ultrafast laser spectroscopy. Femtosecond transient absorption spectroscopy under the one-photon excitation condition revealed that the excited closed-ring isomer is simply deactivated into the initial ground state with a time constant of 2.6 ns without remarkable cycloreversion, the results of which are consistent with the very low cycloreversion reaction yield (<10-5) under steady-state light irradiation. On the other hand, an efficient cycloreversion reaction was observed under irradiation with a picosecond laser pulse at 532 nm. The excitation intensity dependence of the cycloreversion reaction indicates that a highly excited state attained by the stepwise two-photon absorption is responsible for the marked increase of the cycloreversion reaction, and the quantum yield at the highly excited state was estimated to be 0.018 from quantitative analysis, indicating that the reaction is enhanced by a factor of >1800.

A stable frequency comb directly referenced to rubidium electromagnetically induced transparency and two-photon transitions

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

Hou, Dong; Wu, Jiutao; Zhang, Shuangyou

2014-03-17

We demonstrate an approach to create a stable erbium-fiber-based frequency comb at communication band by directly locking the combs to two rubidium atomic transitions resonances (electromagnetically induced transparency absorption and two-photon absorption), respectively. This approach directly transfers the precision and stability of the atomic transitions to the comb. With its distinguishing feature of compactness by removing the conventional octave-spanning spectrum and f-to-2f beating facilities and the ability to directly control the comb's frequency at the atomic transition frequency, this stable optical comb can be widely used in optical communication, frequency standard, and optical spectroscopy and microscopy.

Method and apparatus for producing laser radiation following two-photon excitation of a gaseous medium

DOEpatents

Bischel, William K. [Menlo Park, CA; Jacobs, Ralph R. [Livermore, CA; Prosnitz, Donald [Hamden, CT; Rhodes, Charles K. [Palo Alto, CA; Kelly, Patrick J. [Fort Lewis, WA

1979-02-20

Method and apparatus for producing laser radiation by two-photon optical pumping of an atomic or molecular gaseous medium and subsequent lasing action. A population inversion is created as a result of two-photon absorption of the gaseous species. Stark tuning is utilized, if necessary, in order to tune the two-photon transition into exact resonance. In particular, gaseous ammonia (NH.sub.3) or methyl fluoride (CH.sub.3 F) is optically pumped by a pair of CO.sub.2 lasers to create a population inversion resulting from simultaneous two-photon excitation of a high-lying vibrational state, and laser radiation is produced by stimulated emission of coherent radiation from the inverted level.

Method and apparatus for producing laser radiation following two-photon excitation of a gaseous medium

DOEpatents

Bischel, W.K.; Jacobs, R.R.; Prosnitz, D.P.; Rhodes, C.K.; Kelly, P.J.

1979-02-20

Method and apparatus are disclosed for producing laser radiation by two-photon optical pumping of an atomic or molecular gaseous medium and subsequent lasing action. A population inversion is created as a result of two-photon absorption of the gaseous species. Stark tuning is utilized, if necessary, in order to tune the two-photon transition into exact resonance. In particular, gaseous ammonia (NH[sub 3]) or methyl fluoride (CH[sub 3]F) is optically pumped by a pair of CO[sub 2] lasers to create a population inversion resulting from simultaneous two-photon excitation of a high-lying vibrational state, and laser radiation is produced by stimulated emission of coherent radiation from the inverted level. 3 figs.

High-power, high-repetition-rate performance characteristics of β-BaB₂O₄ for single-pass picosecond ultraviolet generation at 266 nm.

PubMed

Kumar, S Chaitanya; Casals, J Canals; Wei, Junxiong; Ebrahim-Zadeh, M

2015-10-19

We report a systematic study on the performance characteristics of a high-power, high-repetition-rate, picosecond ultraviolet (UV) source at 266 nm based on β-BaB2O4 (BBO). The source, based on single-pass fourth harmonic generation (FHG) of a compact Yb-fiber laser in a two-crystal spatial walk-off compensation scheme, generates up to 2.9 W of average power at 266 nm at a pulse repetition rate of ~80 MHz with a single-pass FHG efficiency of 35% from the green to UV. Detrimental issues such as thermal effects have been studied and confirmed by performing relevant measurements. Angular and temperature acceptance bandwidths in BBO for FHG to 266 nm are experimentally determined, indicating that the effective interaction length is limited by spatial walk-off and thermal gradients under high-power operation. The origin of dynamic color center formation due to two-photon absorption in BBO is investigated by measurements of intensity-dependent transmission at 266 nm. Using a suitable theoretical model, two-photon absorption coefficients as well as the color center densities have been estimated at different temperatures. The measurements show that the two-photon absorption coefficient in BBO at 266 nm is ~3.5 times lower at 200°C compared to that at room temperature. The long-term power stability as well as beam pointing stability is analyzed at different output power levels and focusing conditions. Using cylindrical optics, we have circularized the generated elliptic UV beam to a circularity of >90%. To our knowledge, this is the first time such high average powers and temperature-dependent two-photon absorption measurements at 266 nm are reported at repetition rates as high as ~80 MHz.

Photochemical Upconversion: A Physical or Inorganic Chemistry Experiment for Undergraduates Using a Conventional Fluorimeter

ERIC Educational Resources Information Center

Wilke, Bryn M.; Castellano, Felix N.

2013-01-01

Photochemical upconversion is a regenerative process that transforms lower-energy photons into higher-energy light through two sequential bimolecular reactions, triplet sensitization of an appropriate acceptor followed by singlet fluorescence producing triplet-triplet annihilation derived from two energized acceptors. This laboratory directly…

Autocorrelation measurement of femtosecond laser pulses based on two-photon absorption in GaP photodiode

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

Chong, E. Z.; Watson, T. F.; Festy, F., E-mail: frederic.festy@kcl.ac.uk

2014-08-11

Semiconductor materials which exhibit two-photon absorption characteristic within a spectral region of interest can be useful in building an ultra-compact interferometric autocorrelator. In this paper, we report on the evidence of a nonlinear absorption process in GaP photodiodes which was exploited to measure the temporal profile of femtosecond Ti:sapphire laser pulses with a tunable peak wavelength above 680 nm. The two-photon mediated conductivity measurements were performed at an average laser power of less than a few tenths of milliwatts. Its suitability as a single detector in a broadband autocorrelator setup was assessed by investigating the nonlinear spectral sensitivity bandwidth of amore » GaP photodiode. The highly favourable nonlinear response was found to cover the entire tuning range of our Ti:sapphire laser and can potentially be extended to wavelengths below 680 nm. We also demonstrated the flexibility of GaP in determining the optimum compensation value of the group delay dispersion required to restore the positively chirped pulses inherent in our experimental optical system to the shortest pulse width possible. With the rise in the popularity of nonlinear microscopy, the broad two-photon response of GaP and the simplicity of this technique can provide an alternative way of measuring the excitation laser pulse duration at the focal point of any microscopy systems.« less

Characterization of Photon-Counting Detector Responsivity for Non-Linear Two-Photon Absorption Process

NASA Technical Reports Server (NTRS)

Sburlan, S. E.; Farr, W. H.

2011-01-01

Sub-band absorption at 1550 nm has been demonstrated and characterized on silicon Geiger mode detectors which normally would be expected to have no response at this wavelength. We compare responsivity measurements to singlephoton absorption for wavelengths slightly above the bandgap wavelength of silicon (approx. 1100 microns). One application for this low efficiency sub-band absorption is in deep space optical communication systems where it is desirable to track a 1030 nm uplink beacon on the same flight terminal detector array that monitors a 1550 nm downlink signal for pointingcontrol. The currently observed absorption at 1550 nm provides 60-70 dB of isolation compared to the response at 1064 nm, which is desirable to avoid saturation of the detector by scattered light from the downlink laser.

Laser augmented decomposition. II. D/sub 3/BPF/sub 3/. [Deuterium effects

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

Chien, K.R.; Bauer, S.H.

1976-06-17

The study of the accelerated decomposition of H/sub 3/BPF/sub 3/ induced by laser radiation (930-950 cm/sup -1/ was extended to the fully deuterated species. While in all essential respects the kinetics of the ir photolysis for the two compounds are identical, the few differences which were uncovered proved crucial in pointing to interesting features of the mechanism. These verified predictions were based on a normal mode analysis for the distribution of potential energy among the internal coordinates. For the laser augmented decomposition, E/sub a//sup L/ = 3.5 +- 1 kcal/mol, compared with E/sub a//sup th/ = 29.3 kcal/mol for themore » thermal process. The quantum efficiency is low, approximately 4 x 10/sup 4/ photons/molecule decomposed. The rates of decomposition depend on the isotopic content and are sensitively dependent on the frequency of the irradiating line. For example, with P(24) large fractionation ratios were found for D/sub 3/BPF/sub 3/ vs. H/sub 3/BPF/sub 3/, and small differences for D/sub 3//sup 11/BPF/sub 3/ vs. D/sub 3//sup 10/BPF/sub 3/. The levels of decomposition induced by the sequential three-photon absorption have been semiquantitatively accounted for.« less

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

Makarov, Nikolay S.; Lin, Qianglu; Pietryga, Jeffrey M.

One source of efficiency losses in photovoltaic cells is their transparency toward solar photons with energies below the band gap of the absorbing layer. This loss can be reduced using a process of up-conversion whereby two or more sub-band-gap photons generate a single above-gap exciton. Traditional approaches to up-conversion, such as nonlinear two-photon absorption (2PA) or triplet fusion, suffer from low efficiency at solar light intensities, a narrow absorption bandwidth, nonoptimal absorption energies, and difficulties for implementing in practical devices. We show that these deficiencies can be alleviated using the effect of Auger up-conversion in thick-shell PbSe/CdSe quantum dots. Thismore » process relies on Auger recombination whereby two low-energy, core-based excitons are converted into a single higher-energy, shell-based exciton. When compared to their monocomponent counterparts, the tailored PbSe/CdSe heterostructures feature enhanced absorption cross-sections, a higher efficiency of the “productive” Auger pathway involving re-excitation of a hole, and longer lifetimes of both core- and shell-localized excitons. These features lead to effective up-conversion cross-sections that are more than 6 orders of magnitude higher than for standard nonlinear 2PA, which allows for efficient up-conversion of continuous wave infrared light at intensities as low as a few watts per square centimeter.« less

Energy-Cascaded Upconversion in an Organic Dye-Sensitized Core/Shell Fluoride Nanocrystal.

PubMed

Chen, Guanying; Damasco, Jossana; Qiu, Hailong; Shao, Wei; Ohulchanskyy, Tymish Y; Valiev, Rashid R; Wu, Xiang; Han, Gang; Wang, Yan; Yang, Chunhui; Ågren, Hans; Prasad, Paras N

2015-11-11

Lanthanide-doped upconversion nanoparticles hold promises for bioimaging, solar cells, and volumetric displays. However, their emission brightness and excitation wavelength range are limited by the weak and narrowband absorption of lanthanide ions. Here, we introduce a concept of multistep cascade energy transfer, from broadly infrared-harvesting organic dyes to sensitizer ions in the shell of an epitaxially designed core/shell inorganic nanostructure, with a sequential nonradiative energy transfer to upconverting ion pairs in the core. We show that this concept, when implemented in a core-shell architecture with suppressed surface-related luminescence quenching, yields multiphoton (three-, four-, and five-photon) upconversion quantum efficiency as high as 19% (upconversion energy conversion efficiency of 9.3%, upconversion quantum yield of 4.8%), which is about ~100 times higher than typically reported efficiency of upconversion at 800 nm in lanthanide-based nanostructures, along with a broad spectral range (over 150 nm) of infrared excitation and a large absorption cross-section of 1.47 × 10(-14) cm(2) per single nanoparticle. These features enable unprecedented three-photon upconversion (visible by naked eye as blue light) of an incoherent infrared light excitation with a power density comparable to that of solar irradiation at the Earth surface, having implications for broad applications of these organic-inorganic core/shell nanostructures with energy-cascaded upconversion.

Endoplasmic Reticulum-Localized Two-Photon-Absorbing Boron Dipyrromethenes as Advanced Photosensitizers for Photodynamic Therapy.

PubMed

Zhou, Yimin; Cheung, Ying-Kit; Ma, Chao; Zhao, Shirui; Gao, Di; Lo, Pui-Chi; Fong, Wing-Ping; Wong, Kam Sing; Ng, Dennis K P

2018-05-10

Two advanced boron dipyrromethene (BODIPY) based photosensitizers have been synthesized and characterized. With a glibenclamide analogous moiety, these compounds can localize in the endoplasmic reticulum (ER) of HeLa human cervical carcinoma cells and HepG2 human hepatocarcinoma cells. The BODIPY π skeleton is conjugated with two styryl or carbazolylethenyl groups, which can substantially red-shift the Q-band absorption and fluorescence emission and impart two-photon absorption (TPA) property to the chromophores. The TPA cross section of the carbazole-containing analogue reaches a value of 453 GM at 1010 nm. These compounds also behave as singlet oxygen generators with high photostability. Upon irradiation at λ > 610 nm, these photosensitizers cause photocytotoxicity to these two cell lines with IC 50 values down to 0.09 μM, for which the cell death is triggered mainly by ER stress. The two-photon photodynamic activity of the distyryl derivative upon excitation at λ = 800 nm has also been demonstrated.

Measurement of polarization dependence of two-photon absorption coefficient in InP using extended Z-scan technique for thick materials

NASA Astrophysics Data System (ADS)

Oishi, Masaki; Shinozaki, Tomohisa; Hara, Hikaru; Yamamoto, Kazunuki; Matsusue, Toshio; Bando, Hiroyuki

2018-03-01

The two-photon absorption coefficient β in InP has been measured in the wavelength range of 1640 to 1800 nm by the Z-scan technique in relatively thick materials. The values of β have been evaluated from the fit to the equation including the spatial and temporal profiles of the focused Gaussian beam. The polarization dependence of β has also been measured. The dependence has been expressed very well by the expression of β with the imaginary part of the third-order nonlinear susceptibility tensor χ(3).

Effects of heat induced by two-photon absorption and free-carrier absorption in silicon-on-insulator nanowaveguides operating as all-optical wavelength converters.

PubMed

Abdollahi, Siamak; Moravvej-Farshi, Mohammad Kazem

2009-05-01

We propose a new numerical model to analyze heat induced by two-photon absorption and free-carrier absorption, while high intensity optical pulses propagate along silicon-on-insulator (SOI) nanowaveguides (NWGs). Using this model, we demonstrate that such induced heat causes a shift in the amount of wavelength conversion and hence deteriorates the converter output characteristics for pulses in the picosecond regime. The wavelength shift induced by a pulse with maximum input intensity and full width at half-maximum of I(max)=1.5x10(10) W x cm(-2) and T(FWHM)=30 ps, propagating along a SOI NWG with an effective cross-sectional area of a(eff)=0.15 microm(2), is shown to be Delta lambda(s) approximately 8 pm. We also demonstrate that such a shift can be compensated by tuning the pump intensity down by approximately 6.33%.

Theoretical design and investigation of 1,8-naphthalimide-based two-photon fluorescent probes for detecting cytochrome P450 1A with separated fluorescence signal.

PubMed

Zhang, Chun; Ren, Ai-Min; Guo, Jing-Fu; Wang, Dan; Yu, Li-Ying

2018-05-16

As a type of enzyme with a terminal oxygen, the CYP1A subfamily possesses the ability to catalyze the reactions of many environmental toxins, endogenous substrates and clinical drugs. The development of efficient methods for the rapid and real-time detection of CYP1A enzyme activity in complex biological systems is of considerable significance for identifying potential abnormalities in these cancer-related enzymes. With this goal, we firstly provided a series of 1,8-naphthalimide-based two-photon fluorescent chromophores with large two-photon absorption (TPA) cross-sections (500-7000 GM) and remarkable changes in fluorescence spectra upon recognizing the CYP1A enzyme from its theoretical aspect. Moreover, we have thoroughly studied the effects of cyclic acceptor (dichlorobenzene and benzothiadiazole) and donor (fluorene and carbazole) groups on the one-photon absorption (OPA), TPA, and fluorescence properties of CYP1A enzyme probes and the corresponding reaction products. The connection of a heterocycle as the donor group to a 1,8-naphthalimide-based molecule to form a D-π-A-π-D-type electronic structure can effectively cause red shifts in the absorption and emission wavelengths to facilitate bioimaging in the near infrared (NIR) region, which is attributed to the lower transition energy, larger transition dipole moment and amount of transferred charge. Docking analysis suggests that the two-photon fluorescent probes NCMN-3 and NCMN-5 that were designed will guarantee and achieve excellent selectivity for the CYP1A enzyme.

Near-Infrared Emitting Squaraine Dyes with High 2PA Cross Sections for Multiphoton Fluorescence Imaging

PubMed Central

Ahn, Hyo-Yang; Yao, Sheng; Wang, Xuhua; Belfield, Kevin D.

2012-01-01

Designed to achieve high two-photon absorptivity, new near infrared (NIR) emitting squaraine dyes, (E)-2-(1-(2-(2-methoxyethoxy)ethyl)-5-(3,4,5-trimethoxystyryl)-1H-pyrrol-2-yl)-4-(1-(2-(2-methoxyethoxy)ethyl)-5-(3,4,5-trimethoxystyryl)-2H-pyrrolium-2-ylidene)-3-oxocyclobut-1-enolate (1) and (Z)-2-(4-(dibutylamino)-2-hydroxyphenyl)-4-(4-(dibutyliminio)-2-hydroxycyclohexa-2,5-dienylidene)-3-oxocyclobut-1-enolate (2) were synthesized and characterized. Their linear photophysical properties were investigated via UV-visible absorption spectroscopy and fluorescence spectroscopy in various solvents, while their nonlinear photophysical properties were investigated using a combination of two-photon induced fluorescence and open aperture z-scan methods. Squaraine 1 exhibited a high two-photon absorption (2PA) cross section (δ2PA), ~ 20,000 GM at 800 nm, and high photostability with the photochemical decomposition quantum yield one order of magnitude lower than Cy 5, a commercially available pentamethine cyanine NIR dye. The cytotoxicity of the squaraine dyes were evaluated in HCT 116 and COS 7 cell lines to assess the potential of these probes for biomedical imaging. The viability of both cell lines was maintained above 80% at dye concentrations up to 30 μM, indicating good biocompatibility of the probes. Finally, one-photon fluorescence microscopy (1PFM) and two-photon fluorescence microscopy (2PFM) imaging was accomplished after incubation of micelle-encapsulated squaraine probes with HCT 116 and COS 7 cells, demonstrating their potential in 2PFM bioimaging. PMID:22591003

Double ionization in R -matrix theory using a two-electron outer region

NASA Astrophysics Data System (ADS)

Wragg, Jack; Parker, J. S.; van der Hart, H. W.

2015-08-01

We have developed a two-electron outer region for use within R -matrix theory to describe double ionization processes. The capability of this method is demonstrated for single-photon double ionization of He in the photon energy region between 80 and 180 eV. The cross sections are in agreement with established data. The extended R -matrix with time dependence method also provides information on higher-order processes, as demonstrated by the identification of signatures for sequential double ionization processes involving an intermediate He+ state with n =2 .

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.

Sequential and direct ionic excitation in the strong-field ionization of 1-butene molecules.

PubMed

Schell, Felix; Boguslavskiy, Andrey E; Schulz, Claus Peter; Patchkovskii, Serguei; Vrakking, Marc J J; Stolow, Albert; Mikosch, Jochen

2018-05-18

We study the Strong-Field Ionization (SFI) of the hydrocarbon 1-butene as a function of wavelength using photoion-photoelectron covariance and coincidence spectroscopy. We observe a striking transition in the fragment-associated photoelectron spectra: from a single Above Threshold Ionization (ATI) progression for photon energies less than the cation D0-D1 gap to two ATI progressions for a photon energy greater than this gap. For the first case, electronically excited cations are created by SFI populating the ground cationic state D0, followed by sequential post-ionization excitation. For the second case, direct sub-cycle SFI to the D1 excited cation state contributes significantly. Our experiments access ionization dynamics in a regime where strong-field and resonance-enhanced processes can interplay.

Solvent effects on the vibronic one-photon absorption profiles of dioxaborine heterocycles

NASA Astrophysics Data System (ADS)

Wang, Yan-Hua; Halik, Marcus; Wang, Chuan-Kui; Marder, Seth R.; Luo, Yi

2005-11-01

The vibronic profiles of one-photon absorption spectra of dioxaborine heterocycles in gas phase and solution have been calculated at the Hartree-Fock and density-functional-theory levels. The polarizable continuum model has been applied to simulate the solvent effect, while the linear coupling model is used to compute the Franck-Condon and Herzberg-Teller contributions. It is found that a good agreement between theory and experiment can be achieved when the solvent effect and electron correlation are taken into account simultaneously. For the first excited charge-transfer state, the maximum of its Herzberg-Teller profile is blueshifted from that of the Franck-Condon profile. The shifted energy is found to be around 0.2eV, which agrees well with the measured energy difference between two- and one-photon absorptions of the first excited state.

Two-photon absorption spectra of carotenoids compounds

NASA Astrophysics Data System (ADS)

Vivas, Marcelo Gonçalves; Silva, Daniel Luiz; Boni, Leonardo de; Zalesny, Robert; Bartkowiak, Wojciech; Mendonca, Cleber Renato

2011-05-01

Carotenoids are biosynthetic organic pigments that constitute an important class of one-dimensional π-conjugated organic molecules with enormous potential for application in biophotonic devices. In this context, we studied the degenerate two-photon absorption (2PA) cross-section spectra of two carotenoid compounds (β-carotene and β-apo-8'-carotenal) employing the conventional and white-light-continuum Z-scan techniques and quantum chemistry calculations. Because carotenoids coexist at room temperature as a mixture of isomers, the 2PA spectra reported here are due to samples containing a distribution of isomers, presenting distinct conjugation length and conformation. We show that these compounds present a defined structure on the 2PA spectra, that peaks at 650 nm with an absorption cross-section of approximately 5000 GM, for both compounds. In addition, we observed a 2PA band at 990 nm for β-apo-8'-carotenal, which was attributed to a overlapping of 11Bu+-like and 21Ag--like states, which are strongly one- and two-photon allowed, respectively. Spectroscopic parameters of the electronic transitions to singlet-excited states, which are directly related to photophysical properties of these compounds, were obtained by fitting the 2PA spectra using the sum-over-states approach. The analysis and interpretations of the 2PA spectra of the investigated carotenoids were supported by theoretical predictions of one- and two-photon transitions carried out using the response functions formalism within the density functional theory framework, using the long-range corrected CAM-B3LYP functional.

Selective Two-Photon Absorptive Resonance Femtosecond-Laser Electronic-Excitation Tagging (STARFLEET) Velocimetry in Flow and Combustion Diagnostics

NASA Technical Reports Server (NTRS)

Jiang, Naibo; Halls, Benjamin R.; Stauffer, Hans U.; Roy, Sukesh; Danehy, Paul M.; Gord, James R.

2016-01-01

Selective Two-Photon Absorptive Resonance Femtosecond-Laser Electronic-Excitation Tagging (STARFLEET), a non-seeded ultrafast-laser-based velocimetry technique, is demonstrated in reactive and non-reactive flows. STARFLEET is pumped via a two-photon resonance in N2 using 202.25-nm 100-fs light. STARFLEET greatly reduces the per-pulse energy required (30 µJ/pulse) to generate the signature FLEET emission compared to the conventional FLEET technique (1.1 mJ/pulse). This reduction in laser energy results in less energy deposited in the flow, which allows for reduced flow perturbations (reactive and non-reactive), increased thermometric accuracy, and less severe damage to materials. Velocity measurements conducted in a free jet of N2 and in a premixed flame show good agreement with theoretical velocities and further demonstrate the significantly less-intrusive nature of STARFLEET.

High-accuracy reference standards for two-photon absorption in the 680–1050 nm wavelength range

PubMed Central

de Reguardati, Sophie; Pahapill, Juri; Mikhailov, Alexander; Stepanenko, Yuriy; Rebane, Aleksander

2016-01-01

Degenerate two-photon absorption (2PA) of a series of organic fluorophores is measured using femtosecond fluorescence excitation method in the wavelength range, λ2PA = 680–1050 nm, and ~100 MHz pulse repetition rate. The function of relative 2PA spectral shape is obtained with estimated accuracy 5%, and the absolute 2PA cross section is measured at selected wavelengths with the accuracy 8%. Significant improvement of the accuracy is achieved by means of rigorous evaluation of the quadratic dependence of the fluorescence signal on the incident photon flux in the whole wavelength range, by comparing results obtained from two independent experiments, as well as due to meticulous evaluation of critical experimental parameters, including the excitation spatial- and temporal pulse shape, laser power and sample geometry. Application of the reference standards in nonlinear transmittance measurements is discussed. PMID:27137334

Theoretical study of the crystal-field energy levels and two-photon absorption intensities of Tb3+ in cubic host lattices.

PubMed

Duan, Chang-Kui; Tanner, Peter A

2011-03-17

Published two photon excitation (TPE) intensities for the cubic elpasolite systems Cs(2)NaTbX(6) (X = Cl, F) have been simulated by a calculation of two photon absorption (TPA) intensities which takes into account electric dipole transitions involving the detailed crystal-field structure of 4f(7)5d intermediate states, as well as the interactions of the 4f(7) core with the d-electron. The intensity calculation employed parameters from an energy level calculation which not only presented an accurate fit, but also yielded parameters consistent with those from other lanthanide ions. The calculated intensities were used to confirm or adjust the previous assignments of energy levels, resulting in some minor revisions. Generally, the TPA intensity simulations were in better agreement with experimental data for the fluoride, rather than the chloride, system and possible reasons for this are given.

Perfect absorption in nanotextured thin films via Anderson-localized photon modes

NASA Astrophysics Data System (ADS)

Aeschlimann, Martin; Brixner, Tobias; Differt, Dominik; Heinzmann, Ulrich; Hensen, Matthias; Kramer, Christian; Lükermann, Florian; Melchior, Pascal; Pfeiffer, Walter; Piecuch, Martin; Schneider, Christian; Stiebig, Helmut; Strüber, Christian; Thielen, Philip

2015-10-01

The enhancement of light absorption in absorber layers is crucial in a number of applications, including photovoltaics and thermoelectrics. The efficient use of natural resources and physical constraints such as limited charge extraction in photovoltaic devices require thin but efficient absorbers. Among the many different strategies used, light diffraction and light localization at randomly nanotextured interfaces have been proposed to improve absorption. Although already exploited in commercial devices, the enhancement mechanism for devices with nanotextured interfaces is still subject to debate. Using coherent two-dimensional nanoscopy and coherent light scattering, we demonstrate the existence of localized photonic states in nanotextured amorphous silicon layers as used in commercial thin-film solar cells. Resonant absorption in these states accounts for the enhanced absorption in the long-wavelength cutoff region. Our observations establish that Anderson localization—that is, strong localization—is a highly efficient resonant absorption enhancement mechanism offering interesting opportunities for the design of efficient future absorber layers.

The two-photon absorptivity of rotational transitions in the A2 Sigma hyperon + (v prime = O) - X-2 pion (v prime prime = O) gamma band of nitric oxide

NASA Technical Reports Server (NTRS)

Gross, K. P.; Mckenzie, R. L.

1982-01-01

A predominantly single-mode pulsed dye laser system giving a well characterized spatial and temporal output suitable for absolute two-photon absorptivity measurements was used to study the NO gamma(0,0) S11 + R21 (J double prime = 7-1/2) transition. Using a calibrated induced-fluorescence technique, an absorptivity parameter of 2.8 + or - 1.4 x 10 to the minus 51st power cm to the 6th power was obtained. Relative strengths of other rotational transitions in the gamma(0,0) band were also measured and shown to compare well with predicted values in all cases except the O12 (J double prime = 10-1/2) transition.

Nanoantenna enhancement for telecom-wavelength superconducting single photon detectors.

PubMed

Heath, Robert M; Tanner, Michael G; Drysdale, Timothy D; Miki, Shigehito; Giannini, Vincenzo; Maier, Stefan A; Hadfield, Robert H

2015-02-11

Superconducting nanowire single photon detectors are rapidly emerging as a key infrared photon-counting technology. Two front-side-coupled silver dipole nanoantennas, simulated to have resonances at 1480 and 1525 nm, were fabricated in a two-step process. An enhancement of 50 to 130% in the system detection efficiency was observed when illuminating the antennas. This offers a pathway to increasing absorption into superconducting nanowires, creating larger active areas, and achieving more efficient detection at longer wavelengths.

Thermal emission and absorption of radiation in finite inverted-opal photonic crystals

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

Florescu, Marian; Stimpson, Andrew J.; Lee, Hwang

We study theoretically the optical properties of a finite inverted-opal photonic crystal. The light-matter interaction is strongly affected by the presence of the three-dimensional photonic crystal and the alterations of the light emission and absorption processes can be used to suppress or enhance the thermal emissivity and absorptivity of the dielectric structure. We investigate the influence of the absorption present in the system on the relevant band edge frequencies that control the optical response of the photonic crystal. Our study reveals that the absorption processes cause spectral broadening and shifting of the band edge optical resonances, and determine a strongmore » reduction of the photonic band gap spectral range. Using the angular and spectral dependence of the band edge frequencies for stop bands along different directions, we argue that by matching the blackbody emission spectrum peak with a prescribed maximum of the absorption coefficient, it is possible to achieve an angle-sensitive enhancement of the thermal emission/absorption of radiation. This result opens a way to realize a frequency-sensitive and angle-sensitive photonic crystal absorbers/emitters.« less

Single-photon and two-photon excited fluorescence behavior of a novel fluorene-based compound

NASA Astrophysics Data System (ADS)

Ma, Wenbo; Wu, Yiquan; Gu, Donghong; Gan, Fuxi

2005-09-01

A D-π-D type compound, 2,7-bis(4-methoxystyryl)-9,9-bis(2-ethylhexyl)-9H-fluorene (abbreviated as MO-Flu-MO), where electron-donor D is methoxy group andπis fluorene unit, has been synthesized. The molecular structures of the compound were characterized by elemental analyses, EI-MS and FT-IR spectra. UV-Vis spectra in the region 230--1000 nm and single-photon excited fluorescence in tetrahydrofuran (THF) of the compound were measured. It is found that the new compound exhibits strong two-photon excited fluorescence in the region 380--500 nm and moderate two-photon absorption (TPA) value in the femtoseconds regime (TPA cross-section as high as 55×10-50 cm4 s photon-1 with 13fs laser pulses). The results demonstrate that the compound is a promising candidate for two-photon three-dimensional (3D) optical data storage.

Photonic molecules for improving the optical response of macroporous silicon photonic crystals for gas sensing purposes.

PubMed

Cardador, D; Segura, D; Rodríguez, A

2018-02-19

In this paper, we report the benefits of working with photonic molecules in macroporous silicon photonic crystals. In particular, we theoretically and experimentally demonstrate that the optical properties of a resonant peak produced by a single photonic atom of 2.6 µm wide can be sequentially improved if a second and a third cavity of the same length are introduced in the structure. As a consequence of that, the base of the peak is reduced from 500 nm to 100 nm, while its amplitude remains constant, increasing its Q-factor from its initial value of 25 up to 175. In addition, the bandgap is enlarged almost twice and the noise within it is mostly eliminated. In this study we also provide a way of reducing the amplitude of one or two peaks, depending whether we are in the two- or three-cavity case, by modifying the length of the involved photonic molecules so that the remainder can be used to measure gas by spectroscopic methods.

Tunable angle absorption of hyperbolic metamaterials based on plasma photonic crystals

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

Jiao, Zheng; Ning, Renxia, E-mail: nrxxiner@hsu.edu.cn; Xu, Yuan

2016-06-15

We present the design of a multilayer structure of hyperbolic metamaterials based on plasma photonic crystals which composed of two kinds of traditional dielectric and plasma. The relative permittivity of hyperbolic metamaterials has been studied at certain frequency range. The absorption and reflection of the multilayer period structure at normal and oblique incident have been investigated by the transfer matrix method. We discussed that the absorption is affected by the thickness of material and the electron collision frequency γ of the plasma. The results show that an absorption band at the low frequency can be obtained at normal incident anglemore » and another absorption band at the high frequency can be found at a large incident angle. The results may be applied by logical gate, stealth, tunable angle absorber, and large angle filter.« less

Theoretical study on photophysical properties of three high water solubility polypyridyl complexes for two-photon photodynamic therapy.

PubMed

Liu, Ying-Tao; Yin, Xue; Lai, Xiao-Yong; Wang, Xin

2018-06-22

Two-photon photodynamic therapy (TP-PDT) is a very promising treatment that has drawn much attention in recent years due to its ability to penetrate deeper into tissues and minimize the damage to normal cells. Here, the properties of three highly water soluble Ru(ii) and Zn(ii) polypyridyl complexes as photosensitizers (PSs) were examined, including the one-photon and two-photon absorption (OPA and TPA) spectra, singlet-triplet energy gap (ΔH-L), TPA cross-section and spin-orbit coupling constant via Density Function Theory (DFT) and Time-Dependent Density Functional Theory (TD-DFT). Their potential therapeutic use as photosensitizers in TP-PDT is proposed, where the reasoning is as follows: first, they possess strong absorption in the therapeutic window; second, the vertical excitation energy is greater than 0.98 eV, which can generate a singlet oxygen species and the remarkable coupling between the S1 and T1 states. Moreover, the spin-orbit matrix elements are greater than 0.24 cm-1 for Ru-bpy and Zn-tpy, indicating that the intersystem spin crossing processes are efficient. It is expected that these complexes will be applied to PSs in TP-PDT, and we hope this research can serve as a guideline for the development of efficient two-photon PSs.

Nonlinear optical studies on 1,3-disubstituent chalcones doped polymer films

NASA Astrophysics Data System (ADS)

Poornesh, P.; Shettigar, Seetharam; Umesh, G.; Manjunatha, K. B.; Prakash Kamath, K.; Sarojini, B. K.; Narayana, B.

2009-04-01

We report the measurements of the third-order nonlinear optical properties of recently synthesized and characterized two different 1,3-disubstituent chalcones doped PMMA films, with the prospective of reaching a good compromise between processability and high nonlinear optical properties. The measurements were done using nanosecond Z-scan at 532 nm. The Z-scan spectra reveal a large negative nonlinear refraction coefficient n2 of the order 10 -11 esu and the molecular two photon absorption cross section is 10 -46 cm 4 s/photon. The doped films exhibit good optical power limiting property under nanosecond regime and the two photon absorption (TPA) is the dominating process leading to the nonlinear behavior. The improvement in the nonlinear properties has been observed when methylenedioxy group is replaced by dimethoxy group due to increase in conjugation length. The observed nonlinear parameters of chalcone derivatives doped PMMA film is comparable with stilbazolieum derivatives, a well-known class of optical materials for photonics and biophotonics applications, which suggests that, these moieties have potential for the application of all-optical limiting and switching devices.

Br2 molecular elimination in photolysis of (COBr)2 at 248 nm by using cavity ring-down absorption spectroscopy: a photodissociation channel being ignored.

PubMed

Wu, Chia-Ching; Lin, Hsiang-Chin; Chang, Yuan-Bin; Tsai, Po-Yu; Yeh, Yu-Ying; Fan, He; Lin, King-Chuen; Francisco, J S

2011-12-21

A primary dissociation channel of Br(2) elimination is detected following a single-photon absorption of (COBr)(2) at 248 nm by using cavity ring-down absorption spectroscopy. The technique contains two laser beams propagating in a perpendicular configuration. The tunable laser beam along the axis of the ring-down cell probes the Br(2) fragment in the B(3)Π(ou)(+)-X(1)Σ(g)(+) transition. The measurements of laser energy- and pressure-dependence and addition of a Br scavenger are further carried out to rule out the probability of Br(2) contribution from a secondary reaction. By means of spectral simulation, the ratio of nascent vibrational population for v = 0, 1, and 2 levels is evaluated to be 1:(0.65 ± 0.09):(0.34 ± 0.07), corresponding to a Boltzmann vibrational temperature of 893 ± 31 K. The quantum yield of the ground state Br(2) elimination reaction is determined to be 0.11 ± 0.06. With the aid of ab initio potential energy calculations, the pathway of molecular elimination is proposed on the energetic ground state (COBr)(2) via internal conversion. A four-center dissociation mechanism is followed synchronously or sequentially yielding three fragments of Br(2) + 2CO. The resulting Br(2) is anticipated to be vibrationally hot. The measurement of a positive temperature effect supports the proposed mechanism.

Observation of soliton compression in silicon photonic crystals

PubMed Central

Blanco-Redondo, A.; Husko, C.; Eades, D.; Zhang, Y.; Li, J.; Krauss, T.F.; Eggleton, B.J.

2014-01-01

Solitons are nonlinear waves present in diverse physical systems including plasmas, water surfaces and optics. In silicon, the presence of two photon absorption and accompanying free carriers strongly perturb the canonical dynamics of optical solitons. Here we report the first experimental demonstration of soliton-effect pulse compression of picosecond pulses in silicon, despite two photon absorption and free carriers. Here we achieve compression of 3.7 ps pulses to 1.6 ps with <10 pJ energy. We demonstrate a ~1-ps free-carrier-induced pulse acceleration and show that picosecond input pulses are critical to these observations. These experiments are enabled by a dispersion-engineered slow-light photonic crystal waveguide and an ultra-sensitive frequency-resolved electrical gating technique to detect the ultralow energies in the nanostructured device. Strong agreement with a nonlinear Schrödinger model confirms the measurements. These results further our understanding of nonlinear waves in silicon and open the way to soliton-based functionalities in complementary metal-oxide-semiconductor-compatible platforms. PMID:24423977

Determination of absorption changes from moments of distributions of times of flight of photons: optimization of measurement conditions for a two-layered tissue model.

PubMed

Liebert, Adam; Wabnitz, Heidrun; Elster, Clemens

2012-05-01

Time-resolved near-infrared spectroscopy allows for depth-selective determination of absorption changes in the adult human head that facilitates separation between cerebral and extra-cerebral responses to brain activation. The aim of the present work is to analyze which combinations of moments of measured distributions of times of flight (DTOF) of photons and source-detector separations are optimal for the reconstruction of absorption changes in a two-layered tissue model corresponding to extra- and intra-cerebral compartments. To this end we calculated the standard deviations of the derived absorption changes in both layers by considering photon noise and a linear relation between the absorption changes and the DTOF moments. The results show that the standard deviation of the absorption change in the deeper (superficial) layer increases (decreases) with the thickness of the superficial layer. It is confirmed that for the deeper layer the use of higher moments, in particular the variance of the DTOF, leads to an improvement. For example, when measurements at four different source-detector separations between 8 and 35 mm are available and a realistic thickness of the upper layer of 12 mm is assumed, the inclusion of the change in mean time of flight, in addition to the change in attenuation, leads to a reduction of the standard deviation of the absorption change in the deeper tissue layer by a factor of 2.5. A reduction by another 4% can be achieved by additionally including the change in variance.

Theoretical investigation on ratiometric two-photon fluorescent probe for Zn2+ detection based on ICT mechanism

NASA Astrophysics Data System (ADS)

Huang, Shuang; Yang, Bao-Zhu; Ren, Ai-Min

2016-06-01

OPA (one-photon absorption), TPA (two-photon absorption) and fluorescence properties of a free ligand L upon coordination with Zn2+, and the regeneration with CN- were investigated in theory. According to our research, OPA spectra of ligand L show red-shift binding with Zn2+ while blue-shift with CN-. The fluorescence spectra and TPA wavelength are shifted in the same situation as those of OPA spectra. The value of TPA cross-section decreased at first, and then increased to 1813 GM for [L-Zn(CN)4]2-. Intramolecular charge transfer (ICT) mechanism was investigated by natural bond orbital (NBO) analysis. It demonstrates that L is hopeful to be a good ratiometric fluorescent probe for zinc ion detection in solution, and it can regenerate after CN- was introduced.

Direct quantum process tomography via measuring sequential weak values of incompatible observables.

PubMed

Kim, Yosep; Kim, Yong-Su; Lee, Sang-Yun; Han, Sang-Wook; Moon, Sung; Kim, Yoon-Ho; Cho, Young-Wook

2018-01-15

The weak value concept has enabled fundamental studies of quantum measurement and, recently, found potential applications in quantum and classical metrology. However, most weak value experiments reported to date do not require quantum mechanical descriptions, as they only exploit the classical wave nature of the physical systems. In this work, we demonstrate measurement of the sequential weak value of two incompatible observables by making use of two-photon quantum interference so that the results can only be explained quantum physically. We then demonstrate that the sequential weak value measurement can be used to perform direct quantum process tomography of a qubit channel. Our work not only demonstrates the quantum nature of weak values but also presents potential new applications of weak values in analyzing quantum channels and operations.

Theoretical X-ray production cross sections at incident photon energies across Li (i=1-3) absorption edges of Br

NASA Astrophysics Data System (ADS)

Puri, Sanjiv

2015-08-01

The X-ray production (XRP) cross sections, σLk (k = l, η, α, β6, β1, β3, β4, β9,10, γ1,5, γ2,3) have been evaluated at incident photon energies across the Li(i=1-3) absorption edge energies of 35Br using theoretical data sets of different physical parameters, namely, the Li(i=1-3) sub-shell the X-ray emission rates based on the Dirac-Fock (DF) model, the fluorescence and Coster Kronig yields based on the Dirac-Hartree-Slater (DHS) model, and two sets of the photoionisation cross sections based on the relativistic Hartree-Fock-Slater (RHFS) model and the Dirac-Fock (DF) model, in order to highlight the importance of electron exchange effects at photon energies in vicinity of absorption edge energies.

Enantiopure distorted ribbon-shaped nanographene combining two-photon absorption-based upconversion and circularly polarized luminescence† †Electronic supplementary information (ESI) available: General details, synthesis and spectroscopy data of new compounds. Experimental details on optical, chiroptical, electrochemical and on-surface measurements. Crystal data and structure refinement of compounds 1, and 6. Further details on theoretical calculations and Cartesian coordinates of computed structures. VT-H1NMR, 2D-NMR and HRMS spectra of 1. CCDC 1561552 and 1561553. For ESI and crystallographic data in CIF or other electronic format see DOI: 10.1039/c8sc00427g

PubMed Central

Cruz, Carlos M.; Márquez, Irene R.; Mariz, Inês F. A.; Blanco, Victor; Sánchez-Sánchez, Carlos; Sobrado, Jesús M.; Martín-Gago, José A.; Cuerva, Juan M.

2018-01-01

Herein we describe a distorted ribbon-shaped nanographene exhibiting unprecedented combination of optical properties in graphene-related materials, namely upconversion based on two-photon absorption (TPA-UC) together with circularly polarized luminescence (CPL). The compound is a graphene molecule of ca. 2 nm length and 1 nm width with edge defects that promote the distortion of the otherwise planar lattice. The edge defects are an aromatic saddle-shaped ketone unit and a [5]carbohelicene moiety. This system is shown to combine two-photon absorption and circularly polarized luminescence and a remarkably long emission lifetime of 21.5 ns. The [5]helicene is responsible for the chiroptical activity while the push–pull geometry and the extended network of sp2 carbons are factors favoring the nonlinear absorption. Electronic structure theoretical calculations support the interpretation of the results. PMID:29780523

Auger Up-Conversion of Low-Intensity Infrared Light in Engineered Quantum Dots

DOE PAGES

Makarov, Nikolay S.; Lin, Qianglu; Pietryga, Jeffrey M.; ...

2016-11-29

One source of efficiency losses in photovoltaic cells is their transparency toward solar photons with energies below the band gap of the absorbing layer. This loss can be reduced using a process of up-conversion whereby two or more sub-band-gap photons generate a single above-gap exciton. Traditional approaches to up-conversion, such as nonlinear two-photon absorption (2PA) or triplet fusion, suffer from low efficiency at solar light intensities, a narrow absorption bandwidth, nonoptimal absorption energies, and difficulties for implementing in practical devices. We show that these deficiencies can be alleviated using the effect of Auger up-conversion in thick-shell PbSe/CdSe quantum dots. Thismore » process relies on Auger recombination whereby two low-energy, core-based excitons are converted into a single higher-energy, shell-based exciton. When compared to their monocomponent counterparts, the tailored PbSe/CdSe heterostructures feature enhanced absorption cross-sections, a higher efficiency of the “productive” Auger pathway involving re-excitation of a hole, and longer lifetimes of both core- and shell-localized excitons. These features lead to effective up-conversion cross-sections that are more than 6 orders of magnitude higher than for standard nonlinear 2PA, which allows for efficient up-conversion of continuous wave infrared light at intensities as low as a few watts per square centimeter.« less

Ultrafast two-photon absorption generated free-carrier modulation in a silicon nanoplasmonic resonator

NASA Astrophysics Data System (ADS)

Nielsen, M. P.; Elezzabi, A. Y.

2014-03-01

Ultrafast all-optical modulation in Ag/HfO2/Si/HfO2/Ag metal-insulator-semiconductor-insulator-metal (MISIM) nanoring resonators through two-photon absorption photogenerated free-carriers is studied using self-consistent 3-D finite difference time domain (FDTD) simulations. The self-consistent FDTD simulations incorporate the two-photon absorption, free carrier absorption, and plasma dispersion effects in silicon. The nanorings are aperture coupled to Ag/HfO2/Si(100nm)/HfO2/Ag MISIM waveguides by 300nm wide and 50nm deep apertures. The effects of pump pulse energy, HfO2 spacer thickness, and device footprint on the modulation characteristics are studied. Nanoring radius is varied between 540nm and 1μm, the HfO2 spacer thickness is varied between 10nm and 20nm, and the pump pulse energy is explored up to 60pJ. Modulation amplitude, switching time, average generated carrier density, and wavelength resonant shift is studied for each of the device configurations. In a compact device footprint of only 1.4μm2, a 13.1dB modulation amplitude was obtained with a switching time of only 2ps using a modest pump pulse energy of 16.0pJ. The larger bandwidth associated with more compact nanorings and thinner spacer layers is shown to result in increased modulation amplitude.

Single-photon absorption by single photosynthetic light-harvesting complexes

NASA Astrophysics Data System (ADS)

Chan, Herman C. H.; Gamel, Omar E.; Fleming, Graham R.; Whaley, K. Birgitta

2018-03-01

We provide a unified theoretical approach to the quantum dynamics of absorption of single photons and subsequent excitonic energy transfer in photosynthetic light-harvesting complexes. Our analysis combines a continuous mode < n > -photon quantum optical master equation for the chromophoric system with the hierarchy of equations of motion describing excitonic dynamics in presence of non-Markovian coupling to vibrations of the chromophores and surrounding protein. We apply the approach to simulation of absorption of single-photon coherent states by pigment-protein complexes containing between one and seven chromophores, and compare with results obtained by excitation using a thermal radiation field. We show that the values of excitation probability obtained under single-photon absorption conditions can be consistently related to bulk absorption cross-sections. Analysis of the timescale and efficiency of single-photon absorption by light-harvesting systems within this full quantum description of pigment-protein dynamics coupled to a quantum radiation field reveals a non-trivial dependence of the excitation probability and the excited state dynamics induced by exciton-phonon coupling during and subsequent to the pulse, on the bandwidth of the incident photon pulse. For bandwidths equal to the spectral bandwidth of Chlorophyll a, our results yield an estimation of an average time of ˜0.09 s for a single chlorophyll chromophore to absorb the energy equivalent of one (single-polarization) photon under irradiation by single-photon states at the intensity of sunlight.

Isothermal crystallization of poly(3-hydroxybutyrate) studied by terahertz two-dimensional correlation spectroscopy

NASA Astrophysics Data System (ADS)

Hoshina, Hiromichi; Ishii, Shinya; Morisawa, Yusuke; Sato, Harumi; Noda, Isao; Ozaki, Yukihiro; Otani, Chiko

2012-01-01

The isothermal crystallization of poly(3-hydroxybutylate) (PHB) was studied by monitoring the temporal evolution of terahertz absorption spectra in conjunction with spectral analysis using two-dimensional correlation spectroscopy. Correlation between the absorption peaks and the sequential order of the changes in spectral intensity extracted from synchronous and asynchronous plots indicated that crystallization of PHB at 90 °C is a two step process, in which C-H...O=C hydrogen bonds are initially formed before well-defined crystal structures are established.

Impact of electronic coupling, symmetry, and planarization on one- and two-photon properties of triarylamines with one, two, or three diarylboryl acceptors.

PubMed

Makarov, Nikolay S; Mukhopadhyay, Sukrit; Yesudas, Kada; Brédas, Jean-Luc; Perry, Joseph W; Pron, Agnieszka; Kivala, Milan; Müllen, Klaus

2012-04-19

We have performed a study of the one- and two-photon absorption properties of a systematically varied series of triarylamino-compounds with one, two, or three attached diarylborane arms arranged in linear dipolar, bent dipolar, and octupolar geometries. Two-photon fluorescence excitation spectra were measured over a wide spectral range with femtosecond laser pulses. We found that on going from the single-arm to the two- and three-arm systems, the peak in two-photon absorption (2PA) cross-section is suppressed by factors of 3-11 for the lowest excitonic level associated with the electronic coupling of the arms, whereas it is enhanced by factors of 4-8 for the higher excitonic level. These results show that the coupling of arms redistributes the 2PA cross-section between the excitonic levels in a manner that strongly favors the higher-energy excitonic level. The experimental data on one- and two-photon cross-sections, ground- and excited-state transition dipole moments, and permanent dipole moment differences between the ground and the lowest excited states were compared to the results obtained from a simple Frenkel exciton model and from highly correlated quantum-chemical calculations. It has been found that planarization of the structure around the triarylamine moiety leads to a sizable increase in peak 2PA cross-section for the lowest excitonic level of the two-arm system, whereas for the three-arm system, the corresponding peak was weakened and shifted to lower energy. Our studies show the importance of the interarm coupling, number of arms, and structural planarity on both the enhancement and the suppression of two-photon cross-sections in multiarm molecules. © 2012 American Chemical Society

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

Garrett, W.R.; Moore, M.A.; Payne, M.G.

On the basis of combined experimental and theoretical studies of nonlinear processes associated with two-photon excitations near 3d and 4d states in Na, we show how resonantly enhanced stimulated hyper-Raman emission, parametric four-wave mixing processes and total resonant two-photon absorption can become severely suppressed through the actions of internally generated fields on the total atomic response in extended media. 7 refs., 3 figs.

Improved reference standards for femtosecond three-photon excitation of fluorescence in the wavelength range 950 - 1750 nm

NASA Astrophysics Data System (ADS)

Rebane, Aleksander; Mikhaylov, Alexander

2018-02-01

Fluorescence excited by instantaneous three-photon absorption (3PA) in organic fluorophores is gaining importance as a versatile modality for deep-tissue microscopy and imaging. However, due to technical difficulty of quantifying the higher-order nonlinear absorption cross-section, reliable 3PA cross section values, σ3PA, covering a broad spectral range have been so far not available. This lack of experimental data hinders us from gaining quantitative understanding of relevant structure-property relationships as well as impedes progress towards developing 3-photon fluorophores optimized for various applications. We report on measurement of the absolute 3PA cross section spectra in the 950 - 1750 nm range in a series of common organic fluorophores in various solvents: (a) Rhodamine 6G in deuterated methanol, (b) Coumarin 153 in DMSO and toluene, (c) Prodan in DMSO and toluene, (d) Fluorescein in pH11 buffer, (e) AF455 in toluene, (f) BDPAS in deuterated methylene chloride. In these experiments, we employ femtosecond wavelength-tunable optical parametric amplifier to excite fluorescence signal that has cubic dependence on the incident photon flux. Absolute values of σ3PA are determined using two complementary methods: (i) calibrating the fluorescence signal relative to one-photon (linear) excitation combined with accurate measurement of the pulse temporal- and spatial profile to determine the excitation photon flux and (ii) calibration of the cubic fluorescence signal relative to quadratic florescence excited in fluorophores with known two-photon absorption cross section. Depending on the method utilized, the peak σ3PA values have estimated accuracy 50% and vary in the range, σ3PA = 10-81 - 10-79 cm6 s2 photon-2 , depending on the system studied, with AF455 showing the most enhanced 3PA efficiency. The 3PA spectral shapes have estimated accuracy of 20% and show some unexpected deviations from corresponding one-photon spectral profiles.

Broadband optical limiting and nonlinear optical absorption properties of a novel hyperbranched conjugated polymer

NASA Astrophysics Data System (ADS)

Li, Chao; Liu, Chunling; Li, Quanshui; Gong, Qihuang

2004-12-01

The nonlinear transmittance of a novel hyperbranched conjugated polymer named DMA-HPV has been measured in CHCl 3 solution using a nanosecond optical parametric oscillator. DMA-HPV shows excellent optical limiting performance in the visible region from 490 to 610 nm. An explanation based on the combination of two-photon absorption and reverse saturable absorption was proposed for its huge and broadband nonlinear optical absorption.

Nonlinear Optical Fiber Arrays for Limiting Application

DTIC Science & Technology

2006-09-05

Absorption [ RSA ], Two-Photon Absorption [TPA] and Excited State Absorption [ESA] or Nonlinear Scattering properties [NS] (e.g. carbon black suspension...practical implementation: I. "Saturation Effect and Dynamic Range" - In general, RSA materials have low switching threshold (<<pJ), but are (linearly...transition between the molecular levels involved, RSA materials can be easily ’bleached’, i.e. the absorption electronic state is depopulated by the laser. TPA

Theoretical Studies on Two-Photon Fluorescent Hg2+ Probes Based on the Coumarin-Rhodamine System.

PubMed

Zhang, Yujin; Leng, Jiancai

2017-07-20

The development of fluorescent sensors for Hg 2+ has attracted much attention due to the well-known adverse effects of mercury on biological health. In the present work, the optical properties of two newly-synthesized Hg 2+ chemosensors based on the coumarin-rhodamine system (named Pro1 and Pro2) were systematically investigated using time-dependent density functional theory. It is shown that Pro1 and Pro2 are effective ratiometric fluorescent Hg 2+ probes, which recognize Hg 2+ by Förster resonance energy transfer and through bond energy transfer mechanisms, respectively. To further understand the mechanisms of the two probes, we have developed an approach to predict the energy transfer rate between the donor and acceptor. Using this approach, it can be inferred that Pro1 has a six times higher energy transfer rate than Pro2. Thus the influence of spacer group between the donor and acceptor on the sensing performance of the probe is demonstrated. Specifically, two-photon absorption properties of these two probes are calculated. We have found that both probes show significant two-photon responses in the near-infrared light region. However, only the maximum two-photon absorption cross section of Pro1 is greatly enhanced with the presence of Hg 2+ , indicating that Pro1 can act as a potential two-photon excited fluorescent probe for Hg 2+ . The theoretical investigations would be helpful to build a relationship between the structure and the optical properties of the probes, providing information on the design of efficient two-photon fluorescent sensors that can be used for biological imaging of Hg 2+ in vivo.

Synthesis of novel fluorene-based two-photon absorbing molecules and their applications in optical data storage, microfabrication, and stimulated emission depletion

NASA Astrophysics Data System (ADS)

Yanez, Ciceron

2009-12-01

Two-photon absorption (2PA) has been used for a number of scientific and technological applications, exploiting the fact that the 2PA probability is directly proportional to the square of the incident light intensity (while one-photon absorption bears a linear relation to the incident light intensity). This intrinsic property of 2PA leads to 3D spatial localization, important in fields such as optical data storage, fluorescence microscopy, and 3D microfabrication. The spatial confinement that 2PA enables has been used to induce photochemical and photophysical events in increasingly smaller volumes and allowed nonlinear, 2PA-based, technologies to reach sub-diffraction limit resolutions. The primary focus of this dissertation is the development of novel, efficient 2PA, fluorene-based molecules to be used either as photoacid generators (PAGs) or fluorophores. A second aim is to develop more effective methods of synthesizing these compounds. As a third and final objective, the new molecules were used to develop a write-once-read many (WORM) optical data storage system, and stimulated emission depletion probes for bioimaging. In Chapter I, the microwave-assisted synthesis of triarylsulfonium salt photoacid generators (PAGs) from their diphenyliodonium counterparts is reported. The microwave-assisted synthesis of these novel sulfonium salts afforded reaction times 90 to 420 times faster than conventional thermal conditions, with photoacid quantum yields of new sulfonium PAGs ranging from 0.01 to 0.4. These PAGs were used to develop a fluorescence readout-based, nonlinear three-dimensional (3D) optical data storage system (Chapter II). In this system, writing was achieved by acid generation upon two-photon absorption (2PA) of a PAG (at 710 or 730 nm). Readout was then performed by interrogating two-photon absorbing dyes, after protonation, at 860 nm. Two-photon recording and readout of voxels was demonstrated in five and eight consecutive, crosstalk-free layers within a polymer matrix, generating a data storage capacity of up to 1.8 x 1013 bits/cm3. The possibility of using these PAGs in microfabrication is described in Chapter III, where two-photon induced cationic ring-opening polymerization (CROP) crosslinking of an SU8 resin is employed to produce free-standing microstructures. Chapter IV describes the investigation of one- and two-photon stimulated emission transitions by the fluorescence quenching of a sulfonyl-containing fluorene compound in solution at room temperate using a picosecond pump-probe technique. The nature of stimulated transitions under various fluorescence excitation and quenching conditions were analyzed theoretically, and good agreement with experimental data was demonstrated. Two-photon stimulated transitions S1 → S0 were shown at lambdaq = 1064 nm. The two-photon stimulated emission cross section of the sulfonyl fluorophore was estimated as delta2PE (lambda q) ≈ 240--280 GM, making this compound a good candidate for use in two-photon stimulated emission depletion (STED) microscopy.

Metal-to-metal charge transfer between dopant and host ions: Photoconductivity of Yb-doped CaF{sub 2} and SrF{sub 2} crystals

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

Barandiarán, Zoila, E-mail: zoila.barandiaran@uam.es; Seijo, Luis; Instituto Universitario de Ciencia de Materiales Nicolás Cabrera and Condensed Matter Physics Center

2015-10-14

Dopant-to-host electron transfer is calculated using ab initio wavefunction-based embedded cluster methods for Yb/Ca pairs in CaF{sub 2} and Yb/Sr pairs in SrF{sub 2} crystals to investigate the mechanism of photoconductivity. The results show that, in these crystals, dopant-to-host electron transfer is a two-photon process mediated by the 4f{sup N−1}5d excited states of Y b{sup 2+}: these are reached by the first photon excitation; then, they absorb the second photon, which provokes the Y b{sup 2+} + Ca{sup 2+} (Sr{sup 2+}) → Y b{sup 3+} + Ca{sup +} (Sr{sup +}) electron phototransfer. This mechanism applies to all the observed Ymore » b{sup 2+} 4f–5d absorption bands with the exception of the first one: Electron transfer cannot occur at the first band wavelengths in CaF{sub 2}:Y b{sup 2+} because the Y b{sup 3+}–Ca{sup +} states are not reached by the two-photon absorption. In contrast, Yb-to-host electron transfer is possible in SrF{sub 2}:Y b{sup 2+} at the wavelengths of the first 4f–5d absorption band, but the mechanism is different from that described above: first, the two-photon excitation process occurs within the Y b{sup 2+} active center, then, non-radiative Yb-to-Sr electron transfer can occur. All of these features allow to interpret consistently available photoconductivity experiments in these materials, including the modulation of the photoconductivity by the absorption spectrum, the differences in photoconductivity thresholds observed in both hosts, and the peculiar photosensitivity observed in the SrF{sub 2} host, associated with the lowest 4f–5d band.« less

Mercury in Environmental and Biological Samples Using Online Combustion with Sequential Atomic Absorption and Fluorescence Measurements: A Direct Comparison of Two Fundamental Techniques in Spectrometry

ERIC Educational Resources Information Center

Cizdziel, James V.

2011-01-01

In this laboratory experiment, students quantitatively determine the concentration of an element (mercury) in an environmental or biological sample while comparing and contrasting the fundamental techniques of atomic absorption spectrometry (AAS) and atomic fluorescence spectrometry (AFS). A mercury analyzer based on sample combustion,…

Emerging Low-Dimensional Materials for Nonlinear Optics and Ultrafast Photonics.

PubMed

Liu, Xiaofeng; Guo, Qiangbing; Qiu, Jianrong

2017-04-01

Low-dimensional (LD) materials demonstrate intriguing optical properties, which lead to applications in diverse fields, such as photonics, biomedicine and energy. Due to modulation of electronic structure by the reduced structural dimensionality, LD versions of metal, semiconductor and topological insulators (TIs) at the same time bear distinct nonlinear optical (NLO) properties as compared with their bulk counterparts. Their interaction with short pulse laser excitation exhibits a strong nonlinear character manifested by NLO absorption, giving rise to optical limiting or saturated absorption associated with excited state absorption and Pauli blocking in different materials. In particular, the saturable absorption of these emerging LD materials including two-dimensional semiconductors as well as colloidal TI nanoparticles has recently been utilized for Q-switching and mode-locking ultra-short pulse generation across the visible, near infrared and middle infrared wavelength regions. Beside the large operation bandwidth, these ultrafast photonics applications are especially benefit from the high recovery rate as well as the facile processibility of these LD materials. The prominent NLO response of these LD materials have also provided new avenues for the development of novel NLO and photonics devices for all-optical control as well as optical circuits beyond ultrafast lasers. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Absorption spectrum of a two-level system subjected to a periodic pulse sequence

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

Fotso, H. F.; Dobrovitski, V. V.

We investigate how the quantum control of a two-level system (TLS) coupled to photons can modify and tune the TLS’s photon absorption spectrum. Tuning and controlling the emission and the absorption is of much interest e.g. for the development of efficient interfaces between stationary and flying qubits in modern architectures for quantum computation and quantum communication. We consider the periodic pulse control, where the TLS is subjected to a periodic sequence of the near-resonant Rabi driving pulses, each pulse implementing a 180° rotation. For small inter-pulse delays, the absorption spectrum features a pronounced peak of stimulated emission at the pulsemore » frequency, as well as equidistant satellite peaks with smaller spectral weights. As long as the detuning between the carrier frequency of the driving and the TLS transition frequency remains moderate, this spectral shape shows little change. Therefore, the quantum control allows shifting the absorption peak to a desired position, and locks the absorption peak to the carrier frequency of the driving pulses. Detailed description of the spectrum, and its evolution as a function time, the inter-pulse spacing and the detuning, is presented.« less

Absorption spectrum of a two-level system subjected to a periodic pulse sequence

DOE PAGES

Fotso, H. F.; Dobrovitski, V. V.

2017-06-01

We investigate how the quantum control of a two-level system (TLS) coupled to photons can modify and tune the TLS’s photon absorption spectrum. Tuning and controlling the emission and the absorption is of much interest e.g. for the development of efficient interfaces between stationary and flying qubits in modern architectures for quantum computation and quantum communication. We consider the periodic pulse control, where the TLS is subjected to a periodic sequence of the near-resonant Rabi driving pulses, each pulse implementing a 180° rotation. For small inter-pulse delays, the absorption spectrum features a pronounced peak of stimulated emission at the pulsemore » frequency, as well as equidistant satellite peaks with smaller spectral weights. As long as the detuning between the carrier frequency of the driving and the TLS transition frequency remains moderate, this spectral shape shows little change. Therefore, the quantum control allows shifting the absorption peak to a desired position, and locks the absorption peak to the carrier frequency of the driving pulses. Detailed description of the spectrum, and its evolution as a function time, the inter-pulse spacing and the detuning, is presented.« less

On the sub-band gap optical absorption in heat treated cadmium sulphide thin film deposited on glass by chemical bath deposition technique

NASA Astrophysics Data System (ADS)

Chattopadhyay, P.; Karim, B.; Guha Roy, S.

2013-12-01

The sub-band gap optical absorption in chemical bath deposited cadmium sulphide thin films annealed at different temperatures has been critically analyzed with special reference to Urbach relation. It has been found that the absorption co-efficient of the material in the sub-band gap region is nearly constant up to a certain critical value of the photon energy. However, as the photon energy exceeds the critical value, the absorption coefficient increases exponentially indicating the dominance of Urbach rule. The absorption coefficients in the constant absorption region and the Urbach region have been found to be sensitive to annealing temperature. A critical examination of the temperature dependence of the absorption coefficient indicates two different kinds of optical transitions to be operative in the sub-band gap region. After a careful analyses of SEM images, energy dispersive x-ray spectra, and the dc current-voltage characteristics, we conclude that the absorption spectra in the sub-band gap domain is possibly associated with optical transition processes involving deep levels and the grain boundary states of the material.

Nonlinear optical properties, upconversion and lasing in metal-organic frameworks.

PubMed

Medishetty, Raghavender; Zaręba, Jan K; Mayer, David; Samoć, Marek; Fischer, Roland A

2017-08-14

The building block modular approach that lies behind coordination polymers (CPs) and metal-organic frameworks (MOFs) results not only in a plethora of materials that can be obtained but also in a vast array of material properties that could be aimed at. Optical properties appear to be particularly predetermined by the character of individual structural units and by the intricate interplay between them. Indeed, the "design principles" shaping the optical properties of these materials seem to be well explored for luminescence and second-harmonic generation (SHG) phenomena; these have been covered in numerous previous reviews. Herein, we shine light on CPs and MOFs as optical media for state-of-the-art photonic phenomena such as multi-photon absorption, triplet-triplet annihilation (TTA) and stimulated emission. In the first part of this review we focus on the nonlinear optical (NLO) properties of CPs and MOFs, with a closer look at the two-photon absorption property. We discuss the scope of applicability of most commonly used measurement techniques (Z-scan and two-photon excited fluorescence (TPEF)) that can be applied for proper determination of the NLO properties of these materials; in particular, we suggest recommendations for their use, along with a discussion of the best reporting practices of NLO parameters. We also outline design principles, employing both intramolecular and intermolecular strategies, that are necessary for maximizing the NLO response. A review of recent literature on two-, three- and multi-photon absorption in CPs and MOFs is further supplemented with application-oriented processes such as two-photon 3D patterning and data storage. Additionally, we provide an overview of the latest achievements in the field of frequency doubling (SHG) and tripling (third-harmonic generation, THG) in these materials. Apart from nonlinear processes, in the next sections we also target the photonic properties of MOFs that benefit from their porosity, and resulting from this their ability to serve as containers for optically-active molecules. Thus, we survey dye@MOF composites as novel media in which efficient upconversion via triplet energy migration (TEM) occurs as well as materials for stimulated emission and multi-photon pumped lasing. Prospects for producing lasing as an intrinsic property of MOFs has also been discussed. Overall, further development of the optical processes highlighted herein should allow for realization of various photonic, data storage, biomedical and optoelectronic applications.

Coherent perfect absorption in a quantum nonlinear regime of cavity quantum electrodynamics

NASA Astrophysics Data System (ADS)

Wei, Yang-hua; Gu, Wen-ju; Yang, Guoqing; Zhu, Yifu; Li, Gao-xiang

2018-05-01

Coherent perfect absorption (CPA) is investigated in the quantum nonlinear regime of cavity quantum electrodynamics (CQED), in which a single two-level atom couples to a single-mode cavity weakly driven by two identical laser fields. In the strong-coupling regime and due to the photon blockade effect, the weakly driven CQED system can be described as a quantum system with three polariton states. CPA is achieved at a critical input field strength when the frequency of the input fields matches the polariton transition frequency. In the quantum nonlinear regime, the incoherent dissipation processes such as atomic and photon decays place a lower bound for the purity of the intracavity quantum field. Our results show that under the CPA condition, the intracavity field always exhibits the quadrature squeezing property manifested by the quantum nonlinearity, and the outgoing photon flux displays the super-Poissonian distribution.

Measurement of two-photon-absorption spectra through nonlinear fluorescence produced by a line-shaped excitation beam.

PubMed

Hasani, E; Parravicini, J; Tartara, L; Tomaselli, A; Tomassini, D

2018-05-01

We propose an innovative experimental approach to estimate the two-photon absorption (TPA) spectrum of a fluorescent material. Our method develops the standard indirect fluorescence-based method for the TPA measurement by employing a line-shaped excitation beam, generating a line-shaped fluorescence emission. Such a configuration, which requires a relatively high amount of optical power, permits to have a greatly increased fluorescence signal, thus avoiding the photon counterdetection devices usually used in these measurements, and allowing to employ detectors such as charge-coupled device (CCD) cameras. The method is finally tested on a fluorescent isothiocyanate sample, whose TPA spectrum, which is measured with the proposed technique, is compared with the TPA spectra reported in the literature, confirming the validity of our experimental approach. © 2018 The Authors Journal of Microscopy © 2018 Royal Microscopical Society.

A bioaccumulative cyclometalated platinum(II) complex with two-photon-induced emission for live cell imaging.

PubMed

Koo, Chi-Kin; Wong, Ka-Leung; Man, Cornelia Wing-Yin; Lam, Yun-Wah; So, Leo King-Yan; Tam, Hoi-Lam; Tsao, Sai-Wah; Cheah, Kok-Wai; Lau, Kai-Chung; Yang, Yang-Yi; Chen, Jin-Can; Lam, Michael Hon-Wah

2009-02-02

The cyclometalated platinum(II) complex [Pt(L)Cl], where HL is a new cyclometalating ligand 2-phenyl-6-(1H-pyrazol-3-yl)pyridine containing C(phenyl), N(pyridyl), and N(pyrazolyl) donor moieties, was found to possess two-photon-induced luminescent properties. The two-photon-absorption cross section of the complex in N,N-dimethylformamide at room temperature was measured to be 20.8 GM. Upon two-photon excitation at 730 nm from a Ti:sapphire laser, bright-green emission was observed. Besides its two-photon-induced luminescent properties, [Pt(L)Cl] was able to be rapidly accumulated in live HeLa and NIH3T3 cells. The two-photon-induced luminescence of the complex was retained after live cell internalization and can be observed by two-photon confocal microscopy. Its bioaccumulation properties enabled time-lapse imaging of the internalization process of the dye into living cells. Cytotoxicity of [Pt(L)Cl] to both tested cell lines was low, according to MTT assays, even at loadings as high as 20 times the dose concentration for imaging for 6 h.

A solid state source of photon triplets based on quantum dot molecules

PubMed Central

Khoshnegar, Milad; Huber, Tobias; Predojević, Ana; Dalacu, Dan; Prilmüller, Maximilian; Lapointe, Jean; Wu, Xiaohua; Tamarat, Philippe; Lounis, Brahim; Poole, Philip; Weihs, Gregor; Majedi, Hamed

2017-01-01

Producing advanced quantum states of light is a priority in quantum information technologies. In this context, experimental realizations of multipartite photon states would enable improved tests of the foundations of quantum mechanics as well as implementations of complex quantum optical networks and protocols. It is favourable to directly generate these states using solid state systems, for simpler handling and the promise of reversible transfer of quantum information between stationary and flying qubits. Here we use the ground states of two optically active coupled quantum dots to directly produce photon triplets. The formation of a triexciton in these ground states leads to a triple cascade recombination and sequential emission of three photons with strong correlations. We record 65.62 photon triplets per minute under continuous-wave pumping, surpassing rates of earlier reported sources. Our structure and data pave the way towards implementing multipartite photon entanglement and multi-qubit readout schemes in solid state devices. PMID:28604705

Linear and Nonlinear Optical Properties of Photoresponsive [60]Fullerene Hybrid Triads and Tetrads with Dual NIR Two-Photon Absorption Characteristics

PubMed Central

Jeon, Seaho; Haley, Joy; Flikkema, Jonathan; Nalla, Venkatram; Wang, Min; Sfeir, Matthew; Tan, Loon-Seng; Cooper, Thomas; Ji, Wei; Hamblin, Michael R.; Chiang, Long Y.

2013-01-01

Two C60-(antenna)x analogous compounds having branched hybrid triad C60(>DPAF-C18)(>CPAF-C2M) and tetrad C60(>DPAF-C18)(>CPAF-C2M)2 nanostructures were synthesized and characterized. The structural design was intended to facilitate the ultrafast fs intramolecular energy-transfer from photoexcited C60[>1(DPAF)*-C18](>CPAF-C2M)1or2 or C60(>DPAF-C18)[>1(CPAF)*-C2M]1or2 to the C60> cage moiety upon two-photon pumping at either 780 or 980 nm, respectively. The latter nanostructure showed approximately equal extinction coefficients of optical absorption over 400–550 nm that corresponds to near-IR two-photon based excitation wavelengths at 780–1100 nm for broadband nonlinear optical (NLO) applications. Aside from their enhanced two-photon absorption (2PA) activity at 780 nm, we also demonstrated ultrafast photo-responses at 980 nm showing 2PA cross-section (σ2) values of 995–1100 GM for the hybrid tetrad. These σ2 values were correlated to the observed good efficiency in reducing fs light-transmittance down to 35% at the light intensity of 110 GW/cm2. Accordingly, 2PA characteristics of these nanostructures at multiple NIR wavelengths provided support for their suitability in uses as broadband NLO nanomaterials at 600–1100 nm that includes the 2PA ability of two antenna, DPAF (700–850 nm) and CPAF (850–1100 nm), and the fullerene cage at shorter wavelengths (600–700 nm). PMID:24163713

Resonant two-photon absorption and electromagnetically induced transparency in open ladder-type atomic system.

PubMed

Moon, Han Seb; Noh, Heung-Ryoul

2013-03-25

We have experimentally and theoretically studied resonant two-photon absorption (TPA) and electromagnetically induced transparency (EIT) in the open ladder-type atomic system of the 5S(1/2) (F = 1)-5P(3/2) (F' = 0, 1, 2)-5D(5/2) (F″ = 1, 2, 3) transitions in (87)Rb atoms. As the coupling laser intensity was increased, the resonant TPA was transformed to EIT for the 5S(1/2) (F = 1)-5P(3/2) (F' = 2)-5D(5/2) (F″ = 3) transition. The transformation of resonant TPA into EIT was numerically calculated for various coupling laser intensities, considering all the degenerate magnetic sublevels of the 5S(1/2)-5P(3/2)-5D(5/2) transition. From the numerical results, the crossover from TPA to EIT could be understood by the decomposition of the spectrum into an EIT component owing to the pure two-photon coherence and a TPA component caused by the mixed term.

Resonance-enhanced two-photon excitation of CaI

NASA Astrophysics Data System (ADS)

Casero-Junquera, Elena; Lawruszczuk, Rafal; Rostas, Joëlle; Taieb, Guy

1994-07-01

Induced fluorescence following visible (620-655 nm) laser excitation of the CaI radical has been detected not only in the same region (B, A-X transitions), but also in the UV (315-330 nm). The UV two-photon excitation spectrum consists of narrow bands appearing at laser frequencies located within certain bands of the Δ v = 1, 0 sequences of the B 2Σ +-X 2Σ + and A 2Π 1/2-X 2Σ + systems. The main peaks are tentatively assigned to resonance-enhanced excitation of a single vibrational level of the lowest Rydberg D 2Σ + state from successive vibrational levels of the ground state. The excitation process is a one-color two-photon optical—optical-double-resonance via B 2Σ + and A 2Π 1/2 intermediate levels. This analysis is supported by the absorption spectrum observed long ago by Walters and Barratt. The absorption and laser excitation complementary data have been used to derive approximate molecular constants for the D state.

Two-photon absorption spectra of luminescent conducting polymers measured over wide spectral range

NASA Astrophysics Data System (ADS)

Meyer, Ron K.; Liess, Martin; Benner, Robert E.; Gellermann, Werner; Vardeny, Z. Valy; Ozaki, Masanori; Yoshino, Katsumi; Ding, Yi W.; Barton, Thomas J.

1997-12-01

We report the two-photon absorption (TPA) spectra of poly(2,5-dibutoxy-p-phenylene acetylene) (PPA-DBO), poly(2,5-dioctyloxy-p-phenylene vinylene) (PPV-DOO), and poly(3-hexylthiophene) in the spectral range extending from 576 nm to 846 nm. Using the Z-scan technique on the polymers in solution, we measured a strong two-photon allowed transition in all three materials which we attribute to the mAg essential state. In the case of PPA-DBO and PPV-DOO, TPA peaks were coincident with dispersion in the nonlinear refractive indices as detected by reduced aperture Z scan. In all three polymers this peak occurs at approximately 1.3 the bandgap energy. The excitonic nature of the excited electronic states in PPA-DBO is indicated by the lack of a TPA band at or near the 1Bu exciton position. Saturation was observed in the nonlinear index of refraction near spectral peaks, as well as an apparent reverse Kramers- Kronig effect.

Complete chirp analysis of a gain-switched pulse using an interferometric two-photon absorption autocorrelation.

PubMed

Chin, Sang Hoon; Kim, Young Jae; Song, Ho Seong; Kim, Dug Young

2006-10-10

We propose a simple but powerful scheme for the complete analysis of the frequency chirp of a gain-switched optical pulse using a fringe-resolved interferometric two-photon absorption autocorrelator. A frequency chirp imposed on the gain-switched pulse from a laser diode was retrieved from both the intensity autocorrelation trace and the envelope of the second-harmonic interference fringe pattern. To verify the accuracy of the proposed phase retrieval method, we have performed an optical pulse compression experiment by using dispersion-compensating fibers with different lengths. We have obtained close agreement by less than a 1% error between the compressed pulse widths and numerically calculated pulse widths.

One Photon Can Simultaneously Excite Two or More Atoms.

PubMed

Garziano, Luigi; Macrì, Vincenzo; Stassi, Roberto; Di Stefano, Omar; Nori, Franco; Savasta, Salvatore

2016-07-22

We consider two separate atoms interacting with a single-mode optical or microwave resonator. When the frequency of the resonator field is twice the atomic transition frequency, we show that there exists a resonant coupling between one photon and two atoms, via intermediate virtual states connected by counterrotating processes. If the resonator is prepared in its one-photon state, the photon can be jointly absorbed by the two atoms in their ground state which will both reach their excited state with a probability close to one. Like ordinary quantum Rabi oscillations, this process is coherent and reversible, so that two atoms in their excited state will undergo a downward transition jointly emitting a single cavity photon. This joint absorption and emission process can also occur with three atoms. The parameters used to investigate this process correspond to experimentally demonstrated values in circuit quantum electrodynamics systems.

Near-infrared sub-bandgap all-silicon photodetectors: state of the art and perspectives.

PubMed

Casalino, Maurizio; Coppola, Giuseppe; Iodice, Mario; Rendina, Ivo; Sirleto, Luigi

2010-01-01

Due to recent breakthroughs, silicon photonics is now the most active discipline within the field of integrated optics and, at the same time, a present reality with commercial products available on the market. Silicon photodiodes are excellent detectors at visible wavelengths, but the development of high-performance photodetectors on silicon CMOS platforms at wavelengths of interest for telecommunications has remained an imperative but unaccomplished task so far. In recent years, however, a number of near-infrared all-silicon photodetectors have been proposed and demonstrated for optical interconnect and power-monitoring applications. In this paper, a review of the state of the art is presented. Devices based on mid-bandgap absorption, surface-state absorption, internal photoemission absorption and two-photon absorption are reported, their working principles elucidated and their performance discussed and compared.

Near-Infrared Sub-Bandgap All-Silicon Photodetectors: State of the Art and Perspectives

PubMed Central

Casalino, Maurizio; Coppola, Giuseppe; Iodice, Mario; Rendina, Ivo; Sirleto, Luigi

2010-01-01

Due to recent breakthroughs, silicon photonics is now the most active discipline within the field of integrated optics and, at the same time, a present reality with commercial products available on the market. Silicon photodiodes are excellent detectors at visible wavelengths, but the development of high-performance photodetectors on silicon CMOS platforms at wavelengths of interest for telecommunications has remained an imperative but unaccomplished task so far. In recent years, however, a number of near-infrared all-silicon photodetectors have been proposed and demonstrated for optical interconnect and power-monitoring applications. In this paper, a review of the state of the art is presented. Devices based on mid-bandgap absorption, surface-state absorption, internal photoemission absorption and two-photon absorption are reported, their working principles elucidated and their performance discussed and compared. PMID:22163487

Broadband sensitive pump-probe setup for ultrafast optical switching of photonic nanostructures and semiconductors.

PubMed

Euser, Tijmen G; Harding, Philip J; Vos, Willem L

2009-07-01

We describe an ultrafast time resolved pump-probe spectroscopy setup aimed at studying the switching of nanophotonic structures. Both femtosecond pump and probe pulses can be independently tuned over broad frequency range between 3850 and 21,050 cm(-1). A broad pump scan range allows a large optical penetration depth, while a broad probe scan range is crucial to study strongly photonic crystals. A new data acquisition method allows for sensitive pump-probe measurements, and corrects for fluctuations in probe intensity and pump stray light. We observe a tenfold improvement of the precision of the setup compared to laser fluctuations, allowing a measurement accuracy of better than DeltaR=0.07% in a 1 s measurement time. Demonstrations of the improved technique are presented for a bulk Si wafer, a three-dimensional Si inverse opal photonic bandgap crystal, and z-scan measurements of the two-photon absorption coefficient of Si, GaAs, and the three-photon absorption coefficient of GaP in the infrared wavelength range.

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.

Rapid Three-Dimensional Printing in Water Using Semiconductor-Metal Hybrid Nanoparticles as Photoinitiators.

PubMed

Pawar, Amol Ashok; Halivni, Shira; Waiskopf, Nir; Ben-Shahar, Yuval; Soreni-Harari, Michal; Bergbreiter, Sarah; Banin, Uri; Magdassi, Shlomo

2017-07-12

Additive manufacturing processes enable fabrication of complex and functional three-dimensional (3D) objects ranging from engine parts to artificial organs. Photopolymerization, which is the most versatile technology enabling such processes through 3D printing, utilizes photoinitiators that break into radicals upon light absorption. We report on a new family of photoinitiators for 3D printing based on hybrid semiconductor-metal nanoparticles. Unlike conventional photoinitiators that are consumed upon irradiation, these particles form radicals through a photocatalytic process. Light absorption by the semiconductor nanorod is followed by charge separation and electron transfer to the metal tip, enabling redox reactions to form radicals in aerobic conditions. In particular, we demonstrate their use in 3D printing in water, where they simultaneously form hydroxyl radicals for the polymerization and consume dissolved oxygen that is a known inhibitor. We also demonstrate their potential for two-photon polymerization due to their giant two-photon absorption cross section.

Two-Phonon Absorption

ERIC Educational Resources Information Center

Hamilton, M. W.

2007-01-01

A nonlinear aspect of the acousto-optic interaction that is analogous to multi-photon absorption is discussed. An experiment is described in which the second-order acousto-optically scattered intensity is measured and found to scale with the square of the acoustic intensity. This experiment using a commercially available acousto-optic modulator is…

Nonlinear optical transmittance of semiconductors in the presence of high-intensity radiation fields

NASA Astrophysics Data System (ADS)

Dong, H. M.; Han, F. W.; Duan, Y. F.; Huang, F.; Liu, J. L.

2018-04-01

We developed a systematic theoretical study of nonlinear optical properties of semiconductors. The eight-band kṡp model and the energy-balance equation are employed to calculate the transmission and optical absorption coefficients in the presence of both the linear one-photon absorption and the nonlinear two-photon absorption (TPA) processes. A substantial reduction of the optical transmittance far below the band-gap can be observed under relatively high-intensity radiation fields due to the nonlinear TPA. The TPA-induced optical transmittance decreases with increasing intensity of the radiation fields. Our theoretical results are in line with those observed experimentally. The theoretical approach can be applied to understand the nonlinear optical properties of semiconductors under high-field conditions.

Sequential x-ray diffraction topography at 1-BM x-ray optics testing beamline at the advanced photon source

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

Stoupin, Stanislav, E-mail: sstoupin@aps.anl.gov; Shvyd’ko, Yuri; Trakhtenberg, Emil

2016-07-27

We report progress on implementation and commissioning of sequential X-ray diffraction topography at 1-BM Optics Testing Beamline of the Advanced Photon Source to accommodate growing needs of strain characterization in diffractive crystal optics and other semiconductor single crystals. The setup enables evaluation of strain in single crystals in the nearly-nondispersive double-crystal geometry. Si asymmetric collimator crystals of different crystallographic orientations were designed, fabricated and characterized using in-house capabilities. Imaging the exit beam using digital area detectors permits rapid sequential acquisition of X-ray topographs at different angular positions on the rocking curve of a crystal under investigation. Results on sensitivity andmore » spatial resolution are reported based on experiments with high-quality Si and diamond crystals. The new setup complements laboratory-based X-ray topography capabilities of the Optics group at the Advanced Photon Source.« less

Single-shot measurement of nonlinear absorption and nonlinear refraction.

PubMed

Jayabalan, J; Singh, Asha; Oak, Shrikant M

2006-06-01

A single-shot method for measurement of nonlinear optical absorption and refraction is described and analyzed. A spatial intensity variation of an elliptical Gaussian beam in conjugation with an array detector is the key element of this method. The advantages of this single-shot technique were demonstrated by measuring the two-photon absorption and free-carrier absorption in GaAs as well as the nonlinear refractive index of CS2 using a modified optical Kerr setup.

Third order nonlinear optical properties of bismuth zinc borate glasses

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

Shanmugavelu, B.; Ravi Kanth Kumar, V. V., E-mail: ravi.phy@pondiuni.edu.in; Kuladeep, R.

2013-12-28

Third order nonlinear optical characterization of bismuth zinc borate glasses are reported here using different laser pulse durations. Bismuth zinc borate glasses with compositions xBi{sub 2}O{sub 3}-30ZnO-(70-x) B{sub 2}O{sub 3} (where x = 30, 35, 40, and 45 mol. %) have been prepared by melt quenching method. These glasses were characterized by Raman, UV-Vis absorption, and Z scan measurements. Raman and UV-Vis spectroscopic results indicate that non-bridging oxygens increase with increase of bismuth content in the glass. Nonlinear absorption and refraction behavior in the nanosecond (ns), picosecond (ps), and femtosecond (fs) time domains were studied in detail. Strong reverse saturable absorption due tomore » dominant two-photon absorption (TPA) was observed with both ps and fs excitations. In the case of ns pulse excitations, TPA and free-carrier absorption processes contribute for the nonlinear absorption. Two-photon absorption coefficient (β) and the absorption cross section due to free carriers (σ{sub e}) are estimated by theoretical fit of the open aperture Z-scan measurements and found to be dependent on the amount of bismuth oxide in the glass composition. In both ns and fs regimes the sign and magnitude of the third order nonlinearity are evaluated, and the optical limiting characteristics are also reported.« less

Nonlinear absorption properties of silicene nanosheets.

PubMed

Zhang, Fang; Wang, Mengxia; Wang, Zhengping; Han, Kezhen; Liu, Xiaojuan; Xu, Xinguang

2018-06-01

As the cousins of graphene, i.e. same group IVA element, the nonlinear absorption (NLA) properties of silicene nanosheets were rarely studied. In this paper, we successfully exfoliated the two-dimensional silicene nanosheets from bulk silicon crystal using liquid phase exfoliation method. The NLA properties of silicene nanosheets were systemically investigated for the first time, as we have known. Silicene performed exciting saturable absorption and two photon absorption (2PA) behavior. The lower saturable intensity and larger 2PA coefficient at 532 nm excitation indicates that silicene has potential application in ultrafast lasers and optical limiting devices, especially in visible waveband.

Nonlinear absorption properties of silicene nanosheets

NASA Astrophysics Data System (ADS)

Zhang, Fang; Wang, Mengxia; Wang, Zhengping; Han, Kezhen; Liu, Xiaojuan; Xu, Xinguang

2018-06-01

As the cousins of graphene, i.e. same group IVA element, the nonlinear absorption (NLA) properties of silicene nanosheets were rarely studied. In this paper, we successfully exfoliated the two-dimensional silicene nanosheets from bulk silicon crystal using liquid phase exfoliation method. The NLA properties of silicene nanosheets were systemically investigated for the first time, as we have known. Silicene performed exciting saturable absorption and two photon absorption (2PA) behavior. The lower saturable intensity and larger 2PA coefficient at 532 nm excitation indicates that silicene has potential application in ultrafast lasers and optical limiting devices, especially in visible waveband.

Diffraction and quantum control of wave functions in nonresonant two-photon absorption

NASA Astrophysics Data System (ADS)

Li, Baihong; Pang, Huafeng; Wang, Doudou; Zhang, Tao; Dong, Ruifang; Li, Yongfang

2018-03-01

In this study, the nonresonant two-photon absorption process in a two-level atom, induced by a weak chirped pulse, is theoretically investigated in the frequency domain. An analytical expression of the wave function expressed by Fresnel functions is obtained, and the two-photon transition probability (TPTP) versus the integral bandwidth, spectral width, and chirp parameter is analyzed. The results indicate that the oscillation evolution of the TPTP result from quantum diffraction of the wave function, which can be explained by analogy with Fresnel diffraction from a wide slit in the spatial domain. Moreover, the ratio between the real and imaginary parts of the excited state wave function and, hence, the atomic polarization, can be controlled by the initial phase of the excitation pulse. In some special initial phase of the excitation pulse, the wave functions with purely real or imaginary parts can be obtained by measuring the population probability. This work provides a novel perspective for understanding the physical details of the interactions between atoms and chirped light pulses in the multiphoton process.

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.

Frequency up-shift in the stimulated thermal scattering under two-photon absorption in liquids and colloids of metal nanoparticles

NASA Astrophysics Data System (ADS)

Smetanin, I. V.; Erokhin, A. I.; Baranov, A. N.

2018-07-01

We report the results of the experimental and theoretical study of stimulated temperature scattering in toluene and hexane solutions of Ag-nanoparticles, as well as in pure toluene in the two-photon absorption regime. A four-wave mixing scheme with two counter-propagating pump waves of the same frequency is utilised to demonstrate the lasing effect and the amplification of the backscattered anti-Stokes signal. For the first time, we have measured anti-Stokes spectral shifts which turn out to appreciably exceed the Rayleigh line widths in those liquids. It is shown that the amplification effect is provided predominantly by thermally induced coherent polarisation oscillations, while the dynamic interference temperature grating causes the formation of a self-induced optical cavity inside the interaction region.

Self-assembly of Terbium(III)-based metal-organic complexes with two-photon absorbing active

NASA Astrophysics Data System (ADS)

Li, Dandan; Shao, Nanqi; Sun, Xianshun; Zhang, Guocui; Li, Shengli; Zhou, Hongping; Wu, Jieying; Tian, Yupeng

2014-12-01

Hybrid complexes based on D-π-A type dyes p-aminostyryl-pyridinum and Terbium(III) complex anion (1, 2) have been synthesized by ionic exchange reaction. Meanwhile two different alkyl-substituted amino groups were used as electron donors in organic dyes cations. The synthesized complexes were characterized by element analysis. In addition, the structural features of them were systematic studied by single crystal X-ray diffraction analysis. Their linear properties have been systematically investigated by absorption spectra and fluorescence, the results show that the energy transfer takes place from the trans-4-[4‧-(N,N-diethylamino)styryl]-N-methyl pyridinium (2‧) cation to Tb(III). In addition, complex 2 exhibit a large two-photon absorption coefficient β: 0.044 cm/GW at 710 nm.

Two-photon Shack-Hartmann wavefront sensor.

PubMed

Xia, Fei; Sinefeld, David; Li, Bo; Xu, Chris

2017-03-15

We introduce a simple wavefront sensing scheme for aberration measurement of pulsed laser beams in near-infrared wavelengths (<2200  nm), where detectors are not always available or are very expensive. The method is based on two-photon absorption in a silicon detector array for longer wavelengths detection. We demonstrate the simplicity of such implementations with a commercially available Shack-Hartmann wavefront sensor and discuss the detection sensitivity of this method.

Two-photon absorption spectroscopy using intense phase-chirped entangled beams

NASA Astrophysics Data System (ADS)

Svozilík, Jiří; Peřina, Jan; León-Montiel, Roberto de J.

2018-06-01

We numerically analyze the use of intense entangled twin beams for ultra-sensitive spectroscopic measurements in chemical and biological systems. The examined scheme makes use of intense frequency-modulated (chirped) entangled beams to successfully extract information about the intermediate material states that contribute to the two-photon excitation of an absorbing medium. Robustness of the presented method is examined with respect to the applied intervals of the frequency chirp.

Two-photon-induced cycloreversion reaction of chalcone photodimers

NASA Astrophysics Data System (ADS)

Träger, J.; Härtner, S.; Heinzer, J.; Kim, H.-C.; Hampp, N.

2008-04-01

The photocleavage reaction of chalcone photodimers has been studied using a two-photon process. For this purpose, a novel chalcone dimer has been synthesized as a low molecular weight model substance for polymer bound chalcones and its photochemistry triggered by two-photon-absorption (2PA) has been investigated using a pulsed frequency-doubled Nd:YAG-laser. The 2PA-induced cycloreversion reaction selectively leads to the cleavage of the chalcone photodimers resulting in the formation of monomeric chalcone molecules. Hence, as an application chalcones can be used as a photosensitive linker which can be cleaved beyond an UV-absorbing barrier. The 2PA cross section of the chalcone photodimer was determined to be of 1.1 × 10 -49 cm 4 s photon -1 (11 GM).

Bright long-lived luminescence of silicon nanocrystals sensitized by two-photon absorbing antenna

PubMed Central

Ravotto, Luca; Chen, Qi; Ma, Yuguo; Vinogradov, Sergei A.; Locritani, Mirko; Bergamini, Giacomo; Negri, Fabrizia; Yu, Yixuan; Korgel, Brian A.; Ceroni, Paola

2017-01-01

Summary Silicon nanocrystals of the average diameter of 5 nm, functionalized with 4,7-di(2-thienyl)-2,1,3-benzothiadiazole chromophores (TBT) and dodecyl chains, exhibit near-infrared emission upon one-photon (1P) excitation at 515 nm and two-photon (2P) excitation at 960 nm. By using TBT chromophores as an antenna we were able to enhance both 1P and 2P absorption cross-sections of the silicon nanocrystals to more efficiently excite their long-lived luminescence. These results chart a path to two-photon-excitable imaging probes with long-lived oxygen-independent luminescence - a rare combination of properties that should allow for a substantial increase in imaging contrast. PMID:28966989

Two Photon Absorption And Refraction in Bulk of the Semiconducting Materials

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

Kumari, Vinay; Department of Physics, DCRUST Murthal, Haryana; Kumar, Vinod

2011-10-20

Fast electronic detection systems have opened up a number of new fields like nonlinear optics, optical communication, coherent optics, optical bistability, two/four wave mixing. The interest in this field has been stimulated by the importance of multiphoton processes in many fundamental aspects of physics. It has proved to be an invaluable tool for determining the optical and electronic properties of the solids because of the fact that one gets the information about the bulk of the material rather than the surface one. In this paper we report, the measurement of the nonlinear absorption and refraction from the band gap tomore » half-band gap region of bulk of semiconductors in the direct and indirect band gap crystals with nanosecond laser. The measured theoretical calculated values of two-photon absorption coefficients ({beta}) and nonlinear refraction n{sub 2}({omega}) of direct band gap crystal match the earlier reported theoretical predictions. By making use of these theoretical calculated values, we have estimated {beta} and n{sub 2}({omega}) in the case of indirect band gap crystals. Low value of absorption coefficient in case of indirect band gap crystals have been attributed to phonon assisted transition while reduction in nonlinear refraction is due to the rise in saturation taking place in the absorption.« less

Optical Nonlinearities in Semiconductors for Limiting.

NASA Astrophysics Data System (ADS)

Wu, Yuan-Yen

I have conducted detailed experimental and theoretical studies of the nonlinear optical properties of semiconductor materials useful for optical limiting. I have constructed optical limiters utilizing two-photon absorption along with photogenerated carrier defocusing as well as the bound electronic nonlinearity using the semiconducting material ZnSe. I have optimized the focusing geometry to achieve a large dynamic range while maintaining a low limiting energy for the device. The ZnSe monolithic optical limiter has achieved a limiting energy as low as 13 nJ (corresponding to 300W peak power) and a dynamic range as large as 10 ^5 at 532 nm using psec pulses. Theoretical analysis showed that the ZnSe device has a broad-band response covering the wavelength range from 550 nm to 800 nm. Moreover, I found that existing theoretical models (e.g. the Auston model and the band-resonant model using Boltzmann statistics) adequately describe the photo-generated carriers refractive nonlinearity in ZnSe. Material nonlinear optical parameters, such as the two-photon absorption coefficient beta _2 = 5.5 cm/GW, the refraction per unit carrier density sigma_{rm n} = -0.8cdot 10^ {-21}cm^3 and the bound electronic refraction n_2 = -4cdot 10^{ -11}esu, have been measured via time-integrated beam distortion experiments in the near field. A numerical code has been written to simulate the beam distortion in order to extract the previously mentioned material parameters. In addition, I have performed time-resolved distortion measurements that provide an intuitive picture of the carrier generation process via two-photon absorption. I also characterized the optical nonlinearities in a ZnSe Fabry-Perot thin film structure (an interference filter). I concluded that the nonlinear absorption alone in the thin film is insufficient to build an effective optical limiter, as it did not show a net change in refraction using psec pulses. An innovative numerical program was developed to simulate the nonlinear beam propagation inside the Fabry-Perot structure. For comparison, pump-probe experiments were performed using both thin film and bulk ZnSe. The results showed relatively long carrier lifetimes (>300 psec) in both samples. A numerical code was written to fit the pump-probe experimental results. The fitting yielded that carrier lifetimes (recombination through traps), radiative decay rate, two-photon absorption coefficient as well as the free carrier absorption coefficient for ZnSe bulk material.

Differential phase contrast with a segmented detector in a scanning X-ray microprobe

PubMed Central

Hornberger, B.; de Jonge, M. D.; Feser, M.; Holl, P.; Holzner, C.; Jacobsen, C.; Legnini, D.; Paterson, D.; Rehak, P.; Strüder, L.; Vogt, S.

2008-01-01

Scanning X-ray microprobes are unique tools for the nanoscale investigation of specimens from the life, environmental, materials and other fields of sciences. Typically they utilize absorption and fluorescence as contrast mechanisms. Phase contrast is a complementary technique that can provide strong contrast with reduced radiation dose for weakly absorbing structures in the multi-keV range. In this paper the development of a segmented charge-integrating silicon detector which provides simultaneous absorption and differential phase contrast is reported. The detector can be used together with a fluorescence detector for the simultaneous acquisition of transmission and fluorescence data. It can be used over a wide range of photon energies, photon rates and exposure times at third-generation synchrotron radiation sources, and is currently operating at two beamlines at the Advanced Photon Source. Images obtained at around 2 keV and 10 keV demonstrate the superiority of phase contrast over absorption for specimens composed of light elements. PMID:18552427

Theoretical X-ray production cross sections at incident photon energies across L{sub i} (i=1-3) absorption edges of Br

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

Puri, Sanjiv

The X-ray production (XRP) cross sections, σ{sub Lk} (k = l, η, α, β{sub 6}, β{sub 1}, β{sub 3}, β{sub 4}, β{sub 9,10}, γ{sub 1,5}, γ{sub 2,3}) have been evaluated at incident photon energies across the L{sub i}(i=1-3) absorption edge energies of {sub 35}Br using theoretical data sets of different physical parameters, namely, the L{sub i}(i=1-3) sub-shell the X-ray emission rates based on the Dirac-Fock (DF) model, the fluorescence and Coster Kronig yields based on the Dirac-Hartree-Slater (DHS) model, and two sets of the photoionisation cross sections based on the relativistic Hartree-Fock-Slater (RHFS) model and the Dirac-Fock (DF) model, inmore » order to highlight the importance of electron exchange effects at photon energies in vicinity of absorption edge energies.« less

Emission turn-on and solubility turn-off in conjugated polymers: one- and two-photon-induced removal of fluorescence-quenching solubilizing groups.

PubMed

Schelkle, Korwin M; Becht, Steffy; Faraji, Shirin; Petzoldt, Martin; Müllen, Klaus; Buckup, Tiago; Dreuw, Andreas; Motzkus, Marcus; Hamburger, Manuel

2015-01-01

The synthesis of highly efficient two-photon uncaging groups and their potential use in functional conjugated polymers for post-polymerization modification are reported. Careful structural design of the employed nitrophenethyl caging groups allows to efficiently induce bond scission by a two-photon process through a combination of exceptionally high two-photon absorption cross-sections and high reaction quantum yields. Furthermore, π-conjugated polyfluorenes are functionalized with these photocleavable side groups and it is possible to alter their emission properties and solubility behavior by simple light irradiation. Cleavage of side groups leads to a turn-on of the fluorescence while solubility of the π-conjugated materials is drastically reduced. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Two-Photon Absorption Spectroscopy of Rubidium with a Dual-Comb Tequnique

NASA Astrophysics Data System (ADS)

Nishiyama, Akiko; Yoshida, Satoru; Hariki, Takuya; Nakajima, Yoshiaki; Minoshima, Kaoru

2017-06-01

Dual-comb spectroscopies have great potential for high-resolution molecular and atomic spectroscopies, thanks to the broadband comb spectrum consisting of dense narrow modes. In this study, we apply the dual-comb system to Doppler-free two-photon absorption spectroscopy. The outputs of two frequency combs excite several two-photon transitions of rubidium, and we obtained broadband Doppler-free spectra from dual-comb fluorescence signals. The fluorescence detection scheme circumvents the sensitivity limit which is effectively determined by the dynamic range of photodetectors in absorption-based dual-comb spectroscopies. Our system realized high-sensitive, Doppler-free high-resolution and broadband atomic spectroscopy. A part of observed spectra of 5S_{1/2} - 5D_{5/2} transition is shown in the figure. The hyperfine structures of the F" = 1 - F' = 3,2,1 transitions are fully-resolved and the spectral widths are approximately 5 MHz. The absolute frequency axis is precisely calibrated from comb mode frequencies which were stabilized to a GPS-disciplined clock. This work was supported by JST through the ERATO MINOSHIMA Intelligent Optical Synthesizer Project and Grant-in-Aid for JSPS Fellows (16J02345). A. Nishiyama, S. Yoshida, Y. Nakajima, H. Sasada, K. Nakagawa, A. Onae, K. and Minoshima, Opt. Express 24, 25894 (2016). A. Hipke, S. A. Meek, T. Ideguchi, T.W. Hänsch, and N. Picqué, Phys. Rev. A 90, 011805(R) (2014).

Intensity-dependent resonant transmission of x-rays in solid-density aluminum plasma

NASA Astrophysics Data System (ADS)

Cho, M. S.; Chung, H.-K.; Cho, B. I.

2018-05-01

X-ray free-electron lasers (XFELs) provide unique opportunities to generate and investigate dense plasmas. The absorption and transmission properties of x-ray photons in dense plasmas are important in characterizing the state of the plasmas. Experimental evidence shows that the transmission of x-ray photons through dense plasmas depends greatly on the incident XFEL intensity. Here, we present a detailed analysis of intensity-dependent x-ray transmission in solid-density aluminum using collisional-radiative population kinetics calculations. Reverse saturable absorption (RSA), i.e., an increase in x-ray absorption with intensity has been observed for photon energies below the K-absorption edge and in the intensity range of 1016-1017 W/cm2 for XFEL photons with 1487 eV. At higher intensities, a transition from RSA to saturable absorption (SA) is predicted; thus, the x-ray absorption decreases with intensity above a threshold value. For XFEL photon energies of 1501 eV and 1515 eV, the transition from RSA to SA occurs at XFEL intensities between 1017-1018 W/cm2. Electron temperatures are predicted to be in the range of 30-50 eV for the given experimental conditions. Detailed population kinetics of the charge states explains the intensity-dependent absorption of x-ray photons and the fast modulation of XFEL pulses for both RSA and SA.

A theoretical investigation of two typical two-photon pH fluorescent probes.

PubMed

Xu, Zhong; Ren, Ai-Min; Guo, Jing-Fu; Liu, Xiao-Ting; Huang, Shuang; Feng, Ji-Kang

2013-01-01

Intracellular pH plays an important role in many cellular events, such as cell growth, endocytosis, cell adhesion and so on. Some pH fluorescent probes have been reported, but most of them are one-photon fluorescent probes, studies about two-photon fluorescent probes are very rare. In this work, the geometrical structure, electronic structure and one-photon properties of a series of two-photon pH fluorescent probes have been theoretically studied by using density functional theory (DFT) method. Their two-photon absorption (TPA) properties are calculated using the method of ZINDO/sum-over-states method. Two types of two-photon pH fluorescent probes have been investigated by theoretical methods. The mechanisms of the Photoinduced Charge Transfer (PCT) probes and the Photoinduced Electron Transfer (PET) probes are verified specifically. Some designed strategies of good two-photon pH fluorescent probes are suggested on the basis of the investigated results of two mechanisms. For the PCT probes, substituting a stronger electron-donating group for the terminal methoxyl group is an advisable choice to increase the TPA cross section. For the PET probes, the TPA cross sections increase upon protonation. © 2012 Wiley Periodicals, Inc. Photochemistry and Photobiology © 2012 The American Society of Photobiology.

Transient Absorption of Attosecond Pulses by He Atoms in Presence of Near-Infrared Laser Fields: A TDDFT Analysis of Sub-Cycle Temporal Structures

NASA Astrophysics Data System (ADS)

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

2013-05-01

We study transient absorption of extreme ultraviolet (XUV) attosecond pulses in presence of near-infrared (NIR) laser fields by analyzing the population and photon emission of excited atomic energy levels. We consider He atoms and apply a self-interaction-free fully ab initio time-dependent density functional theory (TDDFT). Our method is based on the Krieger-Li-Iafrate (KLI) treatment of the optimized effective potential and incorporates explicitly the self-interaction correction. We focus on the sub-cycle (with respect to NIR field) temporal behavior of the population of the excited energy levels and related dynamics of photon emission. We observe and identify sub-cycle shifts in the photon emission spectrum as a function of the time delay between the XUV and NIR pulses. In the region where the two pulses overlap, the photon emission peaks have an oscillatory structure with a period of 1.3 fs, which is half of the NIR laser optical cycle. Such a structure was also observed in recent experiments on transient absorption. This work was partially supported by DOE and by MOE-NSC-NTU-Taiwan.

Enhanced absorption in two-dimensional materials via Fano-resonant photonic crystals

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

Wang, Wenyi; Klots, Andrey; Bolotin, Kirill I.

2015-05-04

The use of two-dimensional (2D) materials in optoelectronics has attracted much attention due to their fascinating optical and electrical properties. However, the low optical absorption of 2D materials arising from their atomic thickness limits the maximum attainable external quantum efficiency. For example, in the visible and near-infrared regimes monolayer MoS{sub 2} and graphene absorb only ∼10% and 2.3% of incoming light, respectively. Here, we experimentally demonstrate the use of Fano-resonant photonic crystals to significantly boost absorption in atomically thin materials. Using graphene as a test bed, we demonstrate that absorption in the monolayer thick material can be enhanced to 77%more » within the telecommunications band, the highest value reported to date. We also show that the absorption in the Fano-resonant structure is non-local, with light propagating up to 16 μm within the structure. This property is particularly beneficial in harvesting light from large areas in field-effect-transistor based graphene photodetectors in which separation of photo-generated carriers only occurs ∼0.2 μm adjacent to the graphene/electrode interface.« less

Near-IR Two-Photon Fluorescent Sensor for K(+) Imaging in Live Cells.

PubMed

Sui, Binglin; Yue, Xiling; Kim, Bosung; Belfield, Kevin D

2015-08-19

A new two-photon excited fluorescent K(+) sensor is reported. The sensor comprises three moieties, a highly selective K(+) chelator as the K(+) recognition unit, a boron-dipyrromethene (BODIPY) derivative modified with phenylethynyl groups as the fluorophore, and two polyethylene glycol chains to afford water solubility. The sensor displays very high selectivity (>52-fold) in detecting K(+) over other physiological metal cations. Upon binding K(+), the sensor switches from nonfluorescent to highly fluorescent, emitting red to near-IR (NIR) fluorescence. The sensor exhibited a good two-photon absorption cross section, 500 GM at 940 nm. Moreover, it is not sensitive to pH in the physiological pH range. Time-dependent cell imaging studies via both one- and two-photon fluorescence microscopy demonstrate that the sensor is suitable for dynamic K(+) sensing in living cells.

Arduino Due based tool to facilitate in vivo two-photon excitation microscopy.

PubMed

Artoni, Pietro; Landi, Silvia; Sato, Sebastian Sulis; Luin, Stefano; Ratto, Gian Michele

2016-04-01

Two-photon excitation spectroscopy is a powerful technique for the characterization of the optical properties of genetically encoded and synthetic fluorescent molecules. Excitation spectroscopy requires tuning the wavelength of the Ti:sapphire laser while carefully monitoring the delivered power. To assist laser tuning and the control of delivered power, we developed an Arduino Due based tool for the automatic acquisition of high quality spectra. This tool is portable, fast, affordable and precise. It allowed studying the impact of scattering and of blood absorption on two-photon excitation light. In this way, we determined the wavelength-dependent deformation of excitation spectra occurring in deep tissues in vivo.

Spontaneous Symmetry Breaking Facilitates Metal-to-Ligand Charge Transfer: A Quantitative Two-Photon Absorption Study of Ferrocene-phenyleneethynylene Oligomers.

PubMed

Mikhaylov, Alexander; Uudsemaa, Merle; Trummal, Aleksander; Arias, Eduardo; Moggio, Ivana; Ziolo, Ronald; Cooper, Thomas M; Rebane, Aleksander

2018-04-19

Change of the permanent molecular electric dipole moment, Δμ, in a series of nominally centrosymmetric and noncentrosymmteric ferrocene-phenyleneethynylene oligomers was estimated by measuring the two-photon absorption cross-section spectra of the lower energy metal-to-ligand charge-transfer transitions using femtosecond nonlinear transmission method and was found to vary in the range up to 12 D, with the highest value corresponding to the most nonsymmetric system. Calculations of the Δμ performed by the TD-DFT method show quantitative agreement with the experimental values and reveal that facile rotation of the ferrocene moieties relative to the organic ligand breaks the ground-state inversion symmetry in the nominally symmetric structures.

Hypersonic Wake Diagnostics Using Laser Induced Fluorescence Techniques

NASA Technical Reports Server (NTRS)

Mills, Jack L.; Sukenik, Charles I.; Balla, Robert J.

2011-01-01

A review of recent research performed in iodine that involves a two photon absorption of light at 193 nm will be discussed, and it's potential application to velocimetry measurements in a hypersonic flow field will be described. An alternative seed atom, Krypton, will be presented as a good candidate for performing nonintrusive hypersonic flow diagnostics. Krypton has a metastable state with a lifetime of approximately 43 s which would prove useful for time of flight measurement (TOF) and a sensitivity to collisions that can be utilized for density measurements. Calculations using modest laser energies and experimental values show an efficiency of excited state production to be on the order of 10(exp -6) for a two photon absorption at 193 nm.

Resonant two-photon ionization and laser induced fluorescence spectroscopy of jet-cooled adenine

NASA Astrophysics Data System (ADS)

Kim, Nam Joon; Jeong, Gawoon; Kim, Yung Sam; Sung, Jiha; Keun Kim, Seong; Park, Young Dong

2000-12-01

Electronic spectra of the jet-cooled DNA base adenine were obtained by the resonant two-photon ionization (R2PI) and the laser induced fluorescence (LIF) techniques. The 0-0 band to the lowest electronically excited state was found to be located at 35 503 cm-1. Well-resolved vibronic structures were observed up to 1100 cm-1 above the 0-0 level, followed by a slow rise of broad structureless absorption. The lowest electronic state was proposed to be of nπ* character, which lies ˜600 cm-1 below the onset of the ππ* state. The broad absorption was attributed to the extensive vibronic mixing between the nπ* state and the high-lying ππ* state.

Changes in the optical absorption induced by sequential exposition to short- and long-wavelength radiation in the BTO:Al crystal

NASA Astrophysics Data System (ADS)

Shandarov, S. M.; Dyu, V. G.; Kisteneva, M. G.; Khudyakova, E. S.; Smirnov, S. V.; Akrestina, A. S.; Kargin, Yu F.

2017-02-01

Modifications of the spectral dependences of the optical absorption induced in the Bi12TiO20:Al crystal as a result of sequential exposition to cw laser radiation first with the wavelength λ g = 532 nm and then with the longer wavelength λ l,n = 588, 633, 655, 658, 663, 700, 780, 871, or 1064 nm are investigated. We revealed that after the short-wavelength exposition to radiation with λg = 532 nm, the optical absorption in the crystal increases, and in the range 470-1000 nm, yields the spectrum whose form is independent of a prehistory. The subsequent exposition to longer-wavelength radiation leads to bleaching of the crystal in the examined spectral range. A maximum diminishing of the optical absorption in the crystal is observed upon exposure to radiation with the wavelength λ l,5 = 663 nm. To describe the experimentally observed reversible changes in the optical absorption spectrum in the Bi12TiO20:Al we use the impurity absorption model that takes into account the photoinduced transitions between two metastable states of a deep defect center leading to the change of its position in the crystal lattice under conditions of strong lattice relaxation.

Importance of the green color, absorption gradient, and spectral absorption of chloroplasts for the radiative energy balance of leaves.

PubMed

Kume, Atsushi

2017-05-01

Terrestrial green plants absorb photosynthetically active radiation (PAR; 400-700 nm) but do not absorb photons evenly across the PAR waveband. The spectral absorbance of photosystems and chloroplasts is lowest for green light, which occurs within the highest irradiance waveband of direct solar radiation. We demonstrate a close relationship between this phenomenon and the safe and efficient utilization of direct solar radiation in simple biophysiological models. The effects of spectral absorptance on the photon and irradiance absorption processes are evaluated using the spectra of direct and diffuse solar radiation. The radiation absorption of a leaf arises as a consequence of the absorption of chloroplasts. The photon absorption of chloroplasts is strongly dependent on the distribution of pigment concentrations and their absorbance spectra. While chloroplast movements in response to light are important mechanisms controlling PAR absorption, they are not effective for green light because chloroplasts have the lowest spectral absorptance in the waveband. With the development of palisade tissue, the incident photons per total palisade cell surface area and the absorbed photons per chloroplast decrease. The spectral absorbance of carotenoids is effective in eliminating shortwave PAR (<520 nm), which contains much of the surplus energy that is not used for photosynthesis and is dissipated as heat. The PAR absorptance of a whole leaf shows no substantial difference based on the spectra of direct or diffuse solar radiation. However, most of the near infrared radiation is unabsorbed and heat stress is greatly reduced. The incident solar radiation is too strong to be utilized for photosynthesis under the current CO 2 concentration in the terrestrial environment. Therefore, the photon absorption of a whole leaf is efficiently regulated by photosynthetic pigments with low spectral absorptance in the highest irradiance waveband and through a combination of pigment density distribution and leaf anatomical structures.

Laser- and Particle-Beam Chemical Processes on Surfaces. Volume 129

DTIC Science & Technology

1989-12-26

explosive decomposition of organometallic compounds with single pulse laser irradiation . This new... ultrashort , meaning ultra high intensity , excimer laser pulses , two-photon absorption becomes important and limits the penetration depth of the laser ...requires a higher photon load before suffering damage to its chemical structure. With extremely high light intensities , ultrashort excimer laser pulses

All-optical switch consisting of two-stage interferometers controlled by using saturable absorption of monolayer graphene.

PubMed

Oya, Masayuki; Kishikawa, Hiroki; Goto, Nobuo; Yanagiya, Shin-ichiro

2012-11-19

At routing nodes in future photonic networks, pico-second switching will be a key function. We propose an all-optical switch consisting of two-stage Mach-Zehnder interferometers, whose arms contain graphene saturable absorption films. Optical amplitudes along the interferometers are controlled to perform switching between two output ports instead of phase control used in conventional switches. Since only absorption is used for realizing complete switching, insertion loss of 10.2 dB is accompanied in switching. Picosecond response can be expected because of the fast response of saturable absorption of graphene. The switching characteristics are theoretically analyzed and numerically simulated by the finite-difference beam propagation method (FD-BPM).

Broadband transient absorption spectroscopy with 1- and 2-photon excitations: Relaxation paths and cross sections of a triphenylamine dye in solution

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

Moreno, J.; Dobryakov, A. L.; Hecht, S., E-mail: sh@chemie.hu-berlin.de, E-mail: skovale@chemie.hu-berlin.de

2015-07-14

1-photon (382 nm) and 2-photon (752 nm) excitations to the S{sub 1} state are applied to record and compare transient absorption spectra of a push-pull triphenylamine (TrP) dye in solution. After 1-photon excitation, ultrafast vibrational and structural molecular relaxations are detected on a 0.1 ps time scale in nonpolar hexane, while in polar acetonitrile, the spectral evolution is dominated by dipolar solvation. Upon 2-photon excitation, transient spectra in hexane reveal an unexpected growth of stimulated emission (SE) and excited-state absorption (ESA) bands. The behavior is explained by strong population transfer S{sub 1} → S{sub n} due to resonant absorption ofmore » a third pump photon. Subsequent S{sub n} → S{sub 1} internal conversion (with τ{sub 1} = 1 ps) prepares a very hot S{sub 1} state which cools down with τ{sub 2} = 13 ps. The pump pulse energy dependence proves the 2-photon origin of the bleach signal. At the same time, SE and ESA are strongly affected by higher-order pump absorptions that should be taken into account in nonlinear fluorescence applications. The 2-photon excitation cross sections σ{sup (2)} = 32 ⋅ 10{sup −50} cm{sup 4} s at 752 nm are evaluated from the bleach signal.« less

Two-Photon Fluorescence Spectroscopy and Imaging of 4-Dimethylaminonaphthalimide-Peptide and Protein Conjugates

PubMed Central

McLean, Alan M.; Socher, Elke; Varnavski, Oleg; Clark, Travis B.

2014-01-01

We report detailed photophysical studies on the two-photon fluorescence processes of the solvatochromic fluorophore 4-DMN as a conjugate of the important calmodulin (CaM) and the associated CaM-binding peptide M13. Strong two-photon fluorescence enhancement has been observed which is associated with calcium binding. It is found that the two-photon absorption cross-section is strongly dependent on the local environment surrounding the 4-DMN fluorophore in the CaM conjugates, providing sensitivity between sites of fluorophore attachment. Utilizing time-resolved measurements, the emission dynamics of 4-DMN under various environmental (solvent) conditions are analyzed. In addition, anisotropy measurements reveal that the 4-DMN-S38C-CaM system has restricted rotation in the calcium-bound calmodulin. To establish the utility for cellular imaging, two-photon fluorescence microscopy studies were also carried out with the 4-DMN-modified M13 peptide in cells. Together, these studies provide strong evidence that 4-DMN is a useful probe in two-photon imaging, with advantageous properties for cellular experiments. PMID:24245815

π-Expanded α,β-unsaturated ketones: synthesis, optical properties, and two-photon-induced polymerization.

PubMed

Nazir, Rashid; Bourquard, Florent; Balčiūnas, Evaldas; Smoleń, Sabina; Gray, David; Tkachenko, Nikolai V; Farsari, Maria; Gryko, Daniel T

2015-02-23

A library of π-expanded α,β-unsaturated ketones was designed and synthesized. They were prepared by a combination of Wittig reaction, Sonogashira reaction, and aldol condensation. It was further demonstrated that the double aldol condensation can be performed effectively for highly polarized styrene- and diphenylacetylene-derived aldehydes. The strategic placement of two dialkylamino groups at the periphery of D-π-A-π-D molecules resulted in dyes with excellent solubility. These ketones absorb light in the region 400-550 nm. Many of them display strong solvatochromism so that the emission ranges from 530-580 nm in toluene to the near-IR region in benzonitrile. Ketones based on cyclobutanone as central moieties display very high fluorescence quantum yields in nonpolar solvents, which decrease drastically in polar media. Photophysical studies of these new functional dyes revealed that they possess an enhanced two-photon absorption cross section when compared with simpler ketone derivatives. Due to strong polarization of the resulting dyes, values of two-photon absorption cross sections on the level of 200-300 GM at 800 nm were achieved, and thanks to that as well as the presence of the keto group, these new two-photon initiators display excellent performance so that the operating region is 5-75 mW in some cases. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

UV-Vis Ratiometric Resonance Synchronous Spectroscopy for Determination of Nanoparticle and Molecular Optical Cross Sections.

PubMed

Nettles, Charles B; Zhou, Yadong; Zou, Shengli; Zhang, Dongmao

2016-03-01

Demonstrated herein is a UV-vis Ratiometric Resonance Synchronous Spectroscopic (R2S2, pronounced as "R-two-S-two" for simplicity) technique where the R2S2 spectrum is obtained by dividing the resonance synchronous spectrum of a NP-containing solution by the solvent resonance synchronous spectrum. Combined with conventional UV-vis measurements, this R2S2 method enables experimental quantification of the absolute optical cross sections for a wide range of molecular and nanoparticle (NP) materials that range optically from pure photon absorbers or scatterers to simultaneous photon absorbers and scatterers, simultaneous photon absorbers and emitters, and all the way to simultaneous photon absorbers, scatterers, and emitters in the UV-vis wavelength region. Example applications of this R2S2 method were demonstrated for quantifying the Rayleigh scattering cross sections of solvents including water and toluene, absorption and resonance light scattering cross sections for plasmonic gold nanoparticles, and absorption, scattering, and on-resonance fluorescence cross sections for semiconductor quantum dots (Qdots). On-resonance fluorescence quantum yields were quantified for the model molecular fluorophore Eosin Y and fluorescent Qdots CdSe and CdSe/ZnS. The insights and methodology presented in this work should be of broad significance in physical and biological science research that involves photon/matter interactions.

Effect of anisotropy on defect mode peculiarities in chiral liquid crystals

NASA Astrophysics Data System (ADS)

Gevorgyan, A. H.; Oganesyan, K. B.

2018-01-01

The effect of anisotropy on defect mode peculiarities in cholesteric liquid crystals is investigated. The light transmission through the cholesteric liquid crystal layer with an anisotropic layer defect inside is solved by Ambartsumian’s layer addition modified method. Two cases are considered. In the first case, it is assumed that the defect layer is non-absorbing, and the effect of refraction anisotropy on the reflection, relative photonic density of states and the total field intensity produced in the defect layer are studied. In the second case, the defect layer is assumed to be isotropic for refraction and anisotropic for absorption, and the influence of defect layer absorption anisotropy on reflection, absorption, relative photonic density of states and the total field intensity produced in the defect layer are investigated.

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

Abdel-Baki, Manal; Abdel-Wahab, Fathy A.; El-Diasty, Fouad

Lithium tungsten borate glass of the composition (0.56-x)B{sub 2}O{sub 3}-0.4Li{sub 2}O-xZnO-0.04WO{sub 3} (0 {<=}x{<=} 0.1 mol. %) is prepared for photonics applications. The glass is doped with ZnO to tune the glass absorption characteristics in a wide spectrum range (200-2500 nm). Chemical bond approach, including chemical structure, electronegativity, bond ionicity, nearest-neighbor coordination, and other chemical bonding aspect, is used to analyze and to explain the obtained glass properties such as: transmittance, absorption, electronic structure parameters (bandgap, Fermi level, and Urbach exciton-phonon coupling), Wannier free excitons excitation (applying Elliott's model), and two-photon absorption coefficient as a result of replacement of B{submore » 2}O{sub 3} by ZnO.« less

Tissue characterization with ballistic photons: counting scattering and/or absorption centres

NASA Astrophysics Data System (ADS)

Corral, F.; Strojnik, M.; Paez, G.

2015-03-01

We describe a new method to separate ballistic from the scattered photons for optical tissue characterization. It is based on the hypothesis that the scattered photons acquire a phase delay. The photons passing through the sample without scattering or absorption preserve their coherence so they may participate in interference. We implement a Mach-Zehnder experimental setup where the ballistic photons pass through the sample with the delay caused uniquely by the sample indices of refraction. We incorporate a movable mirror on the piezoelectric actuator in the sample arm to detect the amplitude of the modulation term. We present the theory that predicts the path-integrated (or total) concentration of the scattering and absorption centres. The proposed technique may characterize samples with transmission attenuation of ballistic photons by a factor of 10-14.

Ultrafast studies of the excited-state dynamics of copper and nickel phthalocyanine tetrasulfonates: potential sensitizers for the two-photon photodynamic therapy of tumors.

PubMed

Fournier, Michel; Pépin, Claude; Houde, Daniel; Ouellet, René; van Lier, Johan E

2004-01-01

In order to evaluate the potential of copper and nickel phthalocyanine tetrasulfonates as sensitizers for two-photon photodynamic therapy, we conducted kinetic femtosecond measurements of transient absorption and bleaching of their excited state dynamics in aqueous solution. Samples were pumped with 620 nm and 310 nm laser light, which allowed us to study relaxation processes from both the first and second singlet (or doublet for the copper phthalocyanine) excited states. A second excitation from the first excited triplet state, approximately 685 and 105 ps after the first excitation for copper and nickel phthalocyanine tetrasulfonate respectively, was the most efficient way to bring the molecules to an upper triplet state. Presumably this highest triplet state can inflict molecular damage on adjacent biomolecules int eh absence of oxygen, resulting in the desired cytotoxic cellular response. Transient absorption spectra at different fixed delays indicate that optimum efficiency would require that the second photon has a wavelength of approximately 750 nm.

Nonlinear interferometry approach to photonic sequential logic

NASA Astrophysics Data System (ADS)

Mabuchi, Hideo

2011-10-01

Motivated by rapidly advancing capabilities for extensive nanoscale patterning of optical materials, I propose an approach to implementing photonic sequential logic that exploits circuit-scale phase coherence for efficient realizations of fundamental components such as a NAND-gate-with-fanout and a bistable latch. Kerr-nonlinear optical resonators are utilized in combination with interference effects to drive the binary logic. Quantum-optical input-output models are characterized numerically using design parameters that yield attojoule-scale energy separation between the latch states.

Work on a quantum dipole by a single-photon pulse.

PubMed

Valente, D; Brito, F; Ferreira, R; Werlang, T

2018-06-01

Energy transfer from a quantized field to a quantized dipole is investigated. We find that a single photon can transfer energy to a two-level dipole by inducing a dynamic Stark shift, going beyond the well-known absorption and emission processes. A quantum thermodynamical perspective allows us to unravel these two energy transfer mechanisms and to identify the former as a generalized work and the latter as a generalized heat. We show two necessary conditions for the generalized work transfer by a single photon to occur, namely, off-resonance and finite linewidth of the pulse. We also show that the generalized work performed by a single-photon pulse equals the reactive (dispersive) contribution of the work performed by a semiclassical pulse in the low-excitation regime.

Self-assembly of Terbium(III)-based metal-organic complexes with two-photon absorbing active.

PubMed

Li, Dandan; Shao, Nanqi; Sun, Xianshun; Zhang, Guocui; Li, Shengli; Zhou, Hongping; Wu, Jieying; Tian, Yupeng

2014-12-10

Hybrid complexes based on D-π-A type dyes p-aminostyryl-pyridinum and Terbium(III) complex anion (1, 2) have been synthesized by ionic exchange reaction. Meanwhile two different alkyl-substituted amino groups were used as electron donors in organic dyes cations. The synthesized complexes were characterized by element analysis. In addition, the structural features of them were systematic studied by single crystal X-ray diffraction analysis. Their linear properties have been systematically investigated by absorption spectra and fluorescence, the results show that the energy transfer takes place from the trans-4-[4'-(N,N-diethylamino)styryl]-N-methyl pyridinium (2') cation to Tb(III). In addition, complex 2 exhibit a large two-photon absorption coefficient β: 0.044cm/GW at 710nm. Copyright © 2014 Elsevier B.V. All rights reserved.

Multiple-photon excitation of nitrogen vacancy centers in diamond

NASA Astrophysics Data System (ADS)

Ji, Peng; Balili, R.; Beaumariage, J.; Mukherjee, S.; Snoke, D.; Dutt, M. V. Gurudev

2018-04-01

We report the observation of multiphoton photoluminescence excitation (PLE) below the resonant energies of nitrogen vacancy (NV) centers in diamond. The quadratic and cubic dependence of the integrated fluorescence intensity as a function of excitation power indicates a two-photon excitation pathway for the NV- charge state and a three-photon process involved for the neutral NV0 charge state, respectively. Comparing the total multiphoton energy with its single-photon equivalent, the PLE spectra follows the absorption spectrum of single photon excitation. We also observed that the efficiency of photoluminescence for different charge states, as well as the decay time constant, was dependent on the excitation wavelength and power.

Two-photon high-resolution measurement of partial pressure of oxygen in cerebral vasculature and tissue.

PubMed

Sakadzić, Sava; Roussakis, Emmanuel; Yaseen, Mohammad A; Mandeville, Emiri T; Srinivasan, Vivek J; Arai, Ken; Ruvinskaya, Svetlana; Devor, Anna; Lo, Eng H; Vinogradov, Sergei A; Boas, David A

2010-09-01

Measurements of oxygen partial pressure (pO(2)) with high temporal and spatial resolution in three dimensions is crucial for understanding oxygen delivery and consumption in normal and diseased brain. Among existing pO(2) measurement methods, phosphorescence quenching is optimally suited for the task. However, previous attempts to couple phosphorescence with two-photon laser scanning microscopy have faced substantial difficulties because of extremely low two-photon absorption cross-sections of conventional phosphorescent probes. Here we report to our knowledge the first practical in vivo two-photon high-resolution pO(2) measurements in small rodents' cortical microvasculature and tissue, made possible by combining an optimized imaging system with a two-photon-enhanced phosphorescent nanoprobe. The method features a measurement depth of up to 250 microm, sub-second temporal resolution and requires low probe concentration. The properties of the probe allowed for direct high-resolution measurement of cortical extravascular (tissue) pO(2), opening many possibilities for functional metabolic brain studies.

Room temperature three-photon pumped CH3NH3PbBr3 perovskite microlasers.

PubMed

Gao, Yisheng; Wang, Shuai; Huang, Can; Yi, Ningbo; Wang, Kaiyang; Xiao, Shumin; Song, Qinghai

2017-03-28

Hybrid lead halide perovskites have made great strides in next-generation light-harvesting and light emitting devices. Recently, they have also shown great potentials in nonlinear optical materials. Two-photon absorption and two-photon light emission have been thoroughly studied in past two years. However, the three-photon processes are rarely explored, especially for the laser emissions. Here we synthesized high quality CH 3 NH 3 PbBr 3 perovskite microstructures with solution processed precipitation method and studied their optical properties. When the microstructures are pumped with intense 1240 nm lasers, we have observed clear optical limit effect and the band-to-band photoluminescence at 540 nm. By increasing the pumping density, whispering-gallery-mode based microlasers have been achieved from CH 3 NH 3 PbBr 3 perovskite microplate and microrod for the first time. This work demonstrates the potentials of hybrid lead halide perovskites in nonlinear photonic devices.

Room temperature three-photon pumped CH3NH3PbBr3 perovskite microlasers

NASA Astrophysics Data System (ADS)

Gao, Yisheng; Wang, Shuai; Huang, Can; Yi, Ningbo; Wang, Kaiyang; Xiao, Shumin; Song, Qinghai

2017-03-01

Hybrid lead halide perovskites have made great strides in next-generation light-harvesting and light emitting devices. Recently, they have also shown great potentials in nonlinear optical materials. Two-photon absorption and two-photon light emission have been thoroughly studied in past two years. However, the three-photon processes are rarely explored, especially for the laser emissions. Here we synthesized high quality CH3NH3PbBr3 perovskite microstructures with solution processed precipitation method and studied their optical properties. When the microstructures are pumped with intense 1240 nm lasers, we have observed clear optical limit effect and the band-to-band photoluminescence at 540 nm. By increasing the pumping density, whispering-gallery-mode based microlasers have been achieved from CH3NH3PbBr3 perovskite microplate and microrod for the first time. This work demonstrates the potentials of hybrid lead halide perovskites in nonlinear photonic devices.

Rapid creation of distant entanglement by multi-photon resonant fluorescence

NASA Astrophysics Data System (ADS)

Cohen, Guy Z.; Sham, L. J.

2014-03-01

We study a simple, effective and robust method for entangling two separate stationary quantum dot spin qubits with high fidelity using multi-photon Gaussian state. The fluorescence signals from the two dots interfere at a beam splitter. The bosonic nature of photons leads, in analogy with the Hong-Ou-Mandel (HOM) effect, to selective pairing of photon holes (photon absences in the fluorescent signals). By the HOM effect, two photon holes with the same polarization end up at the same beam splitter output. As a result, two odd photon number detections at the outgoing beams, which must correspond to two photon holes with different polarizations, herald entanglement creation. The robustness of the Gaussian states is evidenced by the ability to compensate for photon absorption and noise by a moderate increase in the number of photons at the input. We calculate the entanglement generation rate in the ideal, non-ideal and near-ideal detector regimes and find substantial improvement over single-photon schemes in all three regimes. Fast and efficient spin-spin entanglement creation can form the basis for a scalable quantum dot quantum computing network. Our predictions can be tested using current experimental capabilities. This research was supported by the U.S. Army Research Office MURI award W911NF0910406, by NSF grant PHY-1104446 and by ARO (IARPA, W911NF-08-1-0487). The authors thank D. G. Steel for useful discussions.

Rise time of voltage pulses in NbN superconducting single photon detectors

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

Smirnov, K. V.; CJSC “Superconducting Nanotechnology”; National Research University Higher School of Economics, Moscow Institute of Electronics and Mathematics, 34 Tallinskaya St., 109028 Moscow

2016-08-01

We have found experimentally that the rise time of voltage pulse in NbN superconducting single photon detectors increases nonlinearly with increasing the length of the detector L. The effect is connected with dependence of resistance of the detector R{sub n}, which appears after photon absorption, on its kinetic inductance L{sub k} and, hence, on the length of the detector. This conclusion is confirmed by our calculations in the framework of two temperature model.

Laser modified processes: bremsstrahlung and inelastic photon atom scattering

NASA Astrophysics Data System (ADS)

Budriga, Olimpia; Dondera, Mihai; Florescu, Viorica

2007-08-01

We consider the influence of a low-frequency monochromatic external electromagnetic field (the laser) on two basic atomic processes: electron Coulomb bremsstrahlung and inelastic photon scattering on an electron bound in the ground state of a hydrogenic atom. We briefly describe the approximations adopted and illustrate in figures how the laser parameters modify the shape of the differential cross-sections and extend the energy domain for emitted electrons, due to simultaneous absorption or emission of a large number (hundreds) of laser photons.

High-speed low-power photonic transistor devices based on optically-controlled gain or absorption to affect optical interference.

PubMed

Huang, Yingyan; Ho, Seng-Tiong

2008-10-13

We show that a photonic transistor device can be realized via the manipulation of optical interference by optically controlled gain or absorption in novel ways, resulting in efficient transistor signal gain and switching action. Exemplary devices illustrate two complementary device types with high operating speed, microm size, microW switching power, and switching gain. They can act in tandem to provide a wide variety of operations including wavelength conversion, pulse regeneration, and logical operations. These devices could have a Transistor Figure-of-Merits >10(5) times higher than current chi((3)) approaches and are highly attractive.

Symmetry Breaking in Platinum Acetylide Chromophores Studied by Femtosecond Two-Photon Absorption Spectroscopy

DTIC Science & Technology

2014-02-01

hand, studies per- formed in conjugated dendrimers have pointed out the impor- tance of conformational changes that may strongly influence the 2PA...Absorption in Dendrimers . J. Phys. Chem. B 2003, 107, 7540−7543. (37) Leng, W.; Bazan, G. C.; Kelley, A. M. Solvent Effects on Resonance Raman and Hyper

Protection layers on a superconducting microwave resonator toward a hybrid quantum system

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

Lee, Jongmin, E-mail: jongmin.lee@sandia.gov; Sandia National Laboratories, Albuquerque, New Mexico 87123; Park, Dong Hun, E-mail: leomac@umd.edu

2015-10-07

We propose a protection scheme of a superconducting microwave resonator to realize a hybrid quantum system, where cold neutral atoms are coupled with a single microwave photon through magnetic dipole interaction at an interface inductor. The evanescent field atom trap, such as a waveguide/nanofiber atom trap, brings both surface-scattered photons and absorption-induced broadband blackbody radiation which result in quasiparticles and a low quality factor at the resonator. A proposed multiband protection layer consists of pairs of two dielectric layers and a thin nanogrid conductive dielectric layer above the interface inductor. We show numerical simulations of quality factors and reflection/absorption spectra,more » indicating that the proposed multilayer structure can protect a lumped-element microwave resonator from optical photons and blackbody radiation while maintaining a reasonably high quality factor.« less

Anisotropic Electron-Photon and Electron-Phonon Interactions in Black Phosphorus

DOE PAGES

Ling, Xi; Huang, Shengxi; Hasdeo, Eddwi; ...

2016-03-10

Orthorhombic black phosphorus (BP) and other layered materials, such as gallium telluride (GaTe) and tin selenide (SnSe), stand out among two-dimensional (2D) materials owing to their anisotropic in-plane structure. This anisotropy adds a new dimension to the properties of 2D materials and stimulates the development of angle-resolved photonics and electronics. However, understanding the effect of anisotropy has remained unsatisfactory to-date, as shown by a number of inconsistencies in the recent literatures. We use angle-resolved absorption and Raman spectroscopies to investigate the role of anisotropy on the electron-photon and electron-phonon interactions in BP. We highlight a non-trivial dependence between anisotropies andmore » flake thickness, photon and phonon energies. We show that once understood, the anisotropic optical absorption appears to be a reliable and simple way to identify the crystalline orientation of BP, which cannot be determined from Raman spectroscopy without the explicit consideration of excitation wavelength and flake thickness, as commonly used previously.« less

Integrated three-dimensional photonic nanostructures for achieving near-unity solar absorption and superhydrophobicity

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

Kuang, Ping; Lin, Shawn-Yu, E-mail: sylin@rpi.edu; Hsieh, Mei-Li

2015-06-07

In this paper, we proposed and realized 3D photonic nanostructures consisting of ultra-thin graded index antireflective coatings (ARCs) and woodpile photonic crystals. The use of the integrated ARC and photonic crystal structure can achieve broadband, broad-angle near unity solar absorption. The amorphous silicon based photonic nanostructure experimentally shows an average absorption of ∼95% for λ = 400–620 nm over a wide angular acceptance of θ = 0°–60°. Theoretical studies show that a Gallium Arsenide (GaAs) based structure can achieve an average absorption of >95% for λ = 400–870 nm. Furthermore, the use of the slanted SiO{sub 2} nanorod ARC surface layer by glancing angle deposition exhibits Cassie-Baxter statemore » wetting, and superhydrophobic surface is obtained with highest water contact angle θ{sub CB} ∼ 153°. These properties are fundamentally important for achieving maximum solar absorption and surface self-cleaning in thin film solar cell applications.« less

Two-photon absorption laser-induced fluorescence of atomic oxygen in the afterglow of pulsed positive corona discharge

NASA Astrophysics Data System (ADS)

Ono, Ryo; Takezawa, Kei; Oda, Tetsuji

2009-08-01

Atomic oxygen is measured in the afterglow of pulsed positive corona discharge using time-resolved two-photon absorption laser-induced fluorescence. The discharge occurs in a 14 mm point-to-plane gap in dry air. After the discharge pulse, the atomic oxygen density decreases at a rate of 5×104 s-1. Simultaneously, ozone density increases at almost the same rate, where the ozone density is measured using laser absorption method. This agreement between the increasing rate of atomic oxygen and decreasing rate of ozone proves that ozone is mainly produced by the well-known three-body reaction, O+O2+M→O3+M. No other process for ozone production such as O2(v)+O2→O3+O is observed. The spatial distribution of atomic oxygen density is in agreement with that of the secondary streamer luminous intensity. This agreement indicates that atomic oxygen is mainly produced in the secondary streamer channels, not in the primary streamer channels.

Second harmonic generation in photonic crystal cavities in (111)-oriented GaAs

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

Buckley, Sonia, E-mail: bucklesm@stanford.edu; Radulaski, Marina; Vučković, Jelena

2013-11-18

We demonstrate second harmonic generation at telecommunications wavelengths in photonic crystal cavities in (111)-oriented GaAs. We fabricate 30 photonic crystal structures in both (111)- and (100)-oriented GaAs and observe an increase in generated second harmonic power in the (111) orientation, with the mean power increased by a factor of 3, although there is a large scatter in the measured values. We discuss possible reasons for this increase, in particular, the reduced two photon absorption for transverse electric modes in (111) orientation, as well as a potential increase due to improved mode overlap.

Structuring β-Ga2O3 photonic crystal photocatalyst for efficient degradation of organic pollutants.

PubMed

Li, Xiaofang; Zhen, Xiuzheng; Meng, Sugang; Xian, Jiangjun; Shao, Yu; Fu, Xianzhi; Li, Danzhen

2013-09-03

Coupling photocatalysts with photonic crystals structure is based on the unique property of photonic crystals in confining, controlling, and manipulating the incident photons. This combination enhances the light absorption in photocatalysts and thus greatly improves their photocatalytic performance. In this study, Ga2O3 photonic crystals with well-arranged skeleton structures were prepared via a dip-coating infiltration method. The positions of the electronic band absorption for Ga2O3 photonic crystals could be made to locate on the red edge, on the blue edge, and away from the edge of their photonic band gaps by changing the pore sizes of the samples, respectively. Particularly, the electronic band absorption of the Ga2O3 photonic crystal with a pore size of 135 nm was enhanced more than other samples by making it locate on the red edge of its photonic band gap, which was confirmed by the higher instantaneous photocurrent and photocatalytic activity for the degradation of various organic pollutants under ultraviolet light irradiation. Furthermore, the degradation mechanism over Ga2O3 photonic crystals was discussed. The design of Ga2O3 photonic crystals presents a prospective application of photonic crystals in photocatalysis to address light harvesting and quantum efficiency problems through manipulating photons or constructing photonic crystal structure as groundwork.

Two-photon absorption in conjugated energetic molecule

DOE PAGES

Bjorgaard, Josiah August; Sifain, Andrew; Nelson, Tammie Renee; ...

2016-06-03

Time-dependent density functional theory (TD-DFT) is used to investigate the relationship between molecular structure and one- and two-photon absorption (OPA and TPA, respectively) properties in novel and recently synthesized conjugated energetic molecules (CEMs). The molecular structure of CEMs can be strategically altered to influence the heat of formation and oxygen balance, two factors that can contribute to the sensitivity and strength of an explosive material. OPA and TPA are sensitive to changes in molecular structure as well, influencing optical range of excitation. We find calculated vertical excitation energies in good agreement with experiment for most molecules. Peak TPA intensities aremore » significant and on the order of 102 GM. Natural transition orbitals for essential electronic states defining TPA peaks of relatively large intensity to examine the character of relevant transitions. Minor modification of molecular substituents, such as additional oxygen and other functional groups, produces significant changes in electronic structure, OPA, TPA, and improves the oxygen balance. Results show that select molecules are apt to nonlinear absorption, opening the possibility for controlled, direct optical initiation of CEMs through photochemical pathways.« less

Optical continuum generation on a silicon chip

NASA Astrophysics Data System (ADS)

Jalali, Bahram; Boyraz, Ozdal; Koonath, Prakash; Raghunathan, Varun; Indukuri, Tejaswi; Dimitropoulos, Dimitri

2005-08-01

Although the Raman effect is nearly two orders of magnitude stronger than the electronic Kerr nonlinearity in silicon, under pulsed operation regime where the pulse width is shorter than the phonon response time, Raman effect is suppressed and Kerr nonlinearity dominates. Continuum generation, made possible by the non-resonant Kerr nonlinearity, offers a technologically and economically appealing path to WDM communication at the inter-chip or intra-chip levels. We have studied this phenomenon experimentally and theoretically. Experimentally, a 2 fold spectral broadening is obtained by launching ~4ps optical pulses with 2.2GW/cm2 peak power into a conventional silicon waveguide. Theoretical calculations, that include the effect of two-photon-absorption, free carrier absorption and refractive index change indicate that up to >30 times spectral broadening is achievable in an optimized device. The broadening is due to self phase modulation and saturates due to two photon absorption. Additionally, we find that free carrier dynamics also contributes to the spectral broadening and cause the overall spectrum to be asymmetric with respect to the pump wavelength.

Arduino Due based tool to facilitate in vivo two-photon excitation microscopy

PubMed Central

Artoni, Pietro; Landi, Silvia; Sato, Sebastian Sulis; Luin, Stefano; Ratto, Gian Michele

2016-01-01

Two-photon excitation spectroscopy is a powerful technique for the characterization of the optical properties of genetically encoded and synthetic fluorescent molecules. Excitation spectroscopy requires tuning the wavelength of the Ti:sapphire laser while carefully monitoring the delivered power. To assist laser tuning and the control of delivered power, we developed an Arduino Due based tool for the automatic acquisition of high quality spectra. This tool is portable, fast, affordable and precise. It allowed studying the impact of scattering and of blood absorption on two-photon excitation light. In this way, we determined the wavelength-dependent deformation of excitation spectra occurring in deep tissues in vivo. PMID:27446677

Two-photon excitation of nitric oxide fluorescence as a temperature indicator in unsteady gas-dynamic processes

NASA Technical Reports Server (NTRS)

Mckenzie, R. L.; Gross, K. P.

1980-01-01

A laser induced fluorescence technique, suitable for measuring fluctuating temperatures in cold turbulent flows containing very low concentrations of nitric oxide is described. Temperatures below 300 K may be resolved with signal to noise ratios greater than 50 to 1 using high peak power, tunable dye lasers. The method relies on the two photon excitation of selected ro-vibronic transitions. The analysis includes the effects of fluorescence quenching and shows the technique to be effective at all densities below ambient. Signal to noise ratio estimates are based on a preliminary measurement of the two photon absorptivity for a selected rotational transition in the NO gamma (0,0) band.

One- and two-photon absorption spectra of the yellow fluorescent protein citrine: effects of intramolecular electron-vibrational coupling and intermolecular interactions

NASA Astrophysics Data System (ADS)

Chen, Fasheng; Zhao, Xinyi; Liang, WanZhen

2018-04-01

Both the vibrationally resolved and statistically averaged one-photon absorption (OPA) and two-photon absorption (TPA) spectra of the anionic form of chromophore (AC) in its micro-environment of yellow fluorescent protein (YFP) Citrine have been calculated. The result comparison has been made with those of the AC model compounds in vacuo and methanol solution, which allows us to allocate the individual contribution of the intramolecular electron-vibrational coupling, the electrostatic π-stacking interaction between Tyr203 and AC, and the interaction between AC and its micro-environment to the spectra. The results reveal that the non-Condon vibronic coupling effect is responsible for the blue shift of TPA absorption maximum compared with its OPA counterpart corresponding to S0 → S1, and that the π-stacking interaction between Tyr203 and AC alters the relative intensities of TPA maxima, which further enhances the higher-energy vibronic peaks and weakens the lowest-energy peak. The statically averaged OPA and TPA spectra calculated by quantum mechanics/molecular mechanics (QM/MM) methods based on Born-Oppenheimer molecular dynamics simulation largely deviate the experimental spectral lineshapes, which further verifies the significant contribution of non-Condon vibronic coupling effect on the spectra. The interaction of individual amino acid residue or water close to AC+Tyr203 has different effects on the spectra, which may increase/decrease the excitation energy depending on its position and electronic property.

Two-Photon Absorption Based Nanoscopic Velocimeter

NASA Astrophysics Data System (ADS)

Wang, Audrey; Abdalrahman, Akrm; Deng, Jianyu; Wang, Guiren

2017-11-01

Most velocimeters in micro/nanofluidics rely on particles as flow tracers, such as micro Particle Image Velocimetry (μPIV). However, for many microflows, such as electrokinetic and near wall flow, magnetophoresis, acoustophoresis, photophoresis and thermophoresis, particles have different velocity from their surrounding fluids. Although most molecular tracer based velocimeters can use neutral dye to measure average velocity, their temporal and spatial resolution are limited. Stimulated emission depletion (STED) based laser-induced fluorescence photobleaching anemometer (LIFPA), i.e. STED-LIFPA has achieved 70 nm spatial resolution. However, STED nanoscopy is very complicated for most users. Here we developed a two-photon absorption LIFPA (TP-LIFPA), which is relatively easier to operate. TP-LIFPA can take advantage of the two-photon microscopy to increase spatial resolution. We use a femtolaser to excite a dye. A microcapillary tube is used to test the feasibility of TP-LIFPA. TP-LIFPA can successfully measure the velocity profile in the capillary. The resolution of TP-LIFPA is estimated to be about 90 nm. The work indicates TP-LIFPA is a new promising nanoscopic velocimeter for interfacial flows, especially within 100 nm at the interfacial area between two phases in the future. The work was supported by NSF under Grant No. MRI CBET-1040227.

Broadband ultrafast nonlinear absorption and ultra-long exciton relaxation time of black phosphorus quantum dots.

PubMed

Chen, Runze; Zheng, Xin; Jiang, Tian

2017-04-03

Black phosphorus (BP) has recently attracted significant attention for its brilliant physical and chemical features. The remarkable strong light-matter interaction and tunable direct wide range band-gap make it an ideal candidate in various application regions, especially saturable absorbers. In this paper, ultrasmall black phosphorus quantum dots (BPQDs), a unique form of phosphorus nanostructures, with average size of 5.7 ± 0.8 nm are synthesized. Compared with BP nanosheets (BPNs) with similar thickness, the ultrafast nonlinear optical (NLO) absorption properties and excited carrier dynamics are investigated in wide spectra. Beyond the saturation absorption (SA), giant two photon absorption (TPA) is observed in BPQDs. BPQDs exhibit quite different excitation intensity and wavelength dependent nonlinear optical (NLO) response from BPNs, which is attributed to the quantum confinement and edge effects. The BPQDs show broadband photon-induced absorption (PIA) under the probe wavelength from 470 nm to 850 nm and a fast and a slow decay time are obtained as long as 92 ± 10 ps and 1100 ± 100 ps, respectively. The substantial independence for ultra-long time scales of pump intensity and temperature reveals that the carrier recombination mechanism may be attributed to a defect-assisted Auger capture process. These findings will help to develop optoelectronic and photonic devices operating in the infrared and visible wavelength region.

Two-photon absorption in diazobenzene compounds

NASA Astrophysics Data System (ADS)

Andrade, A. A.; Yamaki, S. B.; Misoguti, L.; Zilio, S. C.; Atvars, Teresa D. Z.; Oliveira, O. N.; Mendonça, C. R.

2004-12-01

An investigation is made into molecular design strategies to enhance the two-photon absorption (2PA) of organic materials by measuring the 2PA cross-section of diazoaromatic compounds with the femtosecond pulses Z-scan technique at 775 nm. These diazo dyes exhibit a moderate 2PA cross-section, of the order of 300 GM, comparable to those of regular azoaromatic compounds. The increase in the π-electron bridge in the diazoaromatic compounds does not bring, therefore, substantial increase to the measured 2PA intensities, while the main factor to enhance the 2PA cross-section is the presence of charge donor and acceptor groups. It is concluded that current molecular design strategies are unlikely to produce azoaromatic compounds that are useful for applications requiring very high 2PA coefficients.

3He(γ,pp)n cross sections with tagged photons below the Δ resonance energy

NASA Astrophysics Data System (ADS)

Kolb, N. R.; Feldman, G.; O'rielly, G. V.; Pywell, R. E.; Skopik, D. M.; Hackett, E. D.; Quraan, M. A.; Rodning, N. L.

1996-11-01

Cross sections have been measured for the 3He(γ,pp)n reaction with tagged photons in the range Eγ =161-208 MeV using the Saskatchewan-Alberta Large Acceptance Detector (SALAD). The protons were detected over a range of polar angles of 40°-140° and azimuthal angles of 0°-360° with an energy threshold of 40 MeV. Comparisons are made with a microscopic calculation which includes one-, two-, and three-nucleon absorption mechanisms. One- and two-nucleon processes, including final-state interactions, are unable to account for the measured cross sections. The addition of three-nucleon absorption diagrams gives roughly the right strength, but the distribution in phase space is in disagreement with the data.

Effects of two-photon absorption on all optical logic operation based on quantum-dot semiconductor optical amplifiers

NASA Astrophysics Data System (ADS)

Zhang, Xiang; Dutta, Niloy K.

2018-01-01

We investigate all-optical logic operation in quantum-dot semiconductor optical amplifier (QD-SOA) based Mach-Zehnder interferometer considering the effects of two-photon absorption (TPA). TPA occurs during the propagation of sub-picosecond pulses in QD-SOA, which leads to a change in carrier recovery dynamics in quantum-dots. We utilize a rate equation model to take into account carrier refill through TPA and nonlinear dynamics including carrier heating and spectral hole burning in the QD-SOA. The simulation results show the TPA-induced pumping in the QD-SOA can reduce the pattern effect and increase the output quality of the all-optical logic operation. With TPA, this scheme is suitable for high-speed Boolean logic operation at 320 Gb/s.

Extended X-ray Absorption Fine Structure Study of Bond Constraints in Ge-Sb-Te Alloys

DTIC Science & Technology

2011-02-07

Ray Absorption Spectroscopy, or EXAFS. Using the spectroscopic capabilities provided by the MCAT line at the Advanced Photon Source at Argonne...Absorption Spectroscopy, or EXAFS. Using the spectroscopic capabilities provided by the MCAT line at the Advanced Photon Source at Argonne National

Amplification of effects of photons on wound healing

NASA Astrophysics Data System (ADS)

Dyson, Mary

2009-02-01

Following the absorption of photons by cells either resident in or in transit through the skin at and around a wound site, healing can be modulated. This is due to the primary, secondary and tertiary cellular effects of the photons. The main primary effect of phototherapy is photon absorption. This initiates secondary effects within the cells that have absorbed the photons. Secondary effects are restricted to cells that have absorbed a suprathreshold quantity of photonic energy. Photon absorption can lead to an increase in ATP synthesis and the release of reactive oxygen species that can activate specific transcription factors resulting in changes in synthesis of the enzymes needed for cellular proliferation, migration, phagocytosis and protein synthesis, all essential for wound healing. The amount of ATP production is limited in each cell by the availability of ADP and phosphate. Spatial and temporal amplification of the effects of photon absorption increases the range and duration of phototherapy. It may be caused in part by tertiary effects initiated in cells that have not absorbed photons by regulatory proteins such as cytokines secreted by cells that have absorbed photons. Amplification may also be due to changes induced by photons in immune cells, stem cells and soluble protein mediators while in transit through the dermal capillaries. The peripheral location of these capillaries makes their contents readily accessible to photons. The longer the duration of treatment, the greater will be the number of cells in transit that can be affected by photons. Depth of effect may be increased by transduction of electromagnetic energy into mechanical energy. For a treatment to be clinically effective on wound healing, its duration and power may each be important. Components of the immune system, endocrine system and nervous system may also amplify the effects of photons on wound healing.

Theoretical Design of a Two-Photon Fluorescent Probe for Nitric Oxide with Enhanced Emission Induced by Photoninduced Electron Transfer.

PubMed

Zhang, Yujin; Leng, Jiancai; Hu, Wei

2018-04-25

In the present work, we systematically investigate the sensing abilities of two recently literature-reported two-photon fluorescent NO probes, i.e., the o-phenylenediamine derivative of Nile Red and the p-phenylenediamine derivative of coumarin. The recognition mechanisms of these probes are studied by using the molecular orbital classifying method, which demonstrates the photoinduced electron transfer process. In addition, we have designed two new probes by swapping receptor units present on fluorophores, i.e., the p-phenylenediamine derivative of Nile Red and the o-phenylenediamine derivative of coumarin. However, it illustrates that only the latter has ability to function as off-on typed fluorescent probe for NO. More importantly, calculations on the two-photon absorption properties of the probes demonstrate that both receptor derivatives of coumarin possess larger TPA cross-sections than Nile Red derivatives, which makes a better two photon fluorescent probe. Our theoretical investigations reveal that the underlying mechanism satisfactorily explain the experimental results, providing a theoretical basis on the structure-property relationships which is beneficial to developing new two-photon fluorescent probes for NO.

Bright and dark singlet excitons via linear and two-photon spectroscopy in monolayer transition metal dichalcogenides

DOE PAGES

Berkelbach, Timothy C.; Hybertsen, Mark S.; Reichmann, David R.

2015-08-10

We discuss the linear and two-photon spectroscopic selection rules for spin-singlet excitons in monolayer transition-metal dichalcogenides. Our microscopic formalism combines a fully k-dependent few-orbital band structure with a many-body Bethe-Salpeter equation treatment of the electron-hole interaction, using a model dielectric function. We show analytically and numerically that the single-particle, valley-dependent selection rules are preserved in the presence of excitonic effects. Furthermore, we definitively demonstrate that the bright (one-photon allowed) excitons have s-type azimuthal symmetry and that dark p-type excitons can be probed via two-photon spectroscopy. Thus, the screened Coulomb interaction in these materials substantially deviates from the 1/ε₀r form; thismore » breaks the “accidental” angular momentum degeneracy in the exciton spectrum, such that the 2p exciton has a lower energy than the 2s exciton by at least 50 meV. We compare our calculated two-photon absorption spectra to recent experimental measurements.« less

Dopant-Engineered Wide-Band Gap Semiconductors for Deep Tissue Bioimaging

NASA Astrophysics Data System (ADS)

Raghavendra, Achyut; Gregory, Wren; Slonecki, Tyler; Bruce, Terri; Podila, Ramakrishna

Optical spectroscopy promises improved lateral resolution for in vivo imaging but is limited by background fluorescence and photon attenuation. There is clearly an unmet clinical need for new hybrid approaches that use fluorescence to identify cancer margins intraoperatively during the initial operation. An efficient strategy to increase the imaging depth and diagnostic capability, beyond what two-photon absorption (2PA) offers, is to use longer excitation wavelengths outside the water absorption window through three-photon absorption (3PA). Although a variety of existing fluorescent dyes, fluorescent proteins, and calcium indicators could be used in 3PA, they have low or moderate 3PA cross-sections and suffer from photobleaching. The non-linear 3PA coefficient of such fluorescent probes is often low necessitating high excitation powers, which could cause overheating, photodamage, and photo-induced toxicity. To address this demand we have designed dopant-engineered ZnO nanoparticles (d-ZnO NPs) for enabling 3PA with higher penetration depth, lower background noise, and improved spatial resolution (<1 um) at powers below 5 mW.

Analysis of high-efficiency widely-tunable N-resonances in Cs vapor

NASA Astrophysics Data System (ADS)

Krasteva, A.; Gateva, S.; Tzvetkov, S.; Ghosh, P. N.; Sargsyan, A.; Cartaleva, S.

2018-03-01

The narrow-band coherent N-type resonance, promising for the development of advanced atomic clocks, can be considered as a type of three-photon resonance, where a two-photon Raman excitation is combined with a resonant optical pumping field. In this communication, we present an experimental study and a theoretical analysis related to three-photon, bi-chromatic excitation of Cs atomic vapor contained in an 8-mm long cell with 20 Torr of neon. If a coupling laser is fixed at a frequency that is lower by several GHz than the position of the absorption profile of the Fg = 4 set of transitions, and a probe laser is tuned over the D2 line (λ = 852 nm), a narrow high-contrast enhanced absorption N-resonance will be observed in the probe light profile, superimposed on the absorption profile of the Fg = 4 set of transitions. We present theoretical modeling aimed to clarify the processes behind the efficiency of the N-resonance preparation for different frequency positions of the coupling laser within the D2 line of Cs.

Distribution of photon absorption rates across the rat retina.

PubMed

Williams, T P; Webbers, J P; Giordano, L; Henderson, R P

1998-04-15

1. An investigation into the distribution of light intensity across the rat retina was carried out on excised, intact rat eyes exposed to Ganzfeld illumination from a helium-neon laser (543 nm). 2. Some of the light entering the eyes exits through the sclera where its intensity can be monitored with an optical 'pick-up' that samples the intensity coming from a small region of external sclera and underlying retina. The spatial resolution of the pick-up is such that it samples light that has passed through ca 2 % of the rods in the rat eye. 3. Some of the laser light is absorbed by the rod pigment, rhodopsin, which gradually bleaches. Bleaching in the retina, in turn, causes an exponential increase in intensity emanating from the sclera. By monitoring this intensity increase, we are able to measure two important parameters in a single bleaching run: the local rhodopsin concentration and the local intensity falling on the rods. 4. With an ocular transmission photometer, we have measured both the local intensity and the local rhodopsin concentration across wide regions of rat retina. Both pigmented and albino rats were studied. 5. The distributions of rhodopsin and intensity were both nearly uniform; consequently, the product, (rhodopsin concentration) x (intensity), was similarly nearly equal across the retina. This means that the initial rate of photon absorption is about the same at all retinal locations. 6. Interpreted in terms of photostasis (the regulation of daily photon catch), this means that the rate of photon absorption is about the same in each rod, viz. 14 400 photons absorbed per rod per second. Since this rate of absorption is sufficient to saturate the rod, one possible purpose of photostasis is to maintain the rod system in a saturated state during daylight hours.

Antimicrobial Amino-Functionalized Nitrogen-Doped Graphene Quantum Dots for Eliminating Multidrug-Resistant Species in Dual-Modality Photodynamic Therapy and Bioimaging under Two-Photon Excitation.

PubMed

Kuo, Wen-Shuo; Shao, Yu-Ting; Huang, Keng-Shiang; Chou, Ting-Mao; Yang, Chih-Hui

2018-05-02

Developing a nanomaterial, for use in highly efficient dual-modality two-photon photodynamic therapy (PDT) involving reactive oxygen species (ROS) generation and for use as a two-photon imaging contrast probe, is currently desirable. Here, graphene quantum dots (GQDs) doped with nitrogen and functionalized with an amino group (amino-N-GQDs) serving as a photosensitizer in PDT had the superior ability to generate ROS as compared to unmodified GQDs. Multidrug-resistant (MDR) species were completely eliminated at an ultralow energy (239.36 nJ pixel -1 ) through only 12 s two-photon excitation (TPE) in the near-infrared region (800 nm). Furthermore, the amino-N-GQDs had an absorption wavelength of approximately 800 nm, quantum yield of 0.33, strong luminescence, an absolute cross section of approximately 54 356 Göeppert-Mayer units, a lifetime of 1.09 ns, a ratio of the radiative to nonradiative decay rates of approximately 0.49, and high two-photon stability under TPE. These favorable properties enabled the amino-N-GQDs to act as a two-photon contrast probe for tracking and localizing analytes through in-depth two-photon imaging in a three-dimensional biological environment and concurrently easily eliminating MDR species through PDT.

Atmospheric methane measurement instrument using a Zeeman-split He-Ne laser

NASA Technical Reports Server (NTRS)

Mcmanus, J. Barry; Kebabian, Paul L.; Kolb, Charles E.

1989-01-01

The construction of an atmospheric methane measurement instrument based on a Zeeman-split IR He-Ne laser is reported. The laser has a tranverse magnetic field over about 2/3 of its gain length and can oscillate at an (unsplit) frequency (2947.91/cm) centered on a methane absorption line, or on either of two frequencies split by + or - 0.055/cm from the center, with low CH4 absorption. The laser is tuned to dwell sequentially at each frequency, giving two differential absorption measurements in each 46-ms tuning cycle. Atmospheric measurements are made using two multiple pass absorption cells, one with fast (0.75-s) and one with slow (5-s) flow response times. Fluctuations in ambient CH4 of about 20-ppb (rms, 1-s averaging) are detected, with interference fringe effects the dominant noise source. The instrument has operated in a field experiment (NASA GTE/ABLE-3A) in Alaska.

Rapid creation of distant entanglement by multiphoton resonant fluorescence

NASA Astrophysics Data System (ADS)

Cohen, Guy Z.; Sham, L. J.

2013-12-01

We study a simple, effective, and robust method for entangling two separate stationary quantum dot spin qubits with high fidelity using multiphoton Gaussian state. The fluorescence signals from the two dots interfere at a beam splitter. The bosonic nature of photons leads, in analogy with the Hong-Ou-Mandel effect, to selective pairing of photon holes (photon absences in the fluorescent signals). As a result, two odd photon number detections at the outgoing beams herald trion entanglement creation, and subsequent reduction of the trions to the spin ground states leads to spin-spin entanglement. The robustness of the Gaussian states is evidenced by the ability to compensate for photon absorption and noise by a moderate increase in the number of photons at the input. We calculate the entanglement generation rate in the ideal, nonideal, and near-ideal detector regimes and find substantial improvement over single-photon schemes in all three regimes. Fast and efficient spin-spin entanglement creation can form the basis for a scalable quantum dot quantum computing network. Our predictions can be tested using current experimental capabilities.

New two-photon excitation chromophores for cellular imaging

NASA Astrophysics Data System (ADS)

D'Alfonso, Laura; Chirico, Giuseppe; Collini, Maddalena; Baldini, Giancarlo; Diaspro, Alberto; Ramoino, Paola; Abbotto, Alessandro; Beverina, Luca; Pagani, Giorgio A.

2003-10-01

The one photon and two photon excitation spectral properties (absorption, emission spectra, singlet lifetime) of a very efficient two photon absorber, dimethyl-pepep, have been measured in solution. The one photon excitation peak lye near 525 nm and the emission falls at 600 nm, where autofluorescence of cells is weak. The value of the singlet-triplet conversion rate, obtained by two-photon excitation fluorescence correlation spectroscopy, has a quadratic dependence on the excitation power and is comparable to that shown by the dye rhodamine. Preliminary results on stained cells from yeast Saccaromices cerevisiae and Paramecium primaurelia show that the dye preferentially stains DNA in the cell. A direct comparison with a DNA stainer, Dapi, is also performed. Some measurements of the dye functionalized to react with lysine and n-terminal residues of protein are presented. Moreover, this dye can be employed in order to follow in detail some cellular processes such as nuclei division. In vitro fluorescence titration of dimethyl-pepep with calf thymus DNA allowed to estimate the values of the dye-DNA association constant versus ionic strength, and an affinity close to that of ethidium bromide is found.

Secured Optical Communications Using Quantum Entangled Two-Photon Transparency Modulation

NASA Technical Reports Server (NTRS)

Nguyen, Quang-Viet (Inventor); Kojima, Jun (Inventor); Lekki, John (Inventor)

2015-01-01

A system and method is disclosed wherein optical signals are coded in a transmitter by tuning or modulating the interbeam delay time (which modulates the fourth-order coherence) between pairs of entangled photons. The photon pairs are either absorbed or not absorbed (transparent) by an atomic or molecular fluorescer in a receiver, depending on the inter-beam delay that is introduced in the entangled photon pairs. Upon the absorption, corresponding fluorescent optical emissions follow at a certain wavelength, which are then detected by a photon detector. The advantage of the disclosed system is that it eliminates a need of a coincidence counter to realize the entanglement-based secure optical communications because the absorber acts as a coincidence counter for entangled photon pairs.

Molecular specificity in photoacoustic microscopy by time-resolved transient absorption.

PubMed

Shelton, Ryan L; Mattison, Scott P; Applegate, Brian E

2014-06-01

We have recently harnessed transient absorption, a resonant two-photon process, for ultrahigh resolution photoacoustic microscopy, achieving nearly an order of magnitude improvement in axial resolution. The axial resolution is optically constrained due to the two-photon process unlike traditional photoacoustic microscopy where the axial resolution is inversely proportional to the frequency bandwidth of the detector. As a resonant process, the arrival time of the two photons need not be instantaneous. Systematically recording the signal as a function of the delay between two pulses will result in the measurement of an exponential decay whose time constant is related to the molecular dynamics. This time constant, analogous to the fluorescence lifetime, but encompassing nonradiative decay as well, can be used to differentiate between molecular systems with overlapping absorption spectra. This is frequently the situation for closely related yet distinct molecules such as redox pairs. In order to enable the measure of the exponential decay, we have reconfigured our transient absorption ultrasonic microscopy (TAUM) system to incorporate two laser sources with precisely controlled pulse trains. The system was tested by measuring Rhodamine 6G, an efficient laser dye where the molecular dynamics are dominated by the fluorescence pathway. As expected, the measured exponential time constant or ground state recovery time, 3.3±0.7  ns, was similar to the well-known fluorescence lifetime, 4.11±0.05  ns. Oxy- and deoxy-hemoglobin are the quintessential pair whose relative concentration is related to the local blood oxygen saturation. We have measured the ground state recovery times of these two species in fully oxygenated and deoxygenated bovine whole blood to be 3.7±0.8  ns and 7.9±1.0  ns, respectively. Hence, even very closely related pairs of molecules may be differentiated with this technique.

Stepwise photochromism of bisnaphthopyrans exhibiting an excitation intensity-dependent color change.

PubMed

Inagaki, Yuki; Mutoh, Katsuya; Abe, Jiro

2018-06-07

Non-linear photoresponses against excitation light intensity are important for the development of attractive photofunctional materials exhibiting high spatial selective photoswitching that is not affected by weak background light. Biphotochromic systems composed of two fast photochromic units have the potential to show a stepwise two-photon absorption process in which the optical properties can be non-linearly controlled by changing the excitation light conditions. Herein, we designed and synthesized novel bisnaphthopyran derivatives containing fast photoswitchable naphthopyran units. The bisnaphthopyran derivatives show a stepwise two-photon-induced photochromic reaction upon UV light irradiation accompanied by a drastic color change due to a large change in the molecular structure between the one-photon product and the two-photon product. Consequently, the color of the bisnaphthopyran derivatives can be non-linearly controlled by changing the excitation intensity. This characteristic photochromic property of the biphotochromic system provides important insight into advanced photoresponsive materials.

Laser photolysis of caged compounds at 405 nm: photochemical advantages, localisation, phototoxicity and methods for calibration.

PubMed

Trigo, Federico F; Corrie, John E T; Ogden, David

2009-05-30

Rapid, localised photolytic release of neurotransmitters from caged precursors at synaptic regions in the extracellular space is greatly hampered at irradiation wavelengths in the near-UV, close to the wavelength of maximum absorption of the caged precursor, because of inner-filtering by strong absorption of light in the cage solution between the objective and cell. For this reason two-photon excitation is commonly used for photolysis, particularly at multiple points distributed over large fields; or, with near-UV, if combined with local perfusion of the cage. These methods each have problems: the small cross-sections of common cages with two-photon excitation require high cage concentrations and light intensities near the phototoxic limit, while local perfusion gives non-uniform cage concentrations over the field of view. Single-photon photolysis at 405 nm, although less efficient than at 330-350 nm, with present cages is more efficient than two-photon photolysis. The reduced light absorption in the bulk cage solution permits efficient wide-field uncaging at non-toxic intensities with uniform cage concentration. Full photolysis of MNI-glutamate with 100 micros pulses required intensities of 2 mW microm(-2) at the preparation, shown to be non-toxic with repeated exposures. Light scattering at 405 nm was estimated as 50% at 18 microm depth in 21-day rat cerebellum. Methods are described for: (1) varying the laser spot size; (2) photolysis calibration in the microscope with the caged fluorophore NPE-HPTS over the wavelength range 347-405 nm; and (3) determining the point-spread function of excitation. Furthermore, DM-Nitrophen photolysis at 405 nm was efficient for intracellular investigations of Ca2+-dependent processes.

Ultrafast third-order nonlinear optical response of pyrene derivatives

NASA Astrophysics Data System (ADS)

Shi, Yufang; Li, Zhongguo; Fang, Yu; Sun, Jinyu; Zhao, Minggen; Song, Yinglin

2017-05-01

Two mono-substituted pyrene derivatives with delocalized electron system 1-(pyren-1-yl)-3-(4-Methyl thiophene-2-yl) acrylic ketone (13#) and 1-(pyren-1-yl)-3-(4-bromo thiophene-2-yl) acrylic ketone (15#) were successfully synthesized. The resultant compounds were characterized by nuclear magnetic resonance (NMR), infrared spectroscopy (IR), high resolution mass spectrum (HR-MS), and UV-vis spectra. The third-order nonlinear optical properties of the compounds were investigated using Z-scan technique with femtosecond laser pulses at 500 nm and 700 nm, respectively. Both of the compounds showed a decrease in transmittance about the focus, which are typical of two-photon absorption. It was found that the two-photon absorption behavior of the pyrene derivatives were modified by substituents on thiophene ring. These results indicate that both compounds can be promising candidates for future optoelectronic and bio-imaging applications.

Versatile Polymer Nanoparticles as Two-Photon-Triggered Photosensitizers for Simultaneous Cellular, Deep-Tissue Imaging, and Photodynamic Therapy.

PubMed

Guo, Liang; Ge, Jiechao; Liu, Qian; Jia, Qingyan; Zhang, Hongyan; Liu, Weimin; Niu, Guangle; Liu, Sha; Gong, Jianru; Hackbarth, Steffen; Wang, Pengfei

2017-06-01

Clinical applications of current photodynamic therapy (PDT) photosensitizers (PSs) are often limited by their absorption in the UV-vis range that possesses limited tissue penetration ability, leading to ineffective therapeutic response for deep-seated tumors. Alternatively, two-photon excited PS (TPE-PS) using NIR light triggered is one the most promising candidates for PDT improvement. Herein, multimodal polymer nanoparticles (PNPs) from polythiophene derivative as two-photon fluorescence imaging as well as two-photon-excited PDT agent are developed. The prepared PNPs exhibit excellent water dispersibility, high photostability and pH stability, strong fluorescence brightness, and low dark toxicity. More importantly, the PNPs also possess other outstanding features including: (1) the high 1 O 2 quantum yield; (2) the strong two-photon-induced fluorescence and efficient 1 O 2 generation; (3) the specific accumulation in lysosomes of HeLa cells; and (4) the imaging detection depth up to 2100 µm in the mock tissue under two-photon. The multifunctional PNPs are promising candidates as TPE-PDT agent for simultaneous cellular, deep-tissue imaging, and highly efficient in vivo PDT of cancer. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Progress in thin-film silicon solar cells based on photonic-crystal structures

NASA Astrophysics Data System (ADS)

Ishizaki, Kenji; De Zoysa, Menaka; Tanaka, Yoshinori; Jeon, Seung-Woo; Noda, Susumu

2018-06-01

We review the recent progress in thin-film silicon solar cells with photonic crystals, where absorption enhancement is achieved by using large-area resonant effects in photonic crystals. First, a definitive guideline for enhancing light absorption in a wide wavelength range (600–1100 nm) is introduced, showing that the formation of multiple band edges utilizing higher-order modes confined in the thickness direction and the introduction of photonic superlattice structures enable significant absorption enhancement, exceeding that observed for conventional random scatterers. Subsequently, experimental evidence of this enhancement is demonstrated for a variety of thin-film Si solar cells: ∼500-nm-thick ultrathin microcrystalline silicon cells, few-µm-thick microcrystalline silicon cells, and ∼20-µm-thick thin single-crystalline silicon cells. The high short-circuit current densities and/or efficiencies observed for each cell structure confirm the effectiveness of using multiple band-edge resonant modes of photonic crystals for enhancing broadband absorption in actual solar cells.

Nonlinear control of absorption in one-dimensional photonic crystal with graphene-based defect.

PubMed

Vincenti, M A; de Ceglia, D; Grande, M; D'Orazio, A; Scalora, M

2013-09-15

Perfect, narrow-band absorption is achieved in an asymmetric 1D photonic crystal with a monolayer graphene defect. Thanks to the large third-order nonlinearity of graphene and field localization in the defect layer we demonstrate the possibility to achieve controllable, saturable absorption for the pump frequency.

The impact of absorption coefficient on polarimetric determination of Berry phase based depth resolved characterization of biomedical scattering samples: a polarized Monte Carlo investigation

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

Baba, Justin S; Koju, Vijay; John, Dwayne O

2016-01-01

The modulation of the state of polarization of photons due to scatter generates associated geometric phase that is being investigated as a means for decreasing the degree of uncertainty in back-projecting the paths traversed by photons detected in backscattered geometry. In our previous work, we established that polarimetrically detected Berry phase correlates with the mean photon penetration depth of the backscattered photons collected for image formation. In this work, we report on the impact of state-of-linear-polarization (SOLP) filtering on both the magnitude and population distributions of image forming detected photons as a function of the absorption coefficient of the scatteringmore » sample. The results, based on Berry phase tracking implemented Polarized Monte Carlo Code, indicate that sample absorption plays a significant role in the mean depth attained by the image forming backscattered detected photons.« less

Ultrafast responses of two V-shaped compounds with a reverse conjugated structural configuration: an investigation of the reason for the enhanced two-photon absorption cross-section

NASA Astrophysics Data System (ADS)

Wang, Yaochuan; Jiang, Yihua; Liu, Dajun; Wang, Yizhuo; Wang, Guiqiu; Hua, Jianli

2018-06-01

To study the effect of the conjugated structural configuration on the two-photon absorption (TPA) properties of V-shaped compounds, two 1,3,5-triazine-based compounds with the same electron donor (D) and acceptor (A) connected in a reverse-conjugated structural configuration ( T02: D-π-A-π-D; R02: A-π-D-π-A) were systematically investigated using steady-state and transient absorption spectroscopy, open-aperture Z-scan measurements, and two-photon fluorescence measurements. The TPA cross-section of compound R02 connected in a A-π-D-π-A-conjugated structural configuration with triphenylamine as the central core was 203 GM, which showed a 2.3-fold enhancement compared with compound T02 connected in a reverse D-π-A-π-D-conjugated structural configuration (90 GM, with 1,3,5-triazine as the central core). This result indicates that the conjugated structural configuration plays an important role in the TPA properties. A two-color pump-probe experiment was used to investigate the effect of the conjugated structural configuration on the excited state and intra-molecular charge transfer (ICT) properties of these V-shaped compounds. The formation and relaxation lifetimes of the ICT state were determined. The results indicate that the electron-donating/accepting strength of the central group, which serves as a communal group for two D-π-A subunits, was confirmed to be a key role to the overall effect of the ICT for V-shaped compounds. These ultrafast dynamic results are in agreement with the TPA properties.

Effect of midgap defect states on the optical properties of Ge20Se70Te10 nano colloids

NASA Astrophysics Data System (ADS)

Cheruvalath, Ajina; Sebastian, Indu; Sebastian, Mathew; Nampoori, V. P. N.; Thomas, Sheenu

2017-10-01

In this work, we report the linear and nonlinear optical studies on a pseudo binary chalcogenide glass of composition Ge20 Se70 Te10 in its nano colloidal form. The possibility of tuning the band gap, nonlinear refractive index and nonlinear absorption of the material by changing the glass loading in the colloid has been revealed. A red shift in the band edge along with an intermediate peak in the band tail due to defect states is observed with increasing concentration. Photoluminescence studies confirm the existence of intermediate defect states in the bandgap. Nonlinear properties analyzed with open and closed aperture z scan technique reveal that the nonlinear refraction enhances due to resonant effects as the band gap of the colloid gets near the one photon absorption edge. The nonlinear absorption is prominent in the concentrated sample due to the presence of defect states which acts as an intermediate level in two step photon absorption.

Nonlinear refraction and two-photon absorption in dense 2Bi{sub 2}O{sub 3}-B{sub 2}O{sub 3} glasses

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

Paramesh, Gadige; Varma, K. B. R.

2012-06-05

High density transparent glasses (7.86 g/cc) were fabricated in the 2Bi{sub 2}O{sub 3}-B{sub 2}O{sub 3} (BBO) system. Optical band gap of the obtained glasses was found to be 2.6eV. The refractive index measured for these glasses was 2.25{+-}0.05 at {lambda}=543 nm. Nonlinear refraction and absorption studies were carried out on the BBO glasses using z-scan technique at {lambda}=532 nm of 10 ns pulse width. The nonlinear refractive index obtained was n{sub 2}=12.1x10{sup -14} cm{sup 2}/W and nonlinear absorption coefficient was {beta}=15.2 cm/GW. The n{sub 2} and {beta} values of the BBO glasses were large compared to the other reported highmore » index bismuth based oxide glass systems in the literature. These were attributed to the high density, high linear refractive index, low band gap and two photon absorption associated with these glasses. The electronic origin of large nonlinearities was discussed based on bond-orbital theory.« less

Hybrid Photon-Plasmon Coupling and Ultrafast Control of Nanoantennas on a Silicon Photonic Chip.

PubMed

Chen, Bigeng; Bruck, Roman; Traviss, Daniel; Khokhar, Ali Z; Reynolds, Scott; Thomson, David J; Mashanovich, Goran Z; Reed, Graham T; Muskens, Otto L

2018-01-10

Hybrid integration of nanoplasmonic devices with silicon photonic circuits holds promise for a range of applications in on-chip sensing, field-enhanced and nonlinear spectroscopy, and integrated nanophotonic switches. Here, we demonstrate a new regime of photon-plasmon coupling by combining a silicon photonic resonator with plasmonic nanoantennas. Using principles from coherent perfect absorption, we make use of standing-wave light fields to maximize the photon-plasmon interaction strength. Precise placement of the broadband antennas with respect to the narrowband photonic racetrack modes results in controlled hybridization of only a subset of these modes. By combining antennas into groups of radiating dipoles with opposite phase, far-field scattering is effectively suppressed. We achieve ultrafast tuning of photon-plasmon hybridization including reconfigurable routing of the standing-wave input between two output ports. Hybrid photonic-plasmonic resonators provide conceptually new approaches for on-chip integrated nanophotonic devices.

Photon diffusion coefficient in scattering and absorbing media.

PubMed

Pierrat, Romain; Greffet, Jean-Jacques; Carminati, Rémi

2006-05-01

We present a unified derivation of the photon diffusion coefficient for both steady-state and time-dependent transport in disordered absorbing media. The derivation is based on a modal analysis of the time-dependent radiative transfer equation. This approach confirms that the dynamic diffusion coefficient is given by the random-walk result D = cl(*)/3, where l(*) is the transport mean free path and c is the energy velocity, independent of the level of absorption. It also shows that the diffusion coefficient for steady-state transport, often used in biomedical optics, depends on absorption, in agreement with recent theoretical and experimental works. These two results resolve a recurrent controversy in light propagation and imaging in scattering media.

Design concepts for hot carrier-based detectors and energy converters in the near ultraviolet and infrared

NASA Astrophysics Data System (ADS)

Gong, Tao; Krayer, Lisa; Munday, Jeremy N.

2016-10-01

Semiconductor materials are well suited for power conversion when the incident photon energy is slightly larger than the bandgap energy of the semiconductor. However, for photons with energy significantly greater than the bandgap energy, power conversion efficiencies are low. Further, for photons with energy below the bandgap energy, the absence of absorption results in no power generation. Here, we describe photon detection and power conversion of both high- and low-energy photons using hot carrier effects. For the absorption of high-energy photons, excited electrons and holes have excess kinetic energy that is typically lost through thermalization processes between the carriers and the lattice. However, collection of hot carriers before thermalization allows for reduced power loss. Devices utilizing plasmonic nanostructures or simple three-layer stacks (transparent conductor-insulator-metal) can be used to generate and collect these hot carriers. Alternatively, hot carrier collection from sub-bandgap photons can be possible by forming a Schottky junction with an absorbing metal so that hot carriers generated in the metal can be injected across the semiconductor-metal interface. Such structures enable near-IR detection based on sub-bandgap photon absorption. Further, utilization and optimization of localized surface plasmon resonances can increase optical absorption and hot carrier generation (through plasmon decay). Combining these concepts, hot carrier generation and collection can be exploited over a large range of incident wavelengths spanning the UV, visible, and IR.

Determination of band offset using continuous-wave two-photon excitation in a ZnSe quantum-well waveguide structure

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

Wagner, H. P.; Kuhnelt, M.; Wenisch, H.

2001-06-15

We investigate exciton subband transitions in a ZnSe/Zn{sub 1{minus}x}Mg{sub x}S{sub y}Se{sub 1{minus}y} multiple-quantum-well grown by molecular beam epitaxy waveguide structure by photoluminescence excitation and two-photon excitation spectroscopy. A continuous-wave two-photon absorption is realized by an efficient waveguide coupling scheme within the cryostat. From the energetic position of the 1s and 2p exciton transitions exciton binding energies of 33 and 38 meV are deduced for heavy and light-hole excitons, respectively. With these values we are able to determine the strain free and dimensionless conduction-band-offset parameter to Q{sub c}=0.3{+-}0.1.

Ultrabright narrow-band telecom two-photon source for long-distance quantum communication

NASA Astrophysics Data System (ADS)

Niizeki, Kazuya; Ikeda, Kohei; Zheng, Mingyang; Xie, Xiuping; Okamura, Kotaro; Takei, Nobuyuki; Namekata, Naoto; Inoue, Shuichiro; Kosaka, Hideo; Horikiri, Tomoyuki

2018-04-01

We demonstrate an ultrabright narrow-band two-photon source at the 1.5 µm telecom wavelength for long-distance quantum communication. By utilizing a bow-tie cavity, we obtain a cavity enhancement factor of 4.06 × 104. Our measurement of the second-order correlation function G (2)(τ) reveals that the linewidth of 2.4 MHz has been hitherto unachieved in the 1.5 µm telecom band. This two-photon source is useful for obtaining a high absorption probability close to unity by quantum memories set inside quantum repeater nodes. Furthermore, to the best of our knowledge, the observed spectral brightness of 3.94 × 105 pairs/(s·MHz·mW) is also the highest reported over all wavelengths.

A [111]-Cut Si Hemisphere Two-Photon Response Photodetector

NASA Astrophysics Data System (ADS)

Liu, Xiu-Huan; Chen, Zhan-Guo; Jia, Gang; Wang, Hai-Yan; Gao, Yan-Jun; Li, Yi

2011-11-01

Properties of two-photon response in a [111]-cut nearly-intrinsic Si hemisphere photodetector are studied. The measured photocurrent of the photodetector responding to the 1.32μm continuous wave laser shows a quadratic dependence on the coupled optical power and is saturated with the bias voltage. Also, the photocurrent is independent of polarization. Such properties are in good agreement with the theory of two-photon absorption. The isotropic photocurrent generated from the [111]-cut Si hemisphere is compared to the anisotropic one induced in the [110]-cut Si sample and the ratio of χxxxx/χxxyy for silicon performing at 1.32 μm is calculated to be 2.4 via the fitted function of the anisotropic photocurrent from the [110]-cut sample.

Luminescent Fluorene-Based Bis-Pyrazolyl Aniline Ligand for Aluminum Detection.

PubMed

Frazer, Andrew; Morales, Alma R; Woodward, Adam W; Tongwa, Paul; Timofeeva, Tatiana; Belfield, Kevin D

2013-09-29

The design, synthesis, and photophysical properties of a new fluorene-based fluorescent chemosensor, 4-((E)-2-(2-(benzo[d]thiazol-2-yl)-9,9-diethyl-9H-fluoren-7-yl)vinyl)-N,N-bis((3,5-dimethyl-1H-pyrazol-1-yl)methyl)benzenamine (AXF-Al), is described for the detection of Al 3+ . AXF-Al exhibited absorption at 382 nm and strong fluorescence emission at 542 nm (fluorescence quantum yield, Φ F , of 0.80). The capture of Al 3+ by the pyrazolyl aniline receptor resulted in nominal change in the linear absorption (372 nm) but a large hypsochromic shift of 161 nm in the fluorescence spectrum (542 to 433 nm, Φ F  = 0.88), from which Al 3+ was detected both ratiometrically and colorimetrically. The addition of other metal ions, namely Mg 2+ , Ca 2+ , Mn 2+ , Fe 2+ , Co 2+ , Ni 2+ , Cu 2+ , Zn 2+ , Cd 2+ , Hg 2+ and Pb 2+ , produced only minimal changes in the optical properties of this probe. The emission band of this probe was also accessed by two-photon excitation in the near-IR, as two-photon absorption (2PA) is important for potential applications in two-photon fluorescence microscopy (2PFM) imaging. The 2PA cross section of the free fluorenyl ligand AXF-Al was 220 GM at 810 nm and 235 GM at 810 nm for the Al-ligand complex, practically useful properties for 2PFM.

Nonlinear absorption properties of ZnO and Al doped ZnO thin films under continuous and pulsed modes of operations

NASA Astrophysics Data System (ADS)

Sandeep, K. M.; Bhat, Shreesha; Dharmaprakash, S. M.

2018-06-01

In the present investigation, we present the variations in nonlinear optical (NLO) properties of undoped and Al doped ZnO (AZO) films under two different off-resonant regimes using continuous and pulsed mode lasers. Z-scan open aperture experiment is performed to quantify nonlinear absorption constant and imaginary component of third order susceptibility. Reverse saturable absorption (RSA) and saturable absorption (SA) behaviors are noticed in both undoped and AZO films under pulsed mode and continuous wavelength (CW) regime respectively. The RSA and SA behavior observed in the films are attributed to two photon absorption (TPA) and thermal lensing properties respectively. The thermal lensing is assisted by the thermo-optic effects within the films due to the continuous illumination of the laser.

Photonic devices based on patterning by two photon induced polymerization techniques

NASA Astrophysics Data System (ADS)

Fortunati, I.; Dainese, T.; Signorini, R.; Bozio, R.; Tagliazucca, V.; Dirè, S.; Lemercier, G.; Mulatier, J.-C.; Andraud, C.; Schiavuta, P.; Rinaldi, A.; Licoccia, S.; Bottazzo, J.; Franco Perez, A.; Guglielmi, M.; Brusatin, G.

2008-04-01

Two and three dimensional structures with micron and submicron resolution have been achieved in commercial resists, polymeric materials and sol-gel materials by several lithographic techniques. In this context, silicon-based sol-gel materials are particularly interesting because of their versatility, chemical and thermal stability, amount of embeddable active compounds. Compared with other micro- and nano-fabrication schemes, the Two Photon Induced Polymerization is unique in its 3D processing capability. The photopolymerization is performed with laser beam in the near-IR region, where samples show less absorption and less scattering, giving rise to a deeper penetration of the light. The use of ultrashort laser pulses allows the starting of nonlinear processes like multiphoton absorption at relatively low average power without thermally damaging the samples. In this work we report results on the photopolymerization process in hybrid organic-inorganic films based photopolymerizable methacrylate-containing Si-nanobuilding blocks. Films, obtained through sol-gel synthesis, are doped with a photo-initiator allowing a radical polymerization of methacrylic groups. The photo-initiator is activated by femtosecond laser source, at different input energies. The development of the unexposed regions is performed with a suitable solvent and the photopolymerized structures are characterized by microscopy techniques.

Photodynamic therapy and two-photon bio-imaging applications of hydrophobic chromophores through amphiphilic polymer delivery.

PubMed

Gallavardin, Thibault; Maurin, Mathieu; Marotte, Sophie; Simon, Timea; Gabudean, Ana-Maria; Bretonnière, Yann; Lindgren, Mikael; Lerouge, Frédéric; Baldeck, Patrick L; Stéphan, Olivier; Leverrier, Yann; Marvel, Jacqueline; Parola, Stéphane; Maury, Olivier; Andraud, Chantal

2011-07-01

The synthesis and photophysical properties of two lipophilic quadrupolar chromophores featuring anthracenyl (1) or dibromobenzene (2) were described. These two chromophores combined significant two-photon absorption cross-sections with high fluorescence quantum yield for 1 and improved singlet oxygen generation efficiency for 2, in organic solvents. The use of Pluronic nanoparticles allowed a simple and straightforward introduction of these lipophilic chromophores into biological cell media. Their internal distribution in various cell lines was studied using fluorescence microscopy and flow-cytometry following a successful staining that was achieved upon 2 h of incubation. Finally, multiphoton excitation microscopy and photodynamic therapy capability of the chromophores were demonstrated by cell exposure to a 820 nm fs laser and cell death upon one photon resonant irradiation at 436 ± 10 nm, respectively.

Gold nanorods for cell imaging with confocal reflectance microscopy and two-photon fluorescence microscopy

NASA Astrophysics Data System (ADS)

Chen, Ji-Yao; Wang, Pei-Nan

2010-02-01

Gold nanorods have unique optical properties as their two photon absorption cross sections are very high and their spectral positions of extinction bands can be controlled by their aspect ratio only, so that gold nanorods have been considered as agents for cell imaging. Two-photon photoluminescence imaging could be used to detect the cellular gold nanorods with the high power femto-second (fs) infrared laser, but may cause the photothermal effect melting the rods. The 3-D distribution of gold nanorods in living cells also can be measured by confocal reflectance microscopy with a very low laser power, and thus the cell damaging can be avoided. In this work, these two methods were comparatively studied in living rat basophilic leukemia (RBL-2H3) cells.

Cross section asymmetry of two-body carbon disintegration 12C (γ , p)11B with polarized photons at energy 40-50 MeV

NASA Astrophysics Data System (ADS)

Burdeinyi, D.; Brudvik, J.; Fissum, K.; Ganenko, V.; Hansen, K.; Isaksson, L.; Livingston, K.; Lundin, M.; Nilsson, B.; Schroder, B.

2017-01-01

The cross section asymmetry of 12C (γ ,p01)11B and 12C (γ ,p2-6)11B reactions has been studied at the energy range 40-55 MeV, using linearly polarized tagged photons of the MAX-lab facility. The asymmetry of the 12C (γ ,p01)11B processes, which assume the one-body mechanism of the reaction, is Σ ≈ 0.82 ± 0.05 for photon energies 45-50 MeV. The asymmetry for the 12C (γ ,p2-6)11B reactions, which produce a maximum at excitation energy ∼ 6 MeV, is Σ ≈ 0.53 ± 0.13 for a photon energy 49 MeV. It is close to the asymmetry of reaction of the free deuteron photodisintegration, and can be resulted from the two-body mechanism of the photon absorption.

Suppression of population transport and control of exciton distributions by entangled photons

PubMed Central

Schlawin, Frank; Dorfman, Konstantin E.; Fingerhut, Benjamin P.; Mukamel, Shaul

2013-01-01

Entangled photons provide an important tool for secure quantum communication, computing and lithography. Low intensity requirements for multi-photon processes make them idealy suited for minimizing damage in imaging applications. Here we show how their unique temporal and spectral features may be used in nonlinear spectroscopy to reveal properties of multiexcitons in chromophore aggregates. Simulations demostrate that they provide unique control tools for two-exciton states in the bacterial reaction centre of Blastochloris viridis. Population transport in the intermediate single-exciton manifold may be suppressed by the absorption of photon pairs with short entanglement time, thus allowing the manipulation of the distribution of two-exciton states. The quantum nature of the light is essential for achieving this degree of control, which cannot be reproduced by stochastic or chirped light. Classical light is fundamentally limited by the frequency-time uncertainty, whereas entangled photons have independent temporal and spectral characteristics not subjected to this uncertainty. PMID:23653194

Random Photon Absorption Model Elucidates How Early Gain Control in Fly Photoreceptors Arises from Quantal Sampling

PubMed Central

Song, Zhuoyi; Zhou, Yu; Juusola, Mikko

2016-01-01

Many diurnal photoreceptors encode vast real-world light changes effectively, but how this performance originates from photon sampling is unclear. A 4-module biophysically-realistic fly photoreceptor model, in which information capture is limited by the number of its sampling units (microvilli) and their photon-hit recovery time (refractoriness), can accurately simulate real recordings and their information content. However, sublinear summation in quantum bump production (quantum-gain-nonlinearity) may also cause adaptation by reducing the bump/photon gain when multiple photons hit the same microvillus simultaneously. Here, we use a Random Photon Absorption Model (RandPAM), which is the 1st module of the 4-module fly photoreceptor model, to quantify the contribution of quantum-gain-nonlinearity in light adaptation. We show how quantum-gain-nonlinearity already results from photon sampling alone. In the extreme case, when two or more simultaneous photon-hits reduce to a single sublinear value, quantum-gain-nonlinearity is preset before the phototransduction reactions adapt the quantum bump waveform. However, the contribution of quantum-gain-nonlinearity in light adaptation depends upon the likelihood of multi-photon-hits, which is strictly determined by the number of microvilli and light intensity. Specifically, its contribution to light-adaptation is marginal (≤ 1%) in fly photoreceptors with many thousands of microvilli, because the probability of simultaneous multi-photon-hits on any one microvillus is low even during daylight conditions. However, in cells with fewer sampling units, the impact of quantum-gain-nonlinearity increases with brightening light. PMID:27445779

Enhanced photon absorption in spiral nanostructured solar cells using layered 2D materials.

PubMed

Tahersima, Mohammad H; Sorger, Volker J

2015-08-28

Recent investigations of semiconducting two-dimensional (2D) transition metal dichalcogenides have provided evidence for strong light absorption relative to its thickness attributed to high density of states. Stacking a combination of metallic, insulating, and semiconducting 2D materials enables functional devices with atomic thicknesses. While photovoltaic cells based on 2D materials have been demonstrated, the reported absorption is still just a few percent of the incident light due to their sub-wavelength thickness leading to low cell efficiencies. Here we show that taking advantage of the mechanical flexibility of 2D materials by rolling a molybdenum disulfide (MoS(2))/graphene (Gr)/hexagonal boron nitride stack to a spiral solar cell allows for optical absorption up to 90%. The optical absorption of a 1 μm long hetero-material spiral cell consisting of the aforementioned hetero stack is about 50% stronger compared to a planar MoS(2) cell of the same thickness; although the volumetric absorbing material ratio is only 6%. A core-shell structure exhibits enhanced absorption and pronounced absorption peaks with respect to a spiral structure without metallic contacts. We anticipate these results to provide guidance for photonic structures that take advantage of the unique properties of 2D materials in solar energy conversion applications.

Tuning Ag29 nanocluster light emission from red to blue with one and two-photon excitation.

PubMed

Russier-Antoine, Isabelle; Bertorelle, Franck; Hamouda, Ramzi; Rayane, Driss; Dugourd, Philippe; Sanader, Željka; Bonačić-Koutecký, Vlasta; Brevet, Pierre-François; Antoine, Rodolphe

2016-02-07

We demonstrate that the tuning of the light emission from red to blue in dihydrolipoic acid (DHLA) capped Ag29 nanoclusters can be trigged with one and two photon excitations. The cluster stoichiometry was determined with mass spectrometry and found to be Ag29(DHLA)12. In a detailed optical investigation, we show that these silver nanoclusters exhibit a strong red photoluminescence visible to the naked eye and characterized by a quantum yield of nearly ∼2% upon one-photon excitation. In the nonlinear optical (NLO) study of the properties of the clusters, the two-photon excited fluorescence spectra were recorded and their first hyperpolarizability obtained. The two-photon absorption cross-section at ∼800 nm for Ag29(DHLA)12 is higher than 10(4) GM and the hyperpolarizability is 106 × 10(-30) esu at the same excitation wavelength. The two-photon excited fluorescence spectrum appears strongly blue-shifted as compared to the one-photon excited spectrum, displaying a broad band between 400 and 700 nm. The density functional theory (DFT) provides insight into the structural and electronic properties of Ag29(DHLA)12 as well as into interplay between metallic subunit or core and ligands which is responsible for unique optical properties.

Transient absorption phenomena and related structural transformations in femtosecond laser-excited Si

NASA Astrophysics Data System (ADS)

Kudryashov, Sergey I.

2004-09-01

Analysis of processes affecting transient optical absorption and photogeneration of electron-hole plasma in silicon pumped by an intense NIR or visible femtosecond laser pulse has been performed taking into account the most important electron-photon, electron-electron and electron-phonon interactions and, as a result, two main regimes of such laser-matter interaction have been revealed. The first regime is concerned with indirect interband optical absorption in Si, enhanced by a coherent shrinkage of its smallest indirect bandgap due to dynamic Franz-Keldysh effect (DFKE). The second regime takes place due to the critical renormalization of the Si direct bandgap along Λ-axis of its first Brillouin zone because of DFKE and the deformation potential electron-phonon interaction and occurs as intense direct single-photon excitation of electrons into one of the quadruplet of equivalent Λ-valleys in the lowest conduction band, which is split down due to the electron-phonon interaction.

Non-scanning fiber-optic near-infrared beam led to two-photon optogenetic stimulation in-vivo.

PubMed

Dhakal, Kamal R; Gu, Ling; Shivalingaiah, Shivaranjani; Dennis, Torry S; Morris-Bobzean, Samara A; Li, Ting; Perrotti, Linda I; Mohanty, Samarendra K

2014-01-01

Stimulation of specific neurons expressing opsins in a targeted region to manipulate brain function has proved to be a powerful tool in neuroscience. However, the use of visible light for optogenetic stimulation is invasive due to low penetration depth and tissue damage owing to larger absorption and scattering. Here, we report, for the first time, in-depth non-scanning fiber-optic two-photon optogenetic stimulation (FO-TPOS) of neurons in-vivo in transgenic mouse models. In order to optimize the deep-brain stimulation strategy, we characterized two-photon activation efficacy at different near-infrared laser parameters. The significantly-enhanced in-depth stimulation efficiency of FO-TPOS as compared to conventional single-photon beam was demonstrated both by experiments and Monte Carlo simulation. The non-scanning FO-TPOS technology will lead to better understanding of the in-vivo neural circuitry because this technology permits more precise and less invasive anatomical delivery of stimulation.

Multi-phase functionalization of titanium for enhanced photon absorption in the vis-NIR region.

PubMed

Thakur, Pooja; Tan, Bo; Venkatakrishnan, Krishnan

2015-10-19

Inadequate absorption of Near Infrared (NIR) photons by conventional silicon solar cells has been a major stumbling block towards the attainment of a high efficiency "full spectrum" solar cell. An effective enhancement in the absorption of such photons is desired as they account for a considerable portion of the tappable solar energy. In this work, we report a remarkable gain observed in the absorption of photons in the near infrared and visible region (400 nm-1000 nm) by a novel multi-phased oxide of titanium. Synthesised via a single step ultra-fast laser pulse interaction with pure titanium, characterisation studies have identified this oxide of titanium to be multi-phased and composed of Ti3O, (TiO.716)3.76 and TiO2 (rutile). Computed to have an average band gap value of 2.39 eV, this ultrafast laser induced multi-phased titanium oxide has especially exhibited steady absorption capability in the NIR range of 750-1000 nm, which to the best of our knowledge, was never reported before. The unique NIR absorption properties of the laser functionalised titanium coupled with the simplicity and versatility of the ultrafast laser interaction process involved thereby provides tremendous potential towards the photon sensitization of titanium and thereafter for the inception of a "full spectrum" solar device.

Two-Photon-Active Organotin(IV) Complexes for Antibacterial Function and Superresolution Bacteria Imaging.

PubMed

Hu, Lei; Wang, Hui; Xia, Tingting; Fang, Bin; Shen, Yu; Zhang, Qiong; Tian, Xiaohe; Zhou, Hongping; Wu, Jieying; Tian, Yupeng

2018-06-04

Antibacterial agents with two-photon absorption are expected to play a significant role in biomedical science. Herein, two novel organotin complexes, HLSn1 and HLSn2, based on coumarin were designed, synthesized, and systematically investigated. It was found that these complexes possessed suitable two-photon-active cross sections in the near-infrared region. Moreover, complex HLSn1 could efficiently inhibit the growth of Gram-negative Escherichia coli and Gram-positive Bacillus subtilis, especially the latter with a minimum inhibitory concentration (MIC; 90%) of 2 ± 0.14 μg mL -1 , which is lower than that of Kanamycin (Kana, 8 ± 0.42 μg mL -1 ). Importantly, two-photon imaging and superresolution development of bacterial stain revealed that complex HLSn1 can react with bacterial membranes, producing reactive oxygen species (ROS) and leading to cell death. These outcomes provide promising applications in the superresolution bacteria imaging, diagnostics, and treatment of bacterial infectious.

Modification of optical properties by adiabatic shifting of resonances in a four-level atom

NASA Astrophysics Data System (ADS)

Dutta, Bibhas Kumar; Panchadhyayee, Pradipta

2018-04-01

We describe the linear and nonlinear optical properties of a four-level atomic system, after reducing it to an effective two-level atomic model under the condition of adiabatic shifting of resonances driven by two coherent off-resonant fields. The reduced form of the Hamiltonian corresponding to the two-level system is obtained by employing an adiabatic elimination procedure in the rate equations of the probability amplitudes for the proposed four-level model. For a weak probe field operating in the system, the nonlinear dependence of complex susceptibility on the Rabi frequencies and the detuning parameters of the off-resonant driving fields makes it possible to exhibit coherent control of single-photon and two-photon absorption and transparency, the evolution of enhanced Self-Kerr nonlinearity and noticeable dispersive switching. We have shown how the quantum interference results in the generic four-level model at the adiabatic limit. The present scheme describes the appearance of single-photon transparency without invoking any exact two-photon resonance.

Magnetoresponsive discoidal photonic crystals toward active color pigments.

PubMed

Lee, Hye Soo; Kim, Ju Hyeon; Lee, Joon-Seok; Sim, Jae Young; Seo, Jung Yoon; Oh, You-Kwan; Yang, Seung-Man; Kim, Shin-Hyun

2014-09-03

Photonic microdisks with a multilayered structure are designed from photocurable suspensions by step-by-step photolithography. In each step of photolithography, either a colloidal photonic crystal or a magnetic-particle-laden layer is stacked over the windows of a photomask. Sequential photolithography enables the creation of multilayered photonic microdisks that have brilliant structural colors that can be switched by an external magnetic field. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Z-scan measurements using femtosecond continuum generation

NASA Astrophysics Data System (ADS)

de Boni, Leonardo; Andrade, Acácio A.; Misoguti, Lino; Mendonça, Cléber R.; Zilio, Sérgio Carlos

2004-08-01

We present a single beam Z-scan technique using an intense, broadband, white-light continuum (WLC) beam for the direct measurement of nonlinear absorption spectra. In order to demonstrate the validity of our technique, we compared the results of tetraaniline and Sudan 3 solutions obtained with WLC and conventional single wavelength light sources. Both approaches lead to the same nonlinear spectrum, indicating that the association of the Z-scan technique and the WLC source results in an useful method for the measurement of nonlinear spectra of both absorbing (saturable absorption or reverse saturable absorption) and transparent (two-photon absorption) samples.

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.

Subbarrier absorption in a stationary superlattice

NASA Technical Reports Server (NTRS)

Arutyunyan, G. M.; Nerkararyan, K. V.

1984-01-01

The calculation of the interband absorption coefficient was carried out in the classical case, when the frequency of light was assumed to bind two miniband subbarrier states of different bands. The influence of two dimensional Mott excitons on this absorption was studied and a comparison was made with the experiment. All of these considerations were done taking into account the photon wave vector (the phase spatial heterogeneity). The basic traits of the energy spectra of superlattice semiconductors, their kinetic and optical properties, and possible means of electromagnetic wave intensification were examined. By the density matrix method, a theory of electrical and electromagnetic properties of superlattices was suggested.

Kinetics of UV laser radiation defects in high performance glasses

NASA Astrophysics Data System (ADS)

Natura, U.; Feurer, T.; Ehrt, D.

2000-05-01

High purity fluoride phosphate glasses are attractive candidates as UV transmitting materials. The calculated values for the ultraviolet resonance wavelength are comparable with those of pure silica glass or fluoride single crystal CaF2. The formation of radiation-induced defect centers leads to additional absorption bands in the VUV-UV-vis range. The damage and the healing behavior by lamps and lasers are investigated in dependence on phosphate content and the content of impurities, mainly transition metals. Experiments were carried out using pulsed lasers with a duration of femto- and nanoseconds at a wavelength of 248 nm. The initial slope of the induced absorption shows a nonlinear dependence on the pulse energy density. Resonant and non-resonant two-photon mechanisms were observed. Two-photon-absorption coefficients at 248 nm for samples with different phosphate contents were measured. Models of the kinetics of the radiation-induced defects were developed. The inclusion of energy transfer was necessary to explain the difference in the damage behavior for nanosecond (248 nm, 193 nm) and femtosecond (248 nm) laser pulses.

Two-Photon-Absorption Scheme for Optical Beam Tracking

NASA Technical Reports Server (NTRS)

Ortiz, Gerardo G.; Farr, William H.

2011-01-01

A new optical beam tracking approach for free-space optical communication links using two-photon absorption (TPA) in a high-bandgap detector material was demonstrated. This tracking scheme is part of the canonical architecture described in the preceding article. TPA is used to track a long-wavelength transmit laser while direct absorption on the same sensor simultaneously tracks a shorter-wavelength beacon. The TPA responsivity was measured for silicon using a PIN photodiode at a laser beacon wavelength of 1,550 nm. As expected, the responsivity shows a linear dependence with incident power level. The responsivity slope is 4.5 x 10(exp -7) A/W2. Also, optical beam spots from the 1,550-nm laser beacon were characterized on commercial charge coupled device (CCD) and complementary metal-oxide semiconductor (CMOS) imagers with as little as 13.7 microWatts of optical power (see figure). This new tracker technology offers an innovative solution to reduce system complexity, improve transmit/receive isolation, improve optical efficiency, improve signal-to-noise ratio (SNR), and reduce cost for free-space optical communications transceivers.

Deconvolution improves the accuracy and depth sensitivity of time-resolved measurements

NASA Astrophysics Data System (ADS)

Diop, Mamadou; St. Lawrence, Keith

2013-03-01

Time-resolved (TR) techniques have the potential to distinguish early- from late-arriving photons. Since light travelling through superficial tissue is detected earlier than photons that penetrate the deeper layers, time-windowing can in principle be used to improve the depth sensitivity of TR measurements. However, TR measurements also contain instrument contributions - referred to as the instrument-response-function (IRF) - which cause temporal broadening of the measured temporal-point-spread-function (TPSF). In this report, we investigate the influence of the IRF on pathlength-resolved absorption changes (Δμa) retrieved from TR measurements using the microscopic Beer-Lambert law (MBLL). TPSFs were acquired on homogeneous and two-layer tissue-mimicking phantoms with varying optical properties. The measured IRF and TPSFs were deconvolved to recover the distribution of time-of-flights (DTOFs) of the detected photons. The microscopic Beer-Lambert law was applied to early and late time-windows of the TPSFs and DTOFs to access the effects of the IRF on pathlength-resolved Δμa. The analysis showed that the late part of the TPSFs contains substantial contributions from early-arriving photons, due to the smearing effects of the IRF, which reduced its sensitivity to absorption changes occurring in deep layers. We also demonstrated that the effects of the IRF can be efficiently eliminated by applying a robust deconvolution technique, thereby improving the accuracy and sensitivity of TR measurements to deep-tissue absorption changes.

Passive thermo-optic feedback for robust athermal photonic systems

DOEpatents

Rakich, Peter T.; Watts, Michael R.; Nielson, Gregory N.

2015-06-23

Thermal control devices, photonic systems and methods of stabilizing a temperature of a photonic system are provided. A thermal control device thermally coupled to a substrate includes a waveguide for receiving light, an absorption element optically coupled to the waveguide for converting the received light to heat and an optical filter. The optical filter is optically coupled to the waveguide and thermally coupled to the absorption element. An operating point of the optical filter is tuned responsive to the heat from the absorption element. When the operating point is less than a predetermined temperature, the received light is passed to the absorption element via the optical filter. When the operating point is greater than or equal to the predetermined temperature, the received light is transmitted out of the thermal control device via the optical filter, without being passed to the absorption element.

Breast conserving treatment for breast cancer: dosimetric comparison of sequential versus simultaneous integrated photon boost.

PubMed

Van Parijs, Hilde; Reynders, Truus; Heuninckx, Karina; Verellen, Dirk; Storme, Guy; De Ridder, Mark

2014-01-01

Breast conserving surgery followed by whole breast irradiation is widely accepted as standard of care for early breast cancer. Addition of a boost dose to the initial tumor area further reduces local recurrences. We investigated the dosimetric benefits of a simultaneously integrated boost (SIB) compared to a sequential boost to hypofractionate the boost volume, while maintaining normofractionation on the breast. For 10 patients 4 treatment plans were deployed, 1 with a sequential photon boost, and 3 with different SIB techniques: on a conventional linear accelerator, helical TomoTherapy, and static TomoDirect. Dosimetric comparison was performed. PTV-coverage was good in all techniques. Conformity was better with all SIB techniques compared to sequential boost (P = 0.0001). There was less dose spilling to the ipsilateral breast outside the PTVboost (P = 0.04). The dose to the organs at risk (OAR) was not influenced by SIB compared to sequential boost. Helical TomoTherapy showed a higher mean dose to the contralateral breast, but less than 5 Gy for each patient. SIB showed less dose spilling within the breast and equal dose to OAR compared to sequential boost. Both helical TomoTherapy and the conventional technique delivered acceptable dosimetry. SIB seems a safe alternative and can be implemented in clinical routine.

Breast Conserving Treatment for Breast Cancer: Dosimetric Comparison of Sequential versus Simultaneous Integrated Photon Boost

PubMed Central

Reynders, Truus; Heuninckx, Karina; Verellen, Dirk; Storme, Guy; De Ridder, Mark

2014-01-01

Background. Breast conserving surgery followed by whole breast irradiation is widely accepted as standard of care for early breast cancer. Addition of a boost dose to the initial tumor area further reduces local recurrences. We investigated the dosimetric benefits of a simultaneously integrated boost (SIB) compared to a sequential boost to hypofractionate the boost volume, while maintaining normofractionation on the breast. Methods. For 10 patients 4 treatment plans were deployed, 1 with a sequential photon boost, and 3 with different SIB techniques: on a conventional linear accelerator, helical TomoTherapy, and static TomoDirect. Dosimetric comparison was performed. Results. PTV-coverage was good in all techniques. Conformity was better with all SIB techniques compared to sequential boost (P = 0.0001). There was less dose spilling to the ipsilateral breast outside the PTVboost (P = 0.04). The dose to the organs at risk (OAR) was not influenced by SIB compared to sequential boost. Helical TomoTherapy showed a higher mean dose to the contralateral breast, but less than 5 Gy for each patient. Conclusions. SIB showed less dose spilling within the breast and equal dose to OAR compared to sequential boost. Both helical TomoTherapy and the conventional technique delivered acceptable dosimetry. SIB seems a safe alternative and can be implemented in clinical routine. PMID:25162031

Laser isotope separation by multiple photon absorption

DOEpatents

Robinson, C. Paul; Rockwood, Stephen D.; Jensen, Reed J.; Lyman, John L.; Aldridge, III, Jack P.

1987-01-01

Multiple photon absorption from an intense beam of infrared laser light may be used to induce selective chemical reactions in molecular species which result in isotope separation or enrichment. The molecular species must have a sufficient density of vibrational states in its vibrational manifold that, is the presence of sufficiently intense infrared laser light tuned to selectively excite only those molecules containing a particular isotope, multiple photon absorption can occur. By this technique, for example, intense CO.sub.2 laser light may be used to highly enrich .sup.34 S in natural SF.sub.6 and .sup.11 B in natural BCl.sub.3.

Laser isotope separation by multiple photon absorption

DOEpatents

Robinson, C. Paul; Rockwood, Stephen D.; Jensen, Reed J.; Lyman, John L.; Aldridge, III, Jack P.

1977-01-01

Multiple photon absorption from an intense beam of infrared laser light may be used to induce selective chemical reactions in molecular species which result in isotope separation or enrichment. The molecular species must have a sufficient density of vibrational states in its vibrational manifold that, in the presence of sufficiently intense infrared laser light tuned to selectively excite only those molecules containing a particular isotope, multiple photon absorption can occur. By this technique, for example, intense CO.sub.2 laser light may be used to highly enrich .sup.34 S in natural SF.sub.6 and .sup.11 B in natural BCl.sub.3.

Enhanced Broadband Electromagnetic Absorption in Silicon Film with Photonic Crystal Surface and Random Gold Grooves Reflector

PubMed Central

Chen, Zhi-Hui; Qiao, Na; Yang, Yibiao; Ye, Han; Liu, Shaoding; Wang, Wenjie; Wang, Yuncai

2015-01-01

We show a hybrid structure consisting of Si film with photonic crystal surface and random triangular gold grooves reflector at the bottom, which is capable of realizing efficient, broad-band, wide-angle optical absorption. It is numerically demonstrated that the enhanced absorption in a broad wavelength range (0.3–9.9 μm) due to the scattering effect of both sides of the structure and the created resonance modes. Larger thickness and period are favored to enhance the absorption in broader wavelength range. Substantial electric field concentrates in the grooves of surface photonic crystal and in the Si film. Our structure is versatile for solar cells, broadband photodetection and stealth coating. PMID:26238270

Deterministic Remote Entanglement of Superconducting Circuits through Microwave Two-Photon Transitions

NASA Astrophysics Data System (ADS)

Campagne-Ibarcq, P.; Zalys-Geller, E.; Narla, A.; Shankar, S.; Reinhold, P.; Burkhart, L.; Axline, C.; Pfaff, W.; Frunzio, L.; Schoelkopf, R. J.; Devoret, M. H.

2018-05-01

Large-scale quantum information processing networks will most probably require the entanglement of distant systems that do not interact directly. This can be done by performing entangling gates between standing information carriers, used as memories or local computational resources, and flying ones, acting as quantum buses. We report the deterministic entanglement of two remote transmon qubits by Raman stimulated emission and absorption of a traveling photon wave packet. We achieve a Bell state fidelity of 73%, well explained by losses in the transmission line and decoherence of each qubit.

Deterministic Remote Entanglement of Superconducting Circuits through Microwave Two-Photon Transitions.

PubMed

Campagne-Ibarcq, P; Zalys-Geller, E; Narla, A; Shankar, S; Reinhold, P; Burkhart, L; Axline, C; Pfaff, W; Frunzio, L; Schoelkopf, R J; Devoret, M H

2018-05-18

Large-scale quantum information processing networks will most probably require the entanglement of distant systems that do not interact directly. This can be done by performing entangling gates between standing information carriers, used as memories or local computational resources, and flying ones, acting as quantum buses. We report the deterministic entanglement of two remote transmon qubits by Raman stimulated emission and absorption of a traveling photon wave packet. We achieve a Bell state fidelity of 73%, well explained by losses in the transmission line and decoherence of each qubit.

Near-infrared gallium nitride two-dimensional photonic crystal platform on silicon

NASA Astrophysics Data System (ADS)

Roland, I.; Zeng, Y.; Han, Z.; Checoury, X.; Blin, C.; El Kurdi, M.; Ghrib, A.; Sauvage, S.; Gayral, B.; Brimont, C.; Guillet, T.; Semond, F.; Boucaud, P.

2014-07-01

We demonstrate a two-dimensional free-standing gallium nitride photonic crystal platform operating around 1550 nm and fabricated on a silicon substrate. Width-modulated waveguide cavities are integrated and exhibit loaded quality factors up to 34 000 at 1575 nm. We show the resonance tunability by varying the ratio of air hole radius to periodicity, and cavity hole displacement. We deduce a ˜7.9 dB/cm linear absorption loss for the suspended nitride structure from the power dependence of the cavity in-plane transmission.

Near-infrared gallium nitride two-dimensional photonic crystal platform on silicon

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

Roland, I.; Zeng, Y.; Han, Z.

We demonstrate a two-dimensional free-standing gallium nitride photonic crystal platform operating around 1550 nm and fabricated on a silicon substrate. Width-modulated waveguide cavities are integrated and exhibit loaded quality factors up to 34 000 at 1575 nm. We show the resonance tunability by varying the ratio of air hole radius to periodicity, and cavity hole displacement. We deduce a ∼7.9 dB/cm linear absorption loss for the suspended nitride structure from the power dependence of the cavity in-plane transmission.

[Absorption and metabolism of Chuanxiong Rhizoma decoction with multi-component sequential metabolism method].

PubMed

Liu, Yang; Luo, Zhi-Qiang; Lv, Bei-Ran; Zhao, Hai-Yu; Dong, Ling

2016-04-01

The multiple components in Chinese herbal medicines (CHMS) will experience complex absorption and metabolism before entering the blood system. Previous studies often lay emphasis on the components in blood. However, the dynamic and sequential absorption and metabolism process following multi-component oral administration has not been studied. In this study, the in situ closed-loop method combined with LC-MS techniques were employed to study the sequential process of Chuanxiong Rhizoma decoction (RCD). A total of 14 major components were identified in RCD. Among them, ferulic acid, senkyunolide J, senkyunolide I, senkyunolide F, senkyunolide G, and butylidenephthalide were detected in all of the samples, indicating that the six components could be absorbed into blood in prototype. Butylphthalide, E-ligustilide, Z-ligustilide, cnidilide, senkyunolide A and senkyunolide Q were not detected in all the samples, suggesting that the six components may not be absorbed or metabolized before entering the hepatic portal vein. Senkyunolide H could be metabolized by the liver, while senkyunolide M could be metabolized by both liver and intestinal flora. This study clearly demonstrated the changes in the absorption and metabolism process following multi-component oral administration of RCD, so as to convert the static multi-component absorption process into a comprehensive dynamic and continuous absorption and metabolism process. Copyright© by the Chinese Pharmaceutical Association.

An organic dye with very large Stokes-shift and broad tunability of fluorescence: Potential two-photon probe for bioimaging and ultra-sensitive solid-state gas sensor

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

He, Tingchao; Tian, Xiaoqing; Lin, Xiaodong, E-mail: linxd@szu.edu.cn, E-mail: hdsun@ntu.edu.sg

Light-emitting nonlinear optical molecules, especially those with large Stokes shifts and broad tunability of their emission wavelength, have attracted considerable attention for various applications including biomedical imaging and fluorescent sensors. However, most fluorescent chromophores have only limited potential for such applications due to small Stokes shifts, narrow tunability of fluorescence emissions, and small optical nonlinearity in highly polar solvents. In this work, we demonstrate that a two-photon absorbing stilbene chromophore exhibits a large two-photon absorption action cross-section (ηδ = 320 GM) in dimethylsulfoxide (DMSO) and shows broad fluorescence tunability (125 nm) by manipulating the polarity of the surrounding medium. Importantly, a very large Stokesmore » shift of up to 227 nm is achieved in DMSO. Thanks to these features, this chromophore can be utilized as a two-photon probe for bioimaging applications and in an ultrasensitive solid-state gas detector.« less

Detection of TNT using a sensitive two-photon organic dendrimer for remote sensing

NASA Astrophysics Data System (ADS)

Narayanan, Aditya; Varnavski, Oleg; Mongin, Oliver; Majoral, Jean-Pierre; Blanchard-Desce, Mireille; Goodson, Theodore, III

2008-03-01

There is currently a need for superior stand-off detection schemes for protection against explosive weapons of mass destruction. Fluorescence detection at small distances from the target has proven to be attractive. A novel unexplored route in fluorescence chemical sensing that utilizes the exceptional spectroscopic capabilities of nonlinear optical methods is two-photon excited fluorescence. This approach utilizes infra-red light for excitation of remote sensors. Infra-red light suffers less scattering in porous materials which is beneficial for vapor sensing and has greater depth of penetration through the atmosphere, and there are fewer concerns regarding eye safety in remote detection schemes. We demonstrate this method using a novel dendritic system which possesses both excellent fluorescence sensitivity to the presence of TNT with infra-red pulses of light and high two-photon absorption (TPA) response. This illustrates the use of TPA for potential stand-off detection of energetic materials in the infra-red spectral regions in a highly two-photon responsive dendrimer.

A Series of Zn(II) Terpyridine-Based Nitrate Complexes as Two-Photon Fluorescent Probe for Identifying Apoptotic and Living Cells via Subcellular Immigration.

PubMed

Liu, Dandan; Zhang, Mingzhu; Du, Wei; Hu, Lei; Li, Fei; Tian, Xiaohe; Wang, Aidong; Zhang, Qiong; Zhang, Zhongping; Wu, Jieying; Tian, Yupeng

2018-06-19

Two-photon active probe to label apoptotic cells plays a significant role in biological systems. However, discrimination of live/apoptotic cells at subcellular level under microscopy remains unachieved. Here, three novel Zn(II) terpyridine-based nitrate complexes (C1-C3) containing different pull/push units were designed. The structures of the ligands and their corresponding Zn(II) complexes were confirmed by single-crystal X-ray diffraction analysis. On the basis of the comprehensive comparison, C3 had a suitable two-photon absorption cross section in the near-infrared wavelength and good biocompatibility. Under two-photon confocal microscopy and transmission electron microscopy, it is found that C3 could target mitochondria in living cells but immigrate into the nucleolus during the apoptotic process. This dual-functional probe (C3) not only offers a valuable image tool but also acts as an indicator for cell mortality at subcellular level in a real-time manner.

Enhancement of two photon absorption with Ni doping in the dilute magnetic semiconductor ZnO crystalline nanorods

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

Rana, Amit Kumar; Kumar, Yogendra; Arjunan, M.S.

2015-12-07

In this letter, we have investigated the third-order optical nonlinearities of high-quality Ni doped ZnO nanorods crystallized in wurtzite lattice, prepared by the wet chemical method. In our experiments, we found that the two photon absorption coefficient (β) increases by as much as 14 times, i.e., 7.6 ± 0.4 to 112 ± 6 cm/GW, when the Ni doping is increased from 0% to 10%. The substantial enhancement in β is discussed in terms of the bandgap scaling and Ni doping. Furthermore, we also show that the optical bandgap measured by UV-Vis and photoluminescence spectroscopies, continuously redshift with increasing Ni doping concentration.more » We envision that the strong nonlinear optical properties together with their dilute magnetic effects, they form an important class of materials for potential applications in magneto-optical and integrated optical chips.« less

Prediction and Characterization of NaGaS2, A High Thermal Conductivity Mid-Infrared Nonlinear Optical Material for High-Power Laser Frequency Conversion.

PubMed

Hou, Dianwei; Nissimagoudar, Arun S; Bian, Qiang; Wu, Kui; Pan, Shilie; Li, Wu; Yang, Zhihua

2018-06-15

Infrared nonlinear optical (IR NLO) crystals are the major materials to widen the output range of solid-state lasers to mid- or far-infrared regions. The IR NLO crystals used in the middle IR region are still inadequate for high-power laser applications because of deleterious thermal effects (lensing and expansion), low laser-induced damage threshold, and two-photon absorption. Herein, the unbiased global minimum search method was used for the first time to search for IR NLO optical materials and ultimately found a new IR NLO material NaGaS 2 . It meets the stringent demands for IR NLO materials pumped by high-power laser with the highest thermal conductivity among common IR NLO materials able to avoid two-photon absorption, a classic nonlinear coefficient, and wide infrared transparency.

Near resonant and nonresonant third-order optical nonlinearities of colloidal InP/ZnS quantum dots

NASA Astrophysics Data System (ADS)

Wang, Y.; Yang, X.; He, T. C.; Gao, Y.; Demir, H. V.; Sun, X. W.; Sun, H. D.

2013-01-01

We have investigated the third-order optical nonlinearities of high-quality colloidal InP/ZnS core-shell quantum dots (QDs) using Z-scan technique with femtosecond pulses. The two-photon absorption cross-sections as high as 6.2 × 103 GM are observed at 800 nm (non-resonant regime) in InP/ZnS QDs with diameter of 2.8 nm, which is even larger than those of CdSe, CdS, and CdTe QDs at similar sizes. Furthermore, both of the 2.2 nm and 2.8 nm-sized InP/ZnS QDs exhibit strong saturable absorption in near resonant regime, which is attributed to large exciton Bohr radius in this material. These results strongly suggest the promising potential of InP/ZnS QDs for widespread applications, especially in two-photon excited bio-imaging and saturable absorbing.

Enhancement of two photon absorption with Ni doping in the dilute magnetic semiconductor ZnO crystalline nanorods

NASA Astrophysics Data System (ADS)

Rana, Amit Kumar; J, Aneesh; Kumar, Yogendra; M. S, Arjunan; Adarsh, K. V.; Sen, Somaditya; Shirage, Parasharam M.

2015-12-01

In this letter, we have investigated the third-order optical nonlinearities of high-quality Ni doped ZnO nanorods crystallized in wurtzite lattice, prepared by the wet chemical method. In our experiments, we found that the two photon absorption coefficient (β) increases by as much as 14 times, i.e., 7.6 ± 0.4 to 112 ± 6 cm/GW, when the Ni doping is increased from 0% to 10%. The substantial enhancement in β is discussed in terms of the bandgap scaling and Ni doping. Furthermore, we also show that the optical bandgap measured by UV-Vis and photoluminescence spectroscopies, continuously redshift with increasing Ni doping concentration. We envision that the strong nonlinear optical properties together with their dilute magnetic effects, they form an important class of materials for potential applications in magneto-optical and integrated optical chips.

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.

Lighting the Way to See Inside Two-Photon Absorption Materials: Structure–Property Relationship and Biological Imaging

PubMed Central

Zhang, Qiong; Tian, Xiaohe; Zhou, Hongping; Wu, Jieying; Tian, Yupeng

2017-01-01

The application of two-photon absorption (2PA) materials is a classical research field and has recently attracted increasing interest. It has generated a demand for new dyes with high 2PA cross-sections. In this short review, we briefly cover the structure-2PA property relationships of organic fluorophores, organic-inorganic nanohybrids and metal complexes explored by our group. (1) The two-photon absorption cross-section (δ) of organic fluorophores increases with the extent of charge transfer, which is important to optimize the core, donor-acceptor pair, and conjugation-bridge to obtain a large δ value. Among the various cores, triphenylamine appears to be an efficient core. Lengthening of the conjugation with styryl groups in the D-π-D quadrupoles and D-π-A dipoles increased δ over a long wavelength range than when vinylene groups were used. Large values of δ were observed for extended conjugation length and moderate donor-acceptors in the near-IR wavelengths. The δ value of the three-arm octupole is larger than that of the individual arm, if the core has electron accepting groups that allow significant electronic coupling between the arms; (2) Optical functional organic/inorganic hybrid materials usually show high thermal stability and excellent optical activity; therefore the design of functional organic molecules to build functional organic-inorganic hybrids and optimize the 2PA properties are significant. Advances have been made in the design of organic-inorganic nanohybrid materials of different sizes and shapes for 2PA property, which provide useful examples to illustrate the new features of the 2PA response in comparison to the more thoroughly investigated donor-acceptor based organic compounds and inorganic components; (3) Metal complexes are of particular interest for the design of new materials with large 2PA ability. They offer a wide range of metals with different ligands, which can give rise to tunable electronic and 2PA properties. The metal ions, including transition metals and lanthanides, can serve as an important part of the structure to control the intramolecular charge-transfer process that drives the 2PA process. As templates, transition metal ions can assemble simple to more sophisticated ligands in a variety of multipolar arrangements resulting in interesting and tailorable electronic and optical properties, depending on the nature of the metal center and the energetics of the metal-ligand interactions, such as intraligand charge-transfer (ILCT) and metal-ligand charge-transfer (MLCT) processes. Lanthanide complexes are attractive for a number of reasons: (i) their visible emissions are quite long-lived; (ii) their absorption and emission can be tuned with the aid of appropriate photoactive ligands; (iii) the accessible energy-transfer path between the photo-active ligands and the lanthanide ion can facilitate efficient lanthanide-based 2PA properties. Thus, the above materials with excellent 2PA properties should be applied in two-photon applications, especially two-photon fluorescence microscopy (TPFM) and related emission-based applications. Furthermore, the progress of research into the use of those new 2PA materials with moderate 2PA cross section in the near-infrared region, good biocompatibility, and enhanced two-photon excited fluorescence for two-photon bio-imaging is summarized. In addition, several possible future directions in this field are also discussed (146 references). PMID:28772584

Gated photochemical hole burning in photoadducts of polyacenes

NASA Technical Reports Server (NTRS)

Iannone, Mark; Scott, Gary W.; Brinza, David; Coulter, Daniel R.

1986-01-01

A photoadduct of anthracene and tetracene (A-T) in a polymer matrix at 1.5 K generates an absorption spectrum which exhibits two-color, photon-gated photochemical hole burning (PHB) when irradiated with narrowband exciting light into the 0-0 band of the S1-S0 absorption. The efficiency of this PHB process is found to be enhanced by simultaneous irradiation near the maximum of the Tn-T1 absorption of A-T; hole widths of less than 0.07/cm have been observed for this photochemical cleavage of A-T.

High-speed and high-efficiency travelling wave single-photon detectors embedded in nanophotonic circuits

PubMed Central

Pernice, W.H.P.; Schuck, C.; Minaeva, O.; Li, M.; Goltsman, G.N.; Sergienko, A.V.; Tang, H.X.

2012-01-01

Ultrafast, high-efficiency single-photon detectors are among the most sought-after elements in modern quantum optics and quantum communication. However, imperfect modal matching and finite photon absorption rates have usually limited their maximum attainable detection efficiency. Here we demonstrate superconducting nanowire detectors atop nanophotonic waveguides, which enable a drastic increase of the absorption length for incoming photons. This allows us to achieve high on-chip single-photon detection efficiency up to 91% at telecom wavelengths, repeatable across several fabricated chips. We also observe remarkably low dark count rates without significant compromise of the on-chip detection efficiency. The detectors are fully embedded in scalable silicon photonic circuits and provide ultrashort timing jitter of 18 ps. Exploiting this high temporal resolution, we demonstrate ballistic photon transport in silicon ring resonators. Our direct implementation of a high-performance single-photon detector on chip overcomes a major barrier in integrated quantum photonics. PMID:23271658

Excitation Spectra and Brightness Optimization of Two-Photon Excited Probes

PubMed Central

Mütze, Jörg; Iyer, Vijay; Macklin, John J.; Colonell, Jennifer; Karsh, Bill; Petrášek, Zdeněk; Schwille, Petra; Looger, Loren L.; Lavis, Luke D.; Harris, Timothy D.

2012-01-01

Two-photon probe excitation data are commonly presented as absorption cross section or molecular brightness (the detected fluorescence rate per molecule). We report two-photon molecular brightness spectra for a diverse set of organic and genetically encoded probes with an automated spectroscopic system based on fluorescence correlation spectroscopy. The two-photon action cross section can be extracted from molecular brightness measurements at low excitation intensities, while peak molecular brightness (the maximum molecular brightness with increasing excitation intensity) is measured at higher intensities at which probe photophysical effects become significant. The spectral shape of these two parameters was similar across all dye families tested. Peak molecular brightness spectra, which can be obtained rapidly and with reduced experimental complexity, can thus serve as a first-order approximation to cross-section spectra in determining optimal wavelengths for two-photon excitation, while providing additional information pertaining to probe photostability. The data shown should assist in probe choice and experimental design for multiphoton microscopy studies. Further, we show that, by the addition of a passive pulse splitter, nonlinear bleaching can be reduced—resulting in an enhancement of the fluorescence signal in fluorescence correlation spectroscopy by a factor of two. This increase in fluorescence signal, together with the observed resemblance of action cross section and peak brightness spectra, suggests higher-order photobleaching pathways for two-photon excitation. PMID:22385865

Freeze-dried Lactobacillus plantarum 299v increases iron absorption in young females—Double isotope sequential single-blind studies in menstruating women

PubMed Central

Önning, Gunilla; Hulthén, Lena

2017-01-01

Background The probiotic strain Lactobacillus plantarum 299v has earlier been shown to increase iron absorption when added to foods. However, it is not known if the same probiotic strain in a freeze-dried format included in a capsule increases the iron absorption. Objective The aim of this study was to test the hypotheses that non-heme iron absorption from a light meal is promoted by a simultaneous intake of freeze-dried Lactobacillus plantarum 299v (Lp299v, DSM 9843). Study design With a single blinded placebo controlled sequential design, iron absorption from a light breakfast meal administered with or without capsules containing 1010 cfu freeze-dried Lp299v was studied in healthy female volunteers of fertile age. The methodology used was a double isotope technique (59Fe and 55Fe). Two studies were performed using the same protocol. Results In study 1, the absorption of iron from a meal without Lp299v was found to be 17.4 ± 13.4%, and from an identical meal with Lp299v was found to be 22.4 ± 17.3% (mean ± SD). This difference was statistically significant (p = 0.040, n = 14). In study 2, the absorption of iron from a meal without Lp299v was found to be 20.9 ± 13.1%, and from an identical meal with Lp299v found to be 24.5 ± 12.0% (mean ± SD, n = 28), which again was statistically significant (p = 0.003). Conclusion Freeze-dried Lp299v enhances the absorption of iron when administered together with a meal with a high iron bioavailability. Trial registration ClinicalTrials.gov Identifier: NCT02131870 PMID:29236734

Comparison of femtosecond- and nanosecond-two-photon-absorption laser-induced fluorescence (TALIF) of atomic oxygen in atmospheric-pressure plasmas

NASA Astrophysics Data System (ADS)

Schmidt, Jacob B.; Sands, Brian; Scofield, James; Gord, James R.; Roy, Sukesh

2017-05-01

Absolute number densities of atomic species produced by nanosecond (ns)-duration, repetitively pulsed electric discharges are measured by two-photon-absorption laser-induced fluorescence (TALIF). Unique to this work is the development of femtosecond-laser-based TALIF (fs-TALIF) that offers a number of advantages over more conventional nanosecond (ns)-pulse-duration laser techniques, such as higher-fidelity quenching rate measurements over a wide pressure range, significantly reduced photolytic interference (including photo-dissociation and photo-ionization), ability to collect two-dimensional images of atomic-species number densities with high spatial resolution aided by higher signal level, and efficient and accurate measurements of atomic-species number densities due to the higher repetition rates of the laser. For full quantification of these advantages, atomic-oxygen TALIF signals are collected from an atmospheric-pressure plasma jet employing both ns- and fs-duration laser-excitation pulses and the results are compared and contrasted.

Three-photon absorption and nonlinear refraction of BaMgF4 in the ultraviolet region.

PubMed

Ma, Yanzhi; Chen, Junjie; Zheng, Yuanlin; Chen, Xianfeng

2012-08-01

The nonlinear refraction and nonlinear absorption phenomena are investigated in BaMgF(4) single crystal using the Z-scan technique in the ultraviolet region with a pulsed laser at 400 nm with 1 ps pulse duration. The remarkable nonlinear absorption behavior is identified to be three-photon absorption under the experimental conditions. In addition, both nonlinear refraction and nonlinear absorption have relatively large values and possess small anisotropy along three different crystallographic axes. The large values of nonlinear refractive index are demonstrated through the self-phase modulation effect.

Wideband absorption in one dimensional photonic crystal with graphene-based hyperbolic metamaterials

NASA Astrophysics Data System (ADS)

Kang, Yongqiang; Liu, Hongmei

2018-02-01

A broadband absorber which was proposed by one dimensional photonic crystal (1DPC) containing graphene-based hyperbolic metamaterials (GHMM) is theoretically investigated. For TM mode, it was demonstrated to absorb roughly 90% of all available electromagnetic waves at a 14 THz absorption bandwidth at normal incidence. The absorption bandwidth was affected by Fermi energy and thickness of dielectric layer. When the incident angle was increased, the absorption value decreased, and the absorption band had a gradual blue shift. These findings have potential applications for designing broadband optoelectronic devices at mid-infrared and THz frequency range.

Phosphorescent probes for two-photon microscopy of oxygen (Conference Presentation)

NASA Astrophysics Data System (ADS)

Vinogradov, Sergei A.; Esipova, Tatiana V.

2016-03-01

The ability to quantify oxygen in vivo in 3D with high spatial and temporal resolution is much needed in many areas of biological research. Our laboratory has been developing the phosphorescence quenching technique for biological oximetry - an optical method that possesses intrinsic microscopic capability. In the past we have developed dendritically protected oxygen probes for quantitative imaging of oxygen in tissue. More recently we expanded our design on special two-photon enhanced phosphorescent probes. These molecules brought about first demonstrations of the two-photon phosphorescence lifetime microscopy (2PLM) of oxygen in vivo, providing new information for neouroscience and stem cell biology. However, current two-photon oxygen probes suffer from a number of limitations, such as sub-optimal brightness and high cost of synthesis, which dramatically reduce imaging performance and limit usability of the method. In this paper we discuss principles of 2PLM and address the interplay between the probe chemistry, photophysics and spatial and temporal imaging resolution. We then present a new approach to brightly phosphorescent chromophores with internally enhanced two-photon absorption cross-sections, which pave a way to a new generation of 2PLM probes.

Physical mechanisms of timing jitter in photon detection by current-carrying superconducting nanowires

NASA Astrophysics Data System (ADS)

Sidorova, Mariia; Semenov, Alexej; Hübers, Heinz-Wilhelm; Charaev, Ilya; Kuzmin, Artem; Doerner, Steffen; Siegel, Michael

2017-11-01

We studied timing jitter in the appearance of photon counts in meandering nanowires with different fractional amount of bends. Intrinsic timing jitter, which is the probability density function of the random time delay between photon absorption in current-carrying superconducting nanowire and appearance of the normal domain, reveals two different underlying physical mechanisms. In the deterministic regime, which is realized at large photon energies and large currents, jitter is controlled by position-dependent detection threshold in straight parts of meanders. It decreases with the increase in the current. At small photon energies, jitter increases and its current dependence disappears. In this probabilistic regime jitter is controlled by Poisson process in that magnetic vortices jump randomly across the wire in areas adjacent to the bends.

Ultrafast Spectroscopic Studies of Two-Photon States in Third Order Optical Processes of Dye Chromophores.

NASA Astrophysics Data System (ADS)

Yu, Yi-Zhong

1995-01-01

Conjugated organic and polymeric materials usually have large, nonresonant third order optical nonlinearity due to correlations of their delocalized pi -electrons. Most materials studied so far show positive values of third order nonlinear susceptibility when all frequencies that generate the third order effect are below any optical transition. A new class of organic molecules, namely indole squarylium (ISQ) and anilinium squarylium (BSQ), exhibit negative < gamma(-omega_4;omega_1, omega_2,omega_3)> when all three frequencies, omega_1, omega_2 and omega_3, lie below the first electronic transition. Although quantum many-electron calculations based on multiple-excitation configuration interaction have shown that the negative third order coefficient is essentially due to the contribution from high-lying two-photon states, the field of experimental studies exploring the microscopic origins of the negative squaraines remains uncultivated. The work presented in this thesis involves extensive experimental investigation of squaraines using techniques such as time-resolved transit absorption spectroscopy and saturable absorption. Theoretical simulations studying nonlinear absorption behavior of a simplified two-level system with ultrashort pulses are also presented. Part of the thesis is dedicated to the development, fabrication and characterization of our ultrafast laser system which offers tunable femtosecond pulses at wavelengths from UV to IR and served as a major tool in the experimental measurements. The dynamics of the population inversion between the ground state and the first excited state was also investigated through time-resolved experiments. The experiment results agree well with the theoretical predictions. Strong couplings between the gateway state and high-lying two-photon states were observed in BSQ squarylium molecules, which suggested a complete quantum calculation with multiple energy levels is required to correctly describe the negative third order effect.

Self-phase modulation and two-photon absorption imaging of cells and active neurons

NASA Astrophysics Data System (ADS)

Fischer, Martin C.; Liu, Henry; Piletic, Ivan R.; Ye, Tong; Yasuda, Ryohei; Warren, Warren S.

2007-02-01

Even though multi-photon fluorescence microscopy offers higher resolution and better penetration depth than traditional fluorescence microscopy, its use is restricted to the detection of molecules that fluoresce. Two-photon absorption (TPA) imaging can provide contrast in non-fluorescent molecules while retaining the high resolution and sectioning capabilities of nonlinear imaging modalities. In the long-wavelength water window, tissue TPA is dominated by the endogenous molecules melanin and hemoglobin with an almost complete absence of endogenous two-photon fluorescence. A complementary nonlinear contrast mechanism is self-phase modulation (SPM), which can provide intrinsic signatures that can depend on local tissue anisotropy, chemical environment, or other structural properties. We have developed a spectral hole refilling measurement technique for TPA and SPM measurements using shaped ultrafast laser pulses. Here we report on a microscopy setup to simultaneously acquire 3D, high-resolution TPA and SPM images. We have acquired data in mounted B16 melanoma cells with very modest laser power levels. We will also discuss the possible application of this measurement technique to neuronal imaging. Since SPM is sensitive to material structure we can expect SPM properties of neurons to change during neuronal firing. Using our hole-refilling technique we have now demonstrated strong novel intrinsic nonlinear signatures of neuronal activation in a hippocampal brain slice. The observed changes in nonlinear signal upon collective activation were up to factors of two, unlike other intrinsic optical signal changes on the percent level. These results show that TPA and SPM imaging can provide important novel functional contrast in tissue using very modest power levels suitable for in vivo applications.

Characterizing the absorption and aging behavior of DUV optical material by high-resolution excimer laser calorimetry

NASA Astrophysics Data System (ADS)

Mann, Klaus R.; Eva, Eric

1998-06-01

Absorption loss in DUV optics during 193 nm irradiation is investigated by employing a high-resolution calorimetric technique which allows determining both single and two photon absorption coefficients at energy densities of several 10 mJ/cm2, avoiding a significant thermal load on the samples. UV calorimetry is also employed to investigate laser induced aging phenomena, e.g. color center formation in fused silica or CaF2. A separation of transient and cumulative effects as a function of intensity can be achieved, giving insight into various loss mechanisms. Moreover, the influence of dielectric coatings on the absorption characteristics is discussed.

Anomalous nonlinear absorption in epsilon-near-zero materials: optical limiting and all-optical control.

PubMed

Vincenti, M A; de Ceglia, D; Scalora, Michael

2016-08-01

We investigate nonlinear absorption in films of epsilon-near-zero materials. The combination of large local electric fields at the fundamental frequency and material losses at the harmonic frequencies induce unusual intensity-dependent phenomena. We predict that the second-order nonlinearity of a low-damping, epsilon-near-zero slab produces an optical limiting effect that mimics a two-photon absorption process. Anomalous absorption profiles that depend on low permittivity values at the pump frequency are also predicted for third-order nonlinearities. These findings suggest new opportunities for all-optical light control and novel ways to design reconfigurable and tunable nonlinear devices.

Tripartite counterfactual entanglement distribution.

PubMed

Chen, Yuanyuan; Gu, Xuemei; Jiang, Dong; Xie, Ling; Chen, Lijun

2015-08-10

We propose two counterfactual schemes for tripartite entanglement distribution without any physical particles travelling through the quantum channel. One scheme arranges three participators to connect with the absorption object by using switch. Using the "chained" quantum Zeno effect, three participators can accomplish the task of entanglement distribution with unique counterfactual interference probability. Another scheme uses Michelson-type interferometer to swap two entanglement pairs such that the photons of three participators are entangled. Moreover, the distance of entanglement distribution is doubled as two distant absorption objects are used. We also discuss the implementation issues to show that the proposed schemes can be realized with current technology.

Laser isotope separation by multiple photon absorption

DOEpatents

Robinson, C.P.; Rockwood, S.D.; Jensen, R.J.; Lyman, J.L.; Aldridge, J.P. III.

1987-04-07

Multiple photon absorption from an intense beam of infrared laser light may be used to induce selective chemical reactions in molecular species which result in isotope separation or enrichment. The molecular species must have a sufficient density of vibrational states in its vibrational manifold that, is the presence of sufficiently intense infrared laser light tuned to selectively excite only those molecules containing a particular isotope, multiple photon absorption can occur. By this technique, for example, intense CO[sub 2] laser light may be used to highly enrich [sup 34]S in natural SF[sub 6] and [sup 11]B in natural BCl[sub 3]. 8 figs.

Heterometallic Ru-Pt metallacycle for two-photon photodynamic therapy.

PubMed

Zhou, Zhixuan; Liu, Jiangping; Rees, Thomas W; Wang, Heng; Li, Xiaopeng; Chao, Hui; Stang, Peter J

2018-05-29

As an effective and noninvasive treatment of various diseases, photodynamic therapy (PTD) relies on the combination of light, a photosensitizer, and oxygen to generate cytotoxic reactive oxygen species that can damage malignant tissue. Much attention has been paid to covalent modifications of the photosensitizers to improve their photophysical properties and to optimize the pathway of the photosensitizers interacting with cells within the target tissue. Herein we report the design and synthesis of a supramolecular heterometallic Ru-Pt metallacycle via coordination-driven self-assembly. While inheriting the excellent photostability and two-photon absorption characteristics of the Ru(II) polypyridyl precursor, the metallacycle also exhibits red-shifted luminescence to the near-infrared region, a larger two-photon absorption cross-section, and higher singlet oxygen generation efficiency, making it an excellent candidate as a photosensitizer for PTD. Cellular studies reveal that the metallacycle selectively accumulates in mitochondria and nuclei upon internalization. As a result, singlet oxygen generated by photoexcitation of the metallacycle can efficiently trigger cell death via the simultaneous damage to mitochondrial function and intranuclear DNA. In vivo studies on tumor-bearing mice show that the metallacycle can efficiently inhibit tumor growth under a low light dose with minimal side effects. The supramolecular approach presented in this work provides a paradigm for the development of PDT agents with high efficacy.

Ghost Spectroscopy with Classical Thermal Light Emitted by a Superluminescent Diode

NASA Astrophysics Data System (ADS)

Janassek, Patrick; Blumenstein, Sébastien; Elsäßer, Wolfgang

2018-02-01

We propose and realize the first classical ghost-imaging (GI) experiment in the frequency or wavelength domain, thus performing ghost spectroscopy using thermal light exhibiting photon bunching. The required wavelength correlations are provided by light emitted by spectrally broadband near-infrared amplified spontaneous emission of a semiconductor-based superluminescent diode. They are characterized by wavelength-resolved intensity cross-correlation measurements utilizing two-photon-absorption interferometry. Finally, a real-world spectroscopic application of this ghost spectroscopy with a classical light scheme is demonstrated in which an absorption band of trichloromethane (chloroform) at 1214 nm is reconstructed with a spectral resolution of 10 nm as a proof-of-principle experiment. This ghost-spectroscopy work fills the gap of a hitherto missing analogy between the spatial and the spectral domain in classical GI modalities, with the expectation of contributing towards a broader dissemination of correlated photon ghost modalities, hence paving the way towards more applications which exploit the favorable advantages.

Atom beams split by gentle persuasion

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

Pool, R.

1994-02-25

Two different research teams have taken a big step toward atom interferometry. They have succeeded in splitting atomic beams by using atoms in spin states that neither absorb nor reemit laser light. By proper adjustment of experimental conditions, atoms are changed from one spin state to another, without passing through the intermediary excited state. The atoms in essence absorb momentum from the laser photons, without absorption or emission of photons. The change in momentum deflects atoms in the proper spin state.

Photonic Waveguide Choke Joint with Absorptive Loading

NASA Technical Reports Server (NTRS)

Wollack, Edward J. (Inventor); U-Yen, Kongpop (Inventor); Chuss, David T. (Inventor)

2016-01-01

A photonic waveguide choke includes a first waveguide flange member having periodic metal tiling pillars, a dissipative dielectric material positioned within an area between the periodic metal tiling pillars and a second waveguide flange member disposed to be coupled with the first waveguide flange member and in spaced-apart relationship separated by a gap. The first waveguide flange member has a substantially smooth surface, and the second waveguide flange member has an array of two-dimensional pillar structures formed therein.

Research Investigation Directed Toward Extending the Useful Range of the Electromagnetic Spectrum. [atomic spectra and electronic structure of alkali metals

NASA Technical Reports Server (NTRS)

Hartmann, S. R.; Happer, W.

1974-01-01

The report discusses completed and proposed research in atomic and molecular physics conducted at the Columbia Radiation Laboratory from July 1972 to June 1973. Central topics described include the atomic spectra and electronic structure of alkali metals and helium, molecular microwave spectroscopy, the resonance physics of photon echoes in some solid state systems (including Raman echoes, superradiance, and two photon absorption), and liquid helium superfluidity.

Multi-photon excited coherent random laser emission in ZnO powders

NASA Astrophysics Data System (ADS)

Tolentino Dominguez, Christian; Gomes, Maria De A.; Macedo, Zélia S.; de Araújo, Cid B.; Gomes, Anderson S. L.

2014-11-01

We report the observation and analysis of anti-Stokes coherent random laser (RL) emission from zinc oxide (ZnO) powders excited by one-, two- or three-photon femtosecond laser radiation. The ZnO powders were produced via a novel proteic sol-gel, low-cost and environmentally friendly route using coconut water in the polymerization step of the metal precursor. One- and two-photon excitation at 354 nm and 710 nm, respectively, generated single-band emissions centred at about 387 nm. For three-photon excitation, the emission spectra showed a strong ultraviolet (UV) band (380-396 nm) attributed to direct three-photon absorption from the valence band to the conduction band. The presence of an intensity threshold and a bandwidth narrowing of the UV band from about 20 to 4 nm are clear evidence of RL action. The observation of multiple sub-nanometre narrow peaks in the emission spectra for excitation above the RL threshold is consistent with random lasing by coherent feedback.

Observing quantum control of up-conversion luminescence in Dy3+ ion doped glass from weak to intermediate shaped femtosecond laser fields

NASA Astrophysics Data System (ADS)

Liu, Pei; Cheng, Wenjing; Yao, Yunhua; Xu, Cheng; Zheng, Ye; Deng, Lianzhong; Jia, Tianqing; Qiu, Jianrong; Sun, Zhenrong; Zhang, Shian

2017-11-01

Controlling the up-conversion luminescence of rare-earth ions in real-time, in a dynamical and reversible manner, is very important for their application in laser sources, fiber-optic communications, light-emitting diodes, color displays and biological systems. In previous studies, the up-conversion luminescence control mainly focused on the weak femtosecond laser field. Here, we further extend this control behavior from weak to intermediate femtosecond laser fields. In this work, we experimentally and theoretically demonstrate that the up-conversion luminescence in Dy3+ ion doped glass can be artificially controlled by a π phase step modulation, but the up-conversion luminescence control behavior will be affected by the femtosecond laser intensity, and the up-conversion luminescence is suppressed by lower laser intensity while enhanced by higher laser intensity. We establish a new theoretical model (i.e. the fourth-order perturbation theory) to explain the physical control mechanism by considering the two- and four-photon absorption processes, and the theoretical results show that the relative weight of four-photon absorption in the whole excitation process will increase with the increase in laser intensity, and the interference between two- and four-photon absorptions results in up-conversion luminescence control modulation under different laser intensities. These theoretical and experimental works can provide a new method to control and understand up-conversion luminescence in rare-earth ions, and also may open a new opportunity to the related application areas of rare-earth ions.

Emerging technologies in Si active photonics

NASA Astrophysics Data System (ADS)

Wang, Xiaoxin; Liu, Jifeng

2018-06-01

Silicon photonics for synergistic electronic–photonic integration has achieved remarkable progress in the past two decades. Active photonic devices, including lasers, modulators, and photodetectors, are the key challenges for Si photonics to meet the requirement of high bandwidth and low power consumption in photonic datalinks. Here we review recent efforts and progress in high-performance active photonic devices on Si, focusing on emerging technologies beyond conventional foundry-ready Si photonics devices. For emerging laser sources, we will discuss recent progress towards efficient monolithic Ge lasers, mid-infrared GeSn lasers, and high-performance InAs quantum dot lasers on Si for data center applications in the near future. We will then review novel modulator materials and devices beyond the free carrier plasma dispersion effect in Si, including GeSi and graphene electro-absorption modulators and plasmonic-organic electro-optical modulators, to achieve ultralow power and high speed modulation. Finally, we discuss emerging photodetectors beyond epitaxial Ge p–i–n photodiodes, including GeSn mid-infrared photodetectors, all-Si plasmonic Schottky infrared photodetectors, and Si quanta image sensors for non-avalanche, low noise single photon detection and photon counting. These emerging technologies, though still under development, could make a significant impact on the future of large-scale electronicSilicon photonics for synergistic electronic-photonic integration has achieved remarkable progress in the past two decades. Active photonic devices, including lasers, modulators, and photodetectors, are the key challenges for Si photonics to meet the requirement of high bandwidth and low power consumption in photonic datalinks. Here we review recent efforts and progress in high-performance active photonic devices on Si, focusing on emerging technologies beyond conventional foundry-ready Si photonics devices. For emerging laser sources, we will discuss recent progress towards efficient monolithic Ge lasers, mid-infrared GeSn lasers, and high-performance InAs quantum dot lasers on Si for data center applications in the near future. We will then review novel modulator materials and devices beyond the free carrier plasma dispersion effect in Si, including GeSi and graphene electro-absorption modulators and plasmonic-organic electro–optical modulators, to achieve ultralow power and high speed modulation. Finally, we discuss emerging photodetectors beyond epitaxial Ge p–i–n photodiodes, including GeSn mid-infrared photodetectors, all-Si plasmonic Schottky infrared photodetectors, and Si quanta image sensors for non-avalanche, low noise single photon detection and photon counting. These emerging technologies, though still under development, could make a significant impact on the future of large-scale electronic–photonic integration with performance inaccessible from conventional Si photonics technologies-photonic integration with performance inaccessible from conventional Si photonics technologies.

Sensitizers in EUV chemically amplified resist: mechanism of sensitivity improvement

NASA Astrophysics Data System (ADS)

Vesters, Yannick; Jiang, Jing; Yamamoto, Hiroki; De Simone, Danilo; Kozawa, Takahiro; De Gendt, Stefan; Vandenberghe, Geert

2018-03-01

EUV lithography utilizes photons with 91.6 eV energy to ionize resists, generate secondary electrons, and enable electron driven reactions that produce acid in chemically amplified photoresist. Efficiently using the available photons is of key importance. Unlike DUV lithography, where photons are selectively utilized by photoactive compounds, photons at 13.5nm wavelength ionize almost all materials. Nevertheless, specific elements have a significantly higher atomic photon-absorption cross section at 91.6 eV. To increase photon absorption, sensitizer molecules, containing highly absorbing elements, can be added to photoresist formulations. These sensitizers have gained growing attention in recent years, showing significant sensitivity improvement. But there are few experimental evidences that the sensitivity improvement is due to the higher absorption only, as adding metals salts into the resist formulation can induce other mechanisms, like modification of the dissolution rate, potentially affecting patterning performance. In this work, we used different sensitizers in chemically amplified resist. We measured experimentally the absorption of EUV light, the acid yield, the dissolution rate and the patterning performance of the resists. Surprisingly, the absorption of EUV resist was decreased with addition of metal salt sensitizers. Nevertheless, the resist with sensitizer showed a higher acid yield. Sensitizer helps achieving higher PAG conversion to acid, notably due to an increase of the secondary electron generation. Patterning data confirm a significant sensitivity improvement, but at the cost of roughness degradation at high sensitizer loading. This can be explained by the chemical distribution of the sensitizer in the resist combined with a modification of the dissolution contrast, as observed by Dissolution Rate Monitor.

Polarization-independent absorption enhancement in a graphene square array with a cascaded grating structure.

PubMed

Wu, Jun

2018-03-01

The polarization-independent enhanced absorption effect of graphene in the near-infrared range is investigated. This is achieved by placing a graphene square array on top of a dielectric square array backed by a two-dimensional multilayer grating. Total optical absorption in graphene can be attributed to critical coupling, which is achieved through the combined effect of guided-mode resonance with the dielectric square array and the photonic band gap with the two-dimensional multilayer grating. To reveal the physical origin of such a phenomenon, the electromagnetic field distributions for both polarizations are illustrated. The designed graphene absorber exhibits near-unity polarization-independent absorption at resonance with an ultra-narrow spectrum. Moreover, the polarization-independent absorption can be tuned simply by changing the geometric parameters. The results may have promising potential for the design of graphene-based optoelectronic devices.

Stochastic parameterization for light absorption by internally mixed BC/dust in snow grains for application to climate models

NASA Astrophysics Data System (ADS)

Liou, K. N.; Takano, Y.; He, C.; Yang, P.; Leung, L. R.; Gu, Y.; Lee, W. L.

2014-06-01

A stochastic approach has been developed to model the positions of BC (black carbon)/dust internally mixed with two snow grain types: hexagonal plate/column (convex) and Koch snowflake (concave). Subsequently, light absorption and scattering analysis can be followed by means of an improved geometric-optics approach coupled with Monte Carlo photon tracing to determine BC/dust single-scattering properties. For a given shape (plate, Koch snowflake, spheroid, or sphere), the action of internal mixing absorbs substantially more light than external mixing. The snow grain shape effect on absorption is relatively small, but its effect on asymmetry factor is substantial. Due to a greater probability of intercepting photons, multiple inclusions of BC/dust exhibit a larger absorption than an equal-volume single inclusion. The spectral absorption (0.2-5 µm) for snow grains internally mixed with BC/dust is confined to wavelengths shorter than about 1.4 µm, beyond which ice absorption predominates. Based on the single-scattering properties determined from stochastic and light absorption parameterizations and using the adding/doubling method for spectral radiative transfer, we find that internal mixing reduces snow albedo substantially more than external mixing and that the snow grain shape plays a critical role in snow albedo calculations through its forward scattering strength. Also, multiple inclusion of BC/dust significantly reduces snow albedo as compared to an equal-volume single sphere. For application to land/snow models, we propose a two-layer spectral snow parameterization involving contaminated fresh snow on top of old snow for investigating and understanding the climatic impact of multiple BC/dust internal mixing associated with snow grain metamorphism, particularly over mountain/snow topography.

Stochastic Parameterization for Light Absorption by Internally Mixed BC/dust in Snow Grains for Application to Climate Models

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

Liou, K. N.; Takano, Y.; He, Cenlin

2014-06-27

A stochastic approach to model the positions of BC/dust internally mixed with two snow-grain types has been developed, including hexagonal plate/column (convex) and Koch snowflake (concave). Subsequently, light absorption and scattering analysis can be followed by means of an improved geometric-optics approach coupled with Monte Carlo photon tracing to determine their single-scattering properties. For a given shape (plate, Koch snowflake, spheroid, or sphere), internal mixing absorbs more light than external mixing. The snow-grain shape effect on absorption is relatively small, but its effect on the asymmetry factor is substantial. Due to a greater probability of intercepting photons, multiple inclusions ofmore » BC/dust exhibit a larger absorption than an equal-volume single inclusion. The spectral absorption (0.2 – 5 um) for snow grains internally mixed with BC/dust is confined to wavelengths shorter than about 1.4 um, beyond which ice absorption predominates. Based on the single-scattering properties determined from stochastic and light absorption parameterizations and using the adding/doubling method for spectral radiative transfer, we find that internal mixing reduces snow albedo more than external mixing and that the snow-grain shape plays a critical role in snow albedo calculations through the asymmetry factor. Also, snow albedo reduces more in the case of multiple inclusion of BC/dust compared to that of an equal-volume single sphere. For application to land/snow models, we propose a two-layer spectral snow parameterization containing contaminated fresh snow on top of old snow for investigating and understanding the climatic impact of multiple BC/dust internal mixing associated with snow grain metamorphism, particularly over mountains/snow topography.« less

Design on compatible stealth photonic crystal of nearmiddle infrared and 1.06 μm laser

NASA Astrophysics Data System (ADS)

Zhang, Ji-kui; Wang, Jia-Chun; Wang, Qi-Chao

2016-01-01

In the near and middle infrared atmospheric window, infrared stealth material require a low absorptivity (which means a low emissivity according to Kirchhoff's law of black body), at the same time, it also requires high absorptivity so as to decrease the reflectance at military laser wavelength of 1.06μm. Under this circumstances, compatible stealth of infrared and laser is an urgent demand, but the demand is ambivalent for conventional materials. Photonic crystal (PC), as a new type of artificial periodic structure function material, can realize broadband thermal infrared stealth based on its high-reflection photon forbidden band(also called photonic band gap). The high-reflection photon forbidden band of PC can be adjusted to near and middle infrared wave band through some rational methods. When a defect was added into the periodic structure of PC, a "hole-digging" reflection spectrum, which is high absorption at military laser wavelength of 1.06μm, can be achieved, so compatible stealth of near and middle infrared and military laser wavelength of 1.06μm can be achieved too. In this paper, we selected near and middle infrared-transparent materials, Te and MgF2 , as high refractive index and low refractive index material respectively, and designed a one-dimensional one-defect-mode PC whose photon forbidden band was broadened to 1-5μm by constructing two photonic crystals into one. The optical property of the PC was calculated by Transfer matrix method(TMM) of thin-film optical theory, and the results shows that the as-designed PC has a high spectral reflectance in the near and middle infrared band, among which the reflectivity in 1.68μm 5.26μm band reached more than 90%, and the 2.48 5.07μm band even reached 99.99%. The result also shows that between the band gap of 1-5μm, there are one defect mode locating in the wavelength of 1.06μm, whose reflectance is below 0.70%, which means its spectral absorptivity is greater than 99.30%. All the above we have discussed proved that this "hole-digging spectrum" PC can realize the compatible stealth of near and middle infrared and 1.06μm military laser.

Enigmatic photon absorption in plasmas near solar interior conditions

NASA Astrophysics Data System (ADS)

Iglesias, Carlos A.

2015-06-01

Large systematic discrepancies between theoretical and experimental photon absorption of Fe plasmas applicable to the solar interior were reported [Bailey et al., Nature 517, 56 (2015)]. The disagreement is examined in the context of the Thomas-Reiche-Kuhn f-sum rule. The analysis identifies several anomalies in the experimental results.

Silole-Based Red Fluorescent Organic Dots for Bright Two-Photon Fluorescence In vitro Cell and In vivo Blood Vessel Imaging.

PubMed

Chen, Bin; Feng, Guangxue; He, Bairong; Goh, Chiching; Xu, Shidang; Ramos-Ortiz, Gabriel; Aparicio-Ixta, Laura; Zhou, Jian; Ng, Laiguan; Zhao, Zujin; Liu, Bin; Tang, Ben Zhong

2016-02-10

Robust luminescent dyes with efficient two-photon fluorescence are highly desirable for biological imaging applications, but those suitable for organic dots fabrication are still rare because of aggregation-caused quenching. In this work, a red fluorescent silole, 2,5-bis[5-(dimesitylboranyl)thiophen-2-yl]-1-methyl-1,3,4-triphenylsilole ((MesB)2 DTTPS), is synthesized and characterized. (MesB)2 DTTPS exhibits enhanced fluorescence efficiency in nanoaggregates, indicative of aggregation-enhanced emission (AEE). The organic dots fabricated by encapsulating (MesB)2 DTTPS within lipid-PEG show red fluorescence peaking at 598 nm and a high fluorescence quantum yield of 32%. Upon excitation at 820 nm, the dots show a large two-photon absorption cross section of 3.43 × 10(5) GM, which yields a two-photon action cross section of 1.09 × 10(5) GM. These (MesB)2 DTTPS dots show good biocompatibility and are successfully applied to one-photon and two-photon fluorescence imaging of MCF-7 cells and two-photon in vivo visualization of the blood vascular of mouse muscle in a high-contrast and noninvasive manner. Moreover, the 3D blood vasculature located at the mouse ear skin with a depth of over 100 μm can also be visualized clearly, providing the spatiotemporal information about the whole blood vascular network. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Water-Soluble Triarylborane Chromophores for One- and Two-Photon Excited Fluorescence Imaging of Mitochondria in Cells.

PubMed

Griesbeck, Stefanie; Zhang, Zuolun; Gutmann, Marcus; Lühmann, Tessa; Edkins, Robert M; Clermont, Guillaume; Lazar, Adina N; Haehnel, Martin; Edkins, Katharina; Eichhorn, Antonius; Blanchard-Desce, Mireille; Meinel, Lorenz; Marder, Todd B

2016-10-04

Three water-soluble tetracationic quadrupolar chromophores comprising two three-coordinate boron π-acceptor groups bridged by thiophene-containing moieties were synthesised for biological imaging applications. Compound 3 containing the bulkier 5-(3,5-Me2 C6 H2 )-2,2'-(C4 H2 S)2 -5'-(3,5-Me2 C6 H2 ) bridge is stable over a long period of time, exhibits a high fluorescence quantum yield and strong one- and two-photon absorption (TPA), and has a TPA cross section of 268 GM at 800 nm in water. Confocal laser scanning fluorescence microscopy studies in live cells indicated localisation of the chromophore at the mitochondria; moreover, cytotoxicity measurements proved biocompatibility. Thus, chromophore 3 has excellent potential for one- and two-photon-excited fluorescence imaging of mitochondrial function in cells. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Impact of material absorption on supercontinuum generation in liquid core photonic crystal fiber

NASA Astrophysics Data System (ADS)

Nithyanandan, K.; Raja, Vasantha Jayakantha; Uthayakumar, T.; Porsezian, K.

2013-06-01

The impact of material absorption on supercontinuum generation (SCG) in liquid core photonic crystal fiber (LCPCF) is presented. While PCFs with cores made from different glasses are well studied in previous works with saturable nonlinear response (SNL), in this paper, it is planned to investigate the dynamics of nonlinear processes of supercontinuum generation in high-index fiber with material absorption to understand the physical phenomena of pulse propagation.

X-Ray Attenuation and Absorption for Materials of Dosimetric Interest

National Institute of Standards and Technology Data Gateway

SRD 126 X-Ray Attenuation and Absorption for Materials of Dosimetric Interest (Web, free access)   Tables and graphs of the photon mass attenuation coefficient and the mass energy-absorption coefficient are presented for all of the elements Z = 1 to 92, and for 48 compounds and mixtures of radiological interest. The tables cover energies of the photon (x-ray, gamma ray, bremsstrahlung) from 1 keV to 20 MeV.

Chiral quantum optics.

PubMed

Lodahl, Peter; Mahmoodian, Sahand; Stobbe, Søren; Rauschenbeutel, Arno; Schneeweiss, Philipp; Volz, Jürgen; Pichler, Hannes; Zoller, Peter

2017-01-25

Advanced photonic nanostructures are currently revolutionizing the optics and photonics that underpin applications ranging from light technology to quantum-information processing. The strong light confinement in these structures can lock the local polarization of the light to its propagation direction, leading to propagation-direction-dependent emission, scattering and absorption of photons by quantum emitters. The possibility of such a propagation-direction-dependent, or chiral, light-matter interaction is not accounted for in standard quantum optics and its recent discovery brought about the research field of chiral quantum optics. The latter offers fundamentally new functionalities and applications: it enables the assembly of non-reciprocal single-photon devices that can be operated in a quantum superposition of two or more of their operational states and the realization of deterministic spin-photon interfaces. Moreover, engineered directional photonic reservoirs could lead to the development of complex quantum networks that, for example, could simulate novel classes of quantum many-body systems.

Thermally activated delayed fluorescence organic dots for two-photon fluorescence lifetime imaging

NASA Astrophysics Data System (ADS)

He, Tingchao; Ren, Can; Li, Zhuohua; Xiao, Shuyu; Li, Junzi; Lin, Xiaodong; Ye, Chuanxiang; Zhang, Junmin; Guo, Lihong; Hu, Wenbo; Chen, Rui

2018-05-01

Autofluorescence is a major challenge in complex tissue imaging when molecules present in the biological tissue compete with the fluorophore. This issue may be resolved by designing organic molecules with long fluorescence lifetimes. The present work reports the two-photon absorption (TPA) properties of a thermally activated delayed fluorescence (TADF) molecule with carbazole as the electron donor and dicyanobenzene as the electron acceptor (i.e., 4CzIPN). The results indicate that 4CzIPN exhibits a moderate TPA cross-section (˜9 × 10-50 cm4 s photon-1), high fluorescence quantum yield, and a long fluorescence lifetime (˜1.47 μs). 4CzIPN was compactly encapsulated into an amphiphilic copolymer via nanoprecipitation to achieve water-soluble organic dots. Interestingly, 4CzIPN organic dots have been utilized in applications involving two-photon fluorescence lifetime imaging (FLIM). Our work aptly demonstrates that TADF molecules are promising candidates of nonlinear optical probes for developing next-generation multiphoton FLIM applications.

Non-Scanning Fiber-Optic Near-Infrared Beam Led to Two-Photon Optogenetic Stimulation In-Vivo

PubMed Central

Shivalingaiah, Shivaranjani; Dennis, Torry S.; Morris-Bobzean, Samara A.; Li, Ting; Perrotti, Linda I.; Mohanty, Samarendra K.

2014-01-01

Stimulation of specific neurons expressing opsins in a targeted region to manipulate brain function has proved to be a powerful tool in neuroscience. However, the use of visible light for optogenetic stimulation is invasive due to low penetration depth and tissue damage owing to larger absorption and scattering. Here, we report, for the first time, in-depth non-scanning fiber-optic two-photon optogenetic stimulation (FO-TPOS) of neurons in-vivo in transgenic mouse models. In order to optimize the deep-brain stimulation strategy, we characterized two-photon activation efficacy at different near-infrared laser parameters. The significantly-enhanced in-depth stimulation efficiency of FO-TPOS as compared to conventional single-photon beam was demonstrated both by experiments and Monte Carlo simulation. The non-scanning FO-TPOS technology will lead to better understanding of the in-vivo neural circuitry because this technology permits more precise and less invasive anatomical delivery of stimulation. PMID:25383687

Sensing coherent phonons with two-photon interference

NASA Astrophysics Data System (ADS)

Ding, Ding; Yin, Xiaobo; Li, Baowen

2018-02-01

Detecting coherent phonons pose different challenges compared to coherent photons due to the much stronger interaction between phonons and matter. This is especially true for high frequency heat carrying phonons, which are intrinsic lattice vibrations experiencing many decoherence events with the environment, and are thus generally assumed to be incoherent. Two photon interference techniques, especially coherent population trapping (CPT) and electromagnetically induced transparency (EIT), have led to extremely sensitive detection, spectroscopy and metrology. Here, we propose the use of two photon interference in a three-level system to sense coherent phonons. Unlike prior works which have treated phonon coupling as damping, we account for coherent phonon coupling using a full quantum-mechanical treatment. We observe strong asymmetry in absorption spectrum in CPT and negative dispersion in EIT susceptibility in the presence of coherent phonon coupling which cannot be accounted for if only pure phonon damping is considered. Our proposal has application in sensing heat carrying coherent phonons effects and understanding coherent bosonic multi-pathway interference effects in three coupled oscillator systems.

Nonlinear optical and electroabsorption spectra of polydiacetylene crystals and films

NASA Astrophysics Data System (ADS)

Mukhopadhyay, D.; Soos, Z. G.

1996-01-01

Vibronic structure of nonlinear optical (NLO) coefficients is developed within the Condon approximation, displaced harmonic oscillators, and crude adiabatic states. The displacements of backbone modes of conjugated polymers are taken from vibrational data on the ground and 1B excited state. NLO resonances are modeled by three excitations and transition moments taken from Pariser-Parr-Pople (PPP) theory and optimized to polydiacetylene (PDA) spectra in crystals and films, with blue-shifted 1B exciton. The joint analysis of third-harmonic-generation, two-photon absorption, and nondegenerate four-wave-mixing spectra of PDA crystals and films shows weak two-photon absorption to 2A below 1B, leading to overlapping resonances in the THG spectrum, strong two-photon absorption to an nA state some 35% above 1B, and weak Raman resonances in nondegenerate FWM spectra. The full π-π* spectrum contributes to Stark shifts and field-induced transitions, as shown by PPP results for PDA oligomers. The Stark shift dominates high-resolution electroabsorption (EA) spectra of PDA crystals below 10 K. The close correspondence between EA and the first-derivative I'(ω) of the linear absorption above the 1B exciton in PDA crystals provides an experimental separation of vibrational and electronic contributions that limits any even-parity state in this 0.5 eV interval. An oscillator-strength sum rule is applied to the convergence of PDA oligomers with increasing length, N, and the crystal oscillator strengths are obtained without adjustable parameters. The sum rule for the 1B exciton implies large transition moments to higher-energy Ag states, whose locations in recent models are contrasted to PPP results. Joint analysis of NLO and EA spectra clarifies when a few electronic excitations are sufficient, distinguishes between vibrational and electronic contributions, and supports similar π-electron interactions in conjugated molecules and polymers.

Evaluation of mitochondrial activity by two-photon absorption with near-field multioptical fiber probes

NASA Astrophysics Data System (ADS)

Kanazashi, Yasuaki; Takara, Naoshi; Iwami, Kentaro; Ohta, Yoshihiro; Umeda, Norihiro

2018-04-01

pH measurements enable the direct monitoring and evaluation of mitochondrial activity. We constructed a scanning near-field optical microscopy system with multioptical fiber probes using the two-photon absorption of a pH-sensitive fluorescent dye, SNARF-4F, to measure the activity difference of mitochondrial aggregates. pH can be monitored through the fluorescence intensity ratio (FIR) of SNARF-4F. We derived a calibration curve of the FIR as a function of pH. The FIR dynamic responses were measured by adding hydrochloric acid to the buffer solution. Using the developed system, we simultaneously measured the pH changes at two different locations in the SNARF-4F solution. Mitochondrial samples were prepared using optical tweezers to control the number and position of mitochondria. Mitochondrial pH changes (ΔpH) between 0.05 and 0.57 were observed after adding a nutritional supplement (malate and glutamate). In addition, in the comparative experiment on the activities of two mitochondrial populations, the obtained result suggested that the activity differs depending on the difference in the number of mitochondria.

Two-Photon Absorption Characterization of HgCdTe

DTIC Science & Technology

1990-07-30

r17 L3 _ , 952L2 9521- 240 L 976 , 210 979 LU ’~-~’ ~180~ - Eg=136.0 _-0.5 m eV Z-150 T 7K W FIG. 2. Wavelength depend- 0120[0 0 12 > ence of the...8217 / Army Center for Night Vision and Electro-Optics, Contract 0 i No. DAAB07-87-C-FO94. j W 9.329 FIG. 12. Wavelength depend- w ence of the...pres- presented in Fig. I. The two-photon magnetoabsorption ence of impurities and defects in samples of MCT with (TPMA) transitions are indicated by

Time-resolved two-photon spectroscopy of photosystem I determines hidden carotenoid dark-state dynamics.

PubMed

Wehling, Axel; Walla, Peter J

2005-12-29

We present time-resolved fs two-photon pump-probe data measured with photosystem I (PS I) of Thermosynechococcus elongatus. Two-photon excitation (lambda(exc)/2 = 575 nm) in the spectral region of the optically forbidden first excited singlet state of the carotenoids, Car S1, gives rise to a 800 fs and a 9 ps decay component of the Car S1 --> S(n) excited-state absorption with an amplitude of about 47 +/- 16% and 53 +/- 10%, respectively. By measuring a solution of pure beta-carotene under exactly the same conditions, only a 9 ps decay component can be observed. Exciting PS I at exactly the same spectral region via one-photon excitation (lambda(exc) = 575 nm) also does not show any sub-ps component. We ascribe the observed constant of 800 fs to a portion of about 47 +/- 16% beta-carotene states that can potentially transfer their energy efficiently to chlorophyll pigments via the optically dark Car S1 state. We compared these data with conventional one-photon pump-probe data, exciting the optically allowed second excited state, Car S2. This comparison demonstrates that the fast dynamics of the optically forbidden state can hardly be unravelled via conventional one-photon excitation only because the corresponding Car S1 populations are too small after Car S2 --> Car S1 internal conversion. A direct comparison of the amplitudes of the Car S1 --> S(n) excited-state absorption of PS I and beta-carotene observed after Car S2 excitation allows determination of a quantum yield for the Car S1 formation in PS I of 44 +/- 5%. In conclusion, an overall Car S2 --> Chl energy-transfer efficiency of approximately 69 +/- 5% is observed at room temperature with 56 +/- 5% being transferred via Car S2 and probably very hot Car S1 states and 13 +/- 5% being transferred via hot and "cold" Car S1 states.

Photonic crystals for improving light absorption in organic solar cells

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

Duché, D., E-mail: david.duche@im2np.fr; Le Rouzo, J.; Masclaux, C.

2015-02-07

We theoretically and experimentally study the structuration of organic solar cells in the shape of photonic crystal slabs. By taking advantage of the optical properties of photonic crystals slabs, we show the possibility to couple Bloch modes with very low group velocities in the active layer of the cells. These Bloch modes, also called slow Bloch modes (SBMs), allow increasing the lifetime of photons within the active layer. Finally, we present experimental demonstration performed by using nanoimprint to directly pattern the standard poly-3-hexylthiophène:[6,6]-phenyl-C61-butiryc acid methyl ester organic semiconductor blend in thin film form in the shape of a photonic crystalmore » able to couple SBMs. In agreement with the model, optical characterizations will demonstrate significant photonic absorption gains.« less

Photonic light-trapping versus Lambertian limits in thin film silicon solar cells with 1D and 2D periodic patterns.

PubMed

Bozzola, Angelo; Liscidini, Marco; Andreani, Lucio Claudio

2012-03-12

We theoretically investigate the light-trapping properties of one- and two-dimensional periodic patterns etched on the front surface of c-Si and a-Si thin film solar cells with a silver back reflector and an anti-reflection coating. For each active material and configuration, absorbance A and short-circuit current density Jsc are calculated by means of rigorous coupled wave analysis (RCWA), for different active materials thicknesses in the range of interest of thin film solar cells and in a wide range of geometrical parameters. The results are then compared with Lambertian limits to light-trapping for the case of zero absorption and for the general case of finite absorption in the active material. With a proper optimization, patterns can give substantial absorption enhancement, especially for 2D patterns and for thinner cells. The effects of the photonic patterns on light harvesting are investigated from the optical spectra of the optimized configurations. We focus on the main physical effects of patterning, namely a reduction of reflection losses (better impedance matching conditions), diffraction of light in air or inside the cell, and coupling of incident radiation into quasi-guided optical modes of the structure, which is characteristic of photonic light-trapping.

Beyond the electric-dipole approximation: A formulation and implementation of molecular response theory for the description of absorption of electromagnetic field radiation.

PubMed

List, Nanna Holmgaard; Kauczor, Joanna; Saue, Trond; Jensen, Hans Jørgen Aagaard; Norman, Patrick

2015-06-28

We present a formulation of molecular response theory for the description of a quantum mechanical molecular system in the presence of a weak, monochromatic, linearly polarized electromagnetic field without introducing truncated multipolar expansions. The presentation focuses on a description of linear absorption by adopting the energy-loss approach in combination with the complex polarization propagator formulation of response theory. Going beyond the electric-dipole approximation is essential whenever studying electric-dipole-forbidden transitions, and in general, non-dipolar effects become increasingly important when addressing spectroscopies involving higher-energy photons. These two aspects are examined by our study of the near K-edge X-ray absorption fine structure of the alkaline earth metals (Mg, Ca, Sr, Ba, and Ra) as well as the trans-polyenes. In following the series of alkaline earth metals, the sizes of non-dipolar effects are probed with respect to increasing photon energies and a detailed assessment of results is made in terms of studying the pertinent transition electron densities and in particular their spatial extension in comparison with the photon wavelength. Along the series of trans-polyenes, the sizes of non-dipolar effects are probed for X-ray spectroscopies on organic molecules with respect to the spatial extension of the chromophore.

A new Monte Carlo code for light transport in biological tissue.

PubMed

Torres-García, Eugenio; Oros-Pantoja, Rigoberto; Aranda-Lara, Liliana; Vieyra-Reyes, Patricia

2018-04-01

The aim of this work was to develop an event-by-event Monte Carlo code for light transport (called MCLTmx) to identify and quantify ballistic, diffuse, and absorbed photons, as well as their interaction coordinates inside the biological tissue. The mean free path length was computed between two interactions for scattering or absorption processes, and if necessary scatter angles were calculated, until the photon disappeared or went out of region of interest. A three-layer array (air-tissue-air) was used, forming a semi-infinite sandwich. The light source was placed at (0,0,0), emitting towards (0,0,1). The input data were: refractive indices, target thickness (0.02, 0.05, 0.1, 0.5, and 1 cm), number of particle histories, and λ from which the code calculated: anisotropy, scattering, and absorption coefficients. Validation presents differences less than 0.1% compared with that reported in the literature. The MCLTmx code discriminates between ballistic and diffuse photons, and inside of biological tissue, it calculates: specular reflection, diffuse reflection, ballistics transmission, diffuse transmission and absorption, and all parameters dependent on wavelength and thickness. The MCLTmx code can be useful for light transport inside any medium by changing the parameters that describe the new medium: anisotropy, dispersion and attenuation coefficients, and refractive indices for specific wavelength.

Electron-positron pair production by gamma-rays in an anisotropic flux of soft photons, and application to pulsar polar caps

NASA Astrophysics Data System (ADS)

Voisin, Guillaume; Mottez, Fabrice; Bonazzola, Silvano

2018-02-01

Electron-positron pair production by collision of photons is investigated in view of application to pulsar physics. We compute the absorption rate of individual gamma-ray photons by an arbitrary anisotropic distribution of softer photons, and the energy and angular spectrum of the outgoing leptons. We work analytically within the approximation that 1 ≫ mc2/E > ɛ/E, with E and ɛ the gamma-ray and soft-photon maximum energy and mc2 the electron mass energy. We give results at leading order in these small parameters. For practical purposes, we provide expressions in the form of Laurent series which give correct reaction rates in the isotropic case within an average error of ˜ 7 per cent. We apply this formalism to gamma-rays flying downward or upward from a hot neutron star thermally radiating at a uniform temperature of 106 K. Other temperatures can be easily deduced using the relevant scaling laws. We find differences in absorption between these two extreme directions of almost two orders of magnitude, much larger than our error estimate. The magnetosphere appears completely opaque to downward gamma-rays while there are up to ˜ 10 per cent chances of absorbing an upward gamma-ray. We provide energy and angular spectra for both upward and downward gamma-rays. Energy spectra show a typical double peak, with larger separation at larger gamma-ray energies. Angular spectra are very narrow, with an opening angle ranging from 10-3 to 10-7 radians with increasing gamma-ray energies.

A two photon absorption laser induced fluorescence diagnostic for fusion plasmas.

PubMed

Magee, R M; Galante, M E; McCarren, D; Scime, E E; Boivin, R L; Brooks, N H; Groebner, R J; Hill, D N; Porter, G D

2012-10-01

The quality of plasma produced in a magnetic confinement fusion device is influenced to a large extent by the neutral gas surrounding the plasma. The plasma is fueled by the ionization of neutrals, and charge exchange interactions between edge neutrals and plasma ions are a sink of energy and momentum. Here we describe a diagnostic capable of measuring the spatial distribution of neutral gas in a magnetically confined fusion plasma. A high intensity (5 MW/cm(2)), narrow bandwidth (0.1 cm(-1)) laser is injected into a hydrogen plasma to excite the Lyman β transition via the simultaneous absorption of two 205 nm photons. The absorption rate, determined by measurement of subsequent Balmer α emission, is proportional to the number of particles with a given velocity. Calibration is performed in situ by filling the chamber to a known pressure of neutral krypton and exciting a transition close in wavelength to that used in hydrogen. We present details of the calibration procedure, including a technique for identifying saturation broadening, measurements of the neutral density profile in a hydrogen helicon plasma, and discuss the application of the diagnostic to plasmas in the DIII-D tokamak.

A two photon absorption laser induced fluorescence diagnostic for fusion plasmasa)

NASA Astrophysics Data System (ADS)

Magee, R. M.; Galante, M. E.; McCarren, D.; Scime, E. E.; Boivin, R. L.; Brooks, N. H.; Groebner, R. J.; Hill, D. N.; Porter, G. D.

2012-10-01

The quality of plasma produced in a magnetic confinement fusion device is influenced to a large extent by the neutral gas surrounding the plasma. The plasma is fueled by the ionization of neutrals, and charge exchange interactions between edge neutrals and plasma ions are a sink of energy and momentum. Here we describe a diagnostic capable of measuring the spatial distribution of neutral gas in a magnetically confined fusion plasma. A high intensity (5 MW/cm2), narrow bandwidth (0.1 cm-1) laser is injected into a hydrogen plasma to excite the Lyman β transition via the simultaneous absorption of two 205 nm photons. The absorption rate, determined by measurement of subsequent Balmer α emission, is proportional to the number of particles with a given velocity. Calibration is performed in situ by filling the chamber to a known pressure of neutral krypton and exciting a transition close in wavelength to that used in hydrogen. We present details of the calibration procedure, including a technique for identifying saturation broadening, measurements of the neutral density profile in a hydrogen helicon plasma, and discuss the application of the diagnostic to plasmas in the DIII-D tokamak.

Gamma–Gamma Absorption in the γ-ray Binary System PSR B1259-63/LS 2883

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

Sushch, Iurii; Van Soelen, Brian, E-mail: iurii.sushch@desy.de, E-mail: vansoelenb@ufs.ac.za

2017-03-10

The observed TeV light curve from the γ -ray binary PSR B1259-63/LS 2883 shows a decrease in the flux at periastron that has not been fully explained by emission mechanisms alone. This observed decrease can, however, be explained by γγ absorption due to the stellar and disk photons. We calculate the γγ absorption in PSR B1259-63/LS 2883 taking into account photons from both the circumstellar disk and star, assuming that the γ -rays originate at the position of the pulsar. The γγ absorption due to the circumstellar disk photons produces a ≈14% decrease in the flux, and there is amore » total decrease of ≈52% (>1 TeV) within a few days before periastron, accompanied by a hardening of the γ -ray photon index. While the γγ absorption alone is not sufficient to explain the full complexity of the H.E.S.S. γ -ray light curve, it results in a significant decrease in the predicted flux, which is coincident with the observed decrease. In addition, we have calculated an upper limit on the γγ absorption, assuming that the emission is produced at the apex of the bow shock. Future observations with CTA during the 2021 periastron passage may be able to confine the location of the emission based on the degree of γγ absorption, as well as measure the hardening of the spectrum around periastron.« less

Absorption spectrum of a two-level atom in a bad cavity with injected squeezed vacuum

NASA Astrophysics Data System (ADS)

Zhou, Peng; Swain, S.

1996-02-01

We study the absorption spectrum of a coherently driven two-level atom interacting with a resonant cavity mode which is coupled to a broadband squeezed vacuum through its input-output mirror in the bad cavity limit. We study the modification of the two-photon correlation strength of the injected squeezed vacuum inside the cavity, and show that the equations describing probe absorption in the cavity environment are formally identical to these in free space, but with modified parameters describing the squeezed vacuum. The two photon correlations induced by the squeezed vacuum are always weaker than in free space. We pay particular attention to the spectral behaviour at line centre in the region of intermediate trength driving intensities, where anomalous spectral features such as hole-burning and dispersive profiles are displayed. These unusual spectral features are very sensitive to the squeezing phase and the Rabi frequency of the driving field. We also derive the threshold value of the Rabi frequency which gives rise to the transparency of the probe beam at the driving frequency. When the Rabi frequency is less than the threshold value, the probe beam is absorbed, whilst the probe beam is amplified (without population inversion under certain conditions) when the Rabi frequency is larger than this threshold. The anomalous spectral features all take place in the vicinity of the critical point dividing the different dynamical regimes, probe absorption and amplification, of the atomic radiation. The physical origin of the strong amplification without population inversion, and the feasibility of observing it, are discussed.

Phase sensitive amplification in integrated waveguides (Conference Presentation)

NASA Astrophysics Data System (ADS)

Schroeder, Jochen B.; Zhang, Youngbin; Husko, Chad A.; LeFrancois, Simon; Eggleton, Benjamin J.

2017-02-01

Phase sensitive amplification (PSA) is an attractive technology for integrated all-optical signal processing, due to it's potential for noiseless amplification, phase regeneration and generation of squeezed light. In this talk I will review our results on implementing four-wave-mixing based PSA inside integrated photonic devices. In particular I will discuss PSA in chalcogenide ridge waveguides and silicon slow-light photonic crystals. We achieve PSA in both pump- and signal-degenerate schemes with maximum extinction ratios of 11 (silicon) and 18 (chalcogenide) dB. I will further discuss the influence of two-photon absorption and free carrier effects on the performance of silicon-based PSAs.

Method of and apparatus for measuring temperature and pressure. [atmospheric sounding

NASA Technical Reports Server (NTRS)

Korb, C. L.; Kalshoven, J. E., Jr. (Inventor)

1985-01-01

Laser beams are transmitted through gas to a reflecting target, which may be either a solid surface or particulate matter in gas or the gas molecules. The return beams are measured to determine the amount of energy absorbed by the gas. For temperature measurements, the laser beam has a wavelength at which the gas exhibits a relatively temperature sensitive and pressure insensitive absorption characteristic for pressure measurements, the laser beam has a wavelength at which the gas has a relatively pressure sensitive and temperature insensitive absorption characteristic. To reduce the effects of scattering on the absorption measurements a reference laser beam with a weak absorption characteristic is transmitted colinearly with the data beam having a strong absorption characteristic. The two signals are processed as a ratio to eliminate back scattering. Embodiments of transmitters and receivers described include a sequential laser pulse transmitter and receiver, a simultaneous laser pulse transmitter and receiver.

Large nonlinear absorption and refraction coefficients of carbon nanotubes estimated from femtosecond z-scan measurements

NASA Astrophysics Data System (ADS)

Kamaraju, N.; Kumar, Sunil; Sood, A. K.; Guha, Shekhar; Krishnamurthy, Srinivasan; Rao, C. N. R.

2007-12-01

Nonlinear transmission of 80 and 140fs pulsed light with 0.79μm wavelength through single walled carbon nanotubes suspended in water containing sodium dodecyl sulfate is studied. Pulse-width independent saturation absorption and negative cubic nonlinearity are observed, respectively, in open and closed aperture z-scan experiments. The theoretical expressions derived to analyze the z-dependent transmission in the saturable limit require two photon absorption coefficient β0˜1.4cm/MW and a nonlinear index γ ˜-5.5×10-11cm2/W to fit the data.

Short pulse fiber lasers mode-locked by carbon nanotubes and graphene

NASA Astrophysics Data System (ADS)

Yamashita, Shinji; Martinez, Amos; Xu, Bo

2014-12-01

One and two dimensional forms of carbon, carbon nanotubes and graphene, have interesting and useful, not only electronic but also photonic, properties. For fiber lasers, they are very attractive passive mode lockers for ultra-short pulse generation, since they have saturable absorption with inherently fast recovery time (<1 ps). In this paper, we review the photonic properties of graphene and CNT and our recent works on fabrication of fiber devices and applications to ultra-short pulse mode-locked fiber lasers.

New Materials Directions for the Realization of Ultra-High Performance 3rd Order Non-Linear Optical Organics

DTIC Science & Technology

2015-03-13

Nowacki, H.S. Oh, C. Zanlorenzi, H.S. Jee, A. Baev, P.N. Prasad, and L. Akcelrud, "Design and synthesis of polymers for chiral photonics ...rationally design and create organic materials with high nonlinear refractive index and low single· and two- photon absorption at wavelengths relevant to...can also enhance 3rd-order NLO response through microscopic cascading of 2nd-order nonlinearity. Chiral control of nonlinearity bas also been

Nonlinear optical and multi-photon absorption properties in graphene-ZnO nanocomposites

NASA Astrophysics Data System (ADS)

Tong, Qing; Wang, Yu-Hua; Yu, Xiang-Xiang; Wang, Bo; Liang, Zhuang; Tang, Meng; Wu, An-Shun; Zhang, Hai-Jun; Liang, Feng; Xie, Ya-Feng; Wang, Jun

2018-04-01

Graphene-ZnO (GZO) nanocomposites were synthesized by a modified solvothermal method, and characterized by transmission electron microscopy, x-ray diffraction, Raman spectra, and UV-vis absorption spectra. The controllable nonlinear optical (NLO) properties of as-prepared GZO nanocomposites were tested by an open-aperture Z-scan method with 1030 nm fs laser pulses; the tested results showed that there were five-photon absorption (5PA) at 46.8 GW cm-2, 3PA at 28.1 GW cm-2, 2PA at 18.7 GW cm-2, and a vital change from saturable absorption (SA) to reverse SA (RSA) with the increase of incident intensity. This was the first time that 5PA was found in GZO nanocomposites at such a low intensity, 46.8 GW cm-2. The tunable NLO property from SA to RSA and controllable multi-photon absorption provided a facile approach for their applications in optical, optoelectronic devices, and information storage.

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

Enhanced Absorption in 2D Materials Via Fano- Resonant Photonic Crystals

DOE PAGES

Wang, Wenyi; Klotz, Andrey; Yang, Yuanmu; ...

2015-05-01

The use of two-dimensional (2D) materials in optoelectronics has attracted much attention due to their fascinating optical and electrical properties. For instance, graphenebased devices have been employed for applications such as ultrafast and broadband photodetectors and modulators while transition metal dichalcogenide (TMDC) based photodetectors can be used for ultrasensitive photodetection. However, the low optical absorption of 2D materials arising from their atomic thickness limits the maximum attainable external quantum efficiency. For example, in the visible and NIR regimes monolayer MoS 2 and graphene absorb only ~10% and 2.3% of incoming light, respectively. Here, we experimentally demonstrate the use of Fano-resonantmore » photonic crystals to significantly boost absorption in atomically thin materials. Using graphene as a test bed, we demonstrate that absorption in the monolayer thick material can be enhanced to 77% within the telecommunications band, the highest value reported to date. We also show that the absorption in the Fano-resonant structure is non-local, with light propagating up to 16 μm within the structure. This property is particularly beneficial in harvesting light from large areas in field-effect-transistor based graphene photodetectors in which separation of photo-generated carriers only occurs ~0.2 μm adjacent to the graphene/electrode interface.« less

Ground-based Photon Path Measurements from Solar Absorption Spectra of the O2 A-band

NASA Technical Reports Server (NTRS)

Yang, Z.; Wennberg, P. O.; Cageao, R. P.; Pongetti, T. J.; Toon, G. C.; Sander, S. P.

2005-01-01

High-resolution solar absorption spectra obtained from Table Mountain Facility (TMF, 34.38degN, 117.68degW, 2286 m elevation) have been analyzed in the region of the O2 A-band. The photon paths of direct sunlight in clear sky cases are retrieved from the O2 absorption lines and compared with ray-tracing calculations based on the solar zenith angle and surface pressure. At a given zenith angle, the ratios of retrieved to geometrically derived photon paths are highly precise (approx.0.2%), but they vary as the zenith angle changes. This is because current models of the spectral lineshape in this band do not properly account for the significant absorption that exists far from the centers of saturated lines. For example, use of a Voigt function with Lorentzian far wings results in an error in the retrieved photon path of as much as 5%, highly correlated with solar zenith angle. Adopting a super-Lorentz function reduces, but does not completely eliminate this problem. New lab measurements of the lineshape are required to make further progress.

Near- and Extended-Edge X-Ray-Absorption Fine-Structure Spectroscopy Using Ultrafast Coherent High-Order Harmonic Supercontinua

NASA Astrophysics Data System (ADS)

Popmintchev, Dimitar; Galloway, Benjamin R.; Chen, Ming-Chang; Dollar, Franklin; Mancuso, Christopher A.; Hankla, Amelia; Miaja-Avila, Luis; O'Neil, Galen; Shaw, Justin M.; Fan, Guangyu; Ališauskas, Skirmantas; Andriukaitis, Giedrius; Balčiunas, Tadas; Mücke, Oliver D.; Pugzlys, Audrius; Baltuška, Andrius; Kapteyn, Henry C.; Popmintchev, Tenio; Murnane, Margaret M.

2018-03-01

Recent advances in high-order harmonic generation have made it possible to use a tabletop-scale setup to produce spatially and temporally coherent beams of light with bandwidth spanning 12 octaves, from the ultraviolet up to x-ray photon energies >1.6 keV . Here we demonstrate the use of this light for x-ray-absorption spectroscopy at the K - and L -absorption edges of solids at photon energies near 1 keV. We also report x-ray-absorption spectroscopy in the water window spectral region (284-543 eV) using a high flux high-order harmonic generation x-ray supercontinuum with 109 photons/s in 1% bandwidth, 3 orders of magnitude larger than has previously been possible using tabletop sources. Since this x-ray radiation emerges as a single attosecond-to-femtosecond pulse with peak brightness exceeding 1026 photons/s /mrad2/mm2/1 % bandwidth, these novel coherent x-ray sources are ideal for probing the fastest molecular and materials processes on femtosecond-to-attosecond time scales and picometer length scales.

A fully-automated multiscale kernel graph cuts based particle localization scheme for temporal focusing two-photon microscopy

NASA Astrophysics Data System (ADS)

Huang, Xia; Li, Chunqiang; Xiao, Chuan; Sun, Wenqing; Qian, Wei

2017-03-01

The temporal focusing two-photon microscope (TFM) is developed to perform depth resolved wide field fluorescence imaging by capturing frames sequentially. However, due to strong nonignorable noises and diffraction rings surrounding particles, further researches are extremely formidable without a precise particle localization technique. In this paper, we developed a fully-automated scheme to locate particles positions with high noise tolerance. Our scheme includes the following procedures: noise reduction using a hybrid Kalman filter method, particle segmentation based on a multiscale kernel graph cuts global and local segmentation algorithm, and a kinematic estimation based particle tracking method. Both isolated and partial-overlapped particles can be accurately identified with removal of unrelated pixels. Based on our quantitative analysis, 96.22% isolated particles and 84.19% partial-overlapped particles were successfully detected.

Optical nonlinearities of excitons in monolayer MoS2

NASA Astrophysics Data System (ADS)

Soh, Daniel B. S.; Rogers, Christopher; Gray, Dodd J.; Chatterjee, Eric; Mabuchi, Hideo

2018-04-01

We calculate linear and nonlinear optical susceptibilities arising from the excitonic states of monolayer MoS2 for in-plane light polarizations, using second-quantized bound and unbound exciton operators. Optical selection rules are critical for obtaining the susceptibilities. We derive the valley-chirality rule for the second-order harmonic generation in monolayer MoS2 and find that the third-order harmonic process is efficient only for linearly polarized input light while the third-order two-photon process (optical Kerr effect) is efficient for circularly polarized light using a higher order exciton state. The absence of linear absorption due to the band gap and the unusually strong two-photon third-order nonlinearity make the monolayer MoS2 excitonic structure a promising resource for coherent nonlinear photonics.

Method for universal detection of two-photon polarization entanglement

NASA Astrophysics Data System (ADS)

Bartkiewicz, Karol; Horodecki, Paweł; Lemr, Karel; Miranowicz, Adam; Życzkowski, Karol

2015-03-01

Detecting and quantifying quantum entanglement of a given unknown state poses problems that are fundamentally important for quantum information processing. Surprisingly, no direct (i.e., without quantum tomography) universal experimental implementation of a necessary and sufficient test of entanglement has been designed even for a general two-qubit state. Here we propose an experimental method for detecting a collective universal witness, which is a necessary and sufficient test of two-photon polarization entanglement. It allows us to detect entanglement for any two-qubit mixed state and to establish tight upper and lower bounds on its amount. A different element of this method is the sequential character of its main components, which allows us to obtain relatively complicated information about quantum correlations with the help of simple linear-optical elements. As such, this proposal realizes a universal two-qubit entanglement test within the present state of the art of quantum optics. We show the optimality of our setup with respect to the minimal number of measured quantities.

Coherence in the presence of absorption and heating in a molecule interferometer

PubMed Central

Cotter, J. P.; Eibenberger, S.; Mairhofer, L.; Cheng, X.; Asenbaum, P.; Arndt, M.; Walter, K.; Nimmrichter, S.; Hornberger, K.

2015-01-01

Matter-wave interferometry can be used to probe the foundations of physics and to enable precise measurements of particle properties and fundamental constants. It relies on beam splitters that coherently divide the wave function. In atom interferometers, such elements are often realised using lasers by exploiting the dipole interaction or through photon absorption. It is intriguing to extend these ideas to complex molecules where the energy of an absorbed photon can rapidly be redistributed across many internal degrees of freedom. Here, we provide evidence that center-of-mass coherence can be maintained even when the internal energy and entropy of the interfering particle are substantially increased by absorption of photons from a standing light wave. Each photon correlates the molecular center-of-mass wave function with its internal temperature and splits it into a superposition with opposite momenta in addition to the beam-splitting action of the optical dipole potential. PMID:26066053

Optical nonlinear absorption characteristics of Sb2Se3 nanoparticles

NASA Astrophysics Data System (ADS)

Muralikrishna, Molli; Kiran, Aditha Sai; Ravikanth, B.; Sowmendran, P.; Muthukumar, V. Sai; Venkataramaniah, Kamisetti

2014-04-01

In this work, we report for the first time, the nonlinear optical absorption properties of antimony selenide (Sb2Se3) nanoparticles synthesized through solvothermal route. X-ray diffraction results revealed the crystalline nature of the nanoparticles. Electron microscopy studies revealed that the nanoparticles are in the range of 10 - 40 nm. Elemental analysis was performed using EDAX. By employing open aperture z-scan technique, we have evaluated the effective two-photon absorption coefficient of Sb2Se3 nanoparticles to be 5e-10 m/W at 532 nm. These nanoparticles exhibit strong intensity dependent nonlinear optical absorption and hence could be considered to have optical power limiting applications in the visible range.

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.

Microscopic theory of multiple-phonon-mediated dephasing and relaxation of quantum dots near a photonic band gap

NASA Astrophysics Data System (ADS)

Roy, Chiranjeeb; John, Sajeev

2010-02-01

We derive a quantum theory of the role of acoustic and optical phonons in modifying the optical absorption line shape, polarization dynamics, and population dynamics of a two-level atom (quantum dot) in the “colored” electromagnetic vacuum of a photonic band-gap (PBG) material. This is based on a microscopic Hamiltonian describing both radiative and vibrational processes quantum mechanically. We elucidate the extent to which phonon-assisted decay limits the lifetime of a single photon-atom bound state and derive the modified spontaneous emission dynamics due to coupling to various phonon baths. We demonstrate that coherent interaction with undamped phonons can lead to an enhanced lifetime of a photon-atom bound state in a PBG. This results in reduction of the steady-state atomic polarization but an increase in the fractionalized upper state population in the photon-atom bound state. We demonstrate, on the other hand, that the lifetime of the photon-atom bound state in a PBG is limited by the lifetime of phonons due to lattice anharmonicities (breakup of phonons into lower energy phonons) and purely nonradiative decay. We also derive the modified polarization decay and dephasing rates in the presence of such damping. This leads to a microscopic, quantum theory of the optical absorption line shapes. Our model and formalism provide a starting point for describing dephasing and relaxation in the presence of external coherent fields and multiple quantum dot interactions in electromagnetic reservoirs with radiative memory effects.

The origin of absorptive features in the two-dimensional electronic spectra of rhodopsin.

PubMed

Farag, Marwa H; Jansen, Thomas L C; Knoester, Jasper

2018-05-09

In rhodopsin, the absorption of a photon causes the isomerization of the 11-cis isomer of the retinal chromophore to its all-trans isomer. This isomerization is known to occur through a conical intersection (CI) and the internal conversion through the CI is known to be vibrationally coherent. Recently measured two-dimensional electronic spectra (2DES) showed dramatic absorptive spectral features at early waiting times associated with the transition through the CI. The common two-state two-mode model Hamiltonian was unable to elucidate the origin of these features. To rationalize the source of these features, we employ a three-state three-mode model Hamiltonian where the hydrogen out-of plane (HOOP) mode and a higher-lying electronic state are included. The 2DES of the retinal chromophore in rhodopsin are calculated and compared with the experiment. Our analysis shows that the source of the observed features in the measured 2DES is the excited state absorption to a higher-lying electronic state and not the HOOP mode.

A 64-pixel NbTiN superconducting nanowire single-photon detector array for spatially resolved photon detection.

PubMed

Miki, Shigehito; Yamashita, Taro; Wang, Zhen; Terai, Hirotaka

2014-04-07

We present the characterization of two-dimensionally arranged 64-pixel NbTiN superconducting nanowire single-photon detector (SSPD) array for spatially resolved photon detection. NbTiN films deposited on thermally oxidized Si substrates enabled the high-yield production of high-quality SSPD pixels, and all 64 SSPD pixels showed uniform superconducting characteristics within the small range of 7.19-7.23 K of superconducting transition temperature and 15.8-17.8 μA of superconducting switching current. Furthermore, all of the pixels showed single-photon sensitivity, and 60 of the 64 pixels showed a pulse generation probability higher than 90% after photon absorption. As a result of light irradiation from the single-mode optical fiber at different distances between the fiber tip and the active area, the variations of system detection efficiency (SDE) in each pixel showed reasonable Gaussian distribution to represent the spatial distributions of photon flux intensity.

Single-photon imager based on a superconducting nanowire delay line

NASA Astrophysics Data System (ADS)

Zhao, Qing-Yuan; Zhu, Di; Calandri, Niccolò; Dane, Andrew E.; McCaughan, Adam N.; Bellei, Francesco; Wang, Hao-Zhu; Santavicca, Daniel F.; Berggren, Karl K.

2017-03-01

Detecting spatial and temporal information of individual photons is critical to applications in spectroscopy, communication, biological imaging, astronomical observation and quantum-information processing. Here we demonstrate a scalable single-photon imager using a single continuous superconducting nanowire that is not only a single-photon detector but also functions as an efficient microwave delay line. In this context, photon-detection pulses are guided in the nanowire and enable the readout of the position and time of photon-absorption events from the arrival times of the detection pulses at the nanowire's two ends. Experimentally, we slowed down the velocity of pulse propagation to ∼2% of the speed of light in free space. In a 19.7 mm long nanowire that meandered across an area of 286 × 193 μm2, we were able to resolve ∼590 effective pixels with a temporal resolution of 50 ps (full width at half maximum). The nanowire imager presents a scalable approach for high-resolution photon imaging in space and time.

Thermo-optical interactions in a dye-microcavity photon Bose-Einstein condensate

NASA Astrophysics Data System (ADS)

Alaeian, Hadiseh; Schedensack, Mira; Bartels, Clara; Peterseim, Daniel; Weitz, Martin

2017-11-01

Superfluidity and Bose-Einstein condensation are usually considered as two closely related phenomena. Indeed, in most macroscopic quantum systems, like liquid helium, ultracold atomic Bose gases, and exciton-polaritons, condensation and superfluidity occur in parallel. In photon Bose-Einstein condensates realized in the dye microcavity system, thermalization does not occur by direct interaction of the condensate particles as in the above described systems, i.e. photon-photon interactions, but by absorption and re-emission processes on the dye molecules, which act as a heat reservoir. Currently, there is no experimental evidence for superfluidity in the dye microcavity system, though effective photon interactions have been observed from thermo-optic effects in the dye medium. In this work, we theoretically investigate the implications of effective thermo-optic photon interactions, a temporally delayed and spatially non-local effect, on the photon condensate, and derive the resulting Bogoliubov excitation spectrum. The calculations suggest a linear photon dispersion at low momenta, fulfilling the Landau’s criterion of superfluidity. We envision that the temporally delayed and long-range nature of the thermo-optic photon interaction offer perspectives for novel quantum fluid phenomena.

Achieving an Accurate Surface Profile of a Photonic Crystal for Near-Unity Solar Absorption in a Super Thin-Film Architecture.

PubMed

Kuang, Ping; Eyderman, Sergey; Hsieh, Mei-Li; Post, Anthony; John, Sajeev; Lin, Shawn-Yu

2016-06-28

In this work, a teepee-like photonic crystal (PC) structure on crystalline silicon (c-Si) is experimentally demonstrated, which fulfills two critical criteria in solar energy harvesting by (i) its Gaussian-type gradient-index profile for excellent antireflection and (ii) near-orthogonal energy flow and vortex-like field concentration via the parallel-to-interface refraction effect inside the structure for enhanced light trapping. For the PC structure on 500-μm-thick c-Si, the average reflection is only ∼0.7% for λ = 400-1000 nm. For the same structure on a much thinner c-Si ( t = 10 μm), the absorption is near unity (A ∼ 99%) for visible wavelengths, while the absorption in the weakly absorbing range (λ ∼ 1000 nm) is significantly increased to 79%, comparing to only 6% absorption for a 10-μm-thick planar c-Si. In addition, the average absorption (∼94.7%) of the PC structure on 10 μm c-Si for λ = 400-1000 nm is only ∼3.8% less than the average absorption (∼98.5%) of the PC structure on 500 μm c-Si, while the equivalent silicon solid content is reduced by 50 times. Furthermore, the angular dependence measurements show that the high absorption is sustained over a wide angle range (θinc = 0-60°) for teepee-like PC structure on both 500 and 10-μm-thick c-Si.

Careful measurement of first hyperpolarizability spectrum by hyper-Rayleigh scattering (HRS)

NASA Astrophysics Data System (ADS)

Zhu, Jing; Lu, Changgui; Cui, Yiping

2008-01-01

The first hyperpolarizability (β) spectrum of an azobenzene derivative around its two-photon resonance region is detected carefully by hyper-Rayleigh scattering. The present work uses a fluorescence spectrometer (Edinburgh instruments, F900) as the detector instead of interference filter and photoelectric multiplier tube (PMT). For each wavelength, HRS emission spectrum accompanied with two-photon fluorescence (TPF) is carefully detected by changing the detection wavelength around half of the incident wavelength. Full width to half maximum (FWHM) of the spectrum is about 0.4nm, which is similar to that of the laser. When the incident wavelength moves into the two-photon resonance region, TPF signal increases quickly and should be eliminated. In order to receive accurate β spectrum, the data detected by the oscillograph should be made some emendations, such as TPF, incident energy, absorption and pulse width. Compared with the β spectrum detected in previous works, the spectrum received in this work presents a clearer profile. The β spectrum exhibits a similar profile as its UV-visible spectrum just with blue-shift of wavelength. It could be explained that the electronic vibration structure in two-photon progress is different from that in one-photon progress, while the broadening mechanism may be similar, considering the resonant two-state model (RTSM).

Organic Dots Based on AIEgens for Two-Photon Fluorescence Bioimaging.

PubMed

Lou, Xiaoding; Zhao, Zujin; Tang, Ben Zhong

2016-12-01

Two-photon fluorescence imaging technique is a powerful bioanalytical approach in terms of high photostability, low photodamage, high spatiotemporal resolution. Recently, fluorescent organic dots comprised of organic emissive cores and a polymeric matrix are emerging as promising contrast reagents for two-photon fluorescence imaging, owing to their numerous merits of high and tunable fluorescence, good biocompatibility, strong photobleaching resistance, and multiple surface functionality. The emissive core is crucial for organic dots to get high brightness but many conventional chromophores often encounter a severe problem of fluorescence quenching when they form aggregates. To solve this problem, fluorogens featuring aggregation-induced emission (AIE) can fluoresce strongly in aggregates, and thus become ideal candidates for fluorescent organic dots. In addition, two-photon absorption property of the dots can be readily improved by just increase loading contents of AIE fluorogen (AIEgen). Hence, organic dots based on AIEgens have exhibited excellent performances in two-photon fluorescence in vitro cellular imaging, and in vivo vascular architecture visualization of mouse skin, muscle, brain and skull bone. In view of the rapid advances in this important research field, here, we highlight representative fluorescent organic dots with an emissive core of AIEgen aggregate, and discuss their great potential in bioimaging applications. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Slow light enhanced gas sensing in photonic crystals

NASA Astrophysics Data System (ADS)

Kraeh, Christian; Martinez-Hurtado, J. L.; Popescu, Alexandru; Hedler, Harry; Finley, Jonathan J.

2018-02-01

Infrared spectroscopy allows for highly selective and highly sensitive detection of gas species and concentrations. Conventional gas spectrometers are generally large and unsuitable for on-chip applications. Long absorption path lengths are usually required and impose a challenge for miniaturization. In this work, a gas spectrometer is developed consisting of a microtube photonic crystal structure. This structure of millimetric form factors minimizes the required absorption path length due to slow light effects. The microtube photonic crystal allows for strong transmission in the mid-infrared and, due to its large void space fraction, a strong interaction between light and gas molecules. As a result, enhanced absorption of light increases the gas sensitivity of the device. Slow light enhanced gas absorption by a factor of 5.8 in is experimentally demonstrated at 5400 nm. We anticipate small form factor gas sensors on silicon to be a starting point for on-chip gas sensing architectures.

Low loss liquid crystal photonic bandgap fiber in the near-infrared region

NASA Astrophysics Data System (ADS)

Scolari, Lara; Wei, Lei; Gauza, Sebastian; Wu, Shin-Tson; Bjarklev, Anders

2011-01-01

We infiltrate a perdeuterated liquid crystal with a reduced infrared absorption in a photonic crystal fiber. The H atoms of this liquid crystal were substituted with D atoms in order to move the vibration bands which cause absorption loss to longer wavelengths and therefore reduce the absorption in the spectral range of 1-2 μm. We achieve in the middle of the near-infrared transmission bandgap the lowest loss (about 1 dB) ever reported for this kind of devices.

A small molecular pH-dependent fluorescent probe for cancer cell imaging in living cell.

PubMed

Ma, Junbao; Li, Wenqi; Li, Juanjuan; Shi, Rongguang; Yin, Gui; Wang, Ruiyong

2018-05-15

A novel pH-dependent two-photon fluorescent molecular probe ABMP has been prepared based on the fluorophore of 2, 4, 6-trisubstituted pyridine. The probe has an absorption wavelength at 354 nm and corresponding emission wavelength at 475 nm with the working pH range from 2.20 to 7.00, especially owning a good liner response from pH = 2.40 to pH = 4.00. ABMP also has excellent reversibility, photostability and selectivity which promotes its ability in analytical application. The probe can be excited with a two-photon fluorescence microscopy and the fluorescence cell imaging indicated that the probe can distinguish Hela cancer cells out of normal cells with a two-photon fluorescence microscopy which suggested its potential application in tumor cell detection. Copyright © 2018 Elsevier B.V. All rights reserved.

Theoretical study of chromophores for biological sensing: Understanding the mechanism of rhodol based multi-chromophoric systems

NASA Astrophysics Data System (ADS)

Rivera-Jacquez, Hector J.; Masunov, Artëm E.

2018-06-01

Development of two-photon fluorescent probes can aid in visualizing the cellular environment. Multi-chromophore systems display complex manifolds of electronic transitions, enabling their use for optical sensing applications. Time-Dependent Density Functional Theory (TDDFT) methods allow for accurate predictions of the optical properties. These properties are related to the electronic transitions in the molecules, which include two-photon absorption cross-sections. Here we use TDDFT to understand the mechanism of aza-crown based fluorescent probes for metals sensing applications. Our findings suggest changes in local excitation in the rhodol chromophore between unbound form and when bound to the metal analyte. These changes are caused by a charge transfer from the aza-crown group and pyrazol units toward the rhodol unit. Understanding this mechanism leads to an optimized design with higher two-photon excited fluorescence to be used in medical applications.

An Assembled Nanocomplex for Improving both Therapeutic Efficiency and Treatment Depth in Photodynamic Therapy.

PubMed

Cao, Hongqian; Wang, Lei; Yang, Yang; Li, Juan; Qi, Yanfei; Li, Yue; Li, Ying; Wang, Hao; Li, Junbai

2018-06-25

Photodynamic therapy (PDT) shows unique selectivity and irreversible destruction toward treated tissues or cells, but still has several problems in clinical practice. One is limited therapeutic efficiency, which is attributed to hypoxia in tumor sites. Another is the limited treatment depth because traditional photosensitizes are excited by short wavelength light (<700 nm). An assembled nano-complex system composed of oxygen donor, two-photon absorption (TPA) species, and photosensitizer (PS) was synthesized to address both problems. The photosensitizer is excited indirectly by two-photon laser through intraparticle FRET mechanism for improving treatment depth. The oxygen donor, hemoglobin, can supply extra oxygen into tumor location through targeting effect for enhanced PDT efficiency. The mechanism and PDT effect were verified through both in vitro and in vivo experiments. The simple system is promising to promote two-photon PDT for clinical applications. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Theoretical study of chromophores for biological sensing: Understanding the mechanism of rhodol based multi-chromophoric systems.

PubMed

Rivera-Jacquez, Hector J; Masunov, Artëm E

2018-06-05

Development of two-photon fluorescent probes can aid in visualizing the cellular environment. Multi-chromophore systems display complex manifolds of electronic transitions, enabling their use for optical sensing applications. Time-Dependent Density Functional Theory (TDDFT) methods allow for accurate predictions of the optical properties. These properties are related to the electronic transitions in the molecules, which include two-photon absorption cross-sections. Here we use TDDFT to understand the mechanism of aza-crown based fluorescent probes for metals sensing applications. Our findings suggest changes in local excitation in the rhodol chromophore between unbound form and when bound to the metal analyte. These changes are caused by a charge transfer from the aza-crown group and pyrazol units toward the rhodol unit. Understanding this mechanism leads to an optimized design with higher two-photon excited fluorescence to be used in medical applications. Copyright © 2018 Elsevier B.V. All rights reserved.

Simulation of all-optical logic NOR gate based on two-photon absorption with semiconductor optical amplifier-assisted Mach-Zehnder interferometer with the effect of amplified spontaneous emission

NASA Astrophysics Data System (ADS)

Kotb, Amer

2015-05-01

The performance of an all-optical NOR gate is numerically simulated and investigated. The NOR Boolean function is realized by using a semiconductor optical amplifier (SOA) incorporated in Mach-Zehnder interferometer (MZI) arms and exploiting the nonlinear effect of two-photon absorption (TPA). If the input pulse intensities is adjusting to be high enough, the TPA-induced phase change can be larger than the regular gain-induced phase change and hence support ultrafast operation in the dual rail switching mode. The numerical study is carried out by taking into account the effect of the amplified spontaneous emission (ASE). The dependence of the output quality factor ( Q-factor) on critical data signals and SOAs parameters is examined and assessed. The obtained results confirm that the NOR gate implemented with the proposed scheme is capable of operating at a data rate of 250 Gb/s with logical correctness and high output Q-factor.

Engineering light emission of two-dimensional materials in both the weak and strong coupling regimes

NASA Astrophysics Data System (ADS)

Brotons-Gisbert, Mauro; Martínez-Pastor, Juan P.; Ballesteros, Guillem C.; Gerardot, Brian D.; Sánchez-Royo, Juan F.

2018-01-01

Two-dimensional (2D) materials have promising applications in optoelectronics, photonics, and quantum technologies. However, their intrinsically low light absorption limits their performance, and potential devices must be accurately engineered for optimal operation. Here, we apply a transfer matrix-based source-term method to optimize light absorption and emission in 2D materials and related devices in weak and strong coupling regimes. The implemented analytical model accurately accounts for experimental results reported for representative 2D materials such as graphene and MoS2. The model has been extended to propose structures to optimize light emission by exciton recombination in MoS2 single layers, light extraction from arbitrarily oriented dipole monolayers, and single-photon emission in 2D materials. Also, it has been successfully applied to retrieve exciton-cavity interaction parameters from MoS2 microcavity experiments. The present model appears as a powerful and versatile tool for the design of new optoelectronic devices based on 2D semiconductors such as quantum light sources and polariton lasers.

Two-photon absorption and efficient encapsulation of near-infrared-emitting CdSexTe1-x quantum dots

NASA Astrophysics Data System (ADS)

Szeremeta, Janusz; Lamch, Lukasz; Wawrzynczyk, Dominika; Wilk, Kazimiera A.; Samoc, Marek; Nyk, Marcin

2015-07-01

Hydrophobic CdSexTe1-x quantum dots with near infrared emission in the 700-750 nm range were synthesized by a wet chemistry technique. Their nonlinear optical properties were studied using Z-scan technique with a tunable femtosecond laser system. The peak value of the two-photon absorption cross section was found to be ∼2400 GM at 1400 nm. To demonstrate a possible way of utilizing the CdSexTe1-x quantum dots in aqueous environment we describe here a convenient method of preparation of Brij 58® micellar systems loaded with the quantum dots. The obtained nanoconstructs were characterized using optical spectroscopy, TEM and DLS. The micelles colloidal stability, and the influence of the encapsulation process on the spectroscopic properties of the quantum dots are discussed. In particular, we have observed a 60 nm blue-shift of the emission maxima upon loading quantum dots inside the micelles.

Why Do Silver Trimers Intercalated in DNA Exhibit Unique Nonlinear Properties That Are Promising for Applications?

PubMed

Bonačić-Koutecký, Vlasta; Perić, Martina; Sanader, Željka

2018-05-17

Our investigation of one-photon absorption (OPA) and nonlinear optical (NLO) properties such as two-photon absorption (TPA) of silver trimer intercalated in DNA based on TDDFT approach allowed us to propose a mechanism responsible for large TPA cross sections of such NLO-phores. We present a concept that illustrates the key role of quantum cluster as well as of nucleotide bases from the immediate neighborhood. For this purpose, different surroundings consisting of guanine-cytosine and adenine-thymine such as (GCGC) and (ATAT) have been investigated that are exhibiting substantially different values of TPA cross sections. This has been confirmed by extending the immediate surroundings as well as using the two-layer quantum mechanics/molecular mechanics (QM/MM) approach. We focus on the cationic closed-shell system and illustrate that the neutral open-shell system shifts OPA spectra into the NIR regime, which is suitable for applications. Thus, in this contribution, we propose novel NLO-phores inducing large TPA cross sections, opening the route for multiphoton imaging.